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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 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Two-well injector direct-phonon terahertz quantum cascade lasers

We present an experimental study on a terahertz quantum cascade laser (THz QCL) design that combines both two-well injector and direct-phonon scattering schemes, i.e., a so-called two-well injector direct-phonon design. As a result of the two-well injector direct-phonon scheme presented here, the lasers benefit from both a direct phonon scattering scheme for the lower laser level depopulation and a setback for the doping profile that reduces the overlap of the doped region with active laser states. Additionally, our design also has efficient isolation of the active laser levels from excited and continuum states as indicated by negative differential resistance behavior all the way up to room temperature. This scheme serves as a good platform for improving the temperature performance of THz QCLs as indicated by the encouraging temperature performance results of the device with a relatively high doping level of 7.56 × 10 10 cm −2 and T max ∼ 167 K. With the right optimization of the molecular beam epitaxy growth and interface quality, the injection coupling strength, and the doping density and its profile, the device could potentially reach higher temperatures than the latest records reached for the maximum operating temperature (T max ) of THz QCLs.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Application of wideband pulsed high-frequency EPR to molecular quantum spin science

This presentation provides an overview of a range of new applications in the area of molecular quantum spin science that are now possible at the US National High Magnetic Field Laboratory as a result of the development of a wideband, high-power 94 GHz pulsed EPR spectrometer. Here, this instrument allows true Fourier-transform detected experiments spanning a 1 GHz instantaneous bandwidth, akin to what has been possible in NMR for several decades. The presentation will begin by describing experiments on a nitroxide radical using chirped pulses, enabling acquisition of the full spectrum in a single sequence, thus providing a very efficient and convenient means to measure the field orientation dependence of the spin-lattice relaxation time, T 1 . This will be followed by a discussion of a coherent population transfer protocol involving the 2S + 1 = 8 Zeeman levels associated with the spin S = 7/2 Gd 3+ ion, potentially paving the way towards implementation of well-known quantum search algorithms. It will also be shown how the use of chirped pulses provides a route to achieving highly non-thermal spin populations, suggesting novel initialization schemes.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Slope Efficiency and Voltage Reduction at High Current Densities in AlInGaAs Diode Lasers

Here, the slope efficiency and drive voltage of broad area AlInGaAs laser diodes near 865 nm is observed to decrease significantly under quasi-CW pulsed operation at currents well above threshold, in a manner that cannot be explained by thermal effects or carrier leakage over heterojunction barriers. Simulations show that the slope efficiency reduction is explicable by increased free carrier absorption in the waveguide region. Empirical formulas are presented to represent these effects in a closed analytic form suitable for use in simulators for diode-pumped laser systems.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Strong Structural and Electronic Coupling in Metavalent PbS Moiré Superlattices

Moiré superlattices are twisted bilayer materials in which the tunable interlayer quantum confinement offers access to new physics and novel device functionalities. Previously, moiré superlattices were built exclusively using materials with weak van der Waals interactions, and synthesizing moiré superlattices with strong interlayer chemical bonding was considered to be impractical. Here, in this study, using lead sulfide (PbS) as an example, we report a strategy for synthesizing moiré superlattices coupled by strong chemical bonding. We use water-soluble ligands as a removable template to obtain free-standing ultrathin PbS nanosheets and assemble them into direct-contact bilayers with various twist angles. Atomic-resolution imaging shows the moiré periodic structural reconstruction at the superlattice interface due to the strong metavalent coupling. Electron energy loss spectroscopy and theoretical calculations collectively reveal the twist-angle-dependent electronic structure, especially the emergent separation of flat bands at small twist angles. The localized states of flat bands are similar to well-arranged quantum dots, promising an application in devices. This study opens a new door to the exploration of deep energy modulations within moiré superlattices alternative to van der Waals twistronics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Perspectives of active Si photonics devices for data communication and optical sensing

Si photonics has made rapid progress in research and commercialization in the past two decades. While it started with electronic–photonic integration on Si to overcome the interconnect bottleneck in data communications, Si photonics has now greatly expanded into optical sensing, light detection and ranging (LiDAR), optical computing, and microwave/RF photonics applications. From an applied physics point of view, this perspective discusses novel materials and integration schemes of active Si photonics devices for a broad range of applications in data communications, spectrally extended complementary metal–oxide–semiconductor (CMOS) image sensing, as well as 3D imaging for LiDAR systems. We also present a brief outlook of future synergy between Si photonic integrated circuits and Si CMOS image sensors toward ultrahigh capacity optical I/O, ultrafast imaging systems, and ultrahigh sensitivity lab-on-chip molecular biosensing.

