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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 307 records · Page 17
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Photoconversion in Disordered Semiconductors: Spatial, Spectral, and Temporal Insights through Nonlinear Microscopy (Final Technical Report)

Conversion of solar photons to useable energy requires two processes to occur successfully in a light-harvesting material: 1) the initial photoexcited state must efficiently produce excited states that are free to move, and 2) those states must be transported to a new location where they can do useful work before any potential is lost as heat. The core focus of this project examined the spatial and energetic dynamics of these two primary events of photoconversion in solution-processed semiconducting materials. The electronic properties of these systems are complex and strongly influenced by the cumulative interaction of local morphology and composition, along with defects, interfaces, and trap sites. It is therefore important to interrogate these systems at the local level, where structural and compositional heterogeneity can be precisely correlated to variation in functionality. Utilizing ultrafast laser spectroscopy coupled together with optical microscopy, this project examined how excited states and free charges spatially and energetically evolve on length scales between 10 nanometers and 10 microns and on timescales from 50 femtoseconds to 1 nanosecond. Insights gained from measurements made on these characteristic length and time scales provided new insight into how macroscopic functionality in disordered photovoltaic materials emerges from the interplay of nanoscale and mesoscale interactions.

14 SOLAR ENERGY↗
DOE OSTI2026

Mesoscale atomic engineering in a crystal lattice

Controlling individual atoms using lasers, ion traps and scanning probe tips has transformed our understanding of matter and enabled breakthroughs in quantum science. Extending this control into three-dimensional (3D) solids and across mesoscopic scales, however, remains a foundational challenge. Electron irradiation in electron microscopes is known to induce atomic displacements, and atomic manipulation has been proposed and demonstrated. Yet repeated and deterministic control has remained elusive. Here, in this study, we demonstrate deterministic atomic engineering in a 3D crystal, creating ordered arrangements of more than 40,000 user-defined defects within minutes across a 150 nm × 100 nm × 13 nm volume. By steering individual Cr atoms in the magnetic semiconductor CrSBr into selected interstitial sites using an electron beam directed with sub-20-pm-scale accuracy, we create vacancy–interstitial complexes. The resulting impurity array forms a mesoscale crystal embedded within the host lattice, a new form of engineered artificial matter that remains stable at room temperature and outside the microscope. By tracking Cr atom displacements, we identify conditions under which the defect structures are predictable. Our calculations suggest that these defects form correlated impurity states with intra-defect optical transitions and inter-defect kinetic and Coulomb interactions. This establishes a generalizable platform for atomic defect engineering at mesoscopic, and potentially macroscopic, scales, opening opportunities for scalable quantum technologies, including deterministic colour-centre placement, quantum simulation of many-body lattice models and atomic-scale manufacturing.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Signatures of Multiband Effects in High-Harmonic Generation in Monolayer MoS 2

High-harmonic generation (HHG) in solids has been touted as a way to probe ultrafast dynamics and crystal symmetries in condensed matter systems. Here, we investigate the polarization properties of high-order harmonics generated in monolayer MoS 2 , as a function of crystal orientation relative to the mid-infrared laser field polarization. At several different laser wavelengths we experimentally observe a prominent angular shift of the parallel-polarized odd harmonics for energies above approximately 3.5 eV, and our calculations indicate that this shift originates in subtle differences in the recombination dipole strengths involving multiple conduction bands. Further, this observation is material specific and is in addition to the angular dependence imposed by the dynamical symmetry properties of the crystal interacting with the laser field, and may pave the way for probing the vectorial character of multiband recombination dipoles.

2-dimensional systems↗
DOE OSTI2023

Combined Coherent Manipulation and Single-Shot Measurement of an Electron Spin in a Quantum Dot (Final Technical Report)

