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At least 595 records · Page 33
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Magneto-transport study on Sn-rich Sn 1–x Ge x thin films enabled by CdTe buffer layer

α-Sn, generally known as gray tin, has attracted significant scientific interest due to its potential to host novel topological phases. Studying the transport properties of α-Sn thin films grown on the InSb substrate has been challenging, as the InSb substrate also significantly contributes to the transport properties. In this article, we report a novel approach to epitaxially grow α-Sn thin films on an InSb substrate with a resistive buffer layer of CdTe. Thin films of α–Sn 1–x Ge x (x = 0, 0.025) alloy of 15 nm thickness have been grown using molecular beam epitaxy. The high quality of the samples has been determined through high-resolution x-ray diffraction. The CdTe buffer layer has high resistance and acts as an insulating virtual substrate, which significantly suppresses contribution from InSb. Magnetotransport measurements show clear Shubnikov–de Hass oscillations in α–Sn 1–x Ge x (x = 0, 0.025) thin films. A change in oscillation frequency is observed upon alloying with Ge, implying a modification in the electronic structure and demonstrating the effectiveness of the CdTe buffer layer approach. Furthermore, this work provides a new approach that enables the electronic transport characterization of the α–Sn 1–x Ge x alloy system, which enables the study of the topological quantum states using electronic transport and their device applications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Observation of hydrodynamic plasmons and energy waves in graphene

Thermally excited electrons and holes form a quantum-critical Dirac fluid in ultraclean graphene and their electrodynamic responses are described by a universal hydrodynamic theory. The hydrodynamic Dirac fluid can host intriguing collective excitations distinctively different from those in a Fermi liquid. Here we report the observation of the hydrodynamic plasmon and energy wave in ultraclean graphene. In this study, we use the on-chip terahertz (THz) spectroscopy technique to measure the THz absorption spectra of a graphene microribbon as well as the propagation of the energy wave in graphene close to charge neutrality. We observe a prominent high-frequency hydrodynamic bipolar-plasmon resonance and a weaker low-frequency energy-wave resonance of the Dirac fluid in ultraclean graphene. The hydrodynamic bipolar plasmon is characterized by the antiphase oscillation of massless electrons and holes in graphene. The hydrodynamic energy wave is an electron-hole sound mode with both charge carriers oscillating in phase and moving together. The spatial–temporal imaging technique shows that the energy wave propagates at a characteristic speed of $V_f$ / $ \sqrt2$ near the charge neutrality. Our observations open new opportunities to explore collective hydrodynamic excitations in graphene systems.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Illumination-induced modulation of conductivity and Gunn oscillation properties in epitaxial GaAs

In this work, we illuminate a gallium arsenide (GaAs) Gunn device and study the light-induced changes of Gunn oscillation properties. We observe that illumination leads to the modulation of the Gunn threshold voltage, the Gunn oscillation magnitude, and the coherency of Gunn oscillation, with the nature of the modulation being closely related to the position of illumination on the device. These effects are attributed to the generation of optically excited carriers, which results in the modulation of conductivity and the electric field profile along the device. The finite element method is used to simulate the change of the field profile of the Gunn device caused by illumination. We also report an unexpected phenomenon of Gunn oscillation property manipulation with an optical chopper. In addition, wavelength-dependent, power-dependent, and pulsed illumination measurements are performed to help with further understanding the observations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Capturing the sequence of events during the water oxidation reaction in photosynthesis using XFELs

Ever since the discovery that Mn was required for oxygen evolution in plants by Pirson in 1937 and the period-four oscillation in flash-induced oxygen evolution by Joliot and Kok in the 1970s, understanding of this process has advanced enormously using state-of-the-art methods. The most recent in this series of innovative techniques was the introduction of X-ray free-electron lasers (XFELs) a decade ago, which led to another quantum leap in the understanding in this field, by enabling operando X-ray structural and X-ray spectroscopy studies at room temperature. This review summarizes the current understanding of the structure of Photosystem II (PS II) and its catalytic centre, the Mn 4 CaO 5 complex, in the intermediate S i ( i = 0-4)-states of the Kok cycle, obtained using XFELs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Delocalization error poisons the density-functional many-body expansion