electronic band structure↗
DOE OSTI2023

Low Threshold, Long Wavelength Interband Cascade Lasers With High Voltage Efficiencies

Here, we report on the substantial advancement of long wavelength InAs-based interband cascade lasers (ICLs) utilizing advanced waveguides formed from hybrid cladding layers and targeting the 10-12 µm wavelength region. Modifications in the hole injector have improved carrier transport in these ICLs, resulting in significantly reduced threshold voltages (V th ) as low as 3.62 V at 80 K. Consequently, much higher voltage efficiencies were observed, peaking at about 73% at 10.3 µm and allowing for large output powers of more than 100 mW/facet. Also, low threshold current densities (J th ) of 8.8 A/cm 2 in cw mode and 7.6 A/cm 2 in pulsed mode near 10 µm were observed; a result of adjustments in the GaInSb hole well composition intended to reduce the overall strain accumulation in the ICL. Furthermore, an ICL from the second wafer operating at a longer wavelength achieved a peak voltage efficiency of 57% at 11.7 µm, with a peak output power of more than 27 mW/facet. This ICL went on to lase beyond 12 µm in both cw and pulsed modes, representing a new milestone in long wavelength coverage for ICLs with the standard W-QW active region.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Scalable Synthesis of Monolayer Hexagonal Boron Nitride on Graphene with Giant Bandgap Renormalization

Abstract Monolayer hexagonal boron nitride (hBN) has been widely considered a fundamental building block for 2D heterostructures and devices. However, the controlled and scalable synthesis of hBN and its 2D heterostructures has remained a daunting challenge. Here, an hBN/graphene (hBN/G) interface‐mediated growth process for the controlled synthesis of high‐quality monolayer hBN is proposed and further demonstrated. It is discovered that the in‐plane hBN/G interface can be precisely controlled, enabling the scalable epitaxy of unidirectional monolayer hBN on graphene, which exhibits a uniform moiré superlattice consistent with single‐domain hBN, aligned to the underlying graphene lattice. Furthermore, it is identified that the deep‐ultraviolet emission at 6.12 eV stems from the 1s‐exciton state of monolayer hBN with a giant renormalized direct bandgap on graphene. This work provides a viable path for the controlled synthesis of ultraclean, wafer‐scale, atomically ordered 2D quantum materials, as well as the fabrication of 2D quantum electronic and optoelectronic devices.

2D heterostructures↗
DOE OSTI2023

Mechanistic origins of excitonic properties in 2D perovskites: Implications for exciton engineering

As the field of 2D halide perovskites (HPs) matures, state-of-the-art techniques to measure important properties, such as the band gap (E g ) and exciton binding energy (E b ), continue to produce inconsistent values. Here, we tackle this long-standing problem by obtaining direct measurements of E g and E b for 31 unique HP structures. The E b values are lower than in previous literature reports and lower than expected from standard theory that assumes excitons are screened by optical-frequency dielectric constants. These low E b values are shown to be a consequence of unique screening effects, such as superlattice screening and phonon screening. Here, we find a strikingly strong correlation between E b and E g and provide design principles to a priori tune E g and E b to their optimal values. As such, this work offers a blueprint for E g -E b engineering of low-dimensional semiconductors as an even more useful replacement for simply band-gap engineering.

14 SOLAR ENERGY↗
DOE OSTI2021

Anisotropic Transient Disordering of Colloidal, Two-Dimensional CdSe Nanoplatelets upon Optical Excitation

Nanoplatelets (NPLs)-colloidally synthesized, spatially anisotropic, two-dimensional semiconductor quantum wells-are of intense interest owing to exceptionally narrow transition line widths, coupled with solution processability and bandgap tunability. However, given large surface areas and undercoordinated bonding at facet corners and edges, excitation under sufficient intensities may induce anisotropic structural instabilities that impact desired properties. We employ time-resolved X-ray diffraction to study the crystal structure of CdSe NPLs in response to optical excitation. Photoexcitation induces greater out-of-plane than in-plane disordering in 4 and 5 monolayer (ML) NPLs, while 3 ML NPLs display the opposite behavior. Recovery dynamics suggest that out-of-plane cooling slightly outpaces in-plane cooling in 5 ML NPLs with recrystallization occurring on indistinguishable time scales. In comparison, for zero-dimensional CdSe nanocrystals, disordering is isotropic and recovery is faster. These results favor the use of NPLs in optoelectronic applications, where they are likely to exhibit superior performance over traditional, zero-dimensional nanocrystals.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

Engineering Edge States of Graphene Nanoribbons for Narrow-Band Photoluminescence

Solid-state narrow-band light emitters are on-demand for quantum optoelectronics. Current approaches based on defect engineering in low-dimensional materials usually introduce a broad range of emission centers. Here, we report narrow-band light emission from covalent heterostructures fused to the edges of graphene nanoribbons (GNRs) by controllable on-surface reactions from molecular precursors. Two types of heterojunction (HJ) states are realized by sequentially synthesizing GNRs and graphene nanodots (GNDs) and then coupling them together. HJs between armchair GNDs and armchair edges of the GNR are coherent and give rise to narrow-band photoluminescence. In contrast, HJs between the armchair GNDs and the zigzag ends of GNRs are defective and give rise to nonradiative states near the Fermi level. At low temperatures, sharp photoluminescence emissions with peak energy range from 2.03 to 2.08 eV and line widths of 2–5 meV are observed. Furthermore, the radiative HJ states are uniform, and the optical transition energy is controlled by the band gaps of GNRs and GNDs. As these HJs can be synthesized in a large quantity with atomic precision, this finding highlights a route to programmable and deterministic creation of quantum light emitters.

36 MATERIALS SCIENCE↗
DOE OSTI2020

cm 2 -Scale Synthesis of MoTe 2 Thin Films with Large Grains and Layer Control

Owing to the small energy differences between its polymorphs, MoTe 2 can access a full spectrum of electronic states from the 2H semiconducting state to the 1T' semimetallic state and from the T d Weyl semimetallic state to the superconducting state in the 1T' and T d phase at low temperature. Thus, it is a model system for phase transformation studies as well as quantum phenomena such as the quantum spin Hall effect and topological superconductivity. Careful studies of MoTe 2 and its potential applications require large-area MoTe 2 thin films with high crystallinity and thickness control. Here, we present cm 2 -scale synthesis of 2H-MoTe 2 thin films with layer control and large grains that span several microns. Layer control is achieved by controlling the initial thickness of the precursor MoO x thin films, which are deposited on sapphire substrates by atomic layer deposition and subsequently tellurized. Despite the van der Waals epitaxy, the precursor–substrate interface is found to critically determine the uniformity in thickness and grain size of the resulting MoTe 2 films: MoTe 2 grown on sapphire show uniform films while MoTe 2 grown on amorphous SiO 2 substrates form islands. Furthermore, this synthesis strategy decouples the layer control from the variabilities of growth conditions for robust growth results and is applicable to growing other transition-metal dichalcogenides with layer control.

2D materials↗
DOE OSTI2025

One-Dimensional Electron Gas Confined along Nanowrinkles in a Unidirectional Charge Density Wave Material

Two-dimensional (2D) materials inherently exhibit instabilities. Structurally, this may lead to modulations along the third dimension, e.g., wrinkles. Electronically, 2D instabilities can manifest themselves as charge density waves (CDWs). Although wrinkles can alter anisotropic electronic structures susceptible to forming CDWs, less is known about their impact on broken-symmetry ground states. Here, in this study, using scanning tunneling microscopy and spectroscopy, we investigate the CDW states on the wrinkled surface of DyTe 3 . We identify elongated, parallel nanoscale wrinkles stabilized by ribbon-shaped defects. Interestingly, the CDW order persists across the nanowrinkles with a gradual phase shift but is locally suppressed near the defects, where phase windings occur. In addition, these defects induce quantum confinement effects along the nanowrinkles, indicating the presence of one-dimensional metallic states with hole- like dispersion, while angle-resolved photoemission spectroscopy identifies a gap along the wrinkle direction. We ascribe this discrepancy to strain-induced changes in the Fermi surface, which lead to the closure of the gap at the sites of the nanowrinkles. Taken together, our results underscore the complex interplay between structural features and Fermi surface topology, allowing for the deliberate manipulation of quantum states in strongly correlated systems via local crystal deformations.

nanowrinkles↗
DOE OSTI2022

Single-Photon-Induced Electron Spin Polarization of Two Exchange-Coupled Stable Radicals

