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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

A chemical bonding based descriptor for predicting the role of anharmonicity induced by quantum nuclear effects in hydride superconductors

Quantum nuclear effects (QNEs) can significantly alter a material’s crystal structure and phonon spectra, impacting properties such as thermal conductivity and superconductivity. However, predicting a priori whether these effects will enhance or suppress superconductivity, or destabilize a structure, remains a grand challenge. Herein, we address this unresolved problem by introducing two possible descriptors, based upon the integrated crystal orbital bonding index (iCOBI) or the bond valence function, to predict the influence of QNEs on a crystal lattice’s dynamic stability, phonon spectra and superconducting properties. We find that structures with atoms in symmetric chemical bonding environments exhibit greater resilience to structural perturbations induced by QNEs, while those with atoms in asymmetric bonding environments are more susceptible to structural alterations, resulting in enhanced superconducting critical temperatures.

Physical chemistry↗
DOE OSTI2025

Nuclear quantum effects of metal surface-mediated C–H activation

The nuclear quantum effects of surface-mediated C–H activation of surface CH 3 are considered for the pristine Pt(111) and Au(111) surfaces at 300 K. The kinetic barriers without nuclear quantum effects are calculated using both static density functional theory calculations and ab initio molecular dynamics. Static calculations are performed using the harmonic approximation while the free energy pathway is calculated using enhanced sampling molecular dynamics. Machine learning potentials are trained using generated datasets and validated against the ab initio molecular dynamics generated free energy pathways. The machine learning potentials are used to perform centroid molecular dynamics to consider the nuclear quantum effects of C–H activation. Nuclear quantum effects are found to have a very significant effect on the free energy pathway, with reduced importance at higher temperatures and in the CD 3 case.

Bunting, Rhys J. [Lawrence Livermore National Labo↗
DOE OSTI2025

Nuclear quantum effects in molecular liquids across chemical space

Abstract Nuclear quantum effects (NQEs) influence many physical and chemical phenomena, particularly those involving light atoms or occurring at low temperatures. However, their impact has been carefully quantified in few systems-like water-and is rarely considered more broadly. Here we use path-integral molecular dynamics to systematically investigate NQEs on thermophysical properties of 92 organic liquids at ambient conditions. Depending on chemical constitution, we find substantial impact across thermal expansivity, compressibility, dielectric constant, enthalpy of vaporization, and notably molar volume, which shows consistent, positive quantum-classical differences up to 5%; similar, less pronounced trends manifest as isotope effects from deuteration. Using data-driven analysis, we identify three features-molar mass, classical hydrogen density, and classical thermal expansivity-that accurately predict NQEs and facilitate understanding of how characteristics like branching and heteroatom content influence behavior. This work highlights the broad relevance of NQEs in molecular liquids, while also providing a conceptual and practical framework to anticipate their impact.

Science & Technology - Other Topics↗
DOE OSTI2025

Anharmonic phonons, thermal expansion, and nuclear quantum effects in Zn

The anharmonic behavior of phonons and thermal expansion of hexagonal zinc were studied from 15 to 690 K by inelastic neutron scattering (INS) and ab initio simulations. Phonon spectra were measured for Q-points covering the full Brillouin zone, giving the phonon density of states (DOS) and dispersions along high-symmetry directions. The dispersions were sharp at 15 K, but diffuse intensity was observed at energies above them. The dispersions broadened with temperature T and the diffuse intensity became stronger. This diffuse intensity appeared in all INS measurements and simulations, except for classical molecular dynamics at 15 K. The temperature-dependent effective potential (TDEP) method, which included the nuclear quantum effect from zero-point vibrational dynamics, was used to calculate the free energy and thermal expansion. For T < 100 K nuclear quantum effects were important for obtaining the correct negative thermal expansion, and path integral molecular dynamics (PIMD) was particularly effective for obtaining the negative thermal expansion in the basal plane. A Heisenberg-Langevin model for interacting phonons coupled to a thermal bath was able to reproduce the shape and intensity of the diffuse spectral features.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Nuclear Quantum Effects on the Electronic Structure of Water and Ice

