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Results for “Phonon Simulation”

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
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Liquid-like dynamics in a solid-state lithium electrolyte

Superionic materials represent a regime intermediate between the crystalline and liquid states of matter. Despite the considerable interest in potential applications for solid-state batteries or thermoelectric devices, it remains unclear whether the fast ionic diffusion observed in superionic materials reflects liquid-like dynamics or whether the hops of mobile ions are inherently coupled to more conventional lattice phonons. Here we reveal a crossover from crystalline vibrations to relaxational dynamics of ionic diffusion in the superionic compound Li 6 PS 5 Cl, a candidate solid-state electrolyte. By combining inelastic and quasi-elastic neutron-scattering measurements with first-principles-based machine-learned molecular dynamics simulations, we found that the vibrational density of states in the superionic state strongly deviates from the quadratic behaviour expected from the Debye law of lattice dynamics. The superionic dynamics emerges from overdamped phonon quasiparticles to give rise to a linear density of states characteristic of instantaneous normal modes in the liquid state. Further, we showed that the coupling of lattice phonons with a dynamic breathing of the Li+ diffusion bottleneck enables an order-of-magnitude increase in diffusivity. Thus, our results shed insights into superionics for future energy storage and conversion technologies.

25 ENERGY STORAGE↗
DOE OSTI2025

Low spontaneous Brillouin scattering in anti-resonant hollow-core fibers in GHz frequency range

Brillouin light scattering (BLS) is a powerful experimental tool that can be used to gain insights into the fundamental and applied properties of matter, like dispersions of quasiparticles in a solid, as well as their spatiotemporal dynamics. Many applications of light scattering favor the use of optical fibers in place of free-space optics. In this study, we compare the performance of anti-resonant hollow core fibers to that of conventional solid core fused silica fibers for BLS experiments in the GHz frequency range. Conventional fibers are barely suitable for low-noise measurements because of the spontaneous scattering of photons on various phononic modes present in the core and cladding. In the case of the hollow-core fiber, we identify a range of discrete phononic modes and associate them with the various acoustic modes of the structure surrounding the hollow core using finite-element numerical simulations. The measured relative intensity of the spontaneous BLS signal from these modes is orders of magnitude smaller than that of a solid-core fiber, making anti-resonant hollow-core fibers one of the best solutions for the single-mode light guidance for BLS and potentially other low-noise photonic experiments.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Proton Collective Quantum Tunneling Induces Anomalous Thermal Conductivity of Ice under Pressure

Proton tunneling is believed to be nonlocal in ice, but its range has been shown to be limited to only a few molecules. Here, we measured the thermal conductivity of ice under pressure up to 50 GPa and found it increases with pressure until 20 GPa but decreases at higher pressures. We attribute this nonmonotonic thermal conductivity to the collective tunneling of protons at high pressures, supported by large-scale quantum molecular dynamics simulations. The collective tunneling loops span several picoseconds in time and are as large as nanometers in space, which match the phonon periods and wavelengths, leading to strong phonon scattering at high pressures. Finally, our results show direct evidence of global quantum motion existing in high-pressure ice and provide a new perspective to understanding the coupling between phonon propagation and atomic tunneling.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Efficient simulation of open quantum systems coupled to a reservoir through multiple channels

It is challenging to simulate open quantum systems that are connected to a reservoir through multiple channels. For example, vibrations may induce fluctuations in both energy gaps and electronic couplings, which represent two independent channels of system–bath couplings. Systems of this kind are ubiquitous in the processes of excited state radiationless decay. Combined with density matrix renormalization group (DMRG) and matrix product states (MPS) methods, we develop an interaction-picture chain mapping strategy for vibrational reservoirs to simulate the dynamics of these open systems, resulting in time-dependent spatially local system–bath couplings in the chain-mapped Hamiltonian. This transformation causes the entanglement generated by the system–bath interactions to be restricted within a narrow frequency window of vibrational modes, enabling efficient DMRG/MPS dynamical simulations. We demonstrate the utility of this approach by simulating singlet fission dynamics using a generalized spin-boson Hamiltonian with both diagonal and off-diagonal system–bath couplings. This approach generalizes an earlier interaction-picture chain mapping scheme, allowing for efficient and exact simulation of systems with multi-channel system–bath couplings using matrix product states, which may further our understanding of nonlocal exciton–phonon couplings in exciton transport and the non-Condon effect in energy and electron transfer.

