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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Resolving buried optoelectronic features in metal halide perovskites via modulation spectroscopy studies

As research on both bulk and low dimensional metal halide perovskites (MHPs) continues to grow, the tools necessary to gain insights into their exotic and highly convoluted optoelectronic features must also expand. Electroabsorption (EA) is a modulation spectroscopy technique that is exceptionally valuable at deconvoluting overlapping spectral features as well as discerning between different electronic environments in semiconductors. This review outlines the critical shortcomings of traditional optical spectroscopy in determining essential properties such as the bandgap and exciton binding energy. In this report we provide a brief overview of the working principles of EA, focusing on the differences between bound and unbound charge carriers that result in unique behavior when interacting with an applied electric field. We discuss key studies highlighting the unique characterization available when coupling EA spectroscopy with traditional steady-state optical tools to investigate interesting and complex optical features in MHPs. We conclude that EA is a crucial tool for pushing the boundaries of our understanding of the optoelectronic properties of MHP thin films. When other optical characterization methods fall short in the richness of data provided, EA can bridge the knowledge gap to provide a complete optoelectronic characterization of novel MHPs and deepen the understanding of current structures and compositions as a function of their structural and morphological dimensionality.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2022

Electronic and Spintronic Open-Shell Macromolecules, Quo Vadis ?

Open-shell macromolecules (i.e., polymers containing radical sites either along their backbones or at the pendant sites of repeat units) have attracted significant attention owing to their intriguing chemical and physical (e.g., redox, optoelectronic, and magnetic) properties, and they have been proposed and/or implemented in a wide range of potential applications (e.g., energy storage devices, electronic systems, and spintronic modules). These successes span multiple disciplines that range from advanced macromolecular chemistry through nanoscale structural characterization and on to next-generation solid-state physics and the associated devices. In turn, this has allowed different scientific communities to expand the palette of radical-containing polymers relatively quickly. However, critical gaps remain on many fronts, especially regarding the elucidation of key structure–property–function relationships that govern the underlying electrochemical, optoelectronic, and spin phenomena in these materials systems. Here, we highlight vital developments in the history of open-shell macromolecules to explain the current state of the art in the field. Moreover, we provide a critical review of the successes and bring forward open opportunities that, if solved, could propel this class of materials in a meaningful manner. Finally, we provide an outlook to address where it seems most likely that open-shell macromolecules will go in the coming years. Furthermore, our considered view is that the future of radical-containing polymers is extremely bright and the addition of talented researchers with diverse skills to the field will allow these materials and their end-use devices to have a positive impact on the global science and technology enterprise in a relatively rapid manner.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Pick-and-Place Transfer of Arbitrary-Metal Electrodes for van der Waals Device Fabrication

Van der Waals electrode integration is a promising strategy to create nearly perfect interfaces between metals and 2D materials, with advantages such as eliminating Fermi-level pinning and reducing contact resistance. However, the lack of a simple, generalizable pick-and-place transfer technology has greatly hampered the wide use of this technique. Here, we demonstrate the pick-and-place transfer of prefabricated electrodes from reusable polished hydrogenated diamond substrates without the use of any sacrificial layers due to the inherent low-energy and dangling-bond-free nature of the hydrogenated diamond surface. The technique enables transfer of arbitrary-metal electrodes and an electrode array, as demonstrated by successful transfer of eight different elemental metals with work functions ranging from 4.22 to 5.65 eV. We also demonstrate the electrode array transfer for large-scale device fabrication. The mechanical transfer of metal electrodes from diamond to van der Waals materials creates atomically smooth interfaces with no interstitial impurities or disorder, as observed with cross-section high-resolution transmission electron microscopy and energy-dispersive X-ray spectroscopy. As a demonstration of its device application, we use the diamond transfer technique to create metal contacts to monolayer transition metal dichalcogenide semiconductors with high-work-function Pd, low-work-function Ti, and semimetal Bi to create n- and p-type field-effect transistors with low Schottky barrier heights. We also extend this technology to air-sensitive materials (trilayer 1T’ WTe 2 ) and other applications such as ambipolar transistors, Schottky diodes, and optoelectronics. This highly reliable and reproducible technology paves the way for new device architectures and high-performance devices.

