Factors that Control the Direction of Excited-State Electron Transfer at Dye-Sensitized Oxide Interfaces
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catalysis (heterogeneous)↗
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CeO[subscript 2] Modulates the Electronic States of a Palladium Onion-Like Carbon Interface into a H
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Ogada, Jimodo J.↗
Data for Stetten et al. (2025), "Biogeochemical controls on iron speciation and cycling across upland to shoreline gradients in freshwater and estuarine coastal soils (Lake Erie and Chesapeake Bay, United States)"
Coastal environments are dynamic interfaces that mediate carbon and nutrient exchanges between terrestrial landscapes and open waters, but it is unclear how biogeochemical reactions, in particular iron (Fe) redox transformations, affect the understanding and prediction of coastal ecosystem functions. This dataset includes measurements from two freshwater sites in the Western and Central basins of Lake Erie (Ohio, United States) and two estuarine sites in the Chesapeake Bay (Maryland, United States); the analytical results were reported by Stetten et al. (2025) in Science of the Total Environment. It was produced as part of the COMPASS-FME project, which seeks to advance a scalable, predictive understanding of the fundamental biogeochemical processes, ecological structure, and ecosystem dynamics that distinguish coastal terrestrial-aquatic interfaces from the purely terrestrial or aquatic systems to which they are coupled. The sites were sampled in November 2022 (CRC), December 2022 (MSM), February 2023 (GCW), and March 2023 (OWC); site codes follow those used by Pennington et al. (2025).The dataset consists of the following soil data:- Solid data (Fe concentration, etc.)- Porewater data (sulfate, sulfide, etc.)- Linear combination fitting results of X-ray absorption near edge structure (XANES) spectra; i.e., quantitative results of the oxidation state of Fe, indicated as a proportion of pure Fe(III) and Fe(II) model compounds- Linear combination fitting results of EXAFS (extended X-ray absorption fine structure) spectra, indicated as proportion of of Fe-model compounds (illite, smectite, etc.)Each data type has a single file in comma-separated value (CSV) format. No special software is required to read it.
54 ENVIRONMENTAL SCIENCES↗
A Charge‐Separated State that Lives for Almost a Second at a Conductive Metal Oxide Interface
Abstract Transparent conductive oxides (TCOs) are widely used commercially available materials for opto‐electronic applications, yet they have received very little attention for dye‐sensitization applications. Now, mesoporous thin films of conductive indium‐doped tin oxide (ITO) nanocrystallites are shown to support long‐lived charge separation with first‐order recombination kinetics ( k =1.5 s −1 ). A layer‐by‐layer technique was utilized to spatially arrange redox and/or chromophoric molecular components on ITO. Spectroelectrochemical measurements demonstrated that upon light absorption, each component provided a free‐energy gradient to direct electron transfer at the conductive oxide interface. The long‐lived nature of the photogenerated charge separated states provide favorable conditions for photocatalytic solar fuel production. Furthermore, the first‐order recombination kinetics are most ideal for the fundamental understanding of interfacial charge separation dynamics.
Sampaio, Renato N.↗
Ion-Depleted Microenvironments During Lithium Deposition Revealed by Operando Freezing Cryogenic Electron Microscopy
Local structures and chemistry at active electrochemical interfaces are critical to determining safety, lifetime, and energy density in lithium metal batteries and other devices, but they are challenging to characterize at the nanoscale. We address this issue by developing operando freezing cryogenic electron microscopy (cryo-EM) to preserve battery interfaces in an active state for subsequent high-resolution characterization. We find that ion-depleted microenvironments form locally in the electrolyte adjacent to the lithium deposition interface in lithium metal batteries and are linked to heterogenous growth morphologies. These depleted environments arise locally even under conditions for which ion depletion is not predicted at steady state; this provides a mechanistic explanation for why dangerous lithium morphologies can still propagate in such systems and lead to thermal runaway. Operando freezing cryo-EM thus provides a method to directly visualize nanoscale heterogeneities that arise locally at electrochemical interfaces and play key roles in device failure.
CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS,E↗
Many-body entanglement in solid-state emitters
The preparation and control of quantum states lie at the heart of quantum information science. Recent advances in solid-state quantum emitters (QEs) and nanophotonics have transformed the landscape of quantum photonic technologies, enabling scalable generation of quantum states of light and matter. A new frontier in solid-state quantum photonics is the engineering of many-body interactions between QEs and photons to achieve robust coherence and controllable many-body entanglement. These entangled states, including photonic graph and cluster states, superradiant emission and emergent quantum phases, are promising for quantum computation, sensing and simulation. However, intrinsic inhomogeneities and decoherence in solid-state platforms pose considerable challenges in realizing such complex entangled states. This Review provides an overview of fundamental many-body interactions and dynamics at the light–matter interfaces of solid-state QEs and discusses recent advances in mitigating decoherence and harnessing robust many-body coherence.
36 MATERIALS SCIENCE↗
Native Mass Spectrometry, Ion Mobility, Electron-Capture Dissociation, and Modeling Provide Structural Information for Gas-Phase Apolipoprotein E Oligomers
Apolipoprotein E (apoE) is an essential protein in lipid and cholesterol metabolism. Although the three common isoforms in humans differ only at two sites, their consequences in Alzheimer’s disease (AD) are dramatically different: only the ε4 allele is a major genetic risk factor for late-onset Alzheimer’s disease. The isoforms exist as a mixture of oligomers, primarily tetramer, at low μM concentrations in a lipid-free environment. This self-association is involved in equilibrium with the lipid-free state, and the oligomerization interface overlaps with the lipid-binding region. Elucidation of apoE wild-type (WT) structures at an oligomeric state, however, has not yet been achieved. To address this need, we used native electrospray ionization and mass spectrometry (native MS) coupled with ion mobility (IM) to examine the monomer and tetramer of the three WT isoforms. Although collision-induced unfolding (CIU) cannot distinguish the WT isoforms, the monomeric mutant (MM) of apoE3 shows higher stability when submitted to CIU than the WT monomer. From ion-mobility measurements, we obtained the collision cross section and built a coarse-grained model for the tetramer. Application of electron-capture dissociation (ECD) to the tetramer causes unfolding starting from the C-terminal domain, in good agreement with solution denaturation data, and provides additional support for the C4 symmetry structure of the tetramer. .
62 RADIOLOGY AND NUCLEAR MEDICINE↗
Understanding In-Situ Structure and Chemistry at Battery Interfaces Through Time-Resolved Cryo-EM
Transmission and scanning transmission electron microscopy are vital tools for characterizing interfacial structure and chemistry at high spatial resolutions but are limited by the fact that many materials are quickly damaged by electron beam irradiation. This is a challenge particularly for materials relevant to energy applications, such as lithium-containing battery materials, organic-inorganic hybrids, and liquid electrolytes. Cryogenic electron microscopy (cryo-EM) offers a partial solution to this issue by stabilizing beam-sensitive solid-solid or solid-liquid interfaces for characterization, but typical cryo-EM sample preparations are ex situ and thus cannot capture interfaces in their electrified state of interest to applications. Here, we present a method to prepare cryo-EM samples of electrified battery interfaces in situ to preserve the time-resolved structures and chemistry that arise under applied current or bias.
