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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 775 records · Page 43
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Negative Thermal Expansion Near the Precipice of Structural Stability in Open Perovskites

Negative thermal expansion (NTE) describes the anomalous propensity of materials to shrink when heated. Since its discovery, the NTE effect has been found in a wide variety of materials with an array of magnetic, electronic and structural properties. In some cases, the NTE originates from phase competition arising from the electronic or magnetic degrees of freedom but we here focus on a particular class of NTE which originates from intrinsic dynamical origins related to the lattice degrees of freedom, a property we term structural negative thermal expansion (SNTE). Here we review some select cases of NTE which strictly arise from anharmonic phonon dynamics, with a focus on open perovskite lattices. We find that NTE is often present close in proximity to competing structural phases, with structural phase transition lines terminating near T =0 K yielding the most prominent displays of the SNTE effect. We further provide a theoretical model to make precise the proposed relationship among the signature behavior of SNTE, the proximity of these systems to structural quantum phase transitions and the effects of phase fluctuations near these unique regions of the structural phase diagram. Thus, the effects of compositional disorder on NTE and structural phase stability in perovskites are discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Energetic Stability of Freestanding and Metal-Supported Borophenes: Quantum Monte Carlo and Density-Functional Theory Calculations

Quantum Monte Carlo (QMC) and density-functional theory (DFT) calculations were carried out to study cohesion energetics of two-dimensional (2D) sheets of boron atoms called borophenes. Our QMC calculations confirmed the polymorphism among free-standing borophenes that was reported in previous DFT studies. Although Perdew-Burke-Ernzerhof (PBE) calculations significantly overestimate the cohesive energies of 2D boron sheets, DFT-PBE relative energetics with respect to each other among various free-standing borophenes are found to be in quantitative agreement with the corresponding QMC results. This suggests that one can make reliable predictions for relative stability of different boron sheets through DFT-PBE calculations. Our analysis of PBE formation energies of borophenes on metal surfaces shows that the polymorphic range is extended for borophenes on the Ag(111) and the Au(111) surfaces beyond that of free-standing borophenes, reflecting recent experimental synthesis of beta(12) and chi(3) boron sheets on the Ag(111) surface. We have also found that a hexagonal borophene can be stabilized through charge transfer from a metal surface and is energetically favored on the AI(111) surface over other borophene structures. Finally, it is found that the bilayer formation could be energetically favored over its monolayer form for the borophene-Au system, especially for borophenes with hexagonal hole densities eta lower than 1/9. This leads to our prediction that in addition to its monolayer form, a bilayer eta = 1/12 borophene can be synthesized on the Au(111) surface, opening a new possibility for borophene-based electronic devices.

ab initio↗
DOE OSTI2018

Dissipative tunnelling by means of scaled trajectories

Dissipative quantum tunnelling through an inverted parabolic barrier is considered in the presence of an electric field. A Schrödinger–Langevin or Kostin quantum–classical transition wave equation is used and applied resulting in a scaled differential equation of motion. A Gaussian wave packet solution to the resulting scaled Kostin nonlinear equation is assumed and compared to the same solution for the scaled linear Caldirola–Kanai equation. The resulting scaled trajectories are obtained at different dynamical regimes and friction cases, showing the gradual decoherence process in this open dynamics. Theoretical results show that the transmission probabilities are always higher in the Kostin approach than in the Caldirola–Kanai approach in the presence or not of an external electric field. This discrepancy should be understood due to the presence of an environment since the corresponding open dynamics should be governed by nonlinear quantum equations, whereas the second approach is issued from an effective Hamiltonian within a linear theory.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Computing molecular excited states on a D-Wave quantum annealer

Abstract The possibility of using quantum computers for electronic structure calculations has opened up a promising avenue for computational chemistry. Towards this direction, numerous algorithmic advances have been made in the last five years. The potential of quantum annealers, which are the prototypes of adiabatic quantum computers, is yet to be fully explored. In this work, we demonstrate the use of a D-Wave quantum annealer for the calculation of excited electronic states of molecular systems. These simulations play an important role in a number of areas, such as photovoltaics, semiconductor technology and nanoscience. The excited states are treated using two methods, time-dependent Hartree–Fock (TDHF) and time-dependent density-functional theory (TDDFT), both within a commonly used Tamm–Dancoff approximation (TDA). The resulting TDA eigenvalue equations are solved on a D-Wave quantum annealer using the Quantum Annealer Eigensolver (QAE), developed previously. The method is shown to reproduce a typical basis set convergence on the example $$\hbox {H}_2$$ H 2 molecule and is also applied to several other molecular species. Characteristic properties such as transition dipole moments and oscillator strengths are computed as well. Three potential energy profiles for excited states are computed for $$\hbox {NH}_3$$ NH 3 as a function of the molecular geometry. Similar to previous studies, the accuracy of the method is dependent on the accuracy of the intermediate meta-heuristic software called qbsolv.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Advancing molecular machine learning representations with stereoelectronics-infused molecular graphs

