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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 91 records · Page 5
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DOE OSTI2021

Predicting 1 H NMR relaxation in Gd 3+ -aqua using molecular dynamics simulations

Atomistic molecular dynamics simulations are used to predict 1 H NMR T 1 relaxation of water from paramagnetic Gd 3+ ions in solution at 25 °C. Simulations of the T 1 relaxivity dispersion function r 1 computed from the Gd 3+ – 1 H dipole–dipole autocorrelation function agree within ≃8% of measurements in the range f 0 ≃ 5 ↔ 500 MHz, without any adjustable parameters in the interpretation of the simulations, and without any relaxation models. Here the simulation results are discussed in the context of the Solomon-Bloembergen-Morgan inner-sphere relaxation model, and the Hwang-Freed outer-sphere relaxation model. Below f 0 ≲ 5 MHz, the simulation overestimates r 1 compared to measurements, which is used to estimate the zero-field electron-spin relaxation time. The simulations show potential for predicting r 1 at high frequencies in chelated Gd 3+ contrast-agents used for clinical MRI.

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

Reduction of electron-phonon coupling in warm dense iron

The electron-ion relaxation dynamics in warm dense iron were investigated by time-resolved x-ray absorption near-edge spectroscopy (XANES). A novel analysis, combining ab initio density functional theory (DFT) and two temperature model (TTM) simulations, was developed to calculate the x-ray absorption spectra as a function of delay time. Here we present experimental evidence of changes at the XAS L3 edge of iron that are consistent with the reduction of the electron-phonon coupling under warm dense matter conditions. The experimental results are in agreement with the model that takes both the electron ($T_e$) and the ion temperature ($T_i$) dependence of the thermophysical properties into consideration, while models where either constant electron-phonon coupling factor (G) or only $T_e$- dependent G are used do not agree with the observed relaxation dynamics of iron.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Relaxation mechanisms in a disordered system with Poisson-level statistics

Here we discuss the interplay between many-body localization and spin symmetry. To this end, we study the time evolution of several observables in the anisotropic t- j model. Like the Hubbard chain, the studied model contains charge and spin degrees of freedom, yet it has smaller Hilbert space and thus allows for numerical studies of larger systems. We compare the field disorder that breaks the $\mathbb{Z}_2$ spin symmetry and a potential disorder that preserves the latter symmetry. In the former case, sufficiently strong disorder leads to localization of all studied observables, at least for the studied system sizes. However, in the case of symmetry-preserving disorder, we observe that odd operators under the $\mathbb{Z}_2$ spin transformation relax towards the equilibrium value at relatively short timescales that grow only polynomially with the disorder strength. On the other hand, the dynamics of even operators and the level statistics within each symmetry sector are consistent with localization. Our results indicate that localization exists within each symmetry sector for symmetry-preserving disorder. Odd operators' apparent relaxation is due to their time evolution between distinct symmetry sectors.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Electric fields and substrates dramatically accelerate spin relaxation in graphene

Electrons in graphene are theoretically expected to retain spin states much longer than most materials, making graphene a promising platform for spintronics and quantum information technologies. Here, in this work, we use first-principles density-matrix (FPDM) dynamics simulations to show that interaction with electric fields and substrates strongly enhances spin relaxation through scattering with phonons. Consequently, the relaxation time at room temperature reduces from microseconds in free-standing graphene to nanoseconds in graphene on the hexagonal boron nitride (hBN) substrate, which is the order of magnitude typically measured in experiments. Further, inversion symmetry breaking by hBN introduces a stronger asymmetry in electron and hole spin lifetimes than predicted by the conventional D'yakonov-Perel' (DP) model for spin relaxation. Deviations from the conventional DP model are stronger for in-plane spin relaxation, resulting in out-of-plane to in-plane lifetime ratios much greater than 1/2 with a maximum close to the Dirac point. These FPDM results, independent of symmetry-specific assumptions or material-dependent parameters, also validate recent modifications of the DP model to explain such deviations. Overall, our results indicate that spin-phonon relaxation in the presence of substrates may be more important in graphene than typically assumed, requiring consideration for graphene-based spin technologies at room temperature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Molecular-Level Insights into the NMR Relaxivity of Gadobutrol Using Quantum and Classical Molecular Simulations