2D materials↗
DOE OSTI2024

Dynamic metal-linker bonds in metal–organic frameworks

Metal-linker bonds serve as the “glue” that binds metal ions to multitopic organic ligands in the porous materials known as metal–organic frameworks (MOFs). Despite ample evidence of bond lability in molecular and polymeric coordination compounds, the metal-linker bonds of MOFs were long assumed to be rigid and static. Given the importance of ligand fields in determining the behaviour of metal species, labile bonding in MOFs would help explain outstanding questions about MOF behaviour, while providing a design tool for controlling dynamic and stimuli-responsive optoelectronic, magnetic, catalytic, and mechanical phenomena. Here, in this work, we present emerging evidence that MOF metal-linker bonds exist in dynamic equilibria between weakly and tightly bond conformations, and that these equilibria respond to guest–host chemistry, drive phase change behavior, and exhibit size-dependence in MOF nanoparticles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Ultrafast Nanoimaging of Carrier Funneling in Composition-Graded Semiconductor Nanowires

Recent advances in bandgap engineering of low-dimensional semiconductors have enabled high-efficiency carrier transport in miniaturized electronic and optoelectronic devices. The physical properties and functionalities of these materials are governed by complex carrier dynamics coupled with multiple transport mechanisms in tailored band structures. Here, we report ultrafast nanoimaging of carrier funneling and recombination in composition-grade CdSxSe1-x nanowires using pump-probe near-field nanoscopy. Leveraging the high resolution of this technique in both space and time, we resolve nanoscale local carrier dynamics along composition-graded nanowires, revealing the local variation of composition-dependent carrier mobilities and lifetimes that significantly differ from their uniform composition counterparts. Furthermore, we demonstrate a length-dependent behavior wherein shorter nanowires exhibit enhanced funneling effects, accelerating carrier transport by up to 33%. Our findings provide direct visualization of nanoscale carrier transport while supporting an effective approach for investigating complex carrier interactions in inhomogeneous semiconductor nanostructures, with implications for optimizing next-generation optoelectronic devices.

Yang, Rundi↗
DOE OSTI2020

Chemical manipulation of hydrogen induced high p-type and n-type conductivity in Ga 2 O 3

Advancement of optoelectronic and high-power devices is tied to the development of wide band gap materials with excellent transport properties. However, bipolar doping (n-type and p-type doping) and realizing high carrier density while maintaining good mobility have been big challenges in wide band gap materials. Here P-type and n-type conductivity was introduced in β-Ga 2 O 3 , an ultra-wide band gap oxide, by controlling hydrogen incorporation in the lattice without further doping. Hydrogen induced a 9-order of magnitude increase of n-type conductivity with donor ionization energy of 20 meV and resistivity of 10 -4 Ω.cm. The conductivity was switched to p-type with acceptor ionization energy of 42 meV by altering hydrogen incorporation in the lattice. Density functional theory calculations were used to examine hydrogen location in the Ga 2 O 3 lattice and identified a new donor type as the source of this remarkable n-type conductivity. Positron annihilation spectroscopy measurements confirm this finding and the interpretation of the experimental results. This work illustrates a new approach that allows a tunable and reversible way of modifying the conductivity of semiconductors and it is expected to have profound implications on semiconductor field. At the same time, it demonstrates for the first time p-type and remarkable n-type conductivity in Ga 2 O 3 which should usher in the development of Ga 2 O 3 devices and advance optoelectronics and high-power devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Reversible Interlayer Sliding and Conductivity Changes in Adaptive Tetrathiafulvalene-Based Covalent Organic Frameworks