Molecular representation is a critical element in our understanding of the physical world and the foundation for modern molecular machine learning. Previous molecular machine learning models have used strings, fingerprints, global features and simple molecular graphs that are inherently information-sparse representations. However, as the complexity of prediction tasks increases, the molecular representation needs to encode higher fidelity information. This work introduces a new approach to infusing quantum-chemical-rich information into molecular graphs via stereoelectronic effects, enhancing expressivity and interpretability. Learning to predict the stereoelectronics-infused representation with a tailored double graph neural network workflow enables its application to any downstream molecular machine learning task without expensive quantum-chemical calculations. We show that the explicit addition of stereoelectronic information substantially improves the performance of message-passing two-dimensional machine learning models for molecular property prediction. We show that the learned representations trained on small molecules can accurately extrapolate to much larger molecular structures, yielding chemical insight into orbital interactions for previously intractable systems, such as entire proteins, opening new avenues of molecular design. Finally, we have developed a web application (simg.cheme.cmu.edu) where users can rapidly explore stereoelectronic information for their own molecular systems.

Boiko, Daniil A↗
DOE OSTI2018

The finale of a trilogy: comparing terpolymers and ternary blends with structurally similar backbones for use in organic bulk heterojunction solar cells

Building on our previous works that compared the efficacy of terpolymers vs. ternary blends in improving the performance of bulk heterojunction organic solar cells, the final piece of this series of studies focuses on comparing terpolymer and ternary blends constructed with two polymers with structurally similar backbones (monoCNTAZ and FTAZ) yet markedly different open circuit voltage (V oc ) values. Furthermore, terpolymers and ternary blends of five different ratios were studied and the results demonstrate that while the overall performance of both the systems is similar, the ternary blends exhibit higher short circuit current (J sc ) values, while the terpolymers exhibit higher V oc values. Investigation of the charge transfer state using low-energy external quantum efficiency (EQE) indicates that the ternary blends are governed by a parallel-like mechanism, while the terpolymer does not follow this mechanism. Furthermore, the key morphological difference between the systems, as elucidated by resonance soft X-ray scattering (RSoXS), is the slightly smaller size (~60 nm) of domains in the ternary blends compared to that of the terpolymer (~80 nm), which may affect exciton harvesting in the terpolymer system and lead to lower J sc values. In addition, a lower driving force for the formation of charge transfer (CT) state is also likely to contribute to the lower J sc values in the terpolymer system. All together, the data show that structurally similar (perhaps even miscible) polymers still exhibit key differences in performance when paired in terpolymers vs. ternary blends and allow us to further illuminate the underlying mechanisms of such complex systems.

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

An accurate and efficient fragmentation approach via the generalized many-body expansion for density matrices

With relevant chemical space growing larger and larger by the day, the ability to extend computational tractability over that larger space is of paramount importance in virtually all fields of science. The solution we aim to provide here for this issue is in the form of the generalized many-body expansion for building density matrices (GMBE-DM) based on the set-theoretical derivation with overlapping fragments, through which the energy can be obtained by a single Fock build. In combination with the purification scheme and the truncation at the one-body level, the DM-based GMBE(1)-DM-P approach shows both highly accurate absolute and relative energies for medium-to-large size water clusters with about an order of magnitude better than the corresponding energy-based GMBE(1) scheme. Simultaneously, GMBE(1)-DM-P is about an order of magnitude faster than the previously proposed MBE-DM scheme [F. Ballesteros and K. U. Lao, J. Chem. Theory Comput. 18, 179 (2022)] and is even faster than a supersystem calculation without significant parallelization to rescue the fragmentation method. For even more challenging systems including ion–water and ion–pair clusters, GMBE(1)-DM-P also performs about 3 and 30 times better than the energy-based GMBE(1) approach, respectively. In addition, this work provides the first overlapping fragmentation algorithm with a robust and effective binning scheme implemented internally in a popular quantum chemistry software package. Thus, GMBE(1)-DM-P opens a new door to accurately and efficiently describe noncovalent clusters using quantum mechanics.