Semiconductor quantum dots (QDs) are promising candidates to act as single-photon sources and/or quantum bits in future optical quantum information applications. Their excellent optical properties such as high brightness, single-photon purity, and narrow linewidth have potential utility in many areas. One challenge is to control the energy levels of the QD without using a magnetic field. The AC Stark effect offers the opportunity to do this. We have demonstrated record-large AC Stark shifts of the energy states of a single charged QD. We showed that the shifts can be applied in a spin-selective manner by controlling the polarization of the laser producing the AC Stark effect. In order to characterize the effect, we developed a novel spectral filtering scheme to discriminate the high-power AC Stark laser from the QD fluorescence. We also developed a compact, low-cost, homemade polarimeter to help control the polarization of the AC Stark laser, which enabled the spin selectivity of the AC Stark effect. With the practical capabilities thus developed, we learned that the spin-selective AC Stark effect causes electron spin pumping, which in turn causes nuclear spin pumping via the hyperfine interaction. The nuclear spin pumping causes a mean field Zeeman interaction between the nuclear spin ensemble and the electron trapped in the QD, resulting in the so-called Overhauser shift. The magnitude of the Overhauser shift and the measured linewidth of the QD’s optical transitions enabled characterization of the mean nuclear spin polarization and fluctuations. The potentially rapid (ns-scale) control of the QD energy levels and nuclear spin polarization will enable measurements of electron and nuclear spin polarization in the absence of any real magnetic field, which is a completely unique capability. The ability to rapidly apply a spin-selective AC Stark effect in the presence of a weak real magnetic field will allow control of the polarization selection rules of the transitions, enabling all single-qubit operations on the electron spin, i.e., initialization, coherent manipulation, and quantum non-demolition measurement.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Self-driving thin film laboratory: autonomous epitaxial atomic-layer synthesis via real-time computer vision analysis of electron diffraction

Emerging materials science platforms with the ability to make autonomous decisions on the fly are fundamentally changing the outlook and protocols for materials optimization and discovery. Because AI-driven self-navigating schemes can effectively reduce the total number of iterations needed to arrive at the "answer" (i.e. the best stochiometric composition for a desired physical property, optimum materials processing parameters, etc.) by significant margins, they have the potential to revolutionize materials and chemical manufacturing processes at large in research laboratory settings as well as in industrial plants. Here, we demonstrate a successful implementation of real-time closed-loop autonomous navigation of a multi-dimensional materials synthesis parameter space for fabricating phase-pure epitaxial films of a metastable phase of a functional oxide in a combinatorial pulsed laser deposition chamber. Sequential epitaxial growth iterations in search of the optimized recipe to stabilize the desired crystal phase were performed using frame-by-frame quantitative computer vision analysis of reflection high-energy electron diffraction (RHEED) images of the unit-cell level film being deposited. The autonomous scheme regularly resulted in > 30-fold reduction in the number of required experiments compared to a comprehensive mapping of the parameter space. The real-time workflow developed here can be readily extended to a variety of thin film synthesis platforms opening the door for self-driving atomic-level materials design as well as autonomous optimization of semiconductor manufacturing.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Radiative pumping of exciton-polaritons in 2D hybrid perovskites

In addition to their attractive technological applications in photovoltaics and light emitters, the perovskite family of semiconductors has recently emerged as an excellent excitonic material for fundamental studies. Specifically, the 2D hybrid organic-inorganic perovskite (HOIP) offers the added advantage of room temperature investigations owing to their large exciton binding energy. In this work, we strongly couple excitons in 2D HOIP crystals to planar microcavity photons sustaining exciton-polaritons under ambient conditions resulting in a Rabi splitting of 290 meV. Dark excitons directly pump the polariton branch along its dispersion in resonance with the Stokes shifted emission state (radiative pumping), creating a high density of polaritons at higher in-plane momentum ( k || ). We further probe the nonlinear polariton dispersion dynamics at varying input laser fluence, which indicates efficient polariton-polariton scattering and decay to k || = 0 from higher k || . The observation of Stokes shift-assisted energy exchange of dark states with lower polaritons coupled with evidence of efficient polariton-polariton scattering makes 2D HOIPs an attractive platform to study exciton-polariton many-body physics and Bose-Einstein like condensation (BEC) at room temperature.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Stabilization of N6 and N8 anionic units and 2D polynitrogen layers in high-pressure scandium polynitrides

Abstract Nitrogen catenation under high pressure leads to the formation of polynitrogen compounds with potentially unique properties. The exploration of the entire spectrum of poly- and oligo-nitrogen moieties is still in its earliest stages. Here, we report on four novel scandium nitrides, Sc 2 N 6 , Sc 2 N 8 , ScN 5, and Sc 4 N 3 , synthesized by direct reaction between yttrium and nitrogen at 78-125 GPa and 2500 K in laser-heated diamond anvil cells. High-pressure synchrotron single-crystal X-ray diffraction reveals that in the crystal structures of the nitrogen-rich Sc 2 N 6 , Sc 2 N 8, and ScN 5 phases nitrogen is catenated forming previously unknown N 6 6 − and N 8 6 − units and$${\!\,}_{\infty }{\!\,}^{2}({{{{{\rm{N}}}}}}_{5}^{3-})$$ ∞ 2 ( N 5 3 − ) anionic corrugated 2D-polynitrogen layers consisting of fused N 12 rings. Density functional theory calculations, confirming the dynamical stability of the synthesized compounds, show that Sc 2 N 6 and Sc 2 N 8 possess an anion-driven metallicity, while ScN 5 is an indirect semiconductor. Sc 2 N 6 , Sc 2 N 8 , and ScN 5 solids are promising high-energy-density materials with calculated volumetric energy density, detonation velocity, and detonation pressure higher than those of TNT.

Science & Technology - Other Topics↗
DOE OSTI2024

Near-Infrared Optical Gain of Colloidal Quantum Wells via Intraband Transitions

Tunable, unipolar, near-infrared intraband optical gain is demonstrated in semiconductor colloidal quantum wells, expanding the form and optical range for potential infrared applications. Atomically flat colloidal quantum wells of cadmium selenide display photoinduced absorption features in the near-infrared assigned to intraband (alternatively intersubband) transitions from the first to second electron subbands of the quantum wells. Under ultraviolet optical excitation, these same transitions from the first to second electron subbands are shown to exhibit stimulated emission, resulting in optical gain covering the near-infrared spectral region. The modal gain, bandwidth, and lifetime of this intraband gain are manipulated by using excitation energy, fluence, temperature, and surface chemistry. Unlike previous demonstrations of intraband optical gain in epitaxial quantum wells (e.g., quantum cascade lasers), the colloidal quantum wells are undoped. As a result, nearly thresholdless gain is in principle possible and limited in practice by the measurement of small optical losses of the samples in the near-infrared. Furthermore, the observations may be understood as a modified "quantum fountain" employing the valence band, a strategy that may be applied to many other materials.

Optical gain↗
DOE OSTI2023

Suppressing phase disproportionation in quasi-2D perovskite light-emitting diodes

Electroluminescence efficiencies and stabilities of quasi-two-dimensional halide perovskites are restricted by the formation of multiple-quantum-well structures with broad and uncontrollable phase distributions. Here, we report a ligand design strategy to substantially suppress diffusion-limited phase disproportionation, thereby enabling better phase control. We demonstrate that extending the π-conjugation length and increasing the cross-sectional area of the ligand enables perovskite thin films with dramatically suppressed ion transport, narrowed phase distributions, reduced defect densities, and enhanced radiative recombination efficiencies. Consequently, we achieved efficient and stable deep-red light-emitting diodes with a peak external quantum efficiency of 26.3% (average 22.9% among 70 devices and cross-checked) and a half-life of ~220 and 2.8 h under a constant current density of 0.1 and 12 mA/cm 2 , respectively. Our devices also exhibit wide wavelength tunability and improved spectral and phase stability compared with existing perovskite light-emitting diodes. These discoveries provide critical insights into the molecular design and crystallization kinetics of low-dimensional perovskite semiconductors for light-emitting devices.

14 SOLAR ENERGY↗
DOE OSTI2025

Influence of Alkyne Precursor Structure on Carbon Nanotube Chiral Distribution: Data-Dense Analysis Across Multiple Catalyst Types

Carbon nanotubes (CNTs) are a desirable material in the field of optoelectronics and semiconductors due to electronic properties (e.g., bandgap) that are dependent upon their chirality, defined by their diameter and lattice angle. Unfortunately, industrial-scale syntheses have yet to realize growth of a single desired chirality and instead rely on postsynthetic separation techniques to refine a chiral mixture, which increases process complexity and cost. Here, we studied the influence of precursor structure on chiral distribution, using a series of terminal alkyne precursors (acetylene, methylacetylene, vinylacetylene, 1-butyne, two enantiomers of 3-butyn-2-ol and a racemic mixture thereof) to grow CNTs across five transition-metal catalysts (Fe, FeMo, and three proportions of CoMo). Multiwavelength Raman spectroscopy on 5,145 spots (5 catalysts, 7 precursors, 3 lasers, and 49 distinct substrate locations on each) determined that acetylene grew the smallest diameter CNTs, while vinylacetylene produced fewer subnanometer CNTs. Though precursor structure did not dictate a uniform chiral shift, it was shown to broaden or narrow chiral distribution, while catalyst structure played a dominant role. In conclusion, this is consistent with metal-precursor binding occurring through unsaturated bonds in the hydrocarbons via the alkyne polymerization mechanism.