Ordered interlayer stacking is intrinsic in two-dimensional covalent organic frameworks (2D COFs) and has strong implications on COF's optoelectronic properties. Reversible interlayer sliding, corresponding to shearing of 2D layers along their basal plane, is an appealing dynamic control of both structures and properties, yet it remains unexplored in the 2D COF field. In this paper, we demonstrate that the reversible interlayer sliding can be realized in an imine-linked tetrathiafulvalene (TTF)-based COF TTF-DMTA. The solvent treatment induces crystalline phase changes between the proposed staircase-like sql net structure and a slightly slipped eclipsed sql net structure. The solvation-induced crystallinity changes correlate well with reversible spectroscopic and electrical conductivity changes as demonstrated in oriented COF thin films. In contrast, no reversible switching is observed in a related TTF-TA COF, which differs from TTF-DMTA in terms of the absence of methoxy groups on the phenylene linkers. This work represents the first 2D COF example of which eclipsed and staircase-like aggregated states are interchangeably accessed via interlayer sliding, an uncharted structural feature that may enable applications such as chemiresistive sensors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Energy-Resolved Femtosecond Hot Electron Dynamics in Single Plasmonic Nanoparticles

Efficient excitation and harvesting of hot carriers from nanoscale metals is central to many emerging photochemical, photovoltaic, and ultrafast optoelectronic applications. Nevertheless, direct experimental evidence of the energy-dependent femtosecond dynamics in ubiquitous tens-of-nanometer gold structures remains elusive, despite the potentially rich interplay between interfacial and internal plasmonic fields, excitation distributions, and scattering processes. To explore the effects of nanoscale structure on these dynamics, we employ simultaneous time-, angle-, and energy-resolved photoemission spectroscopy of single plasmonic nanoparticles. Photoelectron velocity and electric field distributions reveal bulk-like ballistic hot electron transport in different geometries, lacking any signatures of surface effects. Energy-resolved dynamics are measured in the 1–2 eV range and extrapolated to lower energies via Boltzmann theory, providing a detailed view of hot electron lifetimes within nanoscale gold. Here, we find that particles with relevant dimensions as small as 10 nm serve as exemplary platforms for studying intrinsic metal dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Physical Modeling and Design of a Nonvolatile Optically Gated High‐Power Diamond Transistor

In this work, we present the theory and modeling framework of a diamond optically gated junction field‐effect transistor (DOGFET). The device utilizes nitrogen substitutional centers in type‐1b diamond to optically modulate a p‐ boron doped diamond channel. Using sub‐gap lasers with intensities as low as 100 W/cm 2 , electrons are optically excited from substitutional nitrogen sites to the conduction band of the diamond substrate, thus enabling the optical gate to exercise control on modulating the space‐charge region at the junction and therefore the channel conductivity. We show that the device can deliver a current of 7 μA/μm, or equivalently 1750 A/cm 2 , while switching at a frequency greater than 100 kHz, in a form factor of 5 μm 2 . The breakdown voltage is found to be greater than 1850 V, with a breakdown field strength of ~13 MV/cm. Moreover, the device supports nonvolatile operation with a “memory effect” enabling single transistor state retention. The presented simulation framework provides a physically grounded insight into the limits and opportunities of optoelectronic diamond systems.

Engineering - Electronic and electrical engineerin↗
DOE OSTI2025

Monolithic optoelectronic circuit design for on-chip terahertz applications

We demonstrate a monolithic coplanar stripline platform for on-chip terahertz (THz) generation, transmission, and detection, addressing key challenges of mode purity, bandwidth, and referencing. Capacitive coupling of the photoconductive generator switch enforces pure odd-mode propagation, increases THz field strength, and extends the operational frequency range, achieving 0.05–1.4 THz. Our architecture enables fully monolithic fabrication with amorphous silicon switches, in situ field referencing, and galvanic isolation between generation and detection. Finite-element simulations and experiments confirm that suppressing parasitic modes improves signal integrity, providing a robust platform for high-fidelity THz spectroscopy, ultrafast electronics, and nanoscale quantum materials research.