The many-body expansion is a fragment-based approach to large-scale quantum chemistry that partitions a single monolithic calculation into manageable subsystems. This technique is increasingly being used as a basis for fitting classical force fields to electronic structure data, especially for water and aqueous ions, and for machine learning. Here, we show that the many-body expansion based on semilocal density functional theory affords wild oscillations and runaway error accumulation for ion–water interactions, typified by F − (H 2 O) N with N ≳ 15. We attribute these oscillations to self-interaction error in the density-functional approximation. The effect is minor or negligible in small water clusters, explaining why it has not been noticed previously, but grows to catastrophic proportion in clusters that are only moderately larger. This behavior can be counteracted with hybrid functionals but only if the fraction of exact exchange is ≳50%, whereas modern meta-generalized gradient approximations including ωB97X-V, SCAN, and SCAN0 are insufficient to eliminate divergent behavior. Other mitigation strategies including counterpoise correction, density correction (i.e., exchange–correlation functionals evaluated atop Hartree–Fock densities), and dielectric continuum boundary conditions do little to curtail the problematic oscillations. In contrast, energy-based screening to cull unimportant subsystems can successfully forestall divergent behavior. These results suggest that extreme caution is warranted when the many-body expansion is combined with density functional theory.

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

Supplementary Material for ORNL_AISD-Ex

This dataset provides supplementary material for the previously published dataset ORNL_AISD-Ex (1), which is available at the following website: https://www.osti.gov/biblio/1907919 The dates comprises one compressed folder called ornl_aisd_ex.zip. The compressed folder ornl_aisd_ex.zip contains 1,000 CSV files, each of them titled ornl_aisd_ex_ID.csv, where ID is a number that ranges between 1 and 1,000. The information contained in ornl_aisd_ex_ID.csv corresponds to the information of the molecules compresses inside the ornl_aisd_ex_ID.tar.gz of the dataset ORNL_AISD-Ex. Each row in each .CSV file is associated with a molecule, and the columns contain the following information: 1) molecules ID 2) SMILES string representation 3) DFTB-PE (eV): formation energy 4) first 50 electronic excitation modes 5) oscillators strengths of the first 50 electronic excitation modes The compression of this information into CSV files will allow a more agile extraction and management of information to the users that do not have access to large scale HPC platforms. REFERENCES (1) Lupo Pasini, Massimiliano, Mehta, Kshitij, Yoo, Pilsun, and Irle, Stephan. ORNL_AISD-Ex: Quantum chemical prediction of UV/Vis absorption spectra for over 10 million organic molecules. United States: N. p., 2023. Web. doi:10.13139/OLCF/1907919.

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

Observation of light-driven band structure via multiband high-harmonic spectroscopy

Intense light–matter interactions have revolutionized our ability to probe and manipulate quantum systems at sub-femtosecond timescales, opening routes to the all-optical control of electronic currents in solids at petahertz rates. Such control typically requires electric-field amplitudes in the range of almost volts per angstrom, when the voltage drop across a lattice site becomes comparable to the characteristic bandgap energies. In this regime, intense light–matter interaction induces notable modifications to the electronic and optical properties, dramatically modifying the crystal band structure. Yet, identifying and characterizing such modifications remain an outstanding problem. As the oscillating electric field changes within the driving field’s cycle, does the band structure follow and how can it be defined? Here we address this fundamental question, proposing all-optical spectroscopy to probe the laser-induced closing of the bandgap between adjacent conduction bands. Our work reveals the link between nonlinear light–matter interactions in strongly driven crystals and the sub-cycle modifications in their effective band structure.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Energy-Screened Many-Body Expansion for Protein–Ligand Interactions: Examining Convergence for Metalloenzymes Through Seven–Body Interactions

Fragment-based quantum chemistry is a powerful strategy for calculating protein−ligand interaction energies using quantum chemistry methods. Rigorous convergence often requires hundreds of atoms in the protein binding-site model, especially if that model is constructed using distance-based criteria to select amino acid residues, while three- and four-body calculations exhibit instability related to combinatorial proliferation in the number of subsystem calculations. Here, we report an energy-based screening protocol for the many-body expansion applied to protein−ligand interactions, implemented in the open-source FRAGME∩T code. Using a combination of aggressive screening based on semiempirical quantum chemistry, with an improved graph-theoretical algorithm to eliminate unimportant subsystems, we are able to perform n-body calculations up to n = 7 using density functional theory in triple-ζ basis sets. Distance cutoffs further reduce the cost without compromising accuracy. Rapid and stable convergence of the many-body expansion is obtained by n = 4, for a pair of metalloenzymes in which a divalent ion coordinates directly to the ligand. As compared to previous results that relied solely on distance cutoffs, oscillations in the n-body corrections are reduced or eliminated, although residual errors remain in one case. This work demonstrates that benchmark-quality protein−ligand interaction energies can be systematically converged using a method with excellent parallel efficiency and scalability.

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

High-resolution absorption spectroscopy of room-temperature and jet-cooled ammonia between 59,000 and 93,000 cm -1

Here, we present new high-resolution photoabsorption spectra of ammonia spanning the region between 59,000 cm -1 and 93,000 cm -1 that were recorded by using the Fourier Transform Spectrometer at the Synchrotron SOLEIL. This region extends from just above the Franck-Condon envelope for the $\tilde{A}$ 1 $A$ 2 " ← $\tilde{X}$ 1 $A$ 1 ' transition to well above the NH 3 + $\tilde{X}$ + 2 $A$ 2 " ionization threshold. The spectra were recorded at a measured resolution of 0.23 cm -1 in both a room-temperature cell (293 K) and in a slit-jet supersonic expansion (~70 K). The absolute photoabsorption cross section with an uncertainty of ±5% is also reported for the room-temperature spectrum. The present resolution is a factor of 10 – 100 times higher than in other recently reported broad band spectra of ammonia, and many of the observed bands show partially resolved rotational structure. We have attempted to assign this structure for a number of these bands. The oscillator strengths extracted from the data are in good agreement with previous measurements but, in the case of structured bands, the present higher resolution measurements return higher peak absorption cross sections, that increase further when the sample is cooled. The present higher resolution spectra suggest that a number of previous vibronic band assignments that were based on quantum defect considerations may require some revision. Finally, we discuss the substantial differences between the photoabsorption and photoionization data just above the first ionization threshold.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Kerr-lens mode-locked Cr:ZnS oscillator reaches the spectral span of an optical octave

We report, to the best of our knowledge, the first super-octave femtosecond polycrystalline Cr:ZnS laser at the central wavelength 2.4 µm. The laser is based on a non-polarizing astigmatic X-folded resonator with normal incidence mounting of the gain element. The chromatic dispersion of the resonator is controlled with a set of dispersive mirrors within one third of an optical octave over 2.05–2.6 µm range. The resonator’s optics is highly reflective in the range 1.8–2.9 µm. The components of the oscillator’s output spectrum at the wavelengths 1.6 µm and 3.2 µm are detected at –60 dB with respect to the main peak. Average power of few-cycle Kerr-lens mode-locked laser is 1.4 W at the pulse repetition frequency 79 MHz. That corresponds to 22% conversion of cw radiation of Er-doped fiber laser, which we used for optical pumping of the Cr:ZnS oscillator.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Optical current generation in graphene: CEP control vs. ω + 2 ω control

The injection of directional currents in solids with strong optical fields has attracted tremendous attention as a route to realize ultrafast electronics based on the quantum-mechanical nature of electrons at femto- to attosecond timescales. Such currents are usually the result of an asymmetric population distribution imprinted by the temporal symmetry of the driving field. Here we compare two experimental schemes that allow control over the amplitude and direction of light-field-driven currents excited in graphene. Both schemes rely on shaping the incident laser field with one parameter only: either the carrier-envelope phase (CEP) of a single laser pulse or the relative phase between pulses oscillating at angular frequencies ω and 2ω, both for comparable laser parameters. We observe that the efficiency in generating a current via two-color-control exceeds that of CEP control by more than two orders of magnitude (7 nA vs. 18 pA), as the ω + 2ω field exhibits significantly more asymmetry in its temporal shape. We support this finding with numerical simulations that clearly show that two-color current control in graphene is superior, even down to single-cycle pulse durations. We expect our results to be relevant to experimentally access fundamental properties of any solid at ultrafast timescales, as well as for the emerging field of petahertz electronics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction

Ubiquitous to most molecular scattering methods is the challenge to retrieve bond distance and angle from the scattering signals since this requires convergence of pattern matching algorithms or fitting methods. This problem is typically exacerbated when imaging larger molecules or for dynamic systems with little a priori knowledge. Here, we employ laser-induced electron diffraction (LIED) which is a powerful means to determine the precise atomic configuration of an isolated gas-phase molecule with picometre spatial and attosecond temporal precision. We introduce a simple molecular retrieval method, which is based only on the identification of critical points in the oscillating molecular interference scattering signal that is extracted directly from the laboratory-frame photoelectron spectrum. The method is compared with a Fourier-based retrieval method, and we show that both methods correctly retrieve the asymmetrically stretched and bent field-dressed configuration of the asymmetric top molecule carbonyl sulfide (OCS), which is confirmed by our quantum-classical calculations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Many-Body Collective Neutrino Oscillations: Recent Developments

Neutrino flavor transformations in core-collapse supernovae and binary neutron star mergers represent a complex and unsolved problem that is integral to our understanding of the dynamics and nucleosynthesis in these environments. The high number densities of neutrinos present in these environments can engender various collective effects in neutrino flavor transformations, driven either by neutrino-neutrino coherent scattering, or in some cases, through collisional (incoherent) interactions. An ensemble of neutrinos undergoing coherent scattering among themselves is an interacting quantum many-body system -- as such, there is a tantalising prospect of quantum entanglement developing between the neutrinos, which can leave imprints on their flavor evolution histories. Here, in this study, we seek to summarize recent progress that has been made towards understanding this phenomenon.

Hypernuclei↗
DOE OSTI2025

Anisotropic Response of Defect Bound States to the Magnetic Field in Epitaxial FeSn Films

Crystal defects, whether intrinsic or engineered, drive many fundamental phenomena and novel functionalities of quantum materials. Here, we report symmetry-breaking phenomena induced by Sn vacancy defects on the surface of epitaxial Kagome antiferromagnetic FeSn films using low-temperature scanning tunneling microscopy and spectroscopy. Near the single Sn vacancy, anisotropic quasiparticle interference patterns are observed in the differential conductance dI/dV maps, breaking the 6-fold rotational symmetry of the Kagome layer. Furthermore, the Sn vacancy defects induce bound states that exhibit anomalous Zeeman shift under an out-of-plane magnetic field, where the energy of the bound states moves linearly toward higher energy independent of the direction of the magnetic field. Under an in-plane magnetic field, the shift of the bound state energy also shows a 2-fold oscillating behavior as a function of the azimuth angle. These findings demonstrate defectenabled new functionalities in Kagome antiferromagnets for potential applications in nanoscale spintronic devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