Chemistry↗
DOE OSTI2025

Generalized approach for rapid entropy calculation of liquids and solids

We build a comprehensive methodology for the fast computation of entropy across both solid and liquid phases. The proposed method utilizes a single trajectory of molecular dynamics (MD) to facilitate the calculation of entropy, which is composed of three components. The electronic entropy is determined through the temporal average acquired from density functional theory MD simulations. The vibrational entropy, typically the predominant contributor to the total entropy, even within the liquid state, is evaluated by computing the phonon density of states via the velocity autocorrelation function. The most arduous component to quantify, the configurational entropy, is assessed by probability analysis of the local structural arrangement and atomic distribution. We illustrate, through a variety of examples, that this method is both a versatile and valid technique for characterizing the thermodynamic states of both solids and liquids. Furthermore, this method is employed to expedite the calculation of melting temperatures, demonstrating its practical utility in computational thermodynamics.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Electronic effects in radiation-induced collision cascades in nickel

The accurate treatment of electronic effects in multi-million-atom simulations of radiation-induced collision cascades is crucial for reliable predictions of primary radiation damage. In this work, we explore the fidelity of a recently developed two-temperature molecular dynamics model implementing an electron density-dependent coupling of electronic and atomic subsystems for cascade simulations in nickel. We show that the parameter-free model realistically captures the instantaneous energy losses during all stages of the highly nonequilibrium cascade process. Our simulations predict two distinct coupling regimes, corresponding to the rapid energy losses through electronic stopping in the early stages of the cascade and to the slow equilibration through the electron-phonon coupling mechanism in the later stages, without the use of separate models or coupling terms. The intermediate stage of the cascade dynamics displays a complex energy transfer between the subsystems, which cannot be interpreted by comparison to either electronic stopping or electron-phonon coupling theories. We therefore compare the predicted atomic mixing, which is sensitive to the energy losses during the intermediate cascade stage, with experimental ion beam mixing measurements. We find good agreement with the experiments, validating the coupling model for the intermediate stage of the cascade. Predictions of final defect numbers and cluster sizes are found in line with the results from conventional electronic stopping-based methods, while significantly reducing the theoretical uncertainty in the outcomes of conventional models stemming from arbitrary choices of thresholds for different coupling terms. Our results represent a notable improvement in cascade damage predictions in nickel, providing validation of the electron density-dependent coupling model for radiation damage simulations in general. The results lead us to propose an interpretation of the electronic energy losses in the intermediate regime of velocities, where we find an effectively nonlinear dissipation.

Crystal defects↗
DOE OSTI2026

Measuring quasiparticle dynamics for particle impact reconstruction in a superconducting qubit chip

Quasiparticle poisoning following particle impacts poses a significant challenge to the development of fault-tolerant superconducting quantum computers, as a sudden excess of quasiparticles can simultaneously degrade the coherence of multiple qubits across large device arrays. In this work, we present a statistical analysis that models the time evolution of radiation-induced qubit energy relaxation through quasiparticle density dynamics. This study provides insight into quasiparticle loss processes by distinguishing between recombination and trapping decay channels and assessing their respective impact on qubit performance. We precisely measure quasiparticle recombination in multiple transmon qubits and uncover an unexpected dependence of qubit relaxation dynamics on deposited energy. By linking correlated relaxation events across qubits to ballistic phonon propagation, we introduce a statistical localization approach to extract the energy deposited in the substrate, which is in good agreement with Monte Carlo simulation. This work establishes the quantitative framework for using an arbitrary subset of superconducting transmon qubits in a QPU as energy-resolving witness particle detectors.

Celi, E. [Northwestern U.]↗
DOE OSTI2024

Probing phonon focusing, thermomechanical behavior, and moiré patterns in van der Waals architectures using surface acoustic waves

Surface acoustic waves (SAWs) propagate along solid-air, solid-liquid, and solid-solid interfaces. Their characteristics depend on the elastic properties of the solid. Combining transmission electron microscopy (TEM) experiments with molecular dynamics (MD) simulations, we probe atomic environments around intrinsic defects that generate SAWs in vertically stacked two-dimensional (2D) bilayers of MoS 2 . Our joint experimental-simulation study provides insights into SAW-induced structural and dynamical changes and thermomechanical responses of MoS 2 bilayers. Using MD simulations, we compute mechanical properties from the SAW velocity and thermal conductivity from thermal diffusion of SAWs. The results for Young’s modulus and thermal conductivity of an MoS 2 monolayer are in good agreement with experiments. The presence of defects, such as nanopores which generate SAWs, reduces the thermal conductivity of 2D-MoS 2 by an order of magnitude. We also observe dramatic changes in moiré patterns, phonon focusing, and cuspidal structures on 2D-MoS 2 layers.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Machine learning interatomic potential for predicting the thermal properties of uranium nitride

We present a combined computational and experimental investigation of the thermal properties of uranium nitride (UN), focusing on the development of a machine learning interatomic potential (MLIP) using the moment tensor potential framework. The MLIP was trained on density functional theory (DFT) data and validated against various quantities including energies, forces, elastic constants, phonon dispersion, and defect formation energies, achieving excellent agreement with DFT calculations, prior experimental results, and our thermal conductivity measurement. The potential was then employed in molecular dynamics simulations to predict key thermal properties such as melting point, thermal expansion, specific heat, and lattice thermal conductivity. To further assess model accuracy, we fabricated a UN sample and performed new thermal conductivity measurements representative of single-crystal properties, which showed strong agreement with the MLIP predictions. This work confirms the reliability and predictive capability of the developed potential for determining the thermal properties of UN.

36 - MATERIALS SCIENCE↗
DOE OSTI2025

Resolving the dynamic correlated disorder in KTa 1- x Nb x O 3

Understanding the complex temporal and spatial correlations of ions in disordered perovskite oxides is critical to rationalize their functional properties. Here, in this study, we provide new insights into the longstanding controversy regarding the off-centering of transition metal ions in the archetypal ferroelectric alloy KTa 1-x Nb x O 3 (KTN). By mapping the full energy (E) and wavevector (Q) dependence of the dynamical structure factor S(Q, E) using neutron scattering, and rationalizing our observations with atomistic simulations leveraging machine learning, we fully resolve the static vs dynamic nature of diffuse scattering sheets, as well as their composition (x) and temperature dependence. Our first-principles simulations, extended with machine-learning molecular dynamics, reproduce both inelastic neutron spectra and diffuse features, and establish how dynamically-correlated transition metal off-centerings couple to phonons, unifying local and collective viewpoints. This study sheds new light into an exemplary ferroelectric systems and shows the importance of mapping the full S(Q, E) to reveal critical spatio-temporal correlations of atomic disorder from which functional properties emerge.

42 ENGINEERING↗
DOE OSTI2026

Revealing the Defect‐Driven Ferroelectric Mechanisms of Aluminum Nitride

Wurtzite III-nitride compounds are CMOS-compatible with widespread industrial interest to exercise ferroelectricity, despite their polar structure being highly resistant to polarization reversal. Here, we induce and tune ferroelectric properties in w-AlN via direct-write ion-beam processing, using nanoscale patterned defect engineering as a post-growth alternative to conventional cation substitution. Nanometric piezoresponse spectroscopy of the focused He + beam patterned defect concentrations in ferroelectric Al 0.92 B 0.08 N measures a localized 10x enhancement in effective piezoresponse and 40% reduction in switching barrier. The irradiation-induced point defects convert piezoelectric AlN into a ferroelectric system with site-saturated nucleation and raise the dielectric susceptibility, switched polarization, and effective piezoelectric coefficient. Enhanced defect-lattice interactions in AlN increase carrier conduction and phonon scattering loss but preserve long-range crystallinity. Here, based on atomistic analysis of nudged elastic band density functional theory calculations and reactive force field simulations, both nitrogen vacancies and defect complexes disrupt bond ordering, facilitating a line-by-line low-barrier switching of pristine AlN.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Long-lived polaritonic coherence and polaron decoupling effects in 2D electronic spectra

Molecular polaritons, formed by coupling molecular excitons with cavity photons, offer a promising platform for exploring quantum phenomena. A key challenge is understanding how these hybrid states maintain coherence in the presence of environmental vibrations. Here, we show theoretically that collective coupling of many molecular excitons in a cavity can protect polariton coherence from phonon-induced decoherence. Under realistic conditions, the coherence time can extend up to 200 fs at room temperature, compared with 15 fs for typical molecular systems. Simulations of two-dimensional electronic spectra reveal prolonged oscillations between upper and lower polariton states, and reduced vibrational coupling as indicated by changes in the nodal line slope of the lower polariton peak. These findings provide guidance for experimental efforts to realize long-lived polaritons, such as coupling CdSe nanoplatelets to optical cavities.

2D electronic spectroscopy↗
NASA NTRS2003

Investigarion of the effects of a quantum dot crystal geometry on its brillouin spectrum

We develop a theoretical model and carry out simulation of Brillouin spectrum of three-dimensional (3D) quantum dot (QD) arrays with a high order of 3D periodicity, i.e. quantum dot crystals (QDC). The phonon spectrum of Ge/Si QDC is found from the numerical solution of the elasticity equation for the whole structure. The developed approach is valid for any QD shape and regimentation and allows to include disorder in consider at ion.

quantum dot arrays quantum dot crystal raman spect↗
DOE OSTI2025

Parameterizing empirical interatomic potentials for predicting thermophysical properties via an irreducible derivative approach: the case of ThO 2 and UO 2

The accuracy of classical physical property predictions using molecular dynamics simulations is determined by the quality of the interatomic potentials. Here we introduce a training approach for empirical interatomic potentials (EIPs) which is well suited for capturing phonons and phonon-related properties. Our approach is based on direct comparisons of the second- and third-order irreducible derivatives (IDs) between an EIP and the Born–Oppenheimer potential within density functional theory (DFT) calculations. IDs fully exploit space group symmetry and allow for training without redundant information. We demonstrate the fidelity of our approach in the context of ThO 2 and UO 2 , where we optimize parameters of an embedded-atom method potential in addition to core–shell interactions. Our EIPs provide thermophysical properties in good agreement with DFT and outperform widely utilized EIPs for phonon dispersion and thermal conductivity predictions. Reasonable estimates of thermal expansion and formation energies of Frenkel pairs are also obtained.

empirical interatomic potential↗
DOE OSTI2025

Correlated dynamic disorder, octahedral tilts, and acoustic phonon softening in CsSnBr 3 and CsPbBr 3

Metal halide perovskites (MHPs) have emerged as highly promising materials for optoelectronic applications, with all-inorganic MHPs presenting enhanced stability compared to their hybrid counterparts. Here, in this study, we investigate the atomic dynamics and structural fluctuations in single crystals of CsSnBr⁢ 3 and CsPbBr⁢ 3 through systematic inelastic neutron scattering (INS) measurements as a function of temperature. Our experiments are compared with first-principle simulations, augmented with large-scale molecular dynamics modeling, based on machine-learned neural network potentials. Through both INS and simulations, we find quasi-elastic diffuse rods in reciprocal space in both compounds, originating from fluctuating planar domains featuring correlated tilts of Br octahedron. The diffuse rods exhibit a slow, overdamped dynamic process, modulated across 𝑸 space, reflecting the strong lattice anharmonicity of the inorganic framework. We do not find evidence for dynamic off-centering of the Sn 2+ ions besides phonon vibrations at the center of the Br octahedron. These results offer valuable insights into the unusual anharmonic atomic dynamics and intricate correlated structural distortions in MHPs, which will be critical for rationalizing and further tailoring their thermal and optoelectronic properties.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Excitons in Hematite Fe 2 O 3 : Short-Time Dynamics from TD-DFT and Non-Adiabatic Dynamics Theories

We present a first-principles study of the short-time dynamics of excitons in hematite Fe 2 O 3 . We used time-dependent density functional theory (TD-DFT) with an underlying DFT+U treatment of electron interactions to characterize the electronic structure of excitons and nonadiabatic molecular dynamics theory (NA-MD) to determine their recombination (electronic ground-state recovery) and relaxation dynamics. Decoherence-corrected trajectory surface hopping approaches in NA-MD simulations yielded recovery times of ~1.1 to 1.8 ns and “higher-lying” exciton relaxation times of ~60 to 70 fs, in accord with experimentally derived lifetimes. With hematite phonons in the range of ~100 to 700 cm –1 , higher-lying excitons relax within one or two oscillations of the phonons before getting trapped into an electron–hole pair Exc-3 structure on the first excited state potential energy surface. This structure resembles already a pair of polarons (electron polaron plus hole polaron) with associated lattice distortions three (3) basal planes away. On longer time scales, the electron–hole bipolaronic pair hops to structures Exc-5, then Exc-7, then Exc-9, ... with the electron polaron and hole polaron separated by 5, 7, 9, ... basal planes in a process of charge separation. The largest frequency phonon ~672 cm –1 for the Exc-3 exciton structure is associated with the electron polaron moiety of the exciton. This phonon is a good candidate for giving rise to the recently observed and reported postexcitation transient IR absorption peak.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Efficient simulations of charge density waves in the transition metal Dichalcogenide TiSe 2

Charge density waves (CDWs) in transition metal dichalcogenides are the subject of growing scientific interest due to their rich interplay with exotic phases of matter and their potential technological applications. Here, using density functional theory with advanced meta-generalized gradient approximations (meta-GGAs) and linear response time-dependent density functional theory (TDDFT) with state-of-the-art exchange-correlation kernels, we investigate the electronic, vibrational, and optical properties in 1T-TiSe 2 with and without CDW. In both bulk and monolayer TiSe 2 , the electronic bands and phonon dispersions in either normal or CDW (semiconducting) phase are described well via meta-GGAs, which separate the valence and conduction bands just as HSE06 does but with significantly more computational feasibility. The experimentally observed humps of electron energy loss spectroscopy are successfully reproduced in TDDFT. Our work opens the door to simulating these complexities in CDW compounds from first principles by revealing meta-GGAs as an accurate low-cost alternative to HSE06.

Electronic properties and materials↗
DOE OSTI2025

Transferable dispersion-aware machine learning interatomic potentials for multilayer transition metal dichalcogenide heterostructures

Stacking atomically thin transition metal dichalcogenides (TMDs) into heterostructures enables exploration of exotic quantum phases, particularly through twist-angle-controlled moiré superlattices. These structures exhibit novel electronic and optical behaviors driven by atomic-scale structural reconstruction. However, studying such systems with DFT is computationally demanding due to their large unit cells and van der Waals (vdW) interactions between layers. To address this, we develop a transferable neural network potential (NNP) that includes long-range vdW corrections up to 12Å with minimal overhead. Trained on vdW-corrected DFT data for Mo- and W-based TMDs with S, Se, and Te, the NNP accurately models monolayers, bilayers, heterostructures, and their interaction with h-BN substrates. It reproduces equilibrium structures, energy landscapes, phonon dispersions, and matches experimental atomic reconstructions in twisted WS2 and MoS2/WSe2 systems. We demonstrate that our NNP achieves DFT-level accuracy and high computational efficiency, enabling large-scale simulations of TMD-based moiré superlattices both with and without substrates.

materials for energy and catalysis↗