batteries↗
Kinetic versus Thermodynamic Stability of LLZO in Contact with Lithium Metal
Li 7 La 3 Zr 2 O 12 (LLZO) garnet-based oxides are a promising class of solid electrolytes used as the separator in all-solid-state batteries (ASSBs). While LLZO is considered to have a wide electrochemical stability window, its intrinsic stability in contact with lithium metal is not sufficiently well understood, and there is still a debate on the key question of whether LLZO does or does not form passivation layers before and during cycling. Utilizing both in situ and operando X-ray photoelectron spectroscopy techniques, in this work we reveal the presence of a kinetic barrier to the reduction of LLZO by Li metal, with the extent of oxygen-deficient interphase (ODI) formation depending sensitively on the energetics of Li metal arriving at the Li vertical bar LLZO interface. Despite the clear presence of a kinetic barrier to reduction, the electrochemical response of the Li vertical bar LLZO interface is unchanged by the presence of the ODI, indicating that ODI formation during electrochemical cycling does not hinder charge transfer across the Li vertical bar LLZO interface. Overall, these results reveal that the reactivity of LLZO with Li metal depends not only on the material properties of the adjoining phases (i.e., surface purity and active contact) and their resulting thermodynamic stability but also on the energy input at the interface and the resulting reaction kinetics. Furthermore, the presence of a kinetic barrier to reduction highlights the additional complexities governing the reactivity of solid-state interfaces in ASSBs and underscores the importance of operando characterization of interfacial stability to design more robust, high-performance protection strategies for solid electrolytes in contact with reactive electrodes.
25 ENERGY STORAGE↗
Unconventional quantum oscillations and evidence of nonparabolic electronic states in quasi-two-dimensional electron system at complex oxide interfaces
The simultaneous occurrence of electric-field controlled superconductivity and spin-orbit interaction makes two-dimensional electron systems (2DES) constructed from perovskite transition metal oxides promising candidates for the next generation of spintronics and quantum computing. It is, however, essential to understand the electronic bands thoroughly and verify the predicted electronic states experimentally in these 2DES to advance technological applications. Here, we present insights into the electronic states of the 2DES at oxide interfaces through comprehensive investigations of Shubnikov–de Haas oscillations in three different systems: EuO/KTaO 3 , LaAlO 3 /SrTiO 3 , and amorphous-LaAlO 3 /KTaO 3 . To accurately resolve these oscillations, we conducted transport measurements in high magnetic fields up to 60 T and low temperatures down to 100 mK. For 2D confined electrons at these interfaces, we observed a progressive increase of oscillations frequency and cyclotron mass with the magnetic field. We interpret these universal and intriguing findings by considering the existence of nontrivial electronic bands, for which the 𝐸−𝑘 dispersion incorporates both linear and parabolic relations. In addition to providing experimental evidence for nonparabolic electronic states in KTaO 3 and SrTiO 3 2DES, the unconventional oscillations presented in this study establish a paradigm for quantum oscillations in 2DES based on perovskite transition metal oxides, where the oscillation frequencies in 1/𝐵 exhibit quadratic dependence on the magnetic field.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Emergent c -axis magnetic helix in manganite-nickelate superlattices
Here, the nature of the magnetic order in (La 2/3 Sr 1/3 MnO 3 ) 9 /(LaNiO 3 ) 3 superlattices is investigated using x-ray resonant magnetic reflectometry. We observe a new -axis magnetic helix state in the (LaNiO 3 ) 3 layers that had never been measured in nickelates, and which mediates the ~130° magnetic coupling between the ferromagnetic (La 2/3 Sr 1/3 MnO 3 ) 9 layers, illustrating the power of x-rays for discovering the magnetic state of complex oxide interfaces. Resonant inelastic x-ray scattering and x-ray absorption spectroscopy show that Ni-O ligand hole states from bulk LaNiO 3 are mostly filled due to interfacial electron transfer from Mn, driving the Ni orbitals closer to an atomic-like 3d 8 configuration. We discuss the constraints imposed by this electronic configuration to the microscopic origin of the observed magnetic structure. The presence of a magnetic helix in (La 2/3 Sr 1/3 MnO 3 ) 9 /(LaNiO 3 ) 3 is crucial for modeling the potential spintronic functionality of this system and may be important for designing emergent magnetism in novel devices in general.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Singularity-EOS: Performance Portable Equations of State and Mixed Cell Closures
We present Singularity-EOS, a new performance-portable library for equations of state and related capabilities. Singularity-EOS provides a large set of analytic equations of state, such as the Gruneisen equation of state, and tabulated equation of state data under a unified interface. It also provides support capabilities around these equations of state, such as Python wrappers, solvers for finding pressure-temperature equilibrium between multiple equations of state, and a unique modifier framework, allowing the user to transform a base equation of state, for example by shifting or scaling the specific internal energy. All capabilities are performance portable, meaning they compile and run on both CPU and GPU for a wide variety of architectures.