A Visual Understanding of Circular Dichroism Spectroscopy

Mapping chemical and structural properties to electronic and magnetic responses is critical to many applications such as quantum information science, where the precise storage and transmission of unique information is paramount. Specifically, constructing molecules and materials that provide strong polarized responses at tunable frequencies and with large anisotropies is key to optical processing of quantum information. Chiral molecules provide chiroptical response to circularly polarized light, making them attractive for quantum information science and other applications related to sensing, polarized photodetectors, and spintronics. Predicting a molecular design, a priori, with large anisotropies to circularly polarized light is challenging due to the complex interplay between electric and magnetic components of the optical response. In this work, we explore a visual representation of the electronic chiroptical response by decomposing the rotary strength into its constituent components. Here, we make use of the intuitive electronic oscillator framework to develop classical intuition regarding the rotary strength and its constituents. We explore three model chemical systems that exhibit local and global chirality. Our analysis reveals that local chirality necessarily exhibits competition between the local chiral center and chirality induced in other fragments of the molecule, resulting in both unexpected nonmonotonic trends and sign flips in chemically adjacent geometries. Furthermore, we can visually distinguish between local and global chirality via examination of the transition chiral tensor. Interestingly, we make strong connections to ferromagnetic and antiferromagnetic spin systems in that chiroptically inactive transitions exhibit antiferromagnetic-like alternating orbital patterns while active transitions show domain formation in an ferromagnetic-like alignment that produces a net chiroptical response.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Tuning Hybrid exciton–Photon Fano Resonances in Two-Dimensional Organic–Inorganic Perovskite Thin Films

As easy-to-grow quantum wells with narrow excitonic features at room temperature, two-dimensional (2D) Ruddleson–Popper perovskites are promising for realizing novel nanophotonic devices based on exciton–photon interactions. Here, we demonstrate a distinct hybrid exciton–photon Fano resonance in (C 4 H 9 NH 3 ) 2 PbI 4 thin films prepared via spin coating. Using a classical coupled-oscillator model and finite-difference time-domain simulations, we link the Fano interference to the coupling of the exciton with the Rayleigh-like scattering of the film microstructure. Combining colloidal plasmonic cavities with the 2D perovskite films, we demonstrate tuning of the Fano resonance. In combination with silver nanoparticles, the exciton–photon Fano interference couples to the in-plane plasmonic modes with indications of Rabi splitting. By creating a nanoparticle on mirror geometry, we address the out-of-plane excitonic component, reaching an intermediate coupling regime. Furthermore, these structures suggest possible photonic targets for biomolecular self-assembly applications.

2D perovskites↗
DOE OSTI2022

Light Relics of the Early Universe (Final Technical Report)

The research supported by this award invested two types of signals left over of the early universe that might be observed in maps of the universe: (i) particles produced (thermal relics) during the hot big bang and (ii) signals left in the seeds of structure left from from an inflationary epoch prior to the hot big bang (inflationary relics). The research into thermal relics exposed new signatures of the cosmic neutrino background in the distribution of galaxies, culminating in the first measurement of the neutrino induced phase shift of the baryon acoustic oscillations. Subsequent research explored implications of constraints on hot light particles from the cosmic microwave background and the large scale structure for the physics of dark matter. Green and collaborations also investigated cosmological signatures from the inflationary epoch, including the best constraint to date on oscillatory features in seeds of structure and the first viable proposal to test the quantum origin of structure in the universe.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Neutron Tunneling: A New Mechanism to Power Explosive Phenomena in Neutron Stars, Magnetars, and Neutron Star Mergers

Neutron tunneling between neutron-rich nuclei in inhomogeneous dense matter encountered in neutron star crusts can release enormous energy on a short timescale to power explosive phenomena in neutron stars. In this work, we clarify aspects of this process that can occur in the outer regions of neutron stars when oscillations or cataclysmic events increase the ambient density. We use a time-dependent Hartree–Fock–Bogoliubov formalism to determine the rate of neutron diffusion and find that large amounts of energy can be released rapidly. The roles of nuclear binding, two-body interaction, and pairing in neutron diffusion times are investigated. We consider a one-dimensional quantum diffusion model and extend our analysis to study the impact of diffusion in three dimensions. Here, we find that these novel neutron transfer reactions can generate energy in the amount of ≃ 10 40 –10 44 erg under suitable conditions and assumptions.

79 ASTRONOMY AND ASTROPHYSICS↗