Chemistry↗
DOE OSTI2014

Role of microstructures on the M1-M2 phase transition in epitaxial VO2 thin films

Vanadium dioxide (VO2) with its unique sharp resistivity change at the metal-insulator transition (MIT) has been extensively considered for the near-future terahertz/infrared devices and energy harvesting systems. Controlling the epitaxial quality and microstructures of vanadium dioxide thin films and understanding the metal-insulator transition behaviors are therefore critical to novel device development. The metal-insulator transition behaviors of the epitaxial vanadium dioxide thin films deposited on Al2O3 (0001) substrates were systematically studied by characterizing the temperature dependency of both Raman spectrum and Fourier transform infrared spectroscopy. Our findings on the correlation between the nucleation dynamics of intermediate monoclinic (M2) phase with microstructures will open a new avenue for the design and integration of advanced heterostructures with controllable multifunctionalities for sensing and imaging system applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Robust estimation of charge carrier diffusivity using transient photoluminescence microscopy

Transient microscopy has emerged as a powerful tool for imaging the diffusion of excitons and free charge carriers in optoelectronic materials. In many excitonic materials, extraction of diffusion coefficients can be simplified because of the linear relationship between signal intensity and local excited state population. However, in materials where transport is dominated by free charge carriers, extracting diffusivities accurately from multidimensional data is complicated by the nonlinear dependence of the measured signal on the local charge carrier density. To obtain accurate estimates of charge carrier diffusivity from transient microscopy data, statistically robust fitting algorithms coupled to efficient 3D numerical solvers that faithfully relate local carrier dynamics to raw experimental measurables are sometimes needed. Here, we provide a detailed numerical framework for modeling the spatiotemporal dynamics of free charge carriers in bulk semiconductors with significant solving speed reduction and for simulating the corresponding transient photoluminescence microscopy data. To demonstrate the utility of this approach, we apply a fitting algorithm using a Markov chain Monte Carlo sampler to experimental data on bulk CdS and methylammonium lead bromide (MAPbBr 3 ) crystals. Parameter analyses reveal that transient photoluminescence microscopy can be used to obtain robust estimates of charge carrier diffusivities in optoelectronic materials of interest, but that other experimental approaches should be used for obtaining carrier recombination constants. Additionally, simplifications can be made to the fitting model depending on the experimental conditions and material systems studied. Our open-source simulation code and fitting algorithm are made freely available to the scientific community.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Critical role of intermediate electronic states for spin-flip processes in charge-transfer-type organic molecules with multiple donors and acceptors

Spin-flip in purely organic molecular systems is often described as a forbidden process; however, it is commonly observed and utilized to harvest triplet excitons in a wide variety of organic-material-based applications. Although the initial and final electronic states of the spin-flip between the lowest singlet and lowest triplet excited state are self-evident, the exact process and the role of intermediate states through which spin-flip occurs are still far from being comprehensively determined. Here, via experimental photo-physical investigations in solution combined with first-principles quantum-mechanical calculations, we show that efficient spin-flip in multi-donor-acceptor charge-transfer (CT)-type organic molecular systems involves the critical role of an intermediate triplet excited state that corresponds to a partial molecular structure of the system. Furthermore, our proposed mechanism unifies the understanding of the intersystem crossing mechanism in a wide variety of CT-type molecular systems, opening the way to greater control over the spin-flip rates.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Implementation of a laser–neutron pump–probe capability for inelastic neutron scattering

Knowledge about nonequilibrium dynamics in spin systems is of great importance to both fundamental science and technological applications. Inelastic neutron scattering (INS) is an indispensable tool to study spin excitations in complex magnetic materials. However, conventional INS spectrometers currently only perform steady-state measurements and probe averaged properties over many collision events between spin excitations in thermodynamic equilibrium, while the exact picture of re-equilibration of these excitations remains unknown. In this paper, we report on the design and implementation of a time-resolved laser–neutron pump–probe capability at hybrid spectrometer (beamline 14-B) at the Spallation Neutron Source (SNS) at Oak Ridge National Laboratory. This capability allows us to excite out-of-equilibrium magnons with a nanosecond pulsed laser source and probe the resulting dynamics using INS. Here, we discussed technical aspects to implement such a capability in a neutron beamline, including choices of suitable neutron instrumentation and material systems, laser excitation scheme, experimental configurations, and relevant firmware and software development to allow for time-synchronized pump–probe measurements. We demonstrated that the laser-induced nonequilibrium structure factor is able to be resolved by INS in a quantum magnet. In conclusion, the method developed in this work will provide SNS with advanced capabilities for performing out-of-equilibrium measurements, opening up an entirely new research direction to study out-of-equilibrium phenomena using neutrons.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Sparse adaptive basis set methods for solution of the time dependent Schrodinger equation