Transient electron paramagnetic resonance spectroscopy has been used to probe photoinduced electron spin polarization of a stable exchange-coupled organic biradical in a Pt(II) complex comprising 4,4'-di-tert-butyl-2,2'-bipyridine (bpy) and 3,6-bis(ethynyl-para-phenyl-nitronyl nitroxide)-o-catecholate (CAT(o-C$\equiv$C-Ph-NN) 2 ). Photoexcitation results in four unpaired spins in excited states of this complex, with spins being localized on each of the two radicals, CAT •+ and bpy •– . The four spins are all exchange-coupled in these excited states, and an off-diagonal matrix element in the CAT •+ -NN exchange allows for exchange-enhanced intersystem crossing to the 3 T 1a state, which possesses (bpy •– )Pt(CAT •+ ) chromophoric triplet character. Further, fast mixing between this 3 T 1a state and other thermally accessible excited LL'CT state(s) followed by fast relaxation provides spin polarization of the exchange-coupled NN radicals in the 3 S 0 ground state of the complex. Our results demonstrate that well-defined quantum states of a ground-state biradical can be initialized with single-photon excitation and have the potential for further spin manipulation directed toward quantum information science applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Strain-stabilized superconductivity

Superconductivity is among the most fascinating and well-studied quantum states of matter. Despite over 100 years of research, a detailed understanding of how features of the normal-state electronic structure determine superconducting properties has remained elusive. For instance, the ability to deterministically enhance the superconducting transition temperature by design, rather than by serendipity, has been a long sought-after goal in condensed matter physics and materials science, but achieving this objective may require new tools, techniques and approaches. Here, we report the transmutation of a normal metal into a superconductor through the application of epitaxial strain. We demonstrate that synthesizing RuO 2 thin films on (110)-oriented TiO 2 substrates enhances the density of states near the Fermi level, which stabilizes superconductivity under strain, and suggests that a promising strategy to create new transition-metal superconductors is to apply judiciously chosen anisotropic strains that redistribute carriers within the low-energy manifold of d orbitals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Electron recombination of rotationally cold D 2 H + ions

Dissociative recombination (DR) of electrons with small molecular ions is a fundamental process for the physics and chemistry of the interstellar medium and planetary atmospheres. In previous DR studies, detailed analysis of the experimental rate coefficients has been hindered by the difficulty of preparing the ions in well-defined quantum states. For polyatomic ions in particular, truly state-selective measurements have been elusive, allowing only qualitative benchmarks of theory. Here, we present DR studies of the deuterated triatomic hydrogen ion D 2 H + , where the molecular ions were stored for up to 1000 seconds inside the Cryogenic Storage Ring (CSR) prior to the DR measurements. Our experiments with rotationally cold D 2 H + ions allow for detailed comparison to state-of-the-art theoretical calculations. We obtain very good agreement between experiment and theory even in the important collision energy range from 1 meV to 0.5 eV, where a multitude of Rydberg resonances reveal their imprint on the rate coefficient.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Electromagnetic control of spin ordered Mn 3 qubits: a density functional study

[Mn 3 O(O 2 CMe)(dpd 3/2 )] 2 is composed of two monomers each of which contain three Mn atoms at the vertices of an equilateral triangle. A full analysis of the electronic and magnetic structure of the dimer shows that each Mn atom carries a local spin of S = 2 while other spin states are energetically much higher. This result suggests application for conventional as well as quantum tasks. A detailed analysis of the electronic and magnetic structure of the monomer, on the other hand, suggests that there are three spin states of S = 1, S = 3/2 and S = 2 per monomer which are energetically competitive. Additionally, we found that while monomer–monomer interactions are very weak, the coupling of monomers via covalent linkers affects both the magnetization and electronic energy levels of monomers. In particular, the isolated monomers prefer a ground state with local spin of S = 1 on Mn atoms and an antiferromagnetically ordered structure while the dimers possess a ground state with local spin of S = 2 on Mn atoms and a ferromagnetically ordered structure. The investigation of the polarizability of both monomer and dimer is examined for antiferromagnetically ordered structures which induces a high dipole moment of 0.08 (a.u.) and 0.16 (a.u.) for monomer and dimer, respectively. The energy of the antiferromagnetic structure is also high compared to other spin-electric molecules.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

On the optical anisotropy in 2D metal-halide perovskites

We develop a better understanding of the many contributing factors that give rise to extreme optical anisotropy in 2D perovskites, and we then show that spin-coated films can exhibit excellent order comparable with exfoliated crystals.

14 SOLAR ENERGY↗