MRI is an indispensable diagnostic tool in modern medicine; however, understanding the molecular-level processes governing NMR relaxation of water in the presence of MRI contrast agents remains a challenge, hindering the molecular-guided development of more effective contrast agents. By using quantum-based polarizable force fields, the first-of-its-kind molecular dynamics (MD) simulations of Gadobutrol are reported where the 1 H NMR longitudinal relaxivity r 1 of the aqueous phase is determined without any adjustable parameters. The MD simulations of r 1 dispersion (i.e., frequency dependence) show good agreement with measurements at frequencies of interest in clinical MRI. Importantly, the simulations reveal key insights into the molecular level processes leading to r 1 dispersion by decomposing the NMR dipole–dipole autocorrelation function G(t) into a discrete set of molecular modes, analogous to the eigenmodes of a quantum harmonic oscillator. The molecular modes reveal important aspects of the underlying mechanisms governing r 1 , such as its multiexponential nature and the importance of the second eigenmodal decay. By simply analyzing the MD trajectories on a parameter-free approach, the Gadobutrol simulations show that the outer-shell water contributes ∼50% of the total relaxivity r 1 compared to the inner-shell water, in contrast to simulations of (nonchelated) gadolinium-aqua where the outer shell contributes only ∼15% of r 1 . The deviation between simulations and measurements of r 1 below clinical MRI frequencies is used to determine the low-frequency electron-spin relaxation time for Gadobutrol, in good agreement with independent studies.

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

Similarity of capacitive radio-frequency discharges in nonlocal regimes

Similarity transformations are essential for correlating discharges at different scales, which are mostly utilized with local field or local energy approximations. In this work, we report the fully kinetic results from particle-in-cell/Monte Carlo collision simulations that unambiguously demonstrate the similarity of radio frequency (rf) discharges in nonlocal regimes where the electron energy relaxation length is much larger than the gap dimension. It is found that at a constant rf voltage amplitude, discharges will be similar if the gas pressure, inverse of gap distance, and rf driving frequency are all changed by the same scaling factor. The scaling relations of fundamental parameters are illustrated for rf discharges in the alpha-mode with secondary electron emission ignored, and the temporal electron kinetics are shown to have invariance in similar discharges. The results explicitly validate the scaling laws in nonlocal kinetic regimes, indicating promising application potentials of the similarity transformations across a wide range of kinetic regimes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Accurate tight-binding model for twisted bilayer graphene describes topological flat bands without geometric relaxation

A major hurdle in understanding the phase diagram of twisted bilayer graphene is the roles of lattice relaxation and electronic structure on isolated band flattening near magic twist angles. Here in this work, the authors develop an accurate local environment tight-binding model fit to tight-binding parameters computed from ab initio density-functional theory calculations across many atomic configurations. With the accurate parametrization, it is found that the magic angle shifts to slightly lower angles than often quoted, from around 1.05° to around 0.99°, and that isolated flat bands appear for rigidly rotated graphene layers, with enhancement of the flat bands when the layers are allowed to distort. Study of the orbital localization supports the emergence of fragile topology in the isolated flat bands without the need for lattice relaxation.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Thermal and concentration effects on 1 H NMR relaxation of Gd 3+ -aqua using MD simulations and measurements

We report gadolinium-based contrast agents are key in clinical MRI for enhancing the longitudinal NMR relativity (r 1 ) of hydrogen nuclei ( 1 H) in water and improving the contrast among different tissues. The importance of MRI in clinical practice cannot be gainsaid, yet the interpretation of MRI relies on models with severe assumptions, reflecting a poor understanding of the molecular-scale relaxation processes. In a step towards building a clearer understanding of the relaxation processes, here we investigate thermal and concentration effects on r 1 of the Gd 3+ -aqua complex using both semi-classical molecular dynamics (MD) simulations and measurements. We follow the MD simulation approach recently introduced by [Singer et al., Phys. Chem. Chem. Phys., 2021, 23, 20974], in which no NMR relaxation model or free-parameter is assumed to predict r 1 , thereby bringing new insights into the physics of r 1 on a molecular scale. We expand the autocorrelation function G(t) in terms of molecular modes and determine the thermal activation energies of the two largest modes, both of which are consistent with the range of literature values for rotational diffusion. We also determine the activation energies for translational diffusion and low-field electron-spin relaxation, both of which are consistent with the literature. Furthermore, we validate the MD simulations at human body temperature and concentrations of the paramagnetic ion used in clinical MRI, and we quantify the uncertainties in both simulations and measurements.

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

Hofstadter butterfly and quantum transport benchmarks in PVA-exfoliated graphene heterostructures

Polymer exposure during van der Waals heterostructure fabrication is widely regarded as compromising the integrity of the electronic system required for hosting emergent quantum physics. This assumption has persisted largely because electronic benchmarking of heterostructures from polymer-exposed graphene has remained limited to only foundational transport metrics, such as mobility and charge inhomogeneity. Here, we challenge this assumption by establishing that graphene heterostructures produced by polyvinyl alcohol (PVA)-assisted exfoliation and encapsulated in hexagonal boron nitride using elevated-temperature lamination satisfy demanding quantum transport benchmarks. Beyond exhibiting ultra-high mobility and ballistic transport, these heterostructures yield quantum scattering times comparable to the best polymer-free devices. Most demanding of all, moiré superlattices from PVA-exposed graphene exhibit Hofstadter butterfly spectra, confirming spatially uniform interlayer coupling across the device area. These results establish that PVA exposure is compatible with low-disorder electronic systems, relaxing the trade-off between scalable fabrication and low-disorder quantum transport. This study motivates further development of polymer-assisted assembly with engineered residue-removal protocols.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Dispersive Charge Transfer State Electroluminescence in Organic Solar Cells

Abstract The notion of quasi‐equilibrium is central to most solar cells; however, it has been questioned in organic photovoltaics (OPVs) owing to strong energetic disorder that frustrates efficient relaxation of electrons and holes within their respective density of states (DOS). Here, modulation electroluminescence (EL) spectroscopy is applied to OPVs and it is found that the frequency response of charge transfer (CT) state EL on the high energy side of the spectrum differs from that of the low energy side. This observation confirms that static disorder contributes substantially to the linewidth of the steady‐state EL spectrum and is unambiguous proof that the distribution of CT states formed by electrical injection in the dark is not in quasi‐equilibrium. These results emphasize the need for caution when analyzing OPV cells on the basis of reciprocity models that assume quasi‐equilibrium holds, and highlight a new method to study this unusual aspect of OPV operation.

14 SOLAR ENERGY↗
DOE OSTI2023

Plasmon-enhanced optical nonlinearity in graphene nanomeshes

Using the density-matrix formalism, here we show that graphene nanomeshes (GNMs)—graphene sheets patterned with antidots—have large plasmon-enhanced nonlinear optical response. GNMs can be designed to behave as quasi-one-dimensional plasmonic crystals in which plasmons with large propagation lengths are efficiently excited. The associated third-order Kerr and third-harmonic-generation susceptibility can be as high as 10 –7 and 10 –9 m 2 V –2 , respectively, over the mid-to-near-infrared frequency range. Furthermore, carrier-density tuning in GNMs can flip the propagation direction of plasmonic waves and enables bidirectional switching of optical signals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Average-atom calculations of bound-free and free-free cross sections in dense plasmas

Cross sections for photo-induced bound-free and free-free transitions in plasmas are evaluated in the average-atom approximation and applied to determine opacities of dense plasmas of light elements. Parameters characterizing the plasmas (chemical potential, average ionic charge, free electron density, bound and continuum wave functions, and occupation numbers) are obtained from the average-atom model. Lowest-order calculations of the free-free cross sections, which diverge in the low-frequency limit, are regularized by accounting for the finite electron-ion relaxation time. The resulting analysis provides the basis for average-atom studies of plasma opacities. Such studies are presented for dense lithium, beryllium, boron, and carbon. Applications are given to Rosseland mean opacities of dense hydrogen and deuterium plasmas and to comparisons of free-free to bound-free opacities in shock-compressed plasmas. Average-atom cross section and opacity calculations are extended to plasmas consisting of more than one ionic species, boron nitride, polystyrene, and a composite H, He, C plasma.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Mixed Stochastic-Deterministic Approach for Many-Body Perturbation Theory Calculations

Here, we present an approach for GW calculations of quasiparticle energies with quasi-quadratic scaling by approximating high-energy contributions to the Green's function in its Lehmann representation with effective stochastic vectors. The method is easy to implement without altering the GW code, converges rapidly with stochastic parameters, and treats systems of various dimensionality and screening response. Our calculations on a 5.75° twisted MoS 2 bilayer show how large-scale GW methods include geometry relaxations and electronic correlations on an equal basis in structurally nontrivial materials.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Optimal strategies for optical quantum memories using long-lived noble-gas spins

Nuclear spins of noble gases exhibit exceptionally long coherence times and can potentially serve as a long-lived storage medium for quantum information. We analyze and compare the performance of two mechanisms for mapping the quantum state of light onto the collective spin state of noble gases. The first mechanism utilizes collisional exchange with the electronic spin state of metastable noble-gas atoms, while the second relies on spin-exchange collisions with ground-state alkali-metal atoms. We describe the operation of an optical quantum memory relying on these two mechanisms using a compact model and study strategies that optimize the memory storage efficiency. Through numerical simulations, we identify optimal sequences for storing optical signals with different signal bandwidths and electronic spin relaxation rates. This work highlights the qualitative difference between the two approaches for using noble gases as long-lived quantum memories at noncryogenic conditions and outlines the regimes in which they are expected to be efficient.

atomic ensemble↗
DOE OSTI2020

Ultrafast dynamics in the high-symmetry and in the charge density wave phase of 2 H –NbSe 2

Here we investigate carrier and collective mode dynamics in 2H-NbSe 2 using time-resolved optical pump-probe spectroscopy and compare the results with first-principles calculations. Broadband ultrafast reflectivity studies of 2H-NbSe 2 in a wide temperature interval covering the normal, charge density wave (CDW) and superconducting phase were performed. Spectral features observed in the transient reflectivity experiment were associated with specific optical transitions obtained from band structure calculations. Displacive excitation of coherent phonons showed CDW-associated coherent oscillations of the soft phonon mode across the whole spectral range. Temperature evolution of this coherent phonon mode in the low-excitation linear regime shows softening of the mode down to the CDW transition temperature T CDW with subsequent hardening below T CDW . The global fit of the broadband probe data reveals four different relaxation times associated with characteristic electron-electron, electron-phonon, and phonon-phonon relaxation processes. From first-principles calculations of electron-phonon coupling we associate the few picosecond electron-phonon relaxation time $\tau_2$ with a specific group of phonons with frequencies around 20 meV. On the other hand, the anomalously long relaxation time of $\tau_3 \sim$ to 100 ps is associated with anharmonicity-driven phonon-phonon scattering. All relaxation processes result from anomalies near the second order CDW phase transition that are reflected in the temperature dependencies of the characteristic relaxation times and amplitudes of coherent oscillations. At the highest fluences we observe electronic melting of the CDW and disappearance of the mode hardening below T CDW .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

The impact of stacking and phonon environment on energy transfer in organic chromophores: computational insights

