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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 1,639 records · Page 91
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Exploring the role of electronic structure on photo-catalytic behavior of carbon-nitride polymorphs

A fully self-consistent density-functional theory (DFT) with improved functionals is used herein to provide a comprehensive account of structural, electronic, and optical properties of C 3 N 4 polymorphs. Using our recently developed van Leeuwen-Baerends (vLB) corrected local-density approximation (LDA), we implemented LDA + vLB within full-potential N th -order muffin-tin orbital (FP-NMTO) method and show that it improves structural properties and band gaps compared to semi-local functionals (LDA/GGA). We demonstrate that the LDA + vLB predicts band-structure and work-function for well-studied 2D-graphene and bulk-Si in very good agreement with experiments, and more exact hybrid functional (HSE) calculations as implemented in the Quantum-Espresso (QE) package. The structural and electronic-structure (band gap) properties of C 3 N 4 polymorphs calculated using FP-NMTO-LDA + vLB is compared with more sophisticated hybrid-functional calculations. We also perform detailed investigation of photocatalytic behavior using QE-HSE method of C 3 N 4 polymorphs through work-function, band (valence and conduction) position with respect to water reduction and oxidation potential. Our results show $γ$-C 3 N 4 as the best candidate for photocatalysis among all the C 3 N 4 polymorphs but it is dynamically unstable at ‘zero’ pressure. We show that $γ$-C 3 N 4 can be stabilized under hydrostatic-pressure, which improves its photocatalytic behavior relative to water reduction and oxidation potentials.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Fidelity and entanglement entropy for infinite-order phase transitions

Here, we study the fidelity and the entanglement entropy for the ground states of quantum systems that have infinite-order quantum phase transitions. In particular, we consider the quantum O(2) model with a spin-S truncation, where there is an infinite-order Gaussian (IOG) transition for S = 1 and there are Berezinskii-Kosterlitz-Thouless (BKT) transitions for S ≥ 2. We show that the height of the peak in the fidelity susceptibility (χ F ) converges to a finite thermodynamic value as a power law of 1 / L for the IOG transition and as 1 / ln (L) for BKT transitions. The peak position of χ F resides inside the gapped phase for both the IOG transition and BKT transitions. On the other hand, the derivative of the block entanglement entropy with respect to the coupling constant $S^{'}_{vN}$ has a peak height that diverges as ln 2 (L) for S = 1 and ln 3 (L) for S ≥ 2 and can be used to locate both kinds of transitions accurately. We include higher-order corrections for finite-size scalings and obtain the value of the central charge consistent with c = 1 predicted by conformal field theory. The crossing point of χ F between different system sizes is at the IOG point for S = 1 but is inside the gapped phase for S ≥ 2, while those of $S^{'}_{vN}$ are at the phase-transition points for all S truncations. Our work elaborates on how to use the finite-size scaling of χ F or $S^{'}_{vN}$ to detect infinite-order quantum phase transitions and discusses the efficiency and accuracy of the two methods.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Graph-EAM: An Interpretable and Efficient Graph Neural Network Potential Framework

The development of deep learning interatomic potentials has enabled efficient and accurate computations in quantum chemistry and materials science, circumventing computationally expensive ab initio calculations. However, the huge number of learnable parameters in deep learning models and their complex architectures hinder physical interpretability and affect the robustness of the derived potential. In this work, we propose graph-EAM, a lightweight graph neural network (GNN) inspired by the empirical embedded atom method to model the interatomic potential of single-element structures. Four material systems: platinum, niobium, silicon, and amorphous-carbon, for which quantum simulation data sets are publicly available, are examined to demonstrate that graph-EAM can achieve high energy and force prediction accuracy-comparable or better than existing state-of-the-art machine learning models-with much fewer parameters. It is also shown that the explicit inclusion of the angular information via three-body atomic density increases the prediction accuracy. In conclusion, the accuracy and efficiency of potentials obtained from graph-EAM can help accelerate the molecular dynamics simulation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

2D Exotic Optical Lattice via a Digital‐Coding Circular Airy Beam

Optical lattices have been widely used from classical to quantum physics. The tunable and scalable fabrication of lattices would be of great significance in lattice‐based multipartite applications. This work demonstrates first that a circular Airy beam (CAB), which has the peculiar properties of self‐healing and abrupt autofocusing, can be used to generate two‐dimensional (2D) optical lattices in propagation when encoded by a programmable spatial mask, resulting in the formation of large‐scale and tunable optical lattices with both axis and axial symmetry, and even high‐orbital kaleidoscope shapes. The efficient diffraction of CAB during the spatial crosstalk with the mask enables the realization of tunable lattices with rich periodicity and complexity. The study shows a flexible method to manipulate lattices with large‐scale and versatile structures for potential applications in integrated and scalable optical and photonic devices.

Sun, Peisheng↗
DOE OSTI2021

High-Resolution Momentum Imaging—From Stern’s Molecular Beam Method to the COLTRIMS Reaction Microscope [Book Chapter]

Multi-particle momentum imaging experiments are now capable of providing detailed information on the properties and the dynamics of quantum systems in Atomic, Molecular and Photon (AMO) physics. Historically, Otto Stern can be considered the pioneer of high-resolution momentum measurements of particles moving in a vacuum and he was the first to obtain sub-atomic unit (a.u.) momentum resolution (Schmidt-Böcking et al. in The precision limits in a single-event quantum measurement of electron momentum and position, these proceedings). A major contribution to modern experimental atomic and molecular physics was his so-called molecular beam method, which Stern developed and employed in his experiments. With this method he discovered several fundamental properties of atoms, molecules and nuclei. As corresponding particle detection techniques were lacking during his time, he was only able to observe the averaged footprints of large particle ensembles. Today it is routinely possible to measure the momenta of single particles, because of the tremendous progress in single particle detection and data acquisition electronics. A “state-of-the-art” COLTRIMS reaction microscope can measure, for example, the momenta of several particles ejected in the same quantum process in coincidence with sub-a.u. momentum resolution. Such setups can be used to visualize the dynamics of quantum reactions and image the entangled motion of electrons inside atoms and molecules. This review will briefly summarize Stern’s work and then present in longer detail the historic steps of the development of the COLTRIMS reaction microscope. Furthermore, some benchmark results are shown which initially paved the way for a broad acceptance of the COLTRIMS approach. Finally, a small selection of milestone work is presented which has been performed during the last two decades.

Jahnke, T.↗
DOE OSTI2026

Supercurrents and (partial) supersymmetry in adjoint QCD 2 and its generalizations

1 + 1-dimensional SU(N) gauge theory coupled to an adjoint Majorana fermion, also known as adjoint QCD 2 , has the surprising feature that at fermion mass $\sqrt{\frac{g^2N}{2\pi }}$ it exhibits supersymmetry. In this paper, we obtain a deeper insight into how the supersymmetry works by constructing the gauge invariant, Lorentz covariant supercurrent j μA . Its conservation relies crucially on the presence of a quantum anomaly. We generalize this construction to a class of models where, in addition to an adjoint Majorana fermion of an appropriate mass, the gauge theory is coupled to some collection of massless fermions (SU(N) may be replaced by a more general gauge group). In general, these models have a supersymmetric massive sector and a non-supersymmetric CFT sector [1], but there are cases in which both sectors are supersymmetric. An example of such a gapless, fully supersymmetric model is SU(N) gauge theory coupled to three adjoint Majorana fermions, of which two are massless and the third has mass $\sqrt{\frac{3{g}^2N}{2\pi }}$.

anomalies in field and string theories↗
DOE OSTI2023

Exotic field theories for (hybrid) fracton phases from imposing constraints in foliated field theory

Fracton phases of matter are gapped phases of matter that, by dint of their sensitivity to UV data, demand non-standard quantum field theories to describe them in the IR. Two such approaches are foliated quantum theory and exotic field theory. In this paper, we explicitly construct a map from one to the other and work out several examples. In particular, we recover the equivalence between the foliated and exotic fractonic BF theories recently demonstrated at the level of operator correspondence. We also demonstrate the equivalence of toric code layers and the anisotropic model with lineons and planons to the foliated BF theory with one and two foliations, respectively. Finally, we derive new exotic field theories that provide simple descriptions of hybrid fracton phases from foliated field theries known to do so. Our results both provide new examples of exotic field theories and pave the way toward their systematic construction from foliated field theories.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

First-Principles Dissociation Pathways of BCl 3 on the Si(100)-2 × 1 Surface

BCl 3 is a promising acceptor precursor for atomic-precision δ-doping of silicon, as it has been observed to rapidly dissociate into boron doped into the silicon surface and surface chlorine, which can be removed upon annealing. The chemical pathway and the resulting kinetics, through which BCl 3 adsorbs and dissociates on silicon, however, have only been partially explained. Here, in this work, we use density functional theory to expand the dissociation reactions of BCl 3 to include reactions that take place across multiple silicon dimer rows and reactions which end in a bare B atom either at the surface, substituted for a surface silicon, or in a subsurface position. We further simulate the resulting scanning tunneling microscopy images for each of these BCl x dissociation fragments, demonstrating that they often display distinct features that may allow for relatively confident experimental identification. Finally, we input the full dissociation pathway for BCl 3 into a kinetic Monte Carlo model, which simulates realistic reaction pathways as a function of environmental conditions, such as the pressure and temperature of dosing. We find that BCl 2 is broadly dominant at low temperatures, while high temperatures and ample space on the silicon surface for dissociation encourage the formation of bridging BCl fragments and B substitutions on the surface. This work provides the chemical mechanisms for understanding atomic-precision doping of Si with B, enabling a number of relevant quantum applications, such as bipolar nanoelectronics, acceptor-based qubits, and superconducting Si.

Campbell, Quinn T. [Sandia National Laboratories (↗
DOE OSTI2022

Microbial biofilms as living photoconductors due to ultrafast electron transfer in cytochrome OmcS nanowires

Light-induced microbial electron transfer has potential for efficient production of value-added chemicals, biofuels and biodegradable materials owing to diversified metabolic pathways. However, most microbes lack photoactive proteins and require synthetic photosensitizers that suffer from photocorrosion, photodegradation, cytotoxicity, and generation of photoexcited radicals that are harmful to cells, thus severely limiting the catalytic performance. Therefore, there is a pressing need for biocompatible photoconductive materials for efficient electronic interface between microbes and electrodes. Here we show that living biofilms of Geobacter sulfurreducens use nanowires of cytochrome OmcS as intrinsic photoconductors. Photoconductive atomic force microscopy shows up to 100-fold increase in photocurrent in purified individual nanowires. Photocurrents respond rapidly (<100 ms) to the excitation and persist reversibly for hours. Femtosecond transient absorption spectroscopy and quantum dynamics simulations reveal ultrafast (~200 fs) electron transfer between nanowire hemes upon photoexcitation, enhancing carrier density and mobility. Our work reveals a new class of natural photoconductors for whole-cell catalysis.

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

Cavity-altered superconductivity

Is it feasible to alter the ground-state properties of a material by engineering its electromagnetic environment? Inspired by theoretical predictions, experimental realizations of such cavity-controlled properties without optical excitation are beginning to emerge. Here we devised and implemented a new platform to realize cavity-altered materials. Single crystals of hyperbolic van der Waals (vdW) compounds provide a resonant electromagnetic environment with enhanced density of photonic states and prominent mode confinement. We interfaced hexagonal boron nitride (hBN) with the molecular superconductor κ-(BEDT-TTF) 2 Cu[N(CN) 2 ]Br (κ-ET). The frequencies of infrared hyperbolic modes (HMs) of hBN match the infrared-active carbon–carbon (C=C) stretching molecular resonance of κ-ET implicated in superconductivity. Nano-optical data supported by first-principles molecular Langevin dynamics simulations confirm the presence of resonant coupling between the hBN hyperbolic cavity modes and the C=C stretching mode in κ-ET. Meissner-effect measurements using magnetic force microscopy (MFM) demonstrate a strong suppression of superfluid density near the hBN/κ-ET interface. Non-resonant control heterostructures, including RuCl 3 /κ-ET and hBN/Bi 2 Sr 2 CaCu 2 O 8+x (BSCCO), do not show the pronounced superfluid suppression. These observations suggest that hBN/κ-ET realizes a cavity-altered superconducting ground state. Our work highlights the potential of dark cavities devoid of external photons for engineering electronic ground-state properties of complex quantum materials.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Giant defect emission enhancement from ZnO nanowires through desulfurization process

Zinc oxide (ZnO) is a stable, direct bandgap semiconductor emitting in the UV with a multitude of technical applications. It is well known that ZnO emission can be shifted into the green for visible light applications through the introduction of defects. However, generating consistent and efficient green emission through this process is challenging, particularly given that the chemical or atomic origin of the green emission in ZnO is still under debate. In this work we present a new method, for which we coin term desulfurization, for creating green emitting ZnO with significantly enhanced quantum efficiency. Solution grown ZnO nanowires are partially converted to ZnS, then desulfurized back to ZnO, resulting in a highly controlled concentration of oxygen defects as determined by X-ray photoelectron spectroscopy and electron paramagnetic resonance. Using this controlled placement of oxygen vacancies we observe a greater than 40-fold enhancement of integrated emission intensity and explore the nature of this enhancement through low temperature photoluminescence experiments.

36 MATERIALS SCIENCE↗
DOE OSTI2020

The role of resonant nuclear modes in vibrationally assisted energy transport: The LHCII complex

In this paper, we discuss the explicit role of resonant nuclear/vibrational modes in mediating energy transport among chlorophylls in the Light-harvesting Complex II (LHCII), the major light-harvesting complex in green plants. The vibrational modes are considered to be resonant/quasi-resonant with the energy gap between electronic excitons. These resonant vibrations, along with the remaining nuclear degrees of freedom, constitute the environment/bath to the electronically excited system and contribute to two major phenomena: (a) decoherence and (b) incoherent phonon-mediated population relaxation. In this work, we explore the subtle interplay among the electronic excitation, the resonant vibrations, and the environment in dictating environment assisted quantum transport in light-harvesting complexes. We conclusively show that resonant vibrations are capable of boosting the incoherent population relaxation pathways and cause rapid decoherence.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

An ab initio exciton model for singlet fission

Here we present an ab initio exciton model that extends the Frenkel exciton model and includes valence, charge-transfer, and multiexcitonic excited states. It serves as a general, parameter-free, yet computationally efficient and scalable approach for simulation of singlet fission processes in multichromophoric systems. A comparison with multiconfigurational methods confirms that our exciton model predicts consistent energies and couplings for the pentacene dimer and captures the correct physics. Calculations of larger pentacene clusters demonstrate the computational scalability of the exciton model and suggest that the mixing between local and charge-transfer excitations narrows the gap between singlet and multiexcitonic states. Local vibrations of pentacene molecules are found to facilitate singlet–multiexcitonic state-crossing and hence are important for understanding singlet fission. The exciton model developed in this work also sets the stage for further implementation of the nuclear gradients and nonadiabatic couplings needed for first principles nonadiabatic quantum molecular dynamics simulations of singlet fission.

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

Surrogate Hessian accelerated structural optimization for stochastic electronic structure theories

In this work, we present an efficient energy-based method for structural optimization with stochastic electronic structure theories, such as diffusion quantum Monte Carlo (DMC). This method is based on robust line-search energy minimization in reduced parameter space, exploiting approximate but accurate Hessian information from a surrogate theory, such as density functional theory. The surrogate theory is also used to characterize the potential energy surface, allowing for simple but reliable ways to maximize statistical efficiency while retaining controllable accuracy. We demonstrate the method by finding the minimum DMC energy structures of the selected flake-like aromatic molecules, such as benzene, coronene, and ovalene, represented by 2, 6, and 19 structural parameters, respectively. In each case, the energy minimum is found within two parallel line-search iterations. The method is near-optimal for a line-search technique and suitable for a broad range of applications. It is easily generalized to any electronic structure method where forces and stresses are still under active development and implementation, such as diffusion Monte Carlo, auxiliary-field Monte Carlo, and stochastic configuration interaction, as well as deterministic approaches such as the random-phase approximation. Accurate and efficient means of geometry optimization could shed light on a broad class of materials and molecules, showing high sensitivity of induced properties to structural variables.