97 MATHEMATICS AND COMPUTING↗
Coupled Growth in Hypermonotectics
The overall objective of this project is to obtain a fundamental understanding of the physics controlling solidification processes in immiscible alloy systems. The investigation involves both experimentation and the development of a model describing solidification in monotectic systems. The experimental segment was designed to first demonstrate that it is possible to obtain interface stability and steady state coupled growth in hypermonotectic alloys through microgravity processing. Microgravity results obtained to date have verified this possibility. Future flights will permit experimental determination of the limits of interface stability and the influence of alloy composition and growth rate on microstructure. The objectives of the modeling segment of the investigation include prediction of the limits of interface stability, modeling of convective flow due to residual acceleration, and the influence of surface tension driven flows at the solidification interface. The study of solidification processes in immiscible alloy systems is hindered by the inherent convective flow that occurs on Earth and by the possibility of sedimentation of the higher density immiscible liquid phase. It has been shown that processing using a high thermal gradient and a low growth rate can lead to a stable macroscopically planar growth front even in hypermonotectic alloys. Processing under these growth conditions can avoid constitutional supercooling and prevent the formation of the minor immiscible liquid phase in advance of the solidification front. However, the solute depleted boundary layer that forms in advance of the solidification front is almost always less dense than the liquid away from the solidification front. As a result, convective instability is expected. Ground based testing has indicated that convection is a major problem in these alloy systems and leads to gross compositional variations along the sample and difficulties maintaining interface stability. Sustained low gravity processing conditions are necessary in order to minimize these problems and obtain solidification conditions which approach steady state.
Andrews, J. Barry↗
Highly efficient interface stabilization for ambient-temperature quasi-solid-state sodium metal batteries
Solid-state sodium (Na) batteries (SSSBs) using sulfide-based solid electrolytes (SSEs) hold tremendous promise due to their high theoretical specific capacity, enhanced safety and abundant resources. However, detrimental interfacial issues between SSEs and Na metal present a major challenge to the advancement of sulfide-based SSSBs. To address interfacial issues, we demonstrate an efficient approach by incorporating an ionic liquid electrolyte ((PYR/Na)TFSI) as interlayer to stabilize the Na metal/SSE interface. The presence of the (PYR/Na)TFSI interlayer enables the formation of a stable solid electrolyte interphase (SEI) to prevent the harmful reactions and inhibit Na dendrites. Combination of ab initio molecular dynamics simulations and X-ray photoelectron spectroscopy revealed that this stable SEI is largely composed of reduced products of TFSI -, such as NaF and CF 3 . As a result, the symmetric cells exhibited stable Na plating/striping cycling for 300 h at 0.1 mA cm -2 . In addition, FeS2||Na quasi-solid-state batteries delivered an impressive specific capacity of over 300 mAh g -1 under the current density of 20 mA g -1 at room temperature. Under a higher current density (100 mA g -1 ), such batteries performed with long-term cycling stability and maintained a specific capacity of around 103 mAh g -1 after 330 cycles. This work demonstrates the novel perspective of using an ionic liquid interlayer to address interfacial issues, contributing to the advancement of high-performance SSSBs for the next-generation energy storage systems.