The electronic properties and optical response of ice and water are intricately shaped by their molecular structure, including the quantum mechanical nature of the hydrogen atoms. Despite numerous previous studies, a comprehensive understanding of the nuclear quantum effects (NQEs) on the electronic structure of water and ice at finite temperatures remains elusive. Here, we utilize molecular simulations that harness efficient machine-learning potentials and many-body perturbation theory to assess how NQEs impact the electronic bands of water and hexagonal ice. By comparing path-integral and classical simulations, we find that NQEs lead to a larger renormalization of the fundamental gap of ice, compared to that of water, ultimately yielding similar bandgaps in the two systems, consistent with experimental estimates. Our calculations suggest that the increased quantum mechanical delocalization of protons in ice, relative to water, is a key factor leading to the enhancement of NQEs on the electronic structure of ice.

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

Two-dimensional ring polymer molecular dynamics determination of the MnO + + H 2 /D 2 reaction rates on a Δ-machine learned potential energy surface

In this work, we investigate the impact of nuclear quantum effects in the kinetics of the MnO + + H 2 reaction, a prototypical system for gas-phase H 2 activation by transition metal oxide ions. The DFT based potential energy surfaces (PESs) for the lowest-lying quintet and septet spin states reported in our previous work are improved by 2953 newly calculated CCSD(T)/AVDZ points using a delta-machine learning (Δ-ML) method. To examine nuclear quantum effects, the rate coefficients are computed using ring-polymer molecular dynamics (RPMD). Due to the mechanistic complexity of the reaction, two reaction coordinates are necessary to map out the free-energy surface and an extended RPMD rate theory is developed. The calculated RPMD rate coefficients on the new PES are in better agreement with experimental data. The calculated kinetic isotope effects (KIEs) range from 1.6 to 1.8, also in good agreement with the experimental values. Additionally, the converged RPMD rate coefficients are 2.3 to 3.1 times higher than their classical counterparts across the studied temperature range, suggesting the presence of moderate nuclear quantum effects in this reaction.

Liu, Yang [University of New Mexico, Albuquerque, ↗
DOE OSTI2025

New Methods for Predicting Non-Born-Oppenheimer Chemistry

Current methods for modeling non-adiabatic molecular dynamics face fundamental limitations when treating geometric phase effects: quantum mechanical phenomena where nuclear wavepackets acquire phase shifts when encircling conical intersections. Existing approaches either neglect these effects entirely or rely on potential energy surfaces arising from the Born-Oppenheimer approximation, which introduce artificial singularities and can overestimate geometric phase contributions. This project developed a new theoretical framework based on exact factorization (XF) methods to overcome these limitations. We derived mathematical formulations for hybrid quantum-classical XF dynamics that selectively treat critical nuclear degrees of freedom quantum mechanically while propagating others classically. This approach addresses the computational intractability that has previously limited exact methods to toy systems. Key innovations include a new approach to systematically identifying nuclear coordinates requiring quantum treatment, as well as novel implementation strategies that interface with existing quantum chemistry codes. The project also developed a proof-of-concept code for treating Jahn-Teller systems and creation of educational materials on non-adiabatic dynamics geared at the graduate level. The theoretical framework developed will enable future systematically improvable calculations of nuclear quantum effects in realistic molecular systems, filling a critical gap in non-adiabatic dynamics methods. This foundation supports future development of predictive tools for designing energy-relevant photochemical processes where quantum coherence effects may be exploited to control reaction outcomes.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2026

MixPI: Mixed-time slicing path integral software for quantized molecular dynamics simulations

We introduce the MixPI software to implement path integral molecular dynamics (PIMD) simulations for the study of condensed phase systems where nuclