Recent lbnl_es_mf items

Out-of-time-order correlators bridge classical transport and quantum dynamics.

Thu, 14 May 2026 00:00:00 +0000

The out-of-time-order correlator (OTOC) has emerged as a central tool for quantifying decoherence across wide-ranging physical platforms. Here, we demonstrate its direct measurement in a classical ensemble using nuclear magnetic resonance with a modulated gradient spin echo sequence and extend the method into a multidimensional correlation to track exchange phenomena. Position is encoded through magnetic field gradients and momentum through the velocity autocorrelation function, enabling experimental access to OTOCs for proton motion confined within the self-similar lattice of the metal-organic framework MOF-808. Here, water confined to specified geometries within the MOF pores gives rise to spatially distinct diffusive eigenmodes with characteristic relative entropies. We demonstrate that periodic radio frequency driving combined with gradient modulation yields entropy evolution through the selection of distinct diffusion modes. Frequency-resolved diffusion spectra connect these...

Bypassing the yellow phase for extremely stable formamidinium lead iodide perovskite solar cells.

Thu, 7 May 2026 00:00:00 +0000

Using modeling and structural studies, we show that chloride incorporation in formamidinium lead iodide (FAPI) perovskites alters the energetics of both the formation and degradation pathways. We fabricated films with two coadditives [15 mole % FA chloride (FACl) and 0.5 mole % BA₂PbI₄, where BA is butylammonium)], in which FACl ensures chloride incorporation and both additives collectively create a compressive lattice strain that stabilizes the FAPI black phase and bypasses the formation of a yellow phase during degradation. The coadditive strategy revealed a favorable transition from face-sharing 2H, 4H, 6H, and 8H phases to the corner-sharing 3C black phase. Photovoltaic devices with a p-i-n architecture had an average power conversion efficiency (40 devices) of 24.1% and lost only 2% of their efficiency after 1200 hours at 85° ± 5°C, 1-sun illumination, and open-circuit conditions. Upon stressing at 15-sun illumination at 90°C for >400 hours, the stabilized...

Absorption dissymmetry factor enhancement: A data-driven approach to unravel the synthesis knobs of chiral 2D perovskites

Thu, 7 May 2026 00:00:00 +0000

Chiral 2D metal halide perovskites (MHPs) are promising for spin-optoelectronic applications, yet their absorption dissymmetry factor (g abs ) exhibits significant variability due to complex, co-dependent structural and experimental factors. We established a data-driven framework using Pearson’s correlation, ANOVA, and Gaussian process regression to identify and model key synthesis “knobs” governing these properties. The analysis revealed that solvent choice is the primary factor driving variability. For acetonitrile-based films, g abs was maximized by optimizing annealing temperature and film thickness. Conversely, films from higher boiling point solvents showed complex dependencies on annealing temperature, excitonic integral intensity, and film texture. These statistical correlations provide a roadmap for the rational design of high-performance chiral MHPs and establish a foundation for future machine learning-driven material exploration.

Wireless Bioelectronic Modulation of Membrane Potential in Glioblastoma Using Carbon Nanotube Porins

Tue, 5 May 2026 00:00:00 +0000

Disruption of membrane potential (V_mem) can activate pathways associated with cancer proliferation. Manipulating ion channels may therefore present an effective strategy for treating cancers that fail to respond to conventional therapies. One approach to target these channels is to manipulate the membrane charge, which involves the use of wireless bipolar electrodes such as carbon nanotube porins (CNTPs) inserted into cell membranes to modulate membrane charge and ionic flux. By utilizing membrane dyes, we observed alterations in V_mem induced by CNTPs and externally applied voltages. Analyses of cellular behaviors and processes indicated that V_mem is more receptive to stimuli in invasive cancers, while it leads to increased metabolism in less invasive cancers, with notable changes in the cell cycle occurring at approximately 48 h post-treatment in Glioblastoma (GB) cell lines. This work shows that CNTPs, in combination and with externally...

Patterned, Low-Temperature Growth of Transition Metal Dichalcogenides for Low Resistance Raised Contacts

Tue, 5 May 2026 00:00:00 +0000

Transition metal dichalcogenide (TMD) monolayers are promising channel materials for next-generation electronic devices. A challenge is the high contact resistance between monolayer TMDs and metal contacts, especially for holes. In this regard, raised source/drain contacts are promising. However, the direct, patterned growth of raised contacts at CMOS-compatible temperatures remains largely unresolved. We present plasma-free selenization and sulfurization of metal oxides at substrate temperatures down to 400 °C, compatible with back-end-of-line thermal budgets. To achieve growth at such temperatures, gas-phase chalcogen precursors are first thermally activated at 950 °C. Films grown on single-crystal monolayer TMDs exhibit high crystal quality, as confirmed by transmission electron microscopy. Raised contacts on WSe2 monolayers fabricated using this approach yield a low hole contact resistance of 0.3 kΩ·μm after chemical doping. This process is shown to be applicable to growing...

Navigating the research landscape for hyper-NA EUV lithography and future patterning technologies

Wed, 29 Apr 2026 00:00:00 +0000

Hyper-Numerical Aperture (Hyper-NA) Extreme Ultraviolet (EUV) lithography is gathering growing support as the technology of choice to sustain the dimensional scaling trajectory of Moore's Law. This transition, which targets resolution down to 5 nm, necessitates several research advances across several key lithography areas, such as patterning materials, imaging with polarization control, and the optimization of the mask structure. In this paper, we briefly review the historical role of the government-industrial partnerships enabling Center for X-Ray Optics (CXRO) pathfinding research for prior EUV lithography generations. We also highlight the role of the Department of Energy's Energy Frontier Research Center (EFRC) on High-Precision Patterning Science (CHiPPS) as a critical initiative to fundamentally address the pervasive stochastic challenges in materials science that limit the RLS (Resolution, Sensitivity, Line Edge Roughness) tradeoff, charting a path toward the Angstrom...

Highly Anisotropic Quasi‐Direct Organic Metal Halide Hybrids: A Platform for Polarization‐Sensitive Optoelectronics

Tue, 28 Apr 2026 00:00:00 +0000

ABSTRACT Low‐dimensional organic–inorganic metal halide hybrids (OMHHs) exhibit remarkable optical properties and enhanced environmental stability. We investigate a 1D OMHH with formula C 4 N 2 H 14 PbBr 4 , consisting of Pb–Br chains separated by organic cations, which shows a large Stokes shift (0.83 eV) and broadband emission. Through first‐principles calculations and polarized Raman spectroscopy, we characterize the material's vibrational properties and identify the specific phonon modes that drive exciton self‐trapping. Our novel GW/Bethe‐Salpeter equation force formalism reveals that low‐frequency phonons (100100 cm − 1 , primarily involving Pb–Br motions) couple strongly with excitons, with a remarkably high Huang‐Rhys factor of 137 ± 4, and gives a pathway for ultrafast structural analysis during the absorption process. This phonon‐exciton coupling mechanism explains the material's broadband emission and provides a pathway for controlling optical properties through...

Characterization of Oxidative Modifications to Short Peptides Using Low Dose Rate X-Rays

Thu, 23 Apr 2026 00:00:00 +0000

The method of X-ray footprinting and mass spectrometry (XFMS) using high flux synchrotron X-ray sources has become an established method in structural biology and is based on the radiolytic production of hydroxyl radicals, which oxidatively modify protein sidechains. While other methods of producing hydroxyl radicals are available, one benefit of using high flux density sources is that hydroxyl radical scavenging reactions can be minimized, and exposure times kept short to minimize secondary reactions. Here we present an application of the XFMS method using low dose rate X-rays from a commercial instrument. We demonstrate the feasibility of the approach using short peptides, characterizing the oxidative modifications +14, +16, and +32 Da under both aerobic and low oxygen conditions, and we additionally quantify the hydrogen peroxide production for various doses using the low dose rate source. These results provide fundamental information on the oxidative damage to peptides due...

Localized Heterogeneous Nucleation for Vapor‐Assisted Sequential Deposition of Metal Halide Perovskites

Thu, 23 Apr 2026 00:00:00 +0000

ABSTRACT Vapor‐assisted hybrid two‐step deposition, which combines thermally evaporated inorganic layers with solution‐processed organic halides to form halide perovskites, has emerged as a scalable and industry‐compatible route for textured tandem photovoltaics. However, this process is often hindered by reaction‐limited phase formation, particularly when compact, non‐porous, and highly crystalline inorganic layers formed by thermal evaporation restrict subsequent conversion, resulting in incomplete reaction and pronounced depth‐dependent heterogeneity. In this study, we introduce a strategy to regulate the inorganic precursor layer by incorporating localized heterogeneous nucleation sites. Sparsely distributed hydrophilic metal oxide species serve as effective nucleation centers during vapor deposition, enabling effective control over film morphology and crystal orientation from the early stages of growth. This tailored inorganic framework facilitates the subsequent incorporation...

Structural and Mechanical Analysis of Individual Mineralized Collagen Fibrils Using In Situ Transmission Electron Microscopy

Thu, 23 Apr 2026 00:00:00 +0000

Bone serves as an example of nature's architectured material with its characteristic blend of strength and toughness, all at a lightweight design. Given the hierarchical nature of these materials, it is essential to understand the governing mechanisms and organization of their constituents across length scales for bioinspired structural design. Despite recent advances in transmission electron microscopy (TEM) that have allowed us to witness the hierarchical arrangement of bone at micro-down to the nanoscale, we are still missing the details about the structural organization and mechanical properties of the main building blocks of bone─mineralized collagen fibrils (MCFs). Here, we present a method to extract individual MCFs from nature's model material, mineralized turkey leg tendon, using a dropcasting procedure. By isolating the MCFs onto TEM supporting grids, we visualized the arrangement of organic and mineral phases within individual MCFs at the nanoscale. Using a four-dimensional...

Dynamics of ballistic photocurrents driven by Coulomb scattering in a two-dimensional material

Thu, 23 Apr 2026 00:00:00 +0000

First-principles real-time time-dependent density-functional theory (rt-TDDFT) calculations reveal the existence of ballistic photocurrents generated by Coulomb scattering, which has not previously been considered as a mechanism for the bulk photovoltaic effect. With monolayer GeS as an example, it is predicted that ballistic currents can be comparable to shift currents under experimentally accessible conditions.

Investigation of residue-specific radiation damage of peptides under different radiation doses, dose rates, and oxygen availability

Tue, 21 Apr 2026 00:00:00 +0000

Investigation of residue-specific radiation damage of peptides under different radiation doses, dose rates, and oxygen availability

A large interlaboratory electron diffraction study of monolayer graphene

Mon, 20 Apr 2026 00:00:00 +0000

Standardisation of data collection and analysis is essential to enable commercialisation of 2D materials in a wide range of technologies. Selected area electron diffraction (SAED) in the transmission electron microscope (TEM) is one of the key methods for distinguishing monolayer from bilayer and few-layer graphene by comparing the 1st and 2nd order diffraction spot intensities. Yet there are many factors that can affect the reliability of data collection and interpretation, causing the measurement of monolayer samples to deviate from the literature boundary condition of I{2¯110}/I{11¯00}< 1 for monolayer graphene (1LG). Here we present the results of a large interlaboratory SAED comparison study, where 15 international laboratories measured and analysed nominally identical samples of chemical vapour deposited graphene. Large variations were observed in the measured ratios of diffraction spot intensities, with the largest variance associated with poor quality SAED data resulting...

Global metagenomics reveals plastid diversity and unexplored algal lineages

Fri, 17 Apr 2026 00:00:00 +0000

Photosynthetic organelles in eukaryotes originated through primary endosymbiosis with a cyanobacterium, an event that profoundly shaped the evolutionary landscape of the eukaryotic tree of life. Primary plastids in Archaeplastida, especially in cultivable plants and algae, contribute most to known plastid diversity. Secondary and higher-order endosymbiosis, involving eukaryotic hosts and algal endosymbionts, further spread photosynthesis among protists within the CASH lineages (Cryptophyta, Alveolata, Stramenopila, and Haptophyta). Despite various hypotheses explaining secondary plastid evolution and distribution, empirical support remains limited. Here, we employ cultivation-independent global metagenomics to expand plastid diversity and investigate plastid origins. We capture 1,027 plastid sequences, including 300 novel sequences belonging to previously unsequenced plastids and representing yet-to-be described microeukaryotes. This includes a new lineage that offers insights...

High-throughput methods leveraging robotics and computer vision for the development of therapeutic phage cocktails

Fri, 17 Apr 2026 00:00:00 +0000

We present the high-throughput automated screening techniques that are being used to develop bacteriophage-based therapeutic products currently under investigation in human clinical trials to combat urinary tract infections1. By integrating modern liquid handling robotics, standardized phenotypic assays, and computer vision-based enumeration, we established a platform capable of reproducibly screening large collections of phages against clinically derived bacterial strain panels. This approach enabled systematic assessment of phage-bacteria interactions at scale, facilitating the identification and optimization of phage cocktails with broad in vitro activity. Although bacteriophage therapy has long been investigated as a strategy for treating bacterial infections, few frameworks exist for developing phage combinations in a reproducible and scalable manner. The methods outlined here address this gap and aim to support the broader development of therapeutic assets available to combat...

Strain mapping of three-dimensionally structured two-dimensional materials

Wed, 15 Apr 2026 00:00:00 +0000

Strain plays a crucial role in tuning materials' properties, influencing their optical, electrical, and chemical performances. In two-dimensional (2D) materials, applied stress often induces out-of-plane deformation, resulting in a more intricate three-dimensional (3D) topography, where mapping the strain remains a challenge due to the limitations of conventional characterization techniques. In this work, we introduce BRIGHT (Bragg-Rod Informed, Gradient-based Height-mapping Technique), an integrated method for reconstructing both the topography and planar strain profile of 3D-structured 2D materials using nanobeam four-dimensional scanning transmission electron microscopy (4D-STEM). We apply BRIGHT to a MoS₂-MoSe₂ transition metal dichalcogenide (TMD) lateral heterojunctions exhibiting built-in strain and out-of-plane ripples and show that varying heterojunction widths lead to distinct surface morphologies and corresponding changes in the planar strain distribution....

Precision Labeling of Native Antibodies with Lock Coupling

Wed, 15 Apr 2026 00:00:00 +0000

The formation of stable protein complexes enables much of biotechnology, but even high-affinity complexes can dissociate, limiting potential applications in biomaterials, bioimaging, nanomedicine, and other protein-based technologies. Here, we describe lock coupling, a simple and selective one-step reaction between interfacial lysine and glutamate or aspartate side chains to form stable isopeptide bonds and be used for the precise labeling of native antibodies. We identify conditions in which short-lived activated esters formed by the aqueous carbodiimide EDC promote isopeptide bond formation specifically at preassociated amine-acid pairs. Indiscriminate cross-linking is minimized by formation of protein complexes before addition of catalyst, use of acidic pH to suppress exposed Lys reactivity, and limiting the aqueous stability of activated esters. For native antibody (Ab) labeling, we show that the small IgG-binding protein GB1 can be covalently attached to the Ab Fc domain...

New Directions in Focused Ion Beam Induced Deposition for the Nanoprinting of Functional 3D Heterostructures

Wed, 15 Apr 2026 00:00:00 +0000

ABSTRACT The focused ion beam (FIB) microscope is well established as a high‐resolution machining instrument capable of site‐selectively removing material down to the nanoscale. Beyond subtractive processing, however, the FIB can also add material via a technique known as focused ion beam induced deposition (FIBID). Using FIBID, the FIB can thus be employed for the direct‐write of complex nanostructures. This work explores new directions in three‐dimensional FIBID nanoprinting, harnessing unique features of helium and neon FIBs. In particular, the superior spatial resolution of these novel FIBs is leveraged to fabricate precise multimaterial architectures, an isotope effect is used to create satellite deposits, and dose‐controlled implantation of the gaseous ions is used to engineer internal voids. In the context of voids, the fabrication of hollow nanopillars by helium‐FIBID due to concurrent milling (as shown previously by others) is revisited. Insight into the chemical and...

Deriving effective electrode–ion interactions from free-energy profiles at electrochemical interfaces

Wed, 15 Apr 2026 00:00:00 +0000

Understanding ion adsorption at electrified metal-electrolyte interfaces is essential for accurate modeling of electrochemical systems. Here, we systematically investigate the free energy profiles of Na+, Cl-, and F- ions at the Au(111)-water interface using enhanced sampling molecular dynamics with both classical force fields and machine-learned interatomic potentials (MLIPs). Our classical metadynamics results reveal a strong dependence of predicted ion adsorption on the Lennard-Jones parameters, highlighting that-without due care-standard mixing rules can lead to qualitatively incorrect descriptions of ion-metal interactions. We present a systematic methodology for tuning the cross term LJ parameters to control adsorption energetics in agreement with more accurate models. As a surrogate for an ab initio model, we employed the recently released Universal Models for Atoms MLIP, which validates classical trends and displays strong specific adsorption for chloride, weak adsorption...

Photon Avalanching Nanoparticles.

Mon, 13 Apr 2026 00:00:00 +0000

ConspectusAvalanches within nanoparticles seem like science fiction, but if they are avalanches of photons, they open up real-world innovations in imaging, sensing, optical computing, and other unexplored light-driven technologies. Avalanches are outsized events arising from the integration of many smaller inputs, and photon avalanching (PA) was first reported in bulk crystals in 1979 as an unexpectedly large jump in luminescence as excitation intensity was slowly increased. It would be 41 years before PA would be observed at the nanoscale in photon avalanching nanoparticles (ANPs), Tm³⁺-doped upconverting nanoparticles that show excited-to-ground state absorption inversion greater than 10,000:1 and emission that scales nonlinearly up to the 32nd power of the pump intensity. This extreme nonlinearity enables a real-time 5-fold improvement in the 150-year-old Abbe limit of spatial resolution, achieving 70 nm resolution using only simple scanning confocal microscopy....

Structural Heterogeneity in Medium-Entropy AgMnSbPbTe4 for Glassy Thermal Transport and High Thermoelectric Performance

Thu, 9 Apr 2026 00:00:00 +0000

Medium-entropy semiconductors represent a unique category of entropy-engineered materials. They possess a considerable level of randomness in atomic mixing, although this is not sufficient to conclusively achieve single-phase structure stabilization, in contrast to high-entropy materials. This introduces strong competition between the formation of different phases, which can potentially lead to structural heterogeneity. In this work, we uncover endotaxial nanoprecipitates in the microscopically identified homogeneous medium-entropy semiconductor AgMnSbPbTe₄. These nanoprecipitates initially crystallize in a cubic phase (Fm3̅m) within kinetically stabilized AgMnSbPbTe₄, subsequently evolving into a thermodynamically stable monoclinic phase (P2₁/c) during thermal annealing while maintaining an endotaxial relationship with the matrix lattice. This nanophase segregation and the resultant lattice mismatch at interfaces introduce...

Is there a future for 43 Ca nuclear magnetic resonance in cement science?

Thu, 2 Apr 2026 00:00:00 +0000

Calcium and silicon are critical components of cement. While ²⁹Si nuclear magnetic resonance (NMR) is widely used in cement science, ⁴³Ca NMR has received comparatively less attention given the experimental challenges associated with it. To investigate the potential of ⁴³Ca NMR in cement research, a density functional theory study was carried out. The study focused on distinct calcium sites within the calcium silicate hydrate (C-S-H) structure. Four unique calcium sites were identified, each predicted to display distinct ⁴³Ca chemical shifts due to differences in their local environments. These findings were used to generate theoretical ⁴³Ca NMR spectra for C-S-H. Furthermore, theoretical ⁴³Ca NMR spectra for the hydration reaction of triclinic tricalcium silicate were developed, illustrating the potential of ⁴³Ca NMR for tracking the hydration process in multiphase systems.

Low-temperature curing strength enhancement in cement-based materials containing limestone powder

Thu, 2 Apr 2026 00:00:00 +0000

With the ongoing sustainability movement, the incorporation of limestone powder in cementitious binders for concrete in the U.S. has become a subject of renewed interest. In addition to accelerating the early age hydration reactions of cementitious systems by providing additional surfaces for nucleation and growth of products, limestone powder is also intriguing based on its influence on low-temperature curing. For example, previous results have indicated that the utilization of limestone powder to replace one quarter of the fly ash in a high volume fly ash mixture (40–60% cement replacement) produces a reduction in the apparent activation energy for setting for temperatures below 25 °C. In the present study, the relationship between heat release and compressive strength of mortars at batching/curing temperatures of 10 and 23 °C is investigated. For Portland-limestone cements (PLC) with limestone additions on the order of 10%, a higher strength per unit heat release...

Timely deployment of best-in-class technologies to enable development and decarbonise construction

Thu, 2 Apr 2026 00:00:00 +0000

In the face of two apparently irreconcilable global challenges - housing a growing world population and reducing CO2 emissions - we analyse the current, historic and forecast data on the use of construction materials. Today, cement-based materials make up around three quarters of materials used by mass. Historically, we see that cement-based materials use goes through a peak as Gross Domestic Product per capita increases and then falls. This peak of cement use has been particularly pronounced in China, but is now on a downwards path. From now to 2050, three quarters of construction materials demand will be in low- and middle-income countries. We estimate that adopting the best available construction technologies could reduce CO2 emissions by about 73% compared to business as usual by 2050. In low- and middle-income countries, the housing and infrastructure needed to achieve the Sustainable Development Goals could be supplied while simultaneously reducing their per capita CO2 emissions...

Adsorption-Induced Surface Magnetism

Tue, 31 Mar 2026 00:00:00 +0000

We report the emergence of adsorption-induced magnetism from heterohelicene molecules on a nonmagnetic Cu(100) surface. Spin-polarized low-energy electron microscopy measurements reveal spin-dependent electron reflectivity for enantiopure 7,12,17-trioxa[11]helicene (TO[11]H) monolayers, indicating the formation of a spin-polarized state localized in the topmost copper layer. Control experiments on clean Cu(100) and TO[11]H on highly oriented pyrolytic graphite show no such effect, excluding artifacts and chirality-induced spin selectivity as origins. Spin-polarized density functional theory calculations with hybrid functionals attribute the magnetism to strong chemisorption, which induces hybridization between the molecular HOMO and copper s- and d-states, driving asymmetric spin-polarized charge redistribution at the interface. An extended Newns-Anderson-Grimley model incorporating on-site Coulomb repulsion in Cu d-orbitals reproduces the emergence of interfacial spin polarization...

Microstructure of amide-functionalized polyethylenes determined by NMR relaxometry

Tue, 31 Mar 2026 00:00:00 +0000

NMR relaxation studies reveal that pendant amidyl groups on polyethylenes alter microstructure and chain dynamics. These groups are localized in the rigid amorphous fraction of the polymers and lead to changes in bulk properties.

Generative Thermodynamic Computing

Mon, 30 Mar 2026 00:00:00 +0000

We introduce a generative modeling framework for thermodynamic computing, in which structured data are synthesized from noise by the natural time evolution of a physical system governed by Langevin dynamics. While conventional diffusion models use neural networks to perform denoising, here the information needed to generate structure from noise is encoded by the dynamics of a thermodynamic system. Training proceeds by maximizing the probability with which the computer generates the reverse of a noising trajectory, which ensures that the computer generates data with minimal heat emission. We demonstrate this framework within a digital simulation of a thermodynamic computer. If realized in analog hardware, such a system would function as a generative model that produces structured samples without the need for artificially injected noise or active control of denoising.

NEXAFS Spectroscopy of P3HT and PBTTT at the Sulfur K‑Edge

Mon, 30 Mar 2026 00:00:00 +0000

The sulfur K-edge near-edge X-ray absorption fine-structure (NEXAFS) spectra of the common conjugated polymers P3HT and PBTTT are studied from both experimental and theoretical perspectives. Experimental angle-resolved spectra are measured to characterize both the dominant peaks and the dichroism of the polymers. First-principles calculations using the density functional theory-based many-body X-ray absorption spectroscopy (MBXAS) method are performed for the two polymers as well as for the thiophene and thienothiophene units that make up the conjugated backbones of these polymers. Through this combined approach, we are able to confidently assign the observed peaks to specific molecular orbitals and identify the orientation of their transition dipole moments (TDMs) with respect to the coordinate frame of the polymer backbone. In particular, we are able to establish the character and orthogonal nature of the three main low-energy peaks at: (i) 2473.5 eV, 1s → (S–C)π* with TDM...

Mechanism and Kinetics of Propane and n‑Butane Dehydrogenation over Isolated and Nested SiOZn–OH Sites Grafted onto Silanol Nests of Dealuminated Beta Zeolite

Fri, 27 Mar 2026 00:00:00 +0000

Zn Lewis acid centers were grafted onto the silanol nest created by dealumination of H-BEA zeolite (DeAlBEA). The resulting material was characterized and investigated for propane dehydrogenation to propene and n-butane dehydrogenation to 1,3-butadiene (1,3-BD). For Zn/Al molar ratios (Al is the molar amount in H-BEA) below 0.12, Zn sites are present as isolated (SiOZn–OH) species, but for Zn/Al ratios between 0.12 and 0.60, the SiOZn–OH species form nests in which enhanced electron transfer between Zn and O atoms of the neighboring SiOZn–OH group and H-bonding interaction between adjacent Zn–OH groups occur. The turnover frequency (TOF) for both propane and n-butane dehydrogenation is virtually identical for Zn-DeAlBEA for Zn/Al < 0.12 and then increases almost linearly with increasing Zn/Al ratio from 0.12 to 0.36, indicating the superior activity of Zn atoms in SiOZn–OH nests. In the case of 1-butene dehydrogenation, identical activity is observed for both isolated and...

Atomic-Scale Imaging Reveals Polar‑π Interactions in Two-Dimensional Molecular Superlattices

Wed, 25 Mar 2026 00:00:00 +0000

Controlling coassembly of synthetic oligomers into binary superlattices at the atomic level is challenging. We report a strategy for programming polar-π interactions in oligomeric peptoids, a class of sequence-defined peptidomimetics, facilitating the formation of homogeneous two-dimensional (2D) superlattices. N-2-phenylethyl and N-(2-perfluorophenyl)ethyl side chains, similar in size, but with contrasting electrostatic characteristics, were introduced at defined sequence positions to generate favorable dipolar aromatic interactions. The resulting nanosheets exhibit different crystal motifs depending on the side chain interactions: systems containing only one type of aromatic side chain form a parallel V-shaped motif driven by π-π interactions, whereas a combination of both types of aromatic side chains, either within one backbone or through the coassembly of two distinct peptoids, adopt an antiparallel V-shaped superlattice with higher thermal stability, driven...

Nonlinear thermodynamic computing out of equilibrium

Wed, 25 Mar 2026 00:00:00 +0000

We present the design for a thermodynamic computer that can perform arbitrary nonlinear calculations in or out of equilibrium. Simple thermodynamic circuits, fluctuating degrees of freedom in contact with a thermal bath and confined by a quartic potential, display an activity that is a nonlinear function of their input. Such circuits can therefore be regarded as thermodynamic neurons, and can serve as the building blocks of networked structures that act as thermodynamic neural networks, universal function approximators whose operation is powered by thermal fluctuations. We simulate a digital model of a thermodynamic neural network, and show that its parameters can be adjusted by genetic algorithm to perform nonlinear calculations at specified observation times, regardless of whether the system has attained thermal equilibrium. This work expands the field of thermodynamic computing beyond the regime of thermal equilibrium, enabling fully nonlinear computations, analogous to those...

Locating the atoms at the hard-soft interface of gold nanoparticles

Wed, 25 Mar 2026 00:00:00 +0000

Surface structure affects the growth, shape and properties of nanoparticles. In wet chemical syntheses, metal additives and surfactants are used to modify surfaces and guide nanocrystal growth. To understand this process, it is critical to understand how the surface structure, and hence its energy, is modified. However, measuring the type and arrangement of atoms at hard-soft interfaces on nanoscale surfaces, especially in the presence of surfactants, is extremely challenging. Here, we determine the atomic structure of the hard-soft interface in a metallic nanoparticle by developing low-dose imaging conditions in four-dimensional scanning transmission electron microscopy that are preferentially sensitive to surface adatoms. By revealing experimentally the copper additives and bromide surfactant counterion at the surface of a gold nanocuboid and quantifying their interatomic distances, our direct, low-dose imaging method provides atomic-level understanding of chemically sophisticated...

Isothermal solidification for high-entropy alloy synthesis

Mon, 23 Mar 2026 00:00:00 +0000

Kinetically trapping the high-temperature states through rapid cooling solidification is widely used for the synthesis of high-entropy alloys (HEAs), especially those with intrinsically immiscible elemental combinations1, 2, 3–4. However, strategies need to be developed to overcome the fundamental limitations of rapid cooling solidification in controlling the crystallinity, structure and morphology of HEAs. Here we introduce an isothermal solidification strategy for the synthesis of HEAs by rapidly altering the metal alloy composition through liquid–liquid interface reactions at low temperatures, for example, from 25 °C to 80 °C. We use gallium (Ga)-based metal as the sacrificial reagent and mixing medium. By directing the reactions to the interfaces between the Ga-based liquid metal and an aqueous metal ion solution, the foreign metal ions can be reduced at the interfaces and incorporated into the liquid metal quickly. HEAs with various crystallinity (single crystal, mesocrystal,...

Si content in methacrylamide-containing A-b-(B-r-C) block copolymers and its impact on reactive ion etching properties

Fri, 20 Mar 2026 00:00:00 +0000

Block copolymers (BCPs) of an A-block-(B-random-C) architecture have been explored as materials for nanolithography because the composition and chemistry of the random block enables modification of thermodynamic and wetting properties to meet manufacturing criteria. Here, A-b-(B-r-C) BCPs created by an amidation reaction of polystyrene-block-poly(pentafluorophenyl methacrylate) (PS-b-PPFMA) with controlled amounts of Si add insight to previous conclusions about the dual contributions of BCP chemistry and reactive ion etch (RIE) gas chemistry on etch properties. We focus on two RIE etch characteristics: organosilicon etch resistance in H2/N2 plasma etching and enhanced removal of non-styrenic structures in an Ar/O2 etch. Consistent with previous studies, higher amounts of Si result in greater etch resistance under H2/N2 RIE, where at least ∼10 wt. % Si is necessary to exhibit sufficient etch resistance. By contrast, Ar/O2 etching resulted in etch rates independent of Si content....

Dual interfacial H-bonding-enhanced deep-blue hybrid copper–iodide LEDs

Thu, 19 Mar 2026 00:00:00 +0000

Solution-processed light-emitting diodes based on non-toxic copper–iodide hybrids1 are a compelling solution for efficient and stable deep-blue lighting, owing to their tunability, high photoluminescence efficiency and environmental sustainability2. Here we present a hybrid copper–iodide that shows near-unity photoluminescence quantum yield (99.6%) with an emission wavelength of 449 nm and colour coordinates (0.147, 0.087), alongside its emission mechanism and charge transport characteristics. We use the thin film of this hybrid as the sole active emissive layer to fabricate deep-blue light-emitting diodes and subsequently enhance the device performance through a dual interfacial hydrogen-bond passivation strategy. This synergetic surface modification approach, integrating a hydrogen-bond-acceptor self-assembled monolayer with an ultrathin polymethyl methacrylate capping layer, effectively passivates both heterojunctions of the copper–iodide hybrid emissive layer and optimizes...

Utilizing Single-Crystalline Transformations for Precise Atom Placement in Multicomponent Cluster-Based Coordination Networks

Thu, 19 Mar 2026 00:00:00 +0000

The assembly of cluster or superatom building-blocks into extended solids has revolutionized materials design, enabling the synthesis of modular semiconductors with well-defined structures and tunable electronic, magnetic or optical properties. This strategy has recently advanced the synthesis of complex metal oxides with multifunctional or emergent behaviors, but precise atom placement of multiple elements with similar chemistries or preferred coordination environments remains a significant challenge. Here, we present a strategy for synthesizing polyoxometalate (POM)-based coordination networks with up to three different cations in precisely defined positions. Our approach leverages a single-crystal-to-single-crystal (SCSC) transformation in which the spatial placement of cations is governed by their availability at distinct stages of crystallization and transformation. Specifically, [ZP₅W₃₀O₁₁₀]^(15-n)- (Z = Na⁺, K⁺,...

Accelerating iterative ptychography with an integrated neural network

Thu, 19 Mar 2026 00:00:00 +0000

Electron ptychography is a powerful and versatile tool for high-resolution and dose-efficient imaging. Iterative reconstruction algorithms are powerful but also computationally expensive due to their relative complexity and the many hyperparameters that must be optimised. Gradient descent-based iterative ptychography is a popular method, but it may converge slowly when reconstructing low spatial frequencies. In this work, we present a method for accelerating a gradient descent-based iterative reconstruction algorithm by training a neural network (NN) that is applied in the reconstruction loop. The NN works in Fourier space and selectively boosts low spatial frequencies, thus enabling faster convergence in a manner similar to accelerated gradient descent algorithms. We discuss the difficulties that arise when incorporating a NN into an iterative reconstruction algorithm and show how they can be overcome with iterative training. We apply our method to simulated and experimental...

Temperature‐Dependent Crystallization in Two‐Step Perovskite Deposition Revealed by In Situ GIWAXS and Machine Learning‐Guided Analysis

Wed, 18 Mar 2026 00:00:00 +0000

ABSTRACT The performance and stability of perovskite solar cells are strongly governed by the crystallization behavior of their active layer. In two‐step sequential deposition, early‐stage film formation plays a decisive role in determining final phase purity and device quality. Guided by a data‐driven analysis of nearly 39 000 devices in the FAIR perovskite database, we identified solvent‐mediated quenching and thermal processing as key variables affecting power conversion efficiency (PCE), particularly in two‐step fabrication. To investigate these effects in real time, we designed and implemented a custom‐built, temperature‐controlled spin‐coating system, enabling precise thermal modulation during precursor deposition. Using this platform, we performed in situ GIWAXS measurements to study the crystallization dynamics of FA 0.5 MA 0.5 PbI 3 films over a temperature range of 30°C–90°C. Our results reveal a non‐monotonic relationship between spin‐coating temperature and α‐phase...

Structural Heterogeneity in Medium-Entropy AgMnSbPbTe4 for Glassy Thermal Transport and High Thermoelectric Performance

Tue, 17 Mar 2026 00:00:00 +0000

Structural Heterogeneity in Medium-Entropy AgMnSbPbTe4 for Glassy Thermal Transport and High Thermoelectric Performance

Tue, 17 Mar 2026 00:00:00 +0000

Structural Heterogeneity in Medium-Entropy AgMnSbPbTe4 for Glassy Thermal Transport and High Thermoelectric Performance

Tue, 17 Mar 2026 00:00:00 +0000

Structural Heterogeneity in Medium-Entropy AgMnSbPbTe4 for Glassy Thermal Transport and High Thermoelectric Performance

Tue, 17 Mar 2026 00:00:00 +0000

Ion transport through reconfigurable nanoparticle-surfactant stabilized droplet interface bilayers.

Mon, 16 Mar 2026 00:00:00 +0000

Despite their adaptability and mechanical stability, Pickering emulsions based on the interfacial assembly of colloidal particles have not found use in iontronics, since the dense interfacial packing of micron-sized particles precludes functional connectivity between two droplets. Here, we introduce a chemically reconfigurable droplet interface bilayer (DIB) platform based on the interfacial assembly of nanoparticle-surfactants (NPSs) that enables spontaneous or field-induced formation of ion-conducting nanochannels, eliminating the need of ionophores or nanochannel-forming proteins. These nanoscopic channels emerge from packing defects in the jammed interfacial assemblies of the charged NPSs and support size and charge selective, hysteretic ion transport governed by interfacial electrostatics and dimensional constraints. The NPS-DIBs show short-term and long-term plasticity, hallmarks of neuromorphic behavior, that are mediated by the structural and chemical design of the bilayer....

Unraveling the Origin of Glassy Thermal Transport in Medium-Entropy Semiconductors: From Nanoscale Phase Segregation to Atomic-Scale Lattice Distortion

Thu, 12 Mar 2026 00:00:00 +0000

Unraveling the Origin of Glassy Thermal Transport in Medium-Entropy Semiconductors: From Nanoscale Phase Segregation to Atomic-Scale Lattice Distortion

Automated Nanocrystal Synthesis: Lessons from 25 Years of Robots, Microfluidics, and Machine Learning

Wed, 11 Mar 2026 00:00:00 +0000

This perspective highlights the evolution of techniques for automating the synthesis of colloidal nanocrystals. Over the past 25 years, microfluidic reactors and robotic workflows have been developed to enhance the reproducibility of nanocrystal synthesis, facilitate rapid screening of reaction conditions, optimize material properties, and perform multistep syntheses of high-quality nanoparticles with complex heterostructures. Modern automated systems are now valued for their ability to generate robust data sets for validating physical models, supporting chemical mechanisms, training machine learning models, and for directing autonomous experimentation. We discuss the early challenges and limitations of these technologies and present key lessons for effectively utilizing automated and ML-guided tools to accelerate nanocrystal discovery for the next 25 years.

Interplay between Ultrafast Electronic and Librational Dynamics in Liquid Nitrobenzene Probed with Two-Color Four-Wave Mixing

Wed, 11 Mar 2026 00:00:00 +0000

We present an experimental and theoretical study of the interplay between ultrafast electron dynamics and librational dynamics in liquid nitrobenzene. A femtosecond ultraviolet pulse and two femtosecond near-infrared pulses interact with nitrobenzene molecules, generating a four-wave mixing nonlinear signal measured in the Optical Kerr Effect geometry. The signal is measured to be nonzero only at negative time delays, corresponding to the near-infrared pulses arriving before the ultraviolet pulse. We perform time-dependent Quantum Master Equation calculations with classical libration to simulate the experiment. The simulations support the conclusion that the near-infrared pulses launch librational motion while creating electronic coherences resulting in a libration-modulated electronic nonlinear response. The analysis of the phase-matched four-wave mixing signals suggests a nonparametric process leaving the molecules in an excited electronic state, providing new insight into ultrafast...

Gradient-based optimization of complex nanoparticle heterostructures enabled by deep learning on heterogeneous graphs

Wed, 11 Mar 2026 00:00:00 +0000

Applications of deep learning (DL) to design nanomaterials are hampered by a lack of suitable data representations and training data. Here we report efforts to overcome these limitations and leverage DL to optimize the nonlinear optical properties of core–shell upconverting nanoparticles (UCNPs). UCNPs, which have applications in fields such as biosensing, super-resolution microscopy and three-dimensional printing, can emit visible and ultraviolet light from near-infrared excitations. We report a large-scale dataset of UCNP emission spectra based on accurate but expensive kinetic Monte Carlo simulations (N > 6,000) and use these data to train a heterogeneous graph neural network using a physically motivated representation of UCNP nanostructure. Applying gradient-based optimization on the trained graph neural network, we identify structures with 6.5× higher predicted emission under 800-nm illumination than any UCNP in our training set. Our work reveals design principles for...

Advances in in situ/operando techniques for catalysis research: enhancing insights and discoveries

Tue, 10 Mar 2026 00:00:00 +0000

Catalysis research has witnessed remarkable progress with the advent of in situ and operando techniques. These methods enable the study of catalysts under actual operating conditions, providing unprecedented insights into catalytic mechanisms and dynamic catalyst behavior. This review discusses key in situ techniques and their applications in catalysis research. Advances in in situ electron microscopy allow direct visualization of catalysts at the atomic scale under reaction conditions. In situ spectroscopy techniques like X-ray absorption spectroscopy and nuclear magnetic resonance spectroscopy can track chemical states and reveal transient intermediates. Synchrotron-based techniques offer enhanced capabilities for in situ studies. The integration of in situ methods with machine learning and computational modeling provides a powerful approach to accelerate catalyst optimization. However, challenges remain regarding radiation damage, instrumentation limitations, and data interpretation....

Molecular axis distribution moments in ultrafast transient absorption spectroscopy: A path toward ultrafast quantum state tomography

Tue, 10 Mar 2026 00:00:00 +0000

In ultrafast time-resolved experiments with gas phase molecules, the alignment of the molecular axis relative to the polarization of the interacting laser pulses plays a crucial role in determining the dynamics following this light-matter interaction. The molecular axis distribution is influenced by the interacting pulses and is intrinsically linked to the electronic coherences of the excited molecules. However, in typical theoretical calculations of such interactions, the signal is either calculated for a single molecule in the molecular frame or averaged over all possible molecular orientations to compare with the experiment. Such averaging removes information about anisotropy in the molecular-axis distribution, even though anisotropic contributions can play a significant role in the measured experimental signal. Here, we calculate the laboratory frame transient electronic first-order polarization [P(1)] spectra in terms of separated molecular frame and laboratory frame quantities....

Unsupervised learning of representative local atomic arrangements in molecular dynamics data

Tue, 10 Mar 2026 00:00:00 +0000

Molecular dynamics (MD) simulations present a data-mining challenge, given that they can generate a considerable amount of data but often rely on limited or biased human interpretation to examine their information content. By not asking the right questions of MD data we may miss critical information hidden within it. We combine dimensionality reduction (UMAP) and unsupervised hierarchical clustering (HDBSCAN) to quantitatively characterize the coordination environment of chemical species within MD data. By focusing on local coordination, we significantly reduce the amount of data to be analyzed by extracting all distinct molecular formulas within a given coordination sphere. We then efficiently combine UMAP and HDBSCAN with alignment or shape-matching algorithms to classify these formulas into distinct structural isomer families. The outcome is a quantitative mapping of the multiple coordination environments present in the MD data. The method was employed to reveal details of...

CRAGE-RB-PI-seq reveals transcriptional dynamics of plant-associated bacteria during root colonization

Tue, 10 Mar 2026 00:00:00 +0000

Plant roots release a wide array of metabolites into the rhizosphere, shaping microbial communities and their functions. While metagenomics has expanded our understanding of these communities, little is known about the physiology of their members in host environments. Transcriptome analysis via RNA sequencing is a common approach to learning more, but its use has been challenging because of low bacterial biomass and interference from plant RNA. To overcome this, we developed a randomly-barcoded promoter-library insertion sequencing (RB-PI-seq) combined with chassis-independent recombinase-assisted genome engineering (CRAGE). Using Pseudomonas simiae WCS417 as a model rhizobacterium, this method enabled targeted amplification of barcoded transcripts, bypassing plant RNA interference and allowing measurement of thousands of promoter activities during Arabidopsis root colonization. Our analysis revealed temporally resolved transcriptional regulation, including those associated with...

A Nanoscale Ternary Amide‐rGO Composite with Boosted Kinetics for Reversible H2 Storage (Adv. Mater. Interfaces 27/2023)

Tue, 10 Mar 2026 00:00:00 +0000

Reversible H2 Storage In article 2300310, Vitalie Stavila, Jeffrey J. Urban, and co‐workers unleashed the full potential of hydrogen storage with rGO: This innovative material catalyzes hydrogen bond breakage at the Mg‐amide/Li hydride interface, leading to faster dehydrogenation. The nanosizing effect of rGO shortens hydrogen diffusion paths, boosting the speed of dehydrogenation compared to conventional methods. This discovery offers a cutting‐edge solution for designing metal imide composites that achieve optimal, efficient hydrogen storage performance.

Anomalous Nernst conductivity of Weyl materials is enhanced when the anomalous Hall conductivity exhibits a two-peaked feature

Fri, 6 Mar 2026 00:00:00 +0000

Power generation through the anomalous Nernst effect in topological Weyl materials has several advantages over conventional thermoelectrics due to the transverse geometry. However, the magnitude of the anomalous Nernst conductivity (ANC) in most known materials is too small to be of practical use, and there exist few guiding principles for finding materials with optimal thermoelectric properties. This work shows that the ANC is maximal when there is a “coactive-staggered” feature in the anomalous Hall conductivity (AHC). It is shown that a minimal arrangement of two Weyl pairs leads to such a feature, and tuning the separations between the pairs controls the temperature at which the ANC is maximal. Several methods are proposed for creating such arrangements of Weyl points starting from Dirac semimetal materials. It is also demonstrated how an existing coactive-staggered AHC in a Heusler material can be exploited, by collectively tuning the positions of the Weyl points through...

Carrier Localization and Spontaneous Formation of Two-Dimensional Polarization Domain in Halide Perovskites

Fri, 6 Mar 2026 00:00:00 +0000

Halide perovskites are known for their rich phase diagram and superior performance in diverse optoelectronics applications. The latter property is often attributed to the long electron-hole recombination time, whose underlying physical mechanism has been a long-standing controversy. In this Letter, we investigate the transport and localization properties of electron and hole carriers in a prototypical halide perovskite (CsPbBr_{3}), through ab initio tight-binding nonadiabatic dynamics approach for large-scale (tens of nm size) supercell calculations, to simulate electron and ion dynamics on the same footing. We found distinct structural, lattice polarization, and electron-phonon coupling properties at low (below 100 K) and high temperatures, consistent with experimental observations. In particular, at low temperature we find spontaneous formation of polar grain boundaries in the nonpolar bulk systems, which result in two-dimensional polarization patterns that serve...

Isolation of a Terminal Cobalt Nitride in a Metal–Organic Framework

Thu, 5 Mar 2026 00:00:00 +0000

Transition metal nitrides are reactive intermediates in biological and industrial processes. Chemists have synthesized molecular model complexes of such reactive species to understand their function and electronic requirements for new applications. However, molecular chemistry can suffer from intra- and intermolecular decomposition pathways, which preclude further discovery of unknown reactive species. Metal-organic frameworks offer an opportunity for creating long-lived forms of such species with the vacuum of the pore suppressing degradation while simultaneously enabling substrate access for controlled reactivity studies. Here, we report the characterization of an elusive terminal cobalt nitride species generated through photolysis or thermolysis of a site-isolated cobalt azide within the evacuated metal-organic framework CoN₃-MFU-4l. The first crystal structure of such a species is presented, with vibrational, X-ray absorption, and electron paramagnetic resonance...

Heterogeneous Corrosion Pathways in Pt–Ni Nanododecahedra Revealed by In Situ Liquid Cell TEM

Thu, 26 Feb 2026 00:00:00 +0000

Unraveling nanoscale corrosion pathways is essential for understanding materials degradation mechanisms and designing corrosion-resistant metal alloys. Here, we directly visualize the corrosion of Pt-Ni nanododecahedra in 0.1 M HCl using liquid cell TEM. Each nanoparticle features a Ni-rich core and a Pt-rich frame. Our observation reveals that corrosion proceeds in two distinct stages: first the Ni-rich core dissolves without forming porosity, yielding small Pt nanocrystals and transient NiCl₂·6H₂O at the retreating interfaces; then the Pt-rich frame fragments into ∼5 nm Pt₃Ni nanocrystals that subsequently dissolve uniformly, accompanied by fleeting Pt chlorides. A percolation-based theory explains the observed behaviors: The core's ∼8% Pt lies below the Pt connectivity threshold, preventing Pt scaffold formation, whereas the frame's 48% Ni exceeds the Ni percolation threshold and collapses. Ordered Pt₃Ni suppresses Ni percolation,...

Room-temperature valley-selective emission in Si-MoSe2 heterostructures enabled by high-quality-factor chiroptical cavities

Mon, 23 Feb 2026 00:00:00 +0000

Transition metal dichalcogenides possess valley pseudospin, enabling coupling between photon spin and electron spin for classical and quantum information processing. However, rapid valley-dephasing processes have impeded the development of scalable, high-performance valleytronic devices operating at room temperature. Here we demonstrate that a chiral resonant metasurface can enable room-temperature valley-selective emission in MoSe2 monolayers independent of excitation polarization. This platform provides circular eigen-polarization states with a high quality factor (Q-factor) and strong chiral near-field enhancement. The fabricated Si chiral metasurfaces exhibit chiroptical resonances with Q-factors up to 450 at visible wavelengths. We reveal degrees of circular polarization (DOP) reaching a record high of 0.5 at room temperature. Our measurements show that the high DOP can be attributed to the significantly increased chiroptical local density of states, which enhances valley-specific...

Surface structure of water from soft X-ray second harmonic generation

Mon, 23 Feb 2026 00:00:00 +0000

The microscopic structure of water’s surface is crucial to many natural and industrial processes, but studying its hydrogen bond (H-bond) network directly remains challenging due to the required interfacial sensitivity of experimental techniques. By leveraging advances in flat liquid sheet microjets and terawatt-scale attosecond soft X-ray pulses from the LCLS X-ray free electron laser, we employed soft X-ray second harmonic generation (SXSHG) spectroscopy to examine the liquid water/vapor interface. SXSHG combines the elemental selectivity of X-ray spectroscopies with the surface selectivity of SHG and gives access to the electronic structure of interfacial species. Here, we show the SXSHG spectrum differs from bulk water’s X-ray absorption, with its peak shifted several eV, indicating a vastly different electronic environment at the interface as compared to the bulk. First-principles electronic structure calculations show the signal is highly sensitive to H-bond interactions,...

Polarization Control via Artificial Optical Nonlinearity in Dielectric Metasurfaces

Tue, 17 Feb 2026 00:00:00 +0000

Nonlinear optical phenomena are generally governed by geometry in matter systems, as they depend on the spatial arrangement of atoms within materials or molecules. Metasurfaces, through precisely designed geometries on a subwavelength scale, allow the optical response of a material to be tailored far beyond its natural properties. Therefore, metasurfaces are highly appealing for enabling the engineering of nonlinear optical interactions. Current studies of nonlinear metasurfaces predominantly focus on the phase control of the generated light. Nonetheless, investigating the tensorial nature of the nonlinearity of metasurfaces and its effect on the polarization of the generated light is critical to fully unlocking a range of applications, such as nonlinear vector beam generation and nonlinear polarization imaging. Here, we study the artificial optical nonlinearity of a dielectric metasurface originating from its meta-atom symmetry and describe the third-order nonlinear behavior...

Non‐Equilibrium Synthesis Methods to Create Metastable and High‐Entropy Nanomaterials

Tue, 17 Feb 2026 00:00:00 +0000

Stabilizing multiple elements within a single phase enables the creation of advanced materials with exceptional properties arising from their complex composition. However, under equilibrium conditions, the Hume-Rothery rules impose strict limitations on solid-state miscibility, restricting combinations of elements with mismatched crystal structures, atomic radii, valence states, or electronegativities. This severely narrows the accessible compositional space for creating new inorganic materials. In this review, we highlight how non-equilibrium synthesis methods, featuring ultrafast heating and quenching, can overcome these thermodynamic barriers, enabling integration of immiscible elements into metastable and high-entropy nanostructures. The resulting materials benefit from both kinetic trapping and stabilization by high configurational entropy, leading to enhanced phase stability. These materials can exhibit unique structural and functional properties that are needed for advancing...

PhaseT3M: 3D imaging at 1.6 Å resolution via electron cryo-tomography with nonlinear phase retrieval

Wed, 11 Feb 2026 00:00:00 +0000

Electron cryo-tomography (cryo-ET) enables 3D imaging of complex, radiation-sensitive structures with molecular detail. However, image contrast from the interference of scattered electrons is nonlinear with atomic density and multiple scattering further complicates interpretation. These effects degrade resolution, particularly in conventional reconstruction algorithms, which assume linearity. Particle averaging can reduce such issues but is unsuitable for heterogeneous or dynamic samples ubiquitous in biology, chemistry, and materials sciences. Here, we develop a phase retrieval-based cryo-ET method, PhaseT3M. We experimentally demonstrate its application to an approximately 7 nm Co3O4 nanoparticle on an approximately 30 nm carbon substrate, achieving a maximum resolution of 1.6 Å, surpassing conventional limits using standard cryo-TEM equipment. PhaseT3M uses a multislice model for multiple scattering and Bayesian optimization for alignment and computational aberration correction,...

Influence of hydrogen on the low cycle fatigue behavior of the equiatomic CrMnFeCoNi high entropy alloy

Wed, 11 Feb 2026 00:00:00 +0000

True plastic strain-controlled low cycle fatigue (LCF) tests were performed on the CrMnFeCoNi high-entropy alloy in two conditions: thermally precharged with hydrogen (H-precharged) and non-charged. Serrated flow was observed during the first cycle in the H-precharged condition, likely due to hydrogen pinning mobile dislocations. This behavior is suppressed with further straining, most likely by the increase in dislocation density. Internal hydrogen increases the cyclic strength of this alloy at all plastic strain amplitudes by enhancing the effective component of the flow stresses. Furthermore, the evolution of back stresses during LCF testing at different strain amplitudes is not influenced by the presence of hydrogen, suggesting that the strengths of the dislocation structures evolve similarly in both conditions. However, transmission electron microscopy reveals that dislocation cell formation is similar in specimens with and without hydrogen at high amplitudes but is limited...

Elucidating Compositional Differences in Halide Perovskites for Normal and Inverted Perovskite Solar Cells

Tue, 10 Feb 2026 00:00:00 +0000

Over the recent few years, extensive research efforts have shifted from normal (n-i-p) to inverted (p-i-n) perovskite solar cells (PSCs), owing to their promising efficiency and operational stability, enabled by low-temperature processing. Despite a fundamentally identical operation principle (only structurally inverted), the optimized perovskite compositions for normal and inverted PSCs differ significantly across the literature, suggesting an underlying design principle for perovskite composition. Here, we unveil the role of cesium cation in enhancing interfacial contact between the perovskite layer and the underlying hole-transporting layer (HTL) in inverted PSCs. Comprehensive in situ and device characterization reveal that cesium incorporation promotes the formation of initial nucleation seeds for heterogeneous nucleation at the perovskite/hydrophobic HTL interface, thereby improving their contact. The resulting compositional heterogeneity explains the focus of recent studies...

Fabrication and characterization of boron-terminated tetravacancies in monolayer hBN using STEM, EELS and electron ptychography

Tue, 10 Feb 2026 00:00:00 +0000

Tetravacancies in monolayer hexagonal boron nitride (hBN) with consistent edge termination (boron or nitrogen) form triangular nanopores with electrostatic potentials that can be leveraged for applications such as selective ion transport and neuromorphic computing. In order to quantitatively predict the properties of these structures, an atomic-level understanding of their local electronic and chemical environments is required. Moreover, robust methods for their precision manufacture are needed. Here we use electron irradiation in a scanning transmission electron microscope (STEM) at a high dose rate to drive the formation of boron-terminated tetravacancies in monolayer hBN. Characterization of the defects is achieved using aberration-corrected STEM, monochromated electron energy-loss spectroscopy (EELS), and electron ptychography. Z-contrast in STEM and chemical fingerprinting by core-loss EELS enable identification of the edge terminations, while electron ptychography gives...

Directed self-assembly of block copolymers for high-precision patterning in the era of extreme ultraviolet lithography

Tue, 10 Feb 2026 00:00:00 +0000

Extreme ultraviolet (EUV) lithography enables unprecedented resolution in semiconductor patterning but faces critical challenges in developing resist materials that achieve high-precision at economically viable throughput. Directed self-assembly (DSA) of block copolymers (BCPs) offers a promising solution for pattern rectification by leveraging thermodynamically determined domain structures to decouple BCP pattern quality from the imperfect original lithographic pattern. This prospective presents an overview of recent progress on the EUV + DSA strategy, covering advances in BCP material design, processing, metrology, and pattern transfer. We highlight recent advances in high-χ BCPs with perpendicular orientation and domain spacings compatible with EUV dimensions, leveraging A-b-(B-r-C) architectures. We also discuss progress in chemical pre-pattern fabrication using both positive- and negative tone resists, along with processing strategies to minimize defects and roughness based...

Designing and Utilizing Material Acceleration Platforms: Need for Workforce Development

Tue, 10 Feb 2026 00:00:00 +0000

In the quest to accelerate scientific discovery, the materials science field is rapidly moving toward the implementation of robotics and artificial intelligence driven workflows. Our recent summer school “Future Labs: Robotic Synthesis Coupled with Machine Learning for Energy Materials” provided learning opportunities for students, researchers, and educators in the materials science community. We describe this experience and provide our perspective on which new directions could be pursued to enable the future workforce to acquire cross-disciplinary skills.

Low Frequency Vibrational Modes of Two-Dimensional Lead-Free Metal Halide Double Perovskites

Sat, 7 Feb 2026 00:00:00 +0000

2D layered double perovskites of (S-MPA)4AgBiI8 (MPA-AgBiI8) and (S-MPA)4CuBiI8 (MPA-CuBiI8) (S-MPA, S-β-methylphenethylammonium) were synthesized with a hydrothermal method. The crystal structure of MPA-AgBiI8 was determined using single-crystal X-ray diffraction (scXRD). Powder XRD (pXRD) data suggest that the crystal structure of MPA-CuBiI8 is more complex than that of MPA-AgBiI8. UV–vis electronic absorption spectra of these perovskites reveal a bandgap of 2.03 eV for both. Short exciton lifetime from time-resolved photoluminescence (TRPL) results and low PL intensity of the Cu-based perovskite suggest a high density of trap states within the bandgap. Low frequency Raman spectra of both materials show distinct peaks and a slightly higher frequency for the Cu-based perovskite than the Ag-based perovskite. Density functional theory (DFT) calculations were conducted to simulate the low frequency Raman spectra and help explain the different phonon modes, which are collective vibrations...

Iridium-cobalt oxide synthesized via surfactant-assisted Adams fusion for efficient oxygen evolution in acidic and alkaline media

Wed, 28 Jan 2026 00:00:00 +0000

A series of iridium-cobalt (Ir-Co) oxide catalysts were synthesized using a modified surfactant-assisted Adams fusion method and evaluated for the oxygen evolution reaction (OER) in both acidic and alkaline media. The effect of varying the Ir/Co ratio was systematically studied and compared with commercial Ir black and pure IrO2 samples. The actual elemental ratios were quantified using X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectroscopy (EDS), and inductively coupled plasma-mass spectrometry (ICP-MS). Among the synthesized samples, the Ir6Co4 catalyst exhibited the best performance in acidic media, achieving an iR-corrected overpotential of 292 mV. In alkaline conditions, it demonstrated comparable activity to Ir black, with an iR-corrected overpotential of 263 mV. XPS and electron energy loss spectroscopy analyses revealed that increasing Co content led to a higher fraction of metallic Ir (Ir0) in the catalyst. In addition, the role of Ir3+ in enhancing...

The incommensurate modulation of tetragonal tungsten bronze quantified by high resolution 4D STEM

Tue, 27 Jan 2026 00:00:00 +0000

Many members of the tetragonal tungsten bronze (TTB) family of oxides display an incommensurate periodic lattice distortion, the nature of which has been the subject of some controversy. Here we present a study of this structural modulation in the relaxor ferroelectric Ba5SmSn3Nb7O30 (BSSN) by quantitative scanning transmission electron microscopy (STEM). We characterize the modulation in BSSN by employing a fast, pixelated direct electron detector to perform high resolution phase contrast STEM imaging of the crystalline lattice. By quantitatively analyzing the images, we visualize the atomic structural correlations present in the material on both the cation and anion sublattices. This analysis reveals the incommensurate structure to have an octahedral tilting pattern and cooperative A2 site cation displacements, analogous to an Ama2 commensurate cell. Finally, we show that the modulation is composed of a structural motif with a period of 3 x d 1 1 ¯ 0 and modified by discommensurations,...

Entanglement of a nuclear spin qubit register in silicon photonics

Tue, 27 Jan 2026 00:00:00 +0000

Colour centres provide an optical interface to quantum registers based on electron and nuclear spin qubits in solids. The T centre in silicon is an emerging spin–photon interface that combines telecom O-band optical transitions and an electron spin in a scalable photonics platform. Here we integrate T centres into single-mode photonic waveguides in a silicon-on-insulator platform. We demonstrate the initialization, coherent control and state read-out of a three-qubit register based on the electron spin of a T centre coupled to a hydrogen and a silicon nuclear spin. The spin register exhibits spin echo coherence times of 0.41(2) ms for the electron spin, 112(12) ms for the hydrogen nuclear spin and 67(7) ms for the silicon nuclear spin. We use nuclear–nuclear two-qubit gates to generate entanglement between the two nuclear spins with a fidelity of F = 0.77(3) and a coherence time of T2*=2.60(8)$${T}_{2}^{* }=2.60(8)$$ ms. Our results show that a T centre in silicon photonics can...

Mesoscale variations of the chemical and electronic landscape on the surface of the Weyl semimetal Co3Sn2S2 visualized by ARPES and XPS

Tue, 27 Jan 2026 00:00:00 +0000

The multiple crystalline terminations in magnetic Weyl semimetal Co3Sn2S2 display distinct topological and trivial surface states, which have successfully been distinguished experimentally. However, a model of pure terminations is known to be inadequate because these surfaces exhibit a high degree of spatial heterogeneity and point disorder. Here, we perform a spectromicroscopy study of the surface chemistry and surface electronic structure using photoemission measurements in combination with first-principles calculations of core levels. We identify an intermediate region with properties distinct from both the sulfur and tin terminations, and demonstrate that the spectral features in this region can be associated with a disordered termination with a varying density of surface tin vacancies. This work establishes heuristics for identifying variable surface disorder using photoemission, an important prerequisite to experimentally establishing the behavior of momentum-space topological...

Modeling phase transformations in Mn-rich disordered rocksalt cathodes with machine-learning interatomic potentials

Thu, 22 Jan 2026 00:00:00 +0000

Mn-rich disordered rocksalt (DRX) cathode materials exhibit a phase transformation from a disordered to a partially disordered spinel-like structure (δ-phase) during electrochemical cycling. In this computational study, we use charge-informed molecular dynamics with a fine-tuned CHGNet foundation potential to investigate the phase transformation in LixMn0.8Ti0.1O1.9F0.1. Our results indicate that transition metal migration occurs and reorders to form the spinel-like ordering in an FCC anion framework. The transformed structure contains a higher concentration of nontransition metal (0-TM) face-sharing channels, which are known to improve Li transport kinetics. Analysis of the Mn valence distribution suggests that the appearance of tetrahedral Mn2+ is a consequence of spinel-like ordering, rather than the trigger for cation migration as previously suggested. Calculated equilibrium intercalation voltage profiles demonstrate that the δ-phase, unlike the ordered spinel, exhibits solid-solution...

Sub-10 nm upconversion nanocrystals for long-term single-particle tracking

Thu, 22 Jan 2026 00:00:00 +0000

Lanthanide-doped upconversion nanoparticles are attractive single-molecule imaging probes due to their high photostability and anti-Stokes luminescence. However, achieving both small particle size and strong brightness has remained a major challenge, as reducing size often leads to dimmer emission. Herein, we fabricate a sub-10 nm cascade actively protected upconversion nanoparticles, which shows a 33-fold enhanced upconversion efficiency at the single-particle level compared to larger ~19 nm conventional nanoparticles. Theoretical modeling and time-resolved measurements show that emission loss mainly comes from energy leakage of Er3+ ions to surface defects. By introducing a NaYbF4 layer as photon-harvesting and protective intermediate layer, we minimize this energy loss and significantly boost brightness. A monolayer of inert NaLuF4 can effectively suppress the surface quenching to Yb3+. Using these ultra-small bright probes, we successfully tracked single epidermal growth...

Mining Thermophile Photosynthesis Genes: A Synthetic Operon Expressing Chloroflexota Species Reaction Center Genes in Rhodobacter sphaeroides

Wed, 21 Jan 2026 00:00:00 +0000

Photosynthesis is the foundation of the vast majority of life systems, and is therefore the most important bioenergetic process on earth. The greatest diversity of photosynthetic systems is found in microorganisms. However, our understanding of the biophysical and biochemical processes that transduce light into chemical energy is derived from a relatively small subset of proteins from microbes that are amenable to cultivation, in contrast to the huge number of predicted proteins that catalyze the initial photochemical reactions deposited in databases, such as from metagenomics. We describe the use of a Rhodobacter sphaeroides laboratory strain for the expression of heterologous photosynthesis genes to demonstrate the feasibility of mining this resource, focusing on hot spring Chloroflexota gene sequences. Using a synthetic operon of genes, we produced a photochemically active complex of reaction center proteins in our biological system. We also present bioinformatic...

Ionic‐Liquid Free and Flexible Transistors Made of 2D Material Inks

Wed, 21 Jan 2026 00:00:00 +0000

The development of thin-film transistors (TFTs) using 2D materials is crucial for enabling scalable, low-cost, and flexible electronics. Currently, 2D TFTs with the highest performance have been achieved by using ionic-liquid gating (ILG), a technique suited for proof-of-concept studies. However, ILG suffers from slow switching speeds, temperature sensitivity, poor long-term stability, and integration challenges, making it unsuitable for practical use. Moreover, typical fabrication methods for 2D TFTs involve harsh conditions such as strong acids or high temperatures (>300 °C), limiting integration with flexible substrates. This work provides the first demonstration of an ILG-free, all-2D-material TFT fabricated onto a flexible substrate. Water-based graphene and hexagonal boron nitride (h-BN) inks are printed to deposit the electrodes and dielectric layers, respectively. The MoS₂ channel is produced via supramolecular interfacial self-assembly, yielding uniform,...

Photon blockade in a Tavis-Cummings system

Wed, 21 Jan 2026 00:00:00 +0000

We observe blockade of microwave photons in a Tavis-Cummings system comprising a superconducting cavity and up to transmon qubits. The effect is characterized with photon-number-resolving spectroscopy using an additional dispersively coupled transmon “witness” qubit to directly probe the cavity’s photon-number distribution. We first observe polariton formation with splitting proportional to , confirming the Tavis-Cummings coupling, and subsequently obtain sub-Poissonian cavity photon statistics when the cavity is driven at polariton frequencies.

Quantitative Structure Determination from Experimental Four-Dimensional Scanning Transmission Electron Microscopy via the Scattering Matrix

Thu, 15 Jan 2026 00:00:00 +0000

Considerable inroads have recently been made on algorithms to determine the sample potential from four-dimensional scanning transmission electron microscopy data from thick samples where multiple scattering cannot be neglected. This paper further develops the scattering matrix approach to such structure determination. Through simulation, we demonstrate how this approach can be modified to better handle partial spatial coherence, unknown probe defocus, and information from the dark field region. By combining these developments we reconstruct the electrostatic potential of a monolithic SrTiO3 crystal showing good quantitative agreement with the expected structure.

High sensitivity pressure and temperature quantum sensing in pentacene-doped p-terphenyl single crystals

Thu, 15 Jan 2026 00:00:00 +0000

Quantum sensors’ responsiveness to their physical environment enables detection of variables such as temperature (T), pressure (P), and strain. We present a molecular platform for PT sensing using para-terphenyl crystals doped with pentacene (PDP), leveraging optically detected magnetic resonance (ODMR) of photoexcited triplet electron spins. We observe maximal frequency variations of df/dP=1.8 MHz/bar from 0-8 bar and df/dT=247 kHz/K from 79–330 K, over 1200 times and threefold greater, respectively, than those seen with nitrogen-vacancy centers in diamond and > 85-fold greater pressure sensitivity over the previous record. Density functional theory calculations indicate picometer-level PT-induced molecular orbital shifts are measurable via ODMR. PDP offers additional advantages including high sensor doping levels, narrow ODMR linewidths, high contrast, and low-cost single crystal growth. Overall, this work reports low-cost, optically-interrogated PT sensors and lays the foundation...

Mesh-like structure integrated core-shell-shell nanocomposites for enhanced stability and performance in carbon capture

Wed, 14 Jan 2026 00:00:00 +0000

Carbon capture is essential for mitigating climate change, yet most sorbents struggle to combine high capacity with chemical stability. Here we report core-shell-shell (CSS) nanocomposites that integrate adsorption efficiency with exceptional robustness. The design couples a metal-organic framework (MOF) core, which enriches local CO2 concentration, with a polyamine shell that is reorganized into a porous, ordered network through entanglement with an outer covalent organic framework (COF) shell. This hierarchical architecture enables dual amine functionalization via sequential “click” and Schiff-base reactions, achieving a CO2 uptake of 3.4 mmol g−1 at 1 bar. The COF outer layer also acts as a protective barrier, suppressing humidity interference and doubling cycling stability under simulated flue gas. Remarkably, the nanocomposites maintain structural integrity after one week in strongly acidic (3 M HNO3) or basic (NaOH, pH=14) environments, underscoring their chemical resilience....

Unveiling the role of halide mixing in the crystallization kinetics and charge transfer mechanisms of wide-bandgap organic–inorganic halide perovskites

Tue, 13 Jan 2026 00:00:00 +0000

Understanding the crystallization kinetics of Br–I mixed-halide WBG perovskite films, and their correlation to the crystallographic structure and charge transfer dynamics, is critical for advancing WBG perovskite devices. Despite many efforts to increase the photovoltaic performances of wide-bandgap (WBG, with a Br content above 20%) perovskite solar cells based on bromine–iodine (Br–I) mixed-halide perovskites, understanding the crystallization kinetics of WBG perovskite films, as well as the role of Br mixing in the crystallization kinetics, is still lacking. Furthermore, an overlooked aspect is the correlation of the halide compositions, crystallization kinetics, crystallographic structure, and charge transfer dynamics. Here, we unveil that Br–I mixed-halide WBG perovskite films undergo two intrinsically different crystallization kinetic processes. One is the intermediate solvent-complex phase-assisted growth (I-rich), and the other is top-to-bottom downward growth (Br-rich)....

An AI-accelerated pathway for reproducible and stable halide perovskites

Tue, 13 Jan 2026 00:00:00 +0000

Halide perovskites (HPs) have remarkable optoelectronic properties, and in the last decade their photovoltaic power conversion efficiency and light-emitting diode efficiency have skyrocketed. Despite the surge in research on these burgeoning materials, two key challenges in the field remain: material irreproducibility and instability. Their behavior is especially dynamic in response to environmental stressors, due to complex interactions with the perovskite crystal lattice. In this review, we survey the latest achievements in HP materials research accomplished with the assistance of artificial intelligence (AI), through the implementation of automated experimentation and machine learning (ML) data analysis. Automated synthesis and characterization tackle problems with material irreproducibility by systematically controlling parameters with very high precision, creating massive datasets, and allowing methodical comparisons from which unbiased conclusions can be drawn. AI can reveal...

Ultraselective sequestration of Li+ and Mg2+ from brines via a reusable polyoxoniobate-based ion sponge

Mon, 12 Jan 2026 00:00:00 +0000

Lithium (Li) and magnesium (Mg) are designated as critical mineral materials (CMM) due to their essential roles in clean energy technologies. However, extracting high-purity Li⁺ from brine remains a formidable challenge owing to the presence of Mg²⁺, a physicochemical similar ion that often exists in excess. Here, we introduce a polyoxoniobate-based "Mg-PONb sponge" that enables ultraselective and rapid Li⁺/Mg²⁺ separation across an exceptionally broad range of Mg/Li ratios (0.02 to 200.63). This framework achieves >99.9% Mg²⁺ removal with negligible Li⁺ loss in under 1 min, yielding Li⁺/Mg²⁺ selectivity values exceeding 5000. The sponge demonstrates excellent recyclability, maintaining >99% Mg²⁺ rejection and Li⁺ permeability across five regeneration cycles without structural degradation. Mechanistic investigations reveal that selective Mg²⁺ capture originates...

Resolving SPARC–HSA binding kinetics with an ultrasensitive photonic sensor based on bound states in the continuum

Wed, 7 Jan 2026 00:00:00 +0000

Secreted protein acidic and rich in cysteine (SPARC) is critical in cell-matrix interactions and tissue remodeling. It influences tumor progression through its affinity for human serum albumin (HSA) - the most abundant plasma protein, which also plays a crucial role in drug delivery. Strong molecular binding leads to a dissociation constant K_D in the nanomolar range. Thus, determining K_D requires detecting sub-nanomolar concentrations with ultrasensitive methods. This may be crucial for elucidating the nature of SPARC-HSA binding, as their interaction remains a subject of debate. Capturing these interactions accurately requires a platform capable of resolving rapid binding kinetics at extremely low analyte concentrations. In this work, we report on a microfluidics-integrated photonic nanostructure that supports bound states in the continuum (BICs) and is optimized for studying the fast kinetics of high-affinity protein-protein interactions. The unprecedented...

Modification of Ni-20Cr corrosion dealloying behavior in molten fluorides via cold work induced plastic deformation

Tue, 23 Dec 2025 00:00:00 +0000

The corrosion dealloying behavior of cold-worked (CW) Ni20Cr alloy (wt%) was studied in molten LiF-NaF-KF (or FLiNaK) salts at 600 °C, equal to a homologous temperature (TH) of 0.52. Alloys were cold-rolled to achieve reductions of thickness of 10%, 30%, and 50% introducing plastic deformation and a high density of dislocations. Potentiostatic holds (Eapplied) were applied in two different electrode potential regimes. At 1.75VK+/K$${\text{V}}_{{\text{K}}^{+}/{\text{K}}}$$, Cr dealloying to Cr(II) and Cr(III) is predominant, while at 1.90 VK+/K$${\text{V}}_{{\text{K}}^{+}/{\text{K}}}$$, both Ni and Cr are oxidized in molten FLiNaK at 600 °C. In these potential regimes, dealloyed Ni20Cr displayed bicontinuous porosity within the grain interior and at grain boundaries, driven by the high driving force for Cr dissolution and sustained by defect mediated outward solid state diffusion of Cr in parallel with surface diffusion of Ni. The bicontinuous porous structure developed was observed...

Tailoring the Intermediate Phase to Control Formation of γ‑CsPbI3 Films

Mon, 22 Dec 2025 00:00:00 +0000

Controlling the crystallization pathway of inorganic CsPbI3 perovskite is essential for achieving high efficiency and stability in optoelectronic devices. Here, we report a solvent-engineering strategy that combines an antisolvent process with vacuum treatment (AVT) to modulate evaporation dynamics of the precursor, guiding the formation of highly oriented (CH3)2NH2PbI3 (DMAPbI3) and Cs4PbI6 intermediate phases. Synchrotron and in situ analyses revealed correlations between intermediate orientation and γ-CsPbI3 crystallinity. This directional crystallization pathway promotes vertical alignment and grain enlargement in γ-CsPbI3 films, resulting in fewer voids, lower defect densities, and reduced tensile strain. Photovoltaic devices based on AVT-processed films achieved a power conversion efficiency of 18.47% with a fill factor of 83.14% and retained 101.9% of their initial efficiency after 526 h without encapsulation. This study first reports that the quality of DMAPbI3 and Cs4PbI6...

Lewis Acid‐Activated Charge Trapping in Dielectric Polymers for Superior High‐Temperature Electrostatic Energy Storage

Wed, 17 Dec 2025 00:00:00 +0000

Dielectric polymer capacitors are essential for electrostatic energy storage but suffer from charge transport-induced energy losses, particularly at elevated temperatures where thermally activated charge carriers exacerbate conduction. Conventional mitigation strategies rely on introducing heterogeneous interfaces to create charge traps, complicating scalable film fabrication. A homogeneous molecular trapping mechanism would circumvent these complexities, yet remains underexplored. Herein, a charge trapping strategy is devised by modifying the lowest occupied molecular orbitals of dielectric polymers through Lewis acid-base adduct formation. The use of tris(pentafluorophenyl)boron (BCF) as a Lewis acidic molecular additive introduces deeper charge traps in commercial polyetherimide (PEI) while retaining homogeneity. With only 0.5 wt.% loading, the PEI-BCF film exhibits greatly improved breakdown strength, achieving an ultrahigh discharged energy density of 7.3 J cm^-3...

In Situ Study of Resistive Switching in a Nitride‐Based Memristive Device

Tue, 16 Dec 2025 00:00:00 +0000

Abstract Resistive switching (RS) devices with ultra‐low‐voltage threshold and reliable switching repeatability exhibits great potential applications in energy‐efficient data storage and neuromorphic computing. Understanding switching mechanisms at nanoscale is critical to design RS devices with improved performance. In this work, a lamella memristive device using focused ion beam (FIB) method based on the metal/TiO x /TiN/Si structure device is fabricated. In situ transmission electron microscopy (TEM) and current–voltage ( I–V ) characteristic demonstrate that the lamella device shows a volatile RS behavior with a threshold switching at ≈ ± 0.4 V. In situ scanning transmission electron microscopy (STEM) experiments with electron energy loss spectroscopy (EELS) reveal that the charge carriers such as oxygen vacancies migrate under positive/negative DC bias and modulate Schottky barriers at the top and bottom metal/semiconductor interfaces. The RS mechanism of the lamella...

Ambient mechanosynthesis of flexible two-dimensional covalent organic frameworks

Tue, 16 Dec 2025 00:00:00 +0000

We present the first ambient mechanosynthesis of 16 flexible covalent organic frameworks (COFs) within an hour. Notably, one representative COF exhibited a high iodine uptake capacity of ∼4.3 g g −1 from aqueous solutions and 5.97 g g −1 from vapor. Flexible two-dimensional covalent organic frameworks (2D COFs) constructed from nonplanar building blocks represent an emerging paradigm in COF design. Nevertheless, the prevailing solvothermal synthesis suffers from low time efficiency, environmental unfriendliness, and cumbersome protocols. Here, we address these challenges by developing the first ambient mechanosynthesis of a diverse library of flexible 2D COFs. Sixteen distinct triazine-cored Schiff-base COFs, including five as-yet-unreported ones, were rapidly synthesized via ball milling using 2,4,6-tris(4-aminophenoxy)-1,3,5-triazine (TPT-NH 2 ) and 2,4,6-tris(4-formylphenoxy)-1,3,5-triazine (TPT-CHO) as building blocks. Notably, the representative COF, MC-flexible-COF-1,...

Origin of enhanced performance when Mn-rich rocksalt cathodes transform to δ -DRX

Tue, 16 Dec 2025 00:00:00 +0000

Most Mn-rich cathodes are known to undergo phase transformation into structures resembling spinel-like ordering upon electrochemical cycling. Recently, the irreversible transformation of Ti-containing Mn-rich disordered rock-salt cathodes into a phase — named δ — with nanoscale spinel-like domains has been shown to increase energy density, capacity retention, and rate capability. However, the nature of the boundaries between domains and their relationship with composition and electrochemistry are not well understood. In this work, we discuss how the transformation into the multi-domain structure results in eight variants of Spinel domains, which is crucial for explaining the nanoscale domain formation in the δ -phase. We study the energetics of crystallographically unique boundaries and the possibility of Li-percolation across them with a fine-tuned CHGNet machine learning interatomic potential. Energetics of 16 d vacancies reveal a strong affinity to segregate to the boundaries,...

Digital quantum simulation of cavity quantum electrodynamics: insights from superconducting and trapped ion quantum testbeds

Tue, 16 Dec 2025 00:00:00 +0000

We explore the potential for hybrid development of quantum hardware where currently available quantum computers simulate open cavity quantum electrodynamical (CQED) systems for applications in optical quantum communication, simulation and computing. Our simulations make use of a recent quantum algorithm that maps the dynamics of a singly excited open Tavis–Cummings model containing N atoms coupled to a lossy cavity. We report the results of executing this algorithm on two noisy intermediate-scale quantum computers: a superconducting processor and a trapped ion processor, to simulate the population dynamics of an open CQED system featuring N = 3 atoms. By applying technology-specific transpilation and error mitigation techniques, we minimize the impact of gate errors, noise, and decoherence in each hardware platform, obtaining results which agree closely with the exact solution of the system. These results can be used as a recipe for efficient and platform-specific quantum simulation...

Revealing Coexisting Cu0–Cu+ Sites in Cu3N Nanoensembles for Selective CC Coupling of CO2 Under Low Overpotential

Tue, 16 Dec 2025 00:00:00 +0000

To address a long-existing debate on what copper species are responsible for efficient CC coupling, especially ethanol formation, in electrochemical CO₂ reduction reaction, herein, a comprehensive study using Cu₃N nanocubes with a uniform size and shape, alongside a single crystalline phase is reported. The Cu₃N nanoensemble electrode has a remarkable Faradaic efficiency (FE) of 64% for ethanol production at a relatively low potential of -0.6 V versus reversible hydrogen electrode. Through in-operando X-ray absorption spectroscopy study, a dynamic phase evolution that directly correlates with changes in FE across varying applied potentials is observed. Notably, the nanoensemble with a composition of ≈71% Cu⁺ and 29% Cu⁰ is identified as being selective for ethanol formation at the low overpotential. Conversely, a predominantly metallic Cu phase formed at potentials more negative than -0.6 V favors the hydrogen evolution reaction....

Stabilization of magnetic bubbles in [Ni/Co]n multilayers on an oxygen-reconstructed Nb(110) surface via an ultra-thin Cu interlayer

Thu, 11 Dec 2025 00:00:00 +0000

Magnetic thin films hosting topological spin textures, such as magnetic skyrmions, hold high potential for breakthroughs in the field of spintronics, due to good scalability and energy efficiency. Novel computational architectures such as memory-in-logic devices rely on material platforms able to host those topological spin textures. Furthermore, recently proposed designs of novel quantum information technologies are based on heterostructures where topological spin textures are in direct proximity to a superconducting layer. Here, we demonstrate the stabilization of out-of-plane magnetic bubbles in highly ordered [Ni/Co]n multilayers on a Nb(110) single crystal. This is achieved without the need for the removal of the well-known Nb(110)-oxide surface reconstruction, due to the introduction of an ultra-thin Cu interlayer in between the Nb substrate and the magnetic multilayer. The Cu interlayer generates a well-ordered hexagonal surface, which is key for the epitaxial growth of...

Probing and Tuning Strain‐Localized Exciton Emission in 2D Material Bubbles at Room Temperature

Thu, 11 Dec 2025 00:00:00 +0000

In monolayer transition metal dichalcogenides bubbles-nanoscale deformations typically exhibiting a dome-like shape-Excitons are confined by the strain effect, which exhibits extraordinary emission properties, such as single photon generation, enhanced light emission, and spectrally tunable excitonic states. While the strain profiles of these bubbles are extensively studied, this work provides an approach 1) to directly visualize the associated exciton properties in bubbles formed in WSe₂ monolayer, revealing an intrinsic emission wavelength shift of ≈40 nm, and 2) actively modify local strain, enabling further exciton emission tuning over a range of 50 nm. These are achieved by emission mapping and nanoindentation using a dielectric near-field probe, which enables the detection of local emission spectra and emission lifetimes within individual bubbles. Statistical analysis of 67 bubbles uncovers an emission wavelength distribution centered around 780 nm. Furthermore,...

Improving noisy free-energy measurements by adding more noise

Tue, 9 Dec 2025 00:00:00 +0000

Estimating free-energy differences using nonequilibrium work relations, such as the Jarzynski equality, is hindered by poor convergence when work fluctuations are large. For systems governed by overdamped Langevin dynamics, we propose the counterintuitive approach of adding noise in order to increase the precision of such calculations. By introducing additional stochastic fluctuations to the system and rescaling its potential energy accordingly, we leave the thermodynamics of the system unchanged while increasing its relaxation rate. For a given time-dependent protocol this modification reduces the dissipated reduced work, leading to more accurate free-energy estimates. The method is designed to be used in experiment, and we illustrate its operation using computer simulations applied to two model systems. However, the regime of applicability of this strategy is likely limited, because it requires control of the system's potential energy in a way that is feasible in only a few...

Type IV Pili‐Associated Secretion of a Biofilm Matrix Protein From Clostridium perfringens That Forms Intermolecular Isopeptide Bonds

Fri, 5 Dec 2025 00:00:00 +0000

Clostridium perfringens is a gram-positive, anaerobic, spore-forming bacterial pathogen of humans and animals. C. perfringens also produces type IV pili (T4P) and has two complete sets of T4P-associated genes, one of which has been shown to produce surface pili needed for cell adherence. One hypothesis about the second set of T4P genes is that they comprise a type II secretion system (TTSS) like those found in gram-negative bacteria, but for gram-positive bacteria, the TTSS would aid transit across the thick peptidoglycan (PG) layer. The secretome of mutants lacking type IV pilins was examined, and a single protein, BsaC (CPE0517), was identified as being dependent on pilin PilA3 for secretion. The bsaC gene is in an operon with genes encoding a SipW signal peptidase and two putative biofilm matrix proteins, BsaA and BsaB, both of which have remote homology to Bacillus subtilis biofilm protein TasA. Since BsaA forms long oligomers that are secreted, we analyzed BsaA monomer interactions...

Polypeptoids as promising EUV photoresists: a study of total electron yield and outgassing under EUV exposure

Tue, 2 Dec 2025 00:00:00 +0000

As technology nodes shrink, EUV photoresists are essential for high-resolution nanopatterning. Incident photons as well as electrons generated during EUV exposure can cause both intended and unintended chemical reactions. Understanding these processes is critical for improving resist performance. This study investigates how resist components, particularly Photo Acid Generators (PAGs) and photo decomposable quenchers (PDQ), influence photon- and electron-induced chemistry. It also aims to develop a high-throughput characterization method for efficient screening of novel materials. A high-throughput system combining Total Electron Yield (TEY) and Residual Gas Analysis (RGA) was developed. TEY measures electron generation and capture, while RGA monitors chemical transformations via outgassing. The method was first applied to model resists and later adapted for a large-scale polypeptoid library. TEY and outgassing analysis revealed that PAGs and quenchers strongly influence electron...

Time-dependent characterization of total electron yield and outgassing in model EUV resist materials

Tue, 2 Dec 2025 00:00:00 +0000

As technology nodes shrink, EUV photoresists are critical for high-resolution nanopatterning. However, slow electrons (below 20 eV) generated during EUV exposure can cause electron blur and defect formation through unintended chemical reactions. Understanding the behavior of these electrons is crucial for improving resist performance. This work aims to study how different resist materials, particularly photoacid generators (PAGs) and quenchers, influence electron-induced chemistry under EUV exposure. Additionally, the goal is to develop high-throughput methods to screen hundreds of samples efficiently. Simultaneous total electron yield (TEY) and residual gas analysis (RGA) were used to investigate electron behavior in various polymers and model resists during EUV exposure. TEY measured electron generation and capture, while outgassing experiments explored molecular bond scission. The methods are designed for high-throughput analysis, allowing rapid sample evaluation. TEY measurements...

Multi-angle Precession Electron Diffraction (MAPED): A Versatile Approach to 4D-STEM Precession

Tue, 2 Dec 2025 00:00:00 +0000

Precession of a converged beam during acquisition of a 4D-STEM dataset improves strain, orientation, and phase mapping accuracy by averaging over continuous angles of illumination. Precession experiments usually rely on integrated systems, where automatic alignments lead to fast, high-quality results. The dependence of these experiments on specific hardware and software is evident even when switching to nonintegrated detectors on a precession tool, as experimental set-up becomes challenging and time-consuming. Here, we introduce multi-angle precession electron diffraction (MAPED): a method to perform electron diffraction by collecting sequential 4D-STEM scans at different incident beam tilts. The multiple diffraction datasets are averaged together postacquisition, resulting in a single dataset that minimizes the impact of the curvature and orientation of the Ewald sphere relative to the crystal under study. Our results demonstrate that even four additional tilts improved measurement...

Mapping structures and dynamics with frequency-correlated diffusion exchange

Tue, 25 Nov 2025 00:00:00 +0000

Understanding molecular motion in diffusion-driven complex environments is critical for designing sustainable materials and improving chemical processes. Here, we introduce a multidimensional nuclear magnetic resonance (NMR) method that captures how molecular populations exchange across different dynamic regimes. By extending the modulated gradient spin-echo technique to include frequency-frequency correlations, our approach reveals diffusion pathways that are otherwise obscured in heterogeneous systems. Implemented on a unilateral NMR magnet, the method eliminates gradient pulsing constraints and accesses dynamics in the kilohertz regime. We apply this technique to swelling and acid-catalyzed deconstruction of cross-linked and linear polymers to observe how structural heterogeneity evolves over time. By linking molecular motion to topology and chemical state, we extract physical metrics such as fractal surface dimensionality and reaction wavefront velocity, properties inaccessible...

Advancing microelectronics through nanoscale science: A perspective on needs and opportunities from the nanoscale science research centers

Fri, 21 Nov 2025 00:00:00 +0000

Microelectronics are the cornerstone of the modern world, enhancing our daily lives by providing services such as communications and datacenters. These resources are accessible thanks to the continual pursuit of a deeper understanding of the chemical and physical phenomena underlying the materials synthesis approaches and fabrication processes used to create microelectronic components and subsequently the components' responses to electrical, optical, and other stimuli that are utilized within microelectronic systems. Today, further development of microelectronics requires multidisciplinary expertise across scientific disciplines and fields of study—synthesis, materials characterization, nanoscale fabrication, and performance characterization—with focus placed on comprehending the nanoscale forms and features of microelectronic components. The Nanoscale Science Research Centers (NSRCs) are Department of Energy, Office of Science user facilities that support the international scientific...