25 ENERGY STORAGE↗
Seamless Staircase Electrical Contact to Semiconducting Graphene Nanoribbons
Electrical contact to low-dimensional (low-D) materials is a key to their electronic applications. Traditional metal contacts to low-D semiconductors typically create gap states that can pin the Fermi level (E F ). Yet, low-D metals possessing a limited density of states at E F can enable gate-tunable work functions and contact barriers. Furthermore, a seamless contact with native bonds at the interface, without localized interfacial states, can serve as an optimal electrode. To realize such a seamless contact, one needs to develop atomically precise heterojunctions from the atom up. In this work, we demonstrate an all-carbon staircase contact to ultranarrow armchair graphene nanoribbons (aGNRs). The coherent heterostructures of width-variable aGNRs, consisting of 7, 14, 21, and up to 56 carbon atoms across the width, are synthesized by a surface-assisted self-assembly process with a single molecular precursor. The aGNRs exhibit characteristic vibrational modes in Raman spectroscopy. A combined scanning tunneling microscopy and density functional theory study reveals the native covalent-bond nature and quasi-metallic contact characteristics of the interfaces. Our electronic measurements of such seamless GNR staircase constitute a promising first step toward making low resistance contacts.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Joining of High Strength Low Ductility AA7055 by Friction Self-piercing Rivet
High strength aluminum (Al) alloy is one of higher specific strength materials for decarbonization in transportation industries. Because of low ductility at room temperature, conventional mechanical fastening such as self-piercing riveting produces cracks at the joint. In this work, we applied friction self-piercing riveting to join Al alloy (AA) 7055. No cracks were observed in the joints because of the improved local ductility of Al alloy by the generated frictional heat during joining step. Numerical modeling of joining process was applied to guide rivet geometry design and rivet material strength. Mechanical integrity of the AA7055 joints was assessed by lap shear tensile and cross-tension testing. Metallurgical characterizations revealed solid-state bonding formed not only between the rivet and surround Al materials, but also upper and lower Al sheets at the joint interface. Both solid-state bonding and mechanical interlocking between the flared rivet and bottom AA7055 sheet were the major joint mechanisms.
Lim, Yong Chae↗
AlGaN/GaN metal–insulator–semiconductor high electron mobility transistors (MISHEMTs) using plasma deposited BN as gate dielectric
AlGaN/GaN metal–insulator–semiconductor high electron mobility transistors (MISHEMTs) were fabricated on Si substrates with a 10 nm boron nitride (BN) layer as a gate dielectric deposited by electron cyclotron resonance microwave plasma chemical vapor deposition. The material characterization of the BN/GaN interface was investigated by X-ray photoelectric spectroscopy (XPS) and UV photoelectron spectroscopy. The BN bandgap from the B1s XPS energy loss is ~5 eV consistent with sp2 bonding. The MISHEMTs exhibit a low off-state current of 1 × 10 –8 mA/mm, a high on/off current ratio of 10 9 , a threshold voltage of –2.76 V, a maximum transconductance of 32 mS/mm at a gate voltage of –2.1 V and a drain voltage of 1 V, a subthreshold swing of 69.1 mV/dec, and an on-resistance of 12.75 Ω·mm. The interface state density (D it ) is estimated to be less than 8.49 × 10 11 cm –2 eV –1 . Gate leakage current mechanisms were investigated by temperature-dependent current–voltage measurements from 300 K to 500 K. The maximum breakdown electric field is no less than 8.4 MV/cm. Poole–Frenkel emission and Fowler–Nordheim tunneling are indicated as the dominant mechanisms of the gate leakage through the BN gate dielectric at low and high electric fields, respectively.
36 MATERIALS SCIENCE↗
Two-dimensional electronic–vibrational sum frequency spectroscopy for interactions of electronic and nuclear motions at interfaces
Significance Electronic–vibrational couplings are pivotal in many photo-induced processes at interfaces and surfaces. Two-dimensional electronic–vibrational sum frequency generation spectroscopy is a unique tool to decipher electronic–vibrational couplings for excited states of molecules at interfaces and surfaces, enabling the correlation of photo-induced electronic–vibrational manifolds with their subsequent time evolution of high-frequency vibrational modes. This technique is especially powerful to monitor ultrafast processes such as charge transfer, energy transfer, proton transfer, and proton-coupled charge transfer at interfaces and surfaces on a real-time basis.
Deng, Gang-Hua↗