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At least 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Monte Carlo transport analysis to assess intensity dependent response of a carbon-doped GaN photoconductor

In this report evaluation of the photoresponse in wurtzite GaN photoconductive switches is presented based on kinetic Monte Carlo simulations. The focus is on electron transport physics and assessment of high frequency operation. The roles of GaN band structure, Pauli exclusion, and treatment of internal fields based on the fast multipole method are all comprehensively included. The implementation was validated through comparisons of velocity-field characteristics for GaN with computational results in the literature. Photocurrent widths of less than ~7 ps for the 1 μm device can be expected, which translates into a 100 GHz upper bound. Photocurrent pulse compression below the laser full width at half maxima at high applied fields are predicted based on the interplay of space-charge effects and the negative differential velocity characteristics of GaN.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Robust analytic continuation of Green's functions via projection, pole estimation, and semidefinite relaxation

Green's functions of fermions are described by matrix-valued Herglotz-Nevanlinna functions. Since analytic continuation is fundamentally an ill-posed problem, the causal space described by the matrix-valued Herglotz-Nevanlinna structure can be instrumental in improving the accuracy and in enhancing the robustness with respect to noise. We demonstrate a three-pronged procedure for robust analytic continuation called PES: (1) projection of data to the causal space; (2) estimation of pole locations; and (3) semidefinite relaxation within the causal space. We compare the performance of PES with the recently developed Nevanlinna and Carathéodory continuation methods and find that PES is more robust in the presence of noise and does not require the usage of extended precision arithmetics. We also demonstrate that a causal projection improves the performance of the Nevanlinna and Carathéodory methods. The PES method is generalized to bosonic response functions, for which the Nevanlinna and Carathéodory continuation methods have not yet been developed. Furthermore, it is particularly useful for studying spectra with sharp features, as they occur in the study of molecules and band structures in solids.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Monte Carlo Explicitly Correlated Second-Order Many-Body Green’s Function Calculations of Semiconductor Band Gaps

A systematically converging series of ab initio, post-density-functional, size-consistent, electron-correlated approximations is desired for predictive computing of felectronic band structures of insulating, semiconducting, and metallic solids. A series that meets all of these desiderata (except the applicability to metals) is ab initio many-body Green's function theory based on Gaussian-type-orbital (GTO) basis sets. Here, its leading-order approximation, the second-order Green's function (GF2) method in the diagonal and frequency-independent approximations with the aug-cc-pVDZ basis set, is applied to the fundamental band gaps of three semiconductors (diamond, silicon, and silicon carbide in the zincblende structure) using cluster models. Corrections are made to the basis-set-incompleteness errors by the explicit-correlation (F12) ansatz (GF2-F12) for the valence band edges. The crystals are modeled as surface-passivated clusters of increasing sizes, whose wave functions are expanded by up to 2709 GTO basis functions. Immense computational costs of these calculations are overcome by the highly scalable stochastic algorithm of the Monte Carlo GF2-F12 method, whose operation cost per state increases only as a cubic power of system size, which has a tiny memory footprint and easily achieves near-perfect parallel efficiency on thousands of CPUs or on hundreds of GPUs. The correlated, F12-corrected highest-occupied and lowest-unoccupied molecular-orbital energy (HOMO-LUMO) gap is 5.78 ± 0.07 eV for C 87 H 76 as compared with the experimental value of the fundamental (indirect) band gap of bulk diamond at 5.48 eV. The correlated, F12-corrected HOMO-LUMO gaps for Si 75 H 76 and Si 32 C 43 H 76 are 2.56 ± 0.15 eV and 3.50 ± 0.12 eV, respectively, which are expected to decrease further with increasing cluster sizes. As a result, the experimental fundamental (indirect) band gaps of bulk silicon and silicon carbide are 1.17 eV and 2.42 eV, respectively.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Ultrafast high-harmonic spectroscopy of solids