Energy transfer in organic materials is extensively studied due to many applications in optoelectronics. The electronic and vibrational relaxations within molecular assemblies can be influenced by stacking arrangements or additions of a backbone that unites them. Here, we present the computational study of the photoexcitation dynamics of a perylene diimide monomer, and face-to-face stacked dimer and trimer. By using non-Energy transfer in organic materials is extensively studied due to many applications in optoelectronics. The electronic and vibrational relaxations within molecular assemblies can be influenced by stacking arrangements or additions of a backbone that unites them. In this work, we present the computational study of the photoexcitation dynamics of a perylene diimide monomer, and face-to-face stacked dimer and trimer. By using non-adiabatic excited-state molecular dynamics simulations, we show that the non-radiative relaxation is accelerated with the number of stacked molecules. This effect is explained by differences in the energy splitting between states that impacts their corresponding nonadiabatic couplings. Additionally, our analysis of the vibronic dynamics reveals that the passage through the different conical intersections that participate in the relaxation of the stacked systems, activate a positive feedback mechanism. This effect involves a narrow set of vibrational normal modes that accelerate the process by increasing the efficiency of its vibronic dynamics. In contrast, an addition of a biologically inspired backbone slows down the relaxation rate due to its participation in the vibronic dynamics of the molecular stacking arrangements. Our results suggest the stacking arrangements and common backbones as strategies to modulate the efficiency of electronic and vibrational relaxation of diimide-based systems and other molecular aggregates.

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

Thermal effects mediating the flow induced by laser-induced optical breakdown

Here, a short focused laser pulse can generate a hot plasma, which expands then contracts and can eject a hot jet, the speed and direction of which is sensitive to the details of the plasma kernel. The coupling of thermal and chemical nonequilibrium plasma mechanisms with this hydrodynamic development is assessed with detailed simulations of a two-temperature, three-species plasma model. Time scales for electron recombination, thermal relaxation, and diffusion are compared to that of the plasma expansion to anticipate conditions in which these mechanisms might affect the vorticity generation that leads to the ultimate flow pattern. The effect of these mechanisms are analyzed through comparison with corresponding inert-gas and equilibrium models. Thermal-nonequilibrium effects are found to be weak due to rapid relaxation of the heavy-particle and electronic temperatures. In contrast, chemical equilibration occurs at a rate comparable to the expansion and thereby enhance both it and subsequent hydrodynamic mechanisms as the energy stored in ion formation during the preceding breakdown is released by electron recombination. Thermal conduction, enhanced by high-temperature free electrons, weakens the ejection.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Spin-orbit coupling induced demagnetization in Ni: Ab initio nonadiabatic molecular dynamics perspective

Spin-orbit coupling (SOC), which can induce spin flip during the relaxation of photoexcited charge carrier, plays a crucial role in spin dynamics. Here in this work, we have used time-domain ab initio nonadiabatic molecular dynamics (NAMD) method to study the SOC induced ultrafast demagnetization in Ni at 300K. The spin-diabatic representation using spin-polarized Kohn-Sham (KS) basis sets and spin-adiabatic representation using spinor basis sets have been applied, and both of them achieve demagnetization in Ni with a timescale around 100fs. The spin-diabatic representation suggests a picture that the electron-phonon coupling (EPC) provides direct energy relaxation channel among the same-spin states, while the SOC can induce spin flip. After photoexcitation, it is found the spin-minority electrons relax to the same-spin states rather than the opposite-spin states, since EPC is larger than SOC by one order of magnitude. By contrast, for the spin-majority electrons, spin flip occurs since there are no empty same-spin states as electron acceptor above the Fermi level. The different relaxation pathways for spin-majority and spin-minority electrons induce the demagnetization. The spin-adiabatic representation provides an Elliott-Yafet spin-phonon scattering picture. The SOC induced reduction of magnetic moment in Ni may induce magnon to drive further demagnetization. The ab initio NAMD simulation provides a critical angle to understand how the SOC and EPC affect demagnetization process in Ni.

36 MATERIALS SCIENCE↗