Capacitive coupling↗
DOE OSTI2025

Chemical Compensation Challenges in Processing Antiferroelectric PbZrO 3 Thin Films

The electric field-induced antipolar-to-polar phase transition in antiferroelectric materials is accompanied by large changes in the structural and functional response, making them attractive for many applications ranging from pulsed energy capacitors to high-strain-high (blocking-)force actuators, solid-state heating and cooling systems, and optoelectronic devices. PbZrO 3 , as an end member of the PZT, (x)PbZr 1–x Ti x O 3 , solid solution, has been the subject of many studies. However, processing of perovskite PbZrO 3 is extremely challenging due to phase instabilities induced by Pb loss at the temperatures necessary for perovskite crystallization. Here, we discuss the challenges associated with Pb loss, as well as its compensation through bulk Pb overstoichiometry and interfacial PbO additions, in chemical solution processed, highly oriented PbZrO 3 thin films. For both 042 o - and 001 o -oriented (o-orthorhombic distortion) PbZrO 3 thin films, the crystallization interfaces are the most important contributors to Pb loss and off-stoichiometric outcomes, and no single approach was sufficient to address these challenges. Pb-rich and Pb-deficient nonperovskite phases including ZrO x were only observable through microscopic characterization, and X-ray diffraction alone could not rule out the presence of such secondary phases. “Ideal” macroscopic antiferroelectric polarization-electric field double hysteresis curves were observed despite (at times) the large presence of secondary phases. However, reduced saturation polarization and increased phase transition electric fields were observed concomitantly with the presence of secondary phase(s) and tentatively assigned to the voltage drop across the ZrO x nanocrystals. Based on these results, it is imperative that the presence of secondary phases always be addressed (beyond X-ray diffraction spectra) in order to correctly evaluate the properties of antiferroelectric films.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Regrowth and Selective Area Growth of GaN for Vertical Power Electronics

Gallium Nitride (GaN) has a great potential in high-power and high-frequency applications due to its wide energy gap and good transport property. So far all commercial GaN optoelectronic and electronic devices have planar junctions and heterostructures prepared by epitaxial growth. To take the advantage of the merits of GaN material properties, more sophisticated device configurations such as current-aperture vertical electron transistors (CAVETs), junction field-effect transistors (JFETs), and super-junction (SJ) devices require the ability to form in-plane, lateral junctions by selective area doping (SAD). In this project, we explored a novel approach of realizing SAD through selective-area etching (SAE) followed by selective-area growth (SAG).

36 MATERIALS SCIENCE↗
DOE OSTI2023

Quasiparticle and Optical Properties of Carrier-Doped Monolayer MoTe 2 from First Principles

The intrinsic weak and highly nonlocal dielectric screening of two-dimensional materials is well-known to lead to high sensitivity of their optoelectronic properties to environment. Less studied theoretically is the role of free carriers in those properties. In this report we use ab initio GW and Bethe-Salpeter equation calculations, with a rigorous treatment of dynamical screening and local-field effects, to study the doping dependence of the quasiparticle and optical properties of a monolayer transition-metal dichalcogenide, 2H MoTe 2 . Here we predict a quasiparticle band gap renormalization of several hundreds of meV for experimentally attainable carrier densities and a similarly sizable decrease in the exciton binding energy. This results in an almost constant excitation energy for the lowest-energy exciton resonance with an increasing doping density. Using a newly developed and generally applicable plasmon-pole model and a self-consistent solution of the Bethe-Salpeter equation, we reveal the importance of accurately capturing both dynamical and local-field effects to understand detailed photoluminescence measurements.

2D material↗
DOE OSTI2024

Electrical Control and Transport of Tightly Bound Interlayer Excitons in a MoSe 2 /hBN/MoSe 2 Heterostructure