High-harmonic spectroscopy, an ultrafast all-optical technique initially conceptualized in atomic and molecular systems, has now emerged as a powerful platform for studying the structure and dynamics of condensed matter. Unlike that in the gas phase, solid-state high-harmonic generation relies on the fundamental response from high atomic density and periodicity, leading to interband transitions and coherent driving of electrons and holes in their respective bands. These mechanisms make high-harmonic spectroscopy particularly sensitive to the electronic band structure, topological properties and many-body correlations in condensed media. An advantage of high-harmonic spectroscopy over other spectroscopic methods is its ability to probe ultrafast phenomena, capturing femto- to attosecond dynamics of multi-band and strongly correlated electron interactions in solids. Furthermore, in this Review, we discuss the latest experimental and theoretical advances in ultrafast high-harmonic spectroscopy of solids and provide perspectives for future research in this field.

High-harmonic generation↗
DOE OSTI2024

Colloidal AInSe 2 (A = K, Rb, Cs) Nanocrystals with Tunable Crystal and Band Structures

Wide band gap AInSe 2 (A = K, Rb, Cs) is an important interlayer material for improving the efficiency of Cu(In,Ga)(S,Se) 2 (CIGS) solar cells. Compared to high-vacuum deposition and solid-state synthesis, a less energyintensive method is of interest for its fabrication. Herein, we present the rapid, low-temperature colloidal synthesis of AInSe 2 nanocrystals that opens a pathway for convenient solution processing. The crystal structures and electronic band structures of the nanocrystals were studied, and their particle morphology was found to be dependent on the choice of alkali metal and selenium precursors. Homogeneous solid solution (K,Rb,Cs)InSe 2 nanocrystals were synthesized using a mixture of alkali metal precursors. Their compositions, lattice parameters, and band gaps were easily tuned based on the K:Rb:Cs precursor ratio, providing potential for interface engineering of CIGS nanocrystal-based solar cells.

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

Comparison of interband related optical transitions and excitons in ZnGeN 2 and GaN

The optical dielectric function of ZnGeN 2 is calculated from the interband transitions using the energy bands calculated in the quasiparticle self-consistent (QS)GW^ method using two different levels of approximation: the independent particle approximation (IPA) and the Bethe-Salpeter Equation (BSE) approach. The first allows us to relate peaks in ε 2 to specific bands and k-points but does not include electron-hole interaction effects. The second includes electron-hole interaction or excitonic effects. The corresponding changes in the shape of ε 2 (ω) are found to be similar to those in GaN. The screened Coulomb interaction W^ is here calculated including electron-hole interactions in the polarization function and gives a band structure already going beyond the random phase approximation. The static dielectric constants including only electronic screening, commonly referred to as ε∞ , were calculated separately by extrapolating the wave vector dependent macroscopic dielectric function in the long-wavelength limit. Below the quasiparticle gap, we find three bound excitons optically active for different polarization. The convergence of these bound excitons with respect to the density of the k-mesh used in the BSE is studied and found to require a fine mesh. It is also found that these bound excitons originate from only the lowest conduction band and the top three valence bands. To incorporate the lattice screening, we include a scaling factor (ε∞/ε 0 ) 2 , which allows us to obtain exciton binding energies of the correct order of magnitude similar to those in GaN. Here, the excitons are related to each of the three fold split valence bands and the splittings of the latter are also studied as function of strain. Finally, a relation between the anisotropic effective masses and the valence band splitting is pointed out and explained.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Spin switchable optical phenomena in Rashba band structures through intersystem crossing in momentum space in solution-processing 2D-superlattice perovskite film

Spin-switchable phenomena are a critical element for the development of spintronic and chiroptic devices. Herein we combine a 2D-superlattice perovskite (4,4-DFPD2PbI4) film with a ferromagnetic cobalt (Co) layer to form a multiferroic perovskite/Co interface, and demonstrate spin-switchable circularly polarized luminescence (CPL) between right-handed σ+ and left-handed σ− polarizations. When the ferromagnetic spins of Co at the Co/perovskite interface are altered between positive and negative magnetic field directions, the CPL from the 2D-superlattice perovskite switches from σ+ to σ− polarization. The magnetic field effects present a unique method to confirm that CPL is generated by the circular-orbital momentum of light-emitting excitons within Rashba band structures, eliminating artifacts involving structural birefringence. Our polarized neutron reflectometry measurements confirm a super long-range spin-orbit interaction occurring in the 2D-superlattice perovskite films. The temperature dependence of spin-switchable phenomenon indicates an extraordinarily long orbital polarization lifetime, reaching microseconds at room temperature and milliseconds at 5 K.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Quasiparticle self-consistent GW band structures and phase transitions of LiAlO 2 in tetrahedrally and octahedrally coordinated structures

In this work, a first-principles computational study is presented of various phases of LiAlO 2 . The relative total energies and equations of state of the α, β, and γ phases are determined after structural relaxation of each phase. The β and γ tetrahedral phases are found to be very close in energy and lattice volume with the γ phase having the lowest energy. The octahedral α phase is a high-pressure phase and the transition pressure from the γ and β phases to α is determined to be about 1 GPa. The electronic band structures of each phase at their own equilibrium volume are determined using the quasiparticle self-consistent (QS) GW method as well as using the 0.8 Σ approach in which the QS GW self-energy is reduced by a factor of 0.8 to correct for the underscreening of W in QS GW. The effective masses of the band edges and the nature of the band gaps are presented. The lowest energy γ phase is found to have a pseudodirect gap of 7.69 eV. The gap is direct at Γ but corresponds to a dipole forbidden transition. The imaginary part of the dielectric function and the absorption coefficient are calculated in the long-wavelength limit and the random phase approximation, without local field or electron-hole interaction effects for each phase, and their anisotropies are discussed. Si doping on the Al site is investigated as a possible n-type dopant in γ-LiAlO 2 using a 128-atom supercell corresponding to 3.125% Si on the Al sublattice in the generalized gradient approximation and a smaller 16-atom cell with 25% Si in the QS GW approximation. The Si is found to significantly perturb the conduction band and lower the gap but a clearly separated deep donor defect level is not found. However, the donor binding energy is still expected to be relatively deep, on the order of a few tenths eV in the hydrogenic effective mass approximation.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Many-body electronic structure of LaScO 3 by real-space quantum Monte Carlo

We present real space quantum Monte Carlo (QMC) calculations of the scandate LaSc0 3 that proved to be challenging for traditional electronic structure approaches due to strong correlation effects resulting in inaccurate band gaps from DFT and GW methods when compared with existing experimental data. Besides calculating an accurate QMC band gap corrected for supercell size biases and in agreement with numerous experiments, we also predict the cohesive energy of the crystal using the standard fixed-node QMC without any empirical or non-variational parameters. We show that promotion (optical) gap and fundamental gap agree with each other illustrating a clear absence of significant excitonic effects in the ideal crystal. We obtained these results in perfect consistency in two independent tracks that employ different basis sets (plane wave vs. localized gaussians), different codes for generating orbitals (QUANTUM ESPRESSO vs. CRYSTAL), different QMC codes (QMCPACK vs. QWALK) and different high-accuracy pseudopotentials (ccECPs vs. Troullier-Martins) presenting the maturity and consistency of QMC methodology and tools for studies of strongly correlated problems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Monitoring of dielectric permittivity in accelerated alkali-silica reaction concrete with microwave backscattering