Carbon nanotubes↗
DOE OSTI2021

Near-field imaging of plasmonic nanopatch antennas with integrated semiconductor quantum dots

Plasmonic nanopatch antennas that incorporate dielectric gaps hundreds of picometers to several nanometers thick have drawn increasing attention over the past decade because they confine electromagnetic fields to grossly sub-diffraction-limited volumes. Substantial control over the optical properties of excitons and color centers confined within these plasmonic cavities has already been demonstrated with far-field optical spectroscopies, but near-field optical spectroscopies are essential for an improved understanding of the plasmon–emitter interaction at the nanoscale. Here, we characterize the intensity and phase-resolved plasmonic response of isolated nanopatch antennas by cathodoluminescence microscopy. Furthermore, we explore the distinction between optical and electron beam spectroscopies of coupled plasmon–exciton heterostructures to identify constraints and opportunities for future nanoscale characterization and control of hybrid nanophotonic structures. While we observe substantial Purcell enhancement in time-resolved photoluminescence spectroscopies, negligible Purcell enhancement is observed in cathodoluminescence spectroscopies of hybrid nanophotonic structures. The substantial differences in measured Purcell enhancement for electron beam and laser excitation can be understood as a result of the different selection rules for these complementary experiments. Overall, these results provide a fundamentally new understanding of near-field plasmon–exciton interactions in nanopatch antennas, which is essential for myriad emerging quantum photonic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Controllable superconducting to semiconducting phase transition in topological superconductor 2M-WS 2

The investigation of exotic properties in two-dimensional (2D) topological superconductors has garnered increasing attention in condensed matter physics, particularly for applications in topological qubits. Despite this interest, a reliable way of fabricating topological Josephson junctions (JJs) utilizing topological superconductors has yet to be demonstrated. Controllable structural phase transition presents a unique approach to achieving topological JJs in atomically thin 2D topological superconductors. In this work, we report the pioneering demonstration of a structural phase transition from the superconducting to the semiconducting phase in the 2D topological superconductor 2M-WS 2 . We reveal that the metastable 2M phase of WS 2 remains stable in ambient conditions but transitions to the 2H phase when subjected to temperatures above 150°C. We further locally induced the 2H phase within 2M-WS 2 nanolayers using laser irradiation. Notably, the 2H phase region exhibits a hexagonal shape, and scanning tunneling microscopy (STM) uncovers an atomically sharp crystal structural transition between the 2H and 2M phase regions. Moreover, the 2M to 2H phase transition can be induced at the nanometer scale by a 200 keV electron beam. The electrical transport measurements further confirmed the superconductivity of the pristine 2M-WS 2 and the semiconducting behavior of the laser-irradiated 2M-WS 2 . Furthermore, our results establish a novel approach for controllable topological phase change in 2D topological superconductors, significantly impacting the development of atomically scaled planar topological JJs.

2D materials↗
DOE OSTI2026

Incident excitation effects on ZnO-based photoluminescence

Zinc oxide (ZnO) is an attractive semiconductor material owing to a wide band gap, large exciton binding energy, and strong luminescent properties. Two distinct spectral regions are present in the room temperature emission of this material: a narrow line in the UV/near-UV region that is excitonic in nature and a lower energy broad emission band centered in the green/yellow region. Commercially available ZnO particles containing excess Zn and oxygen vacancy defect sites (referred to as ZnO:Zn) were excited using three light sources to study different radiative recombination regimes of the as-received powders. First, a UV LED at a center wavelength of 365 nm provided low irradiance (0.02–0.08 W/cm 2 ) with varying pulse widths (continuous operation to 16 ns). Second, the third harmonic of a pulsed Nd:YAG laser provided high irradiances (∼10 4 –10 6 W/cm 2 ) at a fixed nominal pulse width of 5 ns. Finally, a continuous polychromatic synchrotron X-ray source was also used to excite the ZnO:Zn powders. During UV LED excitation, a low number of carriers are created in the material, leading to an anticipated linear relationship between luminescence and irradiance. This held true for defect luminescence; however, there was an observed enhancement of exciton emission relative to the UV LED intensity as the pulse width was decreased, independent of irradiance. During UV laser excitation, the number of carriers was significantly increased, raising the material into a bimolecular recombination regime, which produced exciton emission much stronger than visible band emission. Finally, spectra obtained during synchrotron X-ray excitation, whose continuous illumination and higher penetration depth yielded higher emission from defect sites relative to exciton emission. A redshift in the exciton emission was also observed as excitation pulse width and sample temperature were varied, and is discussed.

