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DOE OSTI2025

Rapid Synthesis of Carbon‐Supported Ru‐RuO₂ Heterostructures for Efficient Electrochemical Water Splitting

Abstract Development of high‐performance electrocatalysts for water splitting is crucial for a sustainable hydrogen economy. In this study, rapid heating of ruthenium(III) acetylacetonate by magnetic induction heating (MIH) leads to the one‐step production of Ru‐RuO₂/C nanocomposites composed of closely integrated Ru and RuO₂ nanoparticles. The formation of Mott‐Schottky heterojunctions significantly enhances charge transfer across the Ru‐RuO 2 interface leading to remarkable electrocatalytic activities toward both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in 1 m KOH. Among the series, the sample prepares at 300 A for 10 s exhibits the best performance, with an overpotential of only −31 mV for HER and +240 mV for OER to reach the current density of 10 mA cm⁻ 2 . Additionally, the catalyst demonstrates excellent durability, with minimal impacts of electrolyte salinity. With the sample as the bifunctional catalysts for overall water splitting, an ultralow cell voltage of 1.43 V is needed to reach 10 mA cm⁻ 2 , 160 mV lower than that with a commercial 20% Pt/C and RuO₂/C mixture. These results highlight the significant potential of MIH in the ultrafast synthesis of high‐performance catalysts for electrochemical water splitting and sustainable hydrogen production from seawater.

Pan, Dingjie [Department of Chemistry and Biochemi↗

DOE OSTI2025

Next-generation electronics by co-design with chalcogenide materials

As Moore’s law approaches its limits, chalcogenides offer a promising route to next-generation computing and sensing, thanks to their topological, magnetoelectric, excitonic, and spintronic properties. Yet the same traits that make them appealing, e.g., exotic properties at monolayer thickness, clean van der Waals interfaces, and strong many-body effects, also heighten sensitivity to fabrication, hindering translation into scalable devices. Progress is further constrained by fragmented knowledge across synthesis, processing, and integration, and by the lack of systematic links between fabrication parameters and performance metrics. This Perspective examines key obstacles in controlling chalcogenide heterostructures and stresses the need for an integrated co-design framework, uniting materials growth, processing, and device architecture to accelerate practical technologies.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Resistive Switching in SrFeO2.5/Nb:SrTiO3 Heterostructures with Growth-Controlled Film Orientation

Resistive switching, a behavior found in many oxide materials, has the potential to enable emerging computer hardware technologies and architectures. We present resistive switching devices fabricated from epitaxial brownmillerite SrFeO2.5 films with two distinct film orientations, wherein facile oxygen ion diffusion planes are aligned parallel (in-plane) and perpendicular (out-of-plane) with the electrodes. SrFeO2.5 films were grown on (001) oriented Nb:SrTiO3 to enable high-quality interfaces and future integration with Si CMOS technologies. Post-growth vacuum annealing and growth pressure were used to control film orientations, as confirmed by transmission electron microscopy and x-ray diffraction measurements. Films grown with diffusion planes oriented in-plane had oxygen-rich, perovskite-like nanodomains spread throughout the film, and fabricated devices exhibited worse switching consistency and more stochasticity. In contrast, films grown with diffusion planes oriented out-of-plane had a more uniform oxygen-rich perovskite interfacial layer above the bottom electrode, and devices built from this film orientation showed significant statistical improvements in switching voltages and cycling consistency.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

Magnetic Proximity Effects in Iron Germanium Telluride/Platinum Heterostructures

Van der Waals (vdW) magnetic materials have attracted considerable attention for use in spintronic devices such as those controlled by spin–orbit torque (SOT). Such SOT-driven devices are typically fabricated by bringing a vdW magnet in proximity to a spin–charge conversion layer to achieve current-driven magnetization switching. Here, we show that such structures fabricated with iron germanium telluride (FGT) and platinum can exhibit emergent magnetic properties, which we attribute to magnetic proximity effects at the FGT/Pt interface. These changes manifest as increased perpendicular magnetic anisotropy and the emergence of additional magnetization reversal steps as probed by magneto-transport, with the most significant changes appearing in thinner flakes. The behavior was found to be robust and consistently appeared in samples made with crystals from different vendors. In conclusion, our results demonstrate the potential for engineering vdW spintronic systems through magnetic proximity effects.