Scalable numerical solutions to the time dependent Schrodinger equation remain an outstanding goal in theoretical chemistry. Here we present a method which utilises recent breakthroughs in signal processing to consistently adapt a dictionary of basis functions to the dynamics of the system. Further, we show that for two low-dimensional model problems the size of the basis set does not grow quickly with time and appears only weakly dependent on dimensionality. The generality of this finding remains to be seen. The method primarily uses energies and gradients of the potential, opening the possibility for its use in on-the-fly ab initio quantum wavepacket dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Atomic layer epitaxy of kagome magnet Fe 3 Sn 2 and Sn-modulated heterostructures

Magnetic materials with kagome crystal structure exhibit rich physics, such as frustrated magnetism, skyrmion formation, topological flat bands, and Dirac/Weyl points. Until recently, most studies on kagome magnets have been performed on bulk crystals or polycrystalline films. Here, we report the atomic layer molecular beam epitaxy synthesis of high-quality thin films of topological kagome magnet Fe 3 Sn 2 . The structural and magnetic characterization of Fe 3 Sn 2 on epitaxial Pt(111) identifies highly ordered films with c-plane orientation and an in-plane magnetic easy axis. Studies on the local magnetic structure by anomalous Nernst effect imaging reveal in-plane oriented micrometer size domains. Superlattice structures consisting of Fe 3 Sn 2 and Fe 3 Sn are also synthesized by atomic layer molecular beam epitaxy, demonstrating the ability to modulate the sample structure at the atomic level. The realization of high-quality films by atomic layer molecular beam epitaxy opens the door to explore the rich physics of this system and investigate novel spintronic phenomena by interfacing Fe 3 Sn 2 with other materials.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Visualizing the photovoltaic behavior of a type-II p-n heterojunction superstructure

Photovoltaic behavior of a CaFe{sub 2}O{sub 4}/ZnFe{sub 2}O{sub 4} p-n multi-junction was investigated with electron holography combined with an in situ light irradiation system. Potential profiles of the samples with and without light irradiation were extracted to measure the open circuit photovoltage generated either by the whole heterojunction superstructure or from each p-n junction. Investigation on the variation in the energy band configuration under light irradiation revealed the mechanism involved in the photoelectric effect, with respect to the properties of the heterojunction and its periodic quantum structure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Transcendental equations in the Schwinger-Keldysh nonequilibrium theory and nonvanishing correlations

The Schwinger-Keldysh nonequilibrium theory allows the description of various transport phenomena involving bosons (fermions) embedded in bosonic (fermionic) environments. The retarded Green’s function obeys the Dyson equation and determines via its non-vanishing asymptotic behavior the dissipationless open dynamics. The appearance of this regime is conditioned by the existence of the solution of a general class of transcendental equations in complex domain that we study. Particular cases consist in transcendental equations containing exponential, hyperbolic, power law, logarithmic, and special functions. The present analysis provides an analytical description of the thermal and temporal correlation function of two general observables of a quantum system in terms of the corresponding spectral function. Special integral properties of the spectral function guarantee non-vanishing asymptotic behavior of the correlation function.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Atomic-scale strain manipulation of a charge density wave

Significance Charge density waves (CDWs) are simple periodic reorganizations of charge in a crystal, and yet they are still poorly understood and continue to bear surprises. External perturbations, such as strain or pressure, can in principle push a CDW phase into a different ordering geometry. However, engineering this type of quantum criticality has been experimentally challenging. Here, we implement a simple method for straining bulk materials. By applying it to 2H -NbSe 2 , a prototypical CDW system studied for decades, we discover two dramatic strain-induced CDW phase transitions. Our atomic-scale spectroscopic imaging measurements, combined with theory, reveal the distinct roles of electrons and phonons in forming these emergent states, thus opening a window into the rich phenomenology of CDWs.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Role of non-Gaussian quantum fluctuations in neutrino entanglement

The flavor evolution of neutrinos in environments with large neutrino number densities is an open problem at the nexus of astrophysics and neutrino flavor physics. Among the many unanswered questions pertaining to this problem, it remains to be determined whether neutrino-neutrino coherent scattering can give rise to nontrivial quantum entanglement among neutrinos, and whether this can affect the flavor evolution in a meaningful way. To gain further insight into this question, here we study a simple system of two interacting neutrino beams and obtain the exact phase space explored by this system using the Husimi quasiprobability distribution. We observe that the entanglement induced by the coupling leads to strong delocalization in phase-space with largely non-Gaussian quantum fluctuations. The link between the neutrino entanglement and quantum fluctuations is illustrated using the one- and two-neutrino entropy. In addition, we propose an approximate phase-space method to describe the interacting neutrinos problem, where the exact evolution is replaced by a set of independent mean-field evolutions with a statistical sampling of the initial conditions. The phase-space approach provides a simple and accurate method to describe the gross features of the neutrino entanglement problem. Applications are shown using time-independent and time-dependent Hamiltonians in the nonadiabatic regime.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