Controlling interlayer excitons in Van der Waals heterostructures holds promise for exploring Bose-Einstein condensates and developing novel optoelectronic applications, such as excitonic integrated circuits. Despite intensive studies, several key fundamental properties of interlayer excitons, such as their binding energies and interactions with charges, remain not well understood. Here we report the formation of momentum-direct interlayer excitons in a high-quality MoSe 2 /hBN/MoSe 2 heterostructure under an electric field, characterized by bright photoluminescence (PL) emission with high quantum yield and a narrow linewidth of less than 4 meV. These interlayer excitons show electrically tunable emission energy spanning ~1⁢8⁢0 meV through the Stark effect, and exhibit a sizable binding energy of ~8⁢1 meV in the intrinsic regime, along with trion binding energies of a few millielectronvolts. Remarkably, we demonstrate the long-range transport of interlayer excitons with a characteristic diffusion length exceeding 1⁢0 μ⁢m, which can be attributed, in part, to their dipolar repulsive interactions. Further, spatially and polarization-resolved spectroscopic studies reveal rich exciton physics in the system, such as valley polarization, local trapping, and the possible existence of dark interlayer excitons. Furthermore, the formation and transport of tightly bound interlayer excitons with narrow linewidth, coupled with the ability to electrically manipulate their properties, open exciting new avenues for exploring quantum many-body physics, including excitonic condensate and superfluidity, and for developing novel optoelectronic devices, such as exciton and photon routers.

2-dimensional systems↗
DOE OSTI2024

Computational synthesis of a new generation of 2D-based perovskite quantum materials

Perovskite-based optoelectronic devices have emerged as a promising energy source due to their potential for scalable production. This study introduces “perovskene,” a novel class of 2D materials derived from the ABC3-like perovskites, synthesized via a data-driven, high-throughput computational strategy. We harness machine learning and multitarget deep neural networks to systematically investigate the structure–property relations, paving the way for targeted material design and optimization in fields such as renewable energy, electronics, and catalysis. The characterization of over 1500 synthesized structures shows that more than 500 structures are stable, revealing properties such as ultra-low work function and large magnetic moment, underscoring the potential for advanced technological applications.

2D materials↗
DOE OSTI2025

Single-Atom-Resolved Vibrational Spectroscopy of a Dislocation

Dislocations in III-nitride semiconductors impede heat transport, leading to localized overheating, which severely limits the performance and reliability of optoelectronic and power devices. Current research on phonon–dislocation interactions primarily addresses bulk materials, focusing on the average effects at specific dislocation densities. However, phonon resistance from dislocation scattering arises from both short-range core interactions and long-range strain field interactions, which remain largely unexplored. Here, in this study, electron energy-loss spectroscopy is used to investigate a GaN dislocation. Vibrational modes localized on specific core atoms are revealed, reflecting short-range interactions. Additionally, phonon energy shifts driven by strain fields surrounding the dislocation are observed, reflecting long-range interactions. Ab initio calculations support these findings and draw out additional details. This work establishes a paradigm for probing defect-induced phonon scattering at the single-atom level, revealing how dislocations affect phonon behavior through atomic reconstruction and strain engineering, thus offering insights for designing improved material functionalities.

III-nitride semiconductors↗
DOE OSTI2024

Giant optical nonlinearity of Fermi polarons in atomically thin semiconductors

In this study, realizing strong nonlinear optical responses is a long-standing goal of both fundamental and technological importance. Recently, substantial efforts have been focused on exploring excitons in solids to achieve nonlinearities even down to few-photon levels. However, a crucial tradeoff arises as strong light–matter interactions require large oscillator strength and short radiative lifetime of excitons, which limits their nonlinearity. Here we experimentally demonstrate strong nonlinear optical responses with large oscillator strength by exploiting the coupling between excitons and carriers in an atomically thin semiconductor. By controlling the electric field and electrostatic doping of trilayer WSe 2 , we observe the hybridization between intralayer and interlayer excitons and the formation of Fermi polarons. Substantial optical nonlinearity is observed under continuous-wave and pulsed laser excitation, where the Fermi polaron resonance blueshifts by as much as ~10 meV. Intriguingly, we observe a remarkable asymmetry in the optical nonlinearity between electron and hole doping, which is tunable by the applied electric field. We attribute these features to the optically induced valley polarization due to the interactions between excitons and free charges. Our results establish atomically thin heterostructures as a highly versatile platform for engineering nonlinear optical response with applications to classical and quantum optoelectronics.

2d materials↗