2D magnet↗

DOE OSTI2025

Programmable Cryogenic Memory in a Ge/GeSi Heterostructure

Programmable memory components that operate optimally at cryogenic temperatures are essential for cryogenic computing architectures that seek to implement computing-in-memory. In this work, we demonstrate highly programmable memory in a Ge/GeSi heterostructure field-effect transistor (HFET). To operate, the HFET is gated to introduce positive carriers within the Ge quantum well, creating a high-conductance state. We show that this device can be set to a low-conductance state by sweeping a negative bias on the device drain, and reset it to its high-conductance state by sweeping a more positive bias on the device gate, thereby creating memory. We then determine that the device can be programmed within a 103 range of conductances using either the SET or the RESET operation. We propose that memory is achieved through charge trapping as carriers tunnel out of the quantum well, and that altering the density and spatial distribution of carriers modulates the device conductance. This mechanism exhibits endurance over 1000 cycles at temperatures ≤ 25 K, suggesting that the carrier traps are located at the oxide-semiconductor interface. As a first demonstration of programmable conductance in a Ge/GeSi HFET, this work highlights the potential of group-IV HFETs to perform as analog cryogenic memory components.

cryogenic memory↗

DOE OSTI2026

Performance of Heterostructural TaC/AlGaN Schottky Diodes Based on First Principles Electronic Structure Properties

Advances in ultra-wide bandgap materials, such as high Al-content AlxGa1-xN (AlGaN), are essential for next generation power electronics, but the requirement for lattice matched substrates is currently a significant obstacle. Recently, conductive TaC has emerged as a promising virtual substrate for AlGaN heteroepitaxy, with wurtzite (0001) AlxGa1-xN lattice-matched to rocksalt (111) TaC at x ~ 0.5. Thus, understanding and controlling the electronic properties of the TaC/AlGaN interface is key for developing technological applications based on TaC/AlGaN devices. Using density functional theory and electronic structure calculations, we here investigate TaC/Al0.5Ga0.5N interfaces, where we include explicit alloy models in the slab calculations. We predict the Schottky barrier height and the electric field discontinuity resulting from interface charges. Considering all possible combinations of (Ta, C) substrate termination, (Al/Ga, N) nucleation, and (Al/Ga, N) polarity, we construct a chemical potential phase diagram to identify the stable interfaces that can be accessed through variation of the synthesis conditions. The predicted interface electronic properties are implemented in device performance simulations to demonstrate a practical design for a strain-free, high-efficiency TaC/AlGaN Schottky diode with a low barrier height and without interface charges, underscoring the potential of TaC as a substrate for ultra-wide bandgap devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

Buffer-layer effect on the ferromagnetism of manganite heterojunctions

Identifying and understanding interfacial magnetic structures of transition-metal oxides are of great importance not only for fundamental physics but also for potential device applications. Among them, manganite and ruthenate heterostructures have attracted considerable interest due to their intriguing interfacial properties induced by complex magnetic interactions. Here, we report the observation of dramatic buffer-layer dependence of ferromagnetism in ultrathin (L⁢a 2/3 ⁢C⁢a 1/3 )⁢Mn⁢O 3 (LCMO)-based heterostructures. Though all trilayers are nonmetallic, the SrRu⁢O 3 -buffered LCMO trilayer exhibits enhanced ferromagnetism with the Curie temperature (𝑇 C ∼ 198K) much higher than for CaRu⁢O 3 (𝑇 C ∼ 99K)- and SrTi⁢O 3 (𝑇 C ∼ 42K)-buffered counterparts, as well as the monolithic LCMO films with similar thickness. Combining atomically resolved scanning transmission electron microscopy imaging with electron energy loss spectroscopy mapping, we reveal that asymmetric interfaces exist in the SrRu⁢O 3 buffered trilayer, with one exhibiting 1 unit-cell Sr diffusion into LCMO, which is responsible for the 𝑇 C enhancement. In contrast, charge transfer, which has been proposed previously as a possible mechanism, is excluded in this study. In conclusion, our results may pave a promising road toward effective atomic control of interfacial magnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Antiferromagnetic V 2 ⁢O 3 based exchange coupling

Vanadium sesquioxide (V 2 ⁢O 3 ) is a strongly correlated electronic material that famously undergoes a triple coupled first-order transition where it transitions from a paramagnetic metal with a rhombohedral structure at high temperature to an antiferromagnetic insulator with a monoclinic structure. While several studies have used one of both electronic and structural transitions to control the properties of a heterostructure, evidence of magnetic coupling has notoriously yet to be found. In this paper, we report on a robust magnetic coupling between the antiferromagnetic (AFM) V 2 ⁢O 3 and ferromagnetic (FM) Permalloy (Py) layers that results in a significant exchange bias and strain-induced coercivity enhancement. We provide a temperature and angle-dependent study of magnetic properties, which clearly indicates exchange bias at the AFM/FM interface that appears at the onset of the metal-insulator transition. The magnitude of the exchange bias is strongest when the field is applied along the [001] V 2 ⁢O 3 crystallographic orientation which corresponds to an AFM spin configuration on the [110] surface. Here, this opens the door to designing and implementing novel functionalities in transition metal oxide-based computing using the connection between magnetism and the metal-insulator transition.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