Deterioration of concrete due to the alkali–silica reaction (ASR) involves a reaction between alkaline ions in the cement pore solution and non-crystalline silica found in many aggregates. The product of reaction is a porous hydrophilic ASR gel, which causes expansion and cracking of concrete structure. Currently, there is no reliable method for non-destructive evaluation of ASR. We have investigated the feasibility of using relative dielectric permittivity obtained from X-band microwave backscattering of concrete. Advantages of this method of concrete evaluation are that measurements are non-contact and one-sided, and the approach is scalable to arbitrary-size concrete structures. The exploratory study was performed using an unrestrained set of accelerated ASR concrete prism specimens developed according to the ASTM1293 standard. One set of specimens contained no entrained air, while another set was contained entrained air. The specimens were removed from the environmental chamber at different times during a year-long study to create a set of different ASR maturity specimens. Strain measurements were performed on all specimens. Strain data both air entrained and non-air entrained sets were shown to be in close agreement with Larive model of isothermal unrestrained ASR expansion with similar fitting parameters. Furthermore, relative dielectric permittivity of concrete specimens was correlated with strain data. Both sets show correlation between dielectric permittivity and strain, with stronger linear correlation observed for the air-entrained specimens. Development of such correlation would enable estimating expansion of actual concrete structures from microwave backscattering measurements, which could be used for risk stratification to guide and minimize coring.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Extracting Inelastic Scattering Cross Sections for Finite and Aperiodic Materials from Electronic Dynamics Simulations

Explicit time-dependent electronic structure theory methods are increasingly prevalent in the areas of condensed matter physics and quantum chemistry, with the broad-band optical absorptivity of molecular and small condensed-phase systems nowadays routinely studied with such approaches. Here, in this paper, it is demonstrated that electronic dynamics simulations can similarly be employed to study cross sections for the scattering-induced electronic excitations probed in nonresonant inelastic X-ray scattering and momentum-resolved electron energy loss spectroscopies. A method is put forth for evaluating the electronic dynamic structure factor, which involves the application of a momentum boost-type perturbation and transformation of the resulting reciprocal space density fluctuations into the frequency domain. Good agreement is first demonstrated between the dynamic structure factor extracted from these electronic dynamics simulations and the corresponding transition matrix elements from linear response theory. The method is then applied to some extended (quasi)one-dimensional systems, for which the wave vector becomes a good quantum number in the thermodynamic limit. Finally, the dispersion of many-body excitations in a series of hydrogen-terminated graphene flakes (and twisted bilayers thereof) is investigated to highlight the utility of the presented approach for capturing morphology-dependent effects in the inelastic scattering cross sections of nanostructured and/or noncrystalline materials.

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

Prediction of intrinsic topological superconductivity in Mn-doped GeTe monolayer from first-principles

The recent discovery of topological superconductors (TSCs) has sparked enormous interest. The realization of TSC requires a delicate tuning of multiple microscopic parameters, which remains a great challenge. Here, we develop a first-principles approach to quantify realistic conditions of TSC by solving self-consistently Bogoliubov-de Gennes equation based on a Wannier function construction of band structure, in presence of Rashba spin-orbit coupling, Zeeman splitting and electron-phonon coupling. We further demonstrate the power of this method by predicting the Mn-doped GeTe (Ge 1- x Mn x Te) monolayer—a well-known dilute magnetic semiconductor showing superconductivity under hole doping—to be a Class D TSC with Chern number of -1 and chiral Majorana edge modes. By constructing a first-principles phase diagram in the parameter space of temperature and Mn concentration, we propose the TSC phase can be induced at a lower-limit transition temperature of ~40 mK and the Mn concentration of x ~0.015%. Our approach can be generally applied to TSCs with a phonon-mediated pairing, providing useful guidance for future experiments.

Chemistry↗
DOE OSTI2020

Machine learning the Hubbard U parameter in DFT+U using Bayesian optimization

Abstract Within density functional theory (DFT), adding a Hubbard U correction can mitigate some of the deficiencies of local and semi-local exchange-correlation functionals, while maintaining computational efficiency. However, the accuracy of DFT+U largely depends on the chosen Hubbard U values. We propose an approach to determining the optimal U parameters for a given material by machine learning. The Bayesian optimization (BO) algorithm is used with an objective function formulated to reproduce the band structures produced by more accurate hybrid functionals. This approach is demonstrated for transition metal oxides, europium chalcogenides, and narrow-gap semiconductors. The band structures obtained using the BO U values are in agreement with hybrid functional results. Additionally, comparison to the linear response (LR) approach to determining U demonstrates that the BO method is superior.