Westphal, Eric Robert [Sandia National Lab. (SNL-N↗
DOE OSTI2023

Broadband Photoconductive Sampling in Gallium Phosphide

Abstract Direct measurements of the electric field of light enable new observations of light–matter interactions. In the near‐infrared and visible spectral ranges, this typically relies on techniques that exploit nonlinearities in gases or solids, which limits their sensitivity. Here, a method for the detection of broadband near‐infrared fields spanning more than one octave from 110 to 220 THz based on linear absorption in a semiconductor is demonstrated. This technique, which avoids complex vacuum setups and works under ambient conditions, employs linear photoconductive sampling (LPS) in gallium phosphide. Simulations reveal that the response function of LPS is concerned with the intensity envelope of the gate field, in contrast to electro‐optic sampling, relaxing the stringent temporal requirements on the gate pulse.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Billion-pixel x-ray camera (BiPC-X)

The continuing improvement in quantum efficiency (above 90% for single visible photons), reduction in noise (below 1 electron per pixel), and shrink in pixel pitch (less than 1 μm) enable billion-pixel x-ray cameras (BiPC-X) based on commercial complementary metal–oxide–semiconductor (CMOS) imaging sensors. We describe BiPC-X designs and prototype construction based on flexible tiling of commercial CMOS imaging sensors with millions of pixels. Device models are given for direct detection of low energy x rays (<10 keV) and indirect detection of higher energies using scintillators. Modified Birks’s law is proposed for light yield non-proportionality in scintillators as a function of x-ray energy. Single x-ray sensitivity and spatial resolution have been validated experimentally using a laboratory x-ray source and the Argonne Advanced Photon Source. Possible applications include wide field-of-view or large x-ray aperture measurements in high-temperature plasmas, the state-of-the-art synchrotron, x-ray free electron laser, and pulsed power facilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Through the Lens of a Momentum Microscope: Viewing Light-Induced Quantum Phenomena in 2D Materials

Van der Waals (vdW) materials at their 2D limit are diverse, flexible, and unique laboratories to study fundamental quantum phenomena and their future applications. Their novel properties rely on their pronounced Coulomb interactions, variety of crystal symmetries and spin-physics, and the ease of incorporation of different vdW materials to form sophisticated heterostructures. In particular, the excited state properties of many 2D semiconductors and semi-metals are relevant for their technological applications, particularly those that can be induced by light. In this paper, the recent advances made in studying out-of-equilibrium, light-induced, phenomena in these materials are reviewed using powerful, surface-sensitive, time-resolved photoemission-based techniques, with a particular emphasis on the emerging multi-dimensional photoemission spectroscopy technique of time-resolved momentum microscopy. The advances this technique has enabled in studying the nature and dynamics of occupied excited states in these materials are discussed. Then, the future research directions opened by these scientific and instrumental advancements are projected for studying the physics of 2D materials and the opportunities to engineer their band-structure and band-topology by laser fields.

2D materials↗
DOE OSTI2022

Novel self-assembled two-dimensional layered oxide structure incorporated with Au nanoinclusions towards multifunctionalities

Two-dimensional (2D) layered oxides have recently attracted wide attention owing to the strong coupling among charges, spins, lattice, and strain, which allows great flexibility and opportunities in structure designs as well as multifunctionality exploration. In parallel, plasmonic hybrid nanostructures exhibit exotic localized surface plasmon resonance (LSPR) providing a broad range of applications in nanophotonic devices and sensors. A hybrid material platform combining the unique multifunctional 2D layered oxides and plasmonic nanostructures brings optical tuning into the new level. Here, a novel self-assembled Bi 2 MoO 6 (BMO) 2D layered oxide incorporated with plasmonic Au nanoinclusions has been demonstrated via one-step pulsed laser deposition (PLD) technique. Comprehensive microstructural characterizations, including scanning transmission electron microscopy (STEM), differential phase contrast imaging (DPC), and STEM tomography, have demonstrated the high epitaxial quality and particle-in-matrix morphology of the BMO-Au nanocomposite film. DPC-STEM imaging clarifies the magnetic domain structures of BMO matrix. Three different BMO structures including layered supercell (LSC) and superlattices have been revealed which is attributed to the variable strain states throughout the BMO-Au film. Owing to the combination of plasmonic Au and layered structure of BMO, the nanocomposite film exhibits a typical LSPR in visible wavelength region and strong anisotropy in terms of its optical and ferromagnetic properties. This study opens a new avenue for developing novel 2D layered complex oxides incorporated with plasmonic metal or semiconductor phases showing great potential for applications in multifunctional nanoelectronics devices.

36 MATERIALS SCIENCE↗