Electronic origin of reorganization energy in interfacial electron transfer

Electron transfer (ET) reactions underpin energy conversion and chemical transformations in both biological and a biological systems. The efficiency of any ET process relies on achieving a desired ET rate within an optimal driving force range. Marcus theory provides a microscopic framework for understanding the activation free energy—and therefore the rate—of ET in terms of a key parameter: the reorganization energy. For electrified solid–liquid interfaces, it has long been conventionally understood that only factors in the electrolyte phase are responsible for determining the reorganization energy and that the electronic density of states (DOS) of the electrode only serves to dictate the number of thermally accessible channels for ET. Here we show instead that the electrode DOS plays a central role in governing the reorganization energy, far outweighing its conventionally assumed role. Using atomically layered heterostructures, we tune the DOS of graphene and measure outer-sphere ET kinetics. We find the ensuing variation in ET rate arises from strong modulation in a reorganization energy associated with image potential localization in the electrode. Here we redefine the traditional paradigm of heterogeneous ET kinetics, revealing a deeper role of the electrode electronic structure in interfacial reactivity.

Electrochemistry↗

DOE OSTI2024

Unraveling the origin of antiferromagnetic coupling at YIG/permalloy interface

We investigate the structural and electronic origin of antiferromagnetic (AFM) coupling in the yttrium iron garnet (YIG) and permalloy (Ni 80 ⁢Fe 20 , Py) bilayer system at the atomic level. Ferromagnetic resonance (FMR) spectra reveal unique hybrid modes in samples prepared with surface ion milling, indicative of antiferromagnetic exchange coupling at the YIG/Py interface. Using atomic resolution scanning transmission electron microscopy (STEM), we found that AFM coupling appears at the YIG/Py interface of the tetrahedral YIG surface formed with ion milling. Here, the STEM measurements suggest that the interfacial AFM coupling is predominantly driven by an oxygen-mediated superexchange coupling mechanism, which is confirmed by the density-functional theory (DFT) calculations to be energetically favorable. Thus, the combined experimental and theoretical results reveal the critical role of interfacial atomic structure in determining the type of magnetic coupling in a YIG/ferromagnet heterostructure, and prove that the interfacial structure can be experimentally tuned by surface ion milling.

36 MATERIALS SCIENCE↗

NASA NTRS2012

Terahertz Radiation Heterodyne Detector Using Two-Dimensional Electron Gas in a GaN Heterostructure

High-resolution submillimeter/terahertz spectroscopy is important for studying atmospheric and interstellar molecular gaseous species. It typically uses heterodyne receivers where an unknown (weak) signal is mixed with a strong signal from the local oscillator (LO) operating at a slightly different frequency. The non-linear mixer devices for this frequency range are unique and are not off-the-shelf commercial products. Three types of THz mixers are commonly used: Schottky diode, superconducting hot-electron bolometer (HEB), and superconductor-insulation-superconductor (SIS) junction. A HEB mixer based on the two-dimensional electron gas (2DEG) formed at the interface of two slightly dissimilar semiconductors was developed. This mixer can operate at temperatures between 100 and 300 K, and thus can be used with just passive radiative cooling available even on small spacecraft.

Karasik, Boris S.↗

DOE OSTI2025

Porous CeO 2 /CuO Heterostructure for Efficient Hydrogen Evolution Reaction in an Acidic Medium

A composite electrocatalyst CeO 2 /CuO is fabricated for the hydrogen evolution reaction (HER) via a simple, facile, one‐step hydrothermal method, using F‐127 as a template and structure directing agent. The prepared composite CeO 2 /CuO shows top‐notch HER activities with a small overpotential of 98 mV at 10 mA cm −2 and just 160 mV overpotential to attain a current density of 50 mA cm −2 with good stability for 20 h in an acidic medium. The enhanced catalytic activities of CeO 2 /CuO nanocomposite are attributed to their synergetic interface interaction, which lead to improved conductivity, reactive sites, and oxygen vacancies in their lattices. This study aims to advance the development of earth‐abundant transition metal oxides–based electrocatalysts as economical, durable, and efficient HER electrocatalysts to replace noble metal–based materials in the future.