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

Benchmarking the semi-stochastic CC( P;Q ) approach for singlet–triplet gaps in biradicals

Here, we recently proposed a semi-stochastic approach to converging high-level coupled-cluster (CC) energetics, such as those obtained in the CC calculations with singles, doubles, and triples (CCSDT), in which the deterministic CC(P;Q) framework is merged with the stochastic configuration interaction Quantum Monte Carlo propagations [J. E. Deustua, J. Shen, and P. Piecuch, Phys. Rev. Lett. 119, 223003 (2017)]. In this work, we investigate the ability of the semi-stochastic CC(P;Q) methodology to recover the CCSDT energies of the lowest singlet and triplet states and the corresponding singlet–triplet gaps of biradical systems using methylene, (HFH) − , cyclobutadiene, cyclopentadienyl cation, and trimethylenemethane as examples.

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

Origin of the $ν$ = 1/2 fractional quantum Hall effect in wide quantum wells

The nature of the fractional quantum Hall effect at ν = 1/2, observed in wide quantum wells al- most three decades ago, is still under debate. Previous studies have investigated it by the variational Monte Carlo method, which assumes that the transverse wave function and the gap between the symmetric and antisymmetric subbands obtained in a local density approximation at zero magnetic field remain valid even at high perpendicular magnetic fields; this method also ignores the effect of Landau level mixing. We develop in this work a three-dimensional fixed phase diffusion Monte Carlo method, which gives, in a single framework, the total energies of various candidate states in a finite width quantum well, including Landau level mixing, directly in a large magnetic field. This method can be applied to one-component states, and also to two-component states in the limit where the symmetric and antisymmetric bands are nearly degenerate. Our three-dimensional fixed-phase diffusion Monte Carlo calculations find that the one-component composite-fermion Fermi sea and the one-component Pfaffian states are very close in energy for a range of quantum well widths and densities, suggesting that the observed 1/2 fractional quantum Hall state in wide quantum wells is likely to be the one-component Pfaffian state. Furthermore, we hope that this will motivate further experimental studies of this state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Excitons and trions in monolayer semiconductors with correlated electrons

We revisit low-temperature optical spectra of transition-metal dichalcogenide monolayers and point to a possible crystallization of electrons (or holes) at low to moderate charge densities. To calculate the excitonic spectra under such conditions, we introduce the recursion method and compute how the charge density affects the energies, linewidths, and oscillator strengths of exciton and trion complexes. Equally important, we study how excitons and trions in the monolayer evolve when the charge particles gradually transition to a periodic Wigner lattice. The results provide valuable information on the ability to detect whether the particles are ordered through the exciton spectrum. Finally, we calculate the change in exciton energy in cases where the added charge particles have similar and dissimilar quantum numbers (spin and valley) to those of the electron or hole in the exciton. Here, the results of this work shed new light on the important optical properties of monolayer semiconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Angle-resolved pair photoemission theory for correlated electrons

Here in this paper we consider the possibility and conditions for pair photoemission whereby two incident photons emit pairs of electrons from a candidate material as a novel method to measure and visualize electronic correlations. As opposed to double photoemission - where a single photon precipitates the ejection of a pair electrons via a subsequent electron energy loss scattering process - we show that pair photoemission need not be limited to interference between initial photoelectrons and valence electrons, and moreover, can occur without the energy penalty of two work functions. This enables detection of pairs of electrons at high energy resolution that may be correlated in the same quantum many-body states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