Chemistry↗
DOE OSTI2025

Accelerating Instanton Theory with the Line Integral Nudged Elastic Band Method and Gaussian Process Regression

Quantum tunneling plays a fundamental role in many chemical reactions, particularly proton transfer processes. Ring polymer instanton theory offers a practical framework for computing tunneling rates in complex molecular systems. However, applying the ring polymer instanton method with a potential energy surface generated on-the-fly using electronic structure calculations can be computationally demanding. Here, in this work, we present a new efficient implementation of the ring polymer instanton method by combining the Line Integral Nudged Elastic Band (LI-NEB) approach with Gaussian Process Regression (GPR). We benchmarked this method on prototypical ground-state proton transfer systems, including the benchmark gas-phase hydrogen abstraction reaction H + CH 4 → H 2 + CH 3 , malonaldehyde, and Z-3-amino-propenal (aminopropenal). Our results show that this approach is an order of magnitude faster than traditional instanton algorithms while maintaining excellent agreement with their tunneling rates. This development opens the door to studying proton transfer in larger systems with improved efficiency.

chemical physics↗
DOE OSTI2022

Low Index Contrast Valley Hall Topological Photonics for Robust Transport in the Visible Spectrum

We report topological photonics is an emerging platform to study light-matter interactions with promising features such as robust edge state transmission that could be advantageous for quantum information applications. However, applying common topological photonic designs for visible wavelength light-matter interactions is challenging because materials compatible with the visible spectrum have lower refractive index contrasts. We design and demonstrate a novel valley Hall topological photonic crystal that can support a complete topological band gap in the visible spectrum. We also show an overetch procedure can be used to reduce the leakage loss common for low index contrast materials. To demonstrate these advantages, we fabricate topological photonic devices following these design principles and show that edge states at energies in the complete band gap have robust transmission around sharp corners. The compatibility of this photonic structure with straightforward fabrication methods will facilitate the study of interactions between topologically nontrivial photons and nanomaterials active in the visible spectrum.

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

Solution-Phase Synthesis and Photoluminescence of Quaternary Chalcohalide Semiconductors

Mixed-metal chalcohalide semiconductors have emerged as promising candidates for photovoltaic applications. However, preparation of these multinary compounds using solution-phase techniques remains particularly challenging compared to traditional solid-state methods. To fully harness their potential, it is desirable to develop synthetic methods that enable control over both the phase purity and dimensionality of chalcohalides. In this work, we report the solution-phase synthesis of Pb 2 SbS 2 I 3 and Pb 2 BiS 2 I 3 quaternary chalcohalides using readily available precursors. Fine tuning of reaction parameters allows for the isolation of rod-like morphologies with tunable diameters and aspect ratios. The quaternary chalcohalides display photoluminescence as an ensemble as well as at the single particle level, as demonstrated using fluorescence microscopy. We further evaluate the relative stability and band gap of Pb 2 SbS 2 I 3 polymorphs and their coloring patterns using electronic structure calculations. The synthetic methods developed here will motivate the study of ever more complex chalcohalides and other multinary semiconductors for new technological applications.

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

Effective bands and band-like electron transport in amorphous solids

The localization of electrons caused by atomic disorder is a well-known phenomenon. However, under which circumstances electrons remain delocalized and retain band-like characteristics even when the crystal structure is completely absent, as found in certain amorphous solids, is less well understood. Here, in this study, to probe this phenomenon, we develop a fully first-principles description of the electronic structure and charge transport in amorphous materials, which combines a representation of the amorphous state as a composite (ensemble) of local environments and the state-of-the-art many-body electronic structure methods. Using amorphous In 2 O 3 as an example, we demonstrate the accuracy of our approach in reproducing the band-like nature of the conduction electrons as well as their disorder-limited mobility. Our approach reveals the physical origins responsible for the electron delocalization and survival of the band dispersions despite the absence of long-range order.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