Chemistry↗

DOE OSTI2025

Mechanistic Insight into Tunable Spin Relaxation in Two-Dimensional Type-II Ligand-Perovskite Heterostructures

Two-dimensional (2D) metal-halide perovskites with spin-dependent optical properties hold great promise for spintronic and quantum applications. However, their spin lifetimes, especially for n = 1 2D perovskites, are typically limited to subpicosecond time scales due to rapid spin relaxation driven by strong spin−orbit coupling (SOC), electron−hole exchange interactions, and phonon-mediated scattering. Here, we demonstrate that type-II ligand-perovskite heterostructures overcome these constraints by reducing electron−hole wave function overlap and exciton binding energy. Compared to the type-I 2D perovskite (PEA) 2 PbI 4 with a spin lifetime of 0.29 ps at room temperature, our engineered type-II systems achieve substantially extended spin lifetimes, ∼6.37 ps for (4Tm) 2 PbI 4 and ∼18.47 ps for (4TCNm) 2 PbI 4 . In both materials, spatial charge separation across the perovskite−ligand interface mitigates the Bir−Aronov− Pikus (BAP) mechanism. Temperature- and fluence-dependent measurements reveal Elliott−Yafet (EY)-dominated spin relaxation in (4Tm) 2 PbI 4 , consistent with the observation of coherent phonon oscillation, whereas (4TCNm) 2 PbI 4 exhibits D’yakonov−Perel (DP)-dominated spin relaxation, with weaker phonon coupling further suppressing the EY relaxation, enabling spin lifetimes up to ∼126.81 ps at 5 K. Our findings establish a structural design framework for tailoring spin dynamics in 2D perovskites, offering a promising strategy to engineering spin and optoelectronic properties via rational ligand engineering.

Excitons↗

NASA NTRS2004

Electron-Spin Filters Based on the Rashba Effect

Semiconductor electron-spin filters of a proposed type would be based on the Rashba effect, which is described briefly below. Electron-spin filters more precisely, sources of spin-polarized electron currents have been sought for research on, and development of, the emerging technological discipline of spintronics (spin-based electronics). There have been a number of successful demonstrations of injection of spin-polarized electrons from diluted magnetic semiconductors and from ferromagnetic metals into nonmagnetic semiconductors. In contrast, a device according to the proposal would be made from nonmagnetic semiconductor materials and would function without an applied magnetic field. The Rashba effect, named after one of its discoverers, is an energy splitting, of what would otherwise be degenerate quantum states, caused by a spin-orbit interaction in conjunction with a structural-inversion asymmetry in the presence of interfacial electric fields in a semiconductor heterostructure. The magnitude of the energy split is proportional to the electron wave number. The present proposal evolved from recent theoretical studies that suggested the possibility of devices in which electron energy states would be split by the Rashba effect and spin-polarized currents would be extracted by resonant quantum-mechanical tunneling. Accordingly, a device according to the proposal would be denoted an asymmetric resonant interband tunneling diode [a-RITD]. An a-RITD could be implemented in a variety of forms, the form favored in the proposal being a double-barrier heterostructure containing an asymmetric quantum well. It is envisioned that a-RITDs would be designed and fabricated in the InAs/GaSb/AlSb material system for several reasons: Heterostructures in this material system are strong candidates for pronounced Rashba spin splitting because InAs and GaSb exhibit large spin-orbit interactions and because both InAs and GaSb would be available for the construction of highly asymmetric quantum wells. This mate-rial system affords a variety of energy-band alignments that can be exploited to obtain resonant tunneling and other desired effects. The no-common-atom InAs/GaSb and InAs/AlSb interfaces would present opportunities for engineering interface potentials for optimizing Rashba spin splitting.

Ting, David Z.-Y.↗

DOE OSTI2025

Nanoscale Decoupling of Carrier-Phonon Transport in Carbon Nanotube-Halide Perovskite Heterostructures

In conventional semiconductors, electrical and thermal conductivity are typically coupled, posing a challenge in optimizing both simultaneously. Overcoming this inherent trade-off enables strategies for advancing electronic applications. Herein, a strategy is demonstrated to decouple electrical and thermal conductivity trade-off by creating heterostructures of highly conductive single-walled carbon nanotubes (SWCNTs) coated with low conductivity hybrid perovskites. Coating SWCNTs with methylammonium lead iodide perovskite results in an enhancement in electrical conductivity (408-1266 S cm-1) due to p-type doping followed by a threefold decrease of the in-plane thermal conductivity (3.3-1 W m-1 K-1), compared to pristine SWCNTs. Molecular dynamics simulations uncover phonon boundary scattering at the SWCNT/perovskite interface as well as localization of methylammonium-related and softening of the Pb-I-related phonon modes in methylammonium lead iodide perovskite decreasing the thermal conductivity.

14 SOLAR ENERGY↗

DOE OSTI2026

Ultrafast carrier dynamics in multiple quantum well p–i–n photodiodes

Quantum well (QW) structures are widely used in lasers, semiconductor optical amplifiers, and modulators, enabling their monolithic integration on the same substrate. As optoelectronic systems evolve to meet the growing bandwidth demands in the terahertz regime, a deep understanding of ultrafast carrier dynamics in QW structures becomes essential. We introduce a comprehensive model to analyze the ultrafast dynamics of interband photo-excited carriers in QW p–i–n structures and to calculate their frequency response. This model characterizes the entire photocarrier transport process, including carrier escape from QWs and movement across heterojunction interfaces. Additionally, we outline theoretical methods for calculating carrier escape times from both QWs and heterojunction interfaces. Using a GaAs/AlGaAs QW p–i–n structure as a case study, we discuss the effects of carrier escape times from QWs and heterojunction interfaces, as well as carrier transit time through the intrinsic region, on the frequency response of QW p–i–n structures.

Electronic band structure↗

DOE OSTI2026

Ultrafast Terahertz Field Control of the Emergent Magnetic and Electronic Interactions at Oxide Interfaces

Ultrafast electric-field control of emergent electronic and magnetic states at oxide interfaces offers exciting prospects for the development of the next generation of energy-efficient devices. Here, it is demonstrated that the electronic structure and emergent ferromagnetic interfacial state in epitaxial LaNiO3/CaMnO3 superlattices can be effectively controlled using intense, single-cycle THz electric-field pulses. A suite of advanced X-ray spectroscopic techniques is employed to measure a detailed magneto-optical profile and the thickness of the ferromagnetic interfacial layer. Then, a combination of time-resolved and temperature-dependent optical measurements is used to disentangle several correlated electronic and magnetic processes driven by ultrafast, high-field THz pulses. Sub-picosecond non-equilibrium Joule heating of the electronic system is observed, ultrafast demagnetization of the ferromagnetic interfacial layer, and slower dynamics indicative of a change in the magnetic state of the superlattice due to the transfer of spin-angular momentum to the lattice. These findings suggest a promising avenue for the efficient control of 2D ferromagnetic states at oxide interfaces using ultrafast electric-field pulses.

X-ray spectroscopy and scattering↗

NASA NTRS2005

High Quality GaAs Growth by MBE on Si Using GeSi Buffers and Prospects for Space Photovoltaics

III-V solar cells on Si substrates are of interest for space photovoltaics since this would combine high performance space cells with a strong, lightweight and inexpensive substrate. However, the primary obstacles blocking III-V/Si cells from achieving high performance to date have been fundamental materials incompatabilities, namely the 4% lattice mismatch between GaAs and Si, and the large mismatch in thermal expansion coefficient. In this paper, we report on the molecular beam epitaxial (MBE) growth and properties of GaAs layers and single junction GaAs cells on Si wafers which utilize compositionally graded GeSi Intermediate buffers grown by ultra-high vacuum chemical vapor deposition (UHVCVD) to mitigate the large lattice mismatch between GaAs and Si. Ga As cell structures were found to incorporate a threading dislocation density of 0.9-1.5 x 10 (exp 6) per square centimeter, identical to the underlying relaxed Ge cap of the graded buffer, via a combination of transmission electron microscopy, electron beam induced current, and etch pit density measurements. AlGaAs/GaAs double heterostructures wre grown on the GeSi/Si substrates for time-resolved photoluminescence measurements, which revealed a bulk GaAs minority carrier lifetime in excess of 10 ns, the highest lifetime ever reported for GaAs on Si. A series of growth were performed to ass3ss the impact of a GaAs buffer to a thickness of only 0.1 micrometer. Secondary ion mass spectroscopy studies revealed that there is negligible cross diffusion of Ga, As and Ge at he III-V/Ge interface, identical to our earlier findings for GaAs grown on Ge wafers using MBE. This indicates that there is no need for a buffer to "bury" regions of high autodopjing,a nd that either pn or np configuration cells are easily accomodated by these substrates. Preliminary diodes and single junction Al Ga As heteroface cells were grown and fabricated on the Ge/GeSi/Si substrates for the first time. Diodes fabricated on GaAs, Ge and Ge/GeSi/Si substrate show nearly identical I-V characteristics in both forward and reverse bias regions. External quantum efficiencies of AlGaAs/GaAs cell structures grown on Ge/GeSi/Si and Ge substrates demonstrated nearly identical photoresponse, which indicates that high lifetimes, diffusion lengths and efficient minority carrier collection is maintained after complete cell processing.

Carlin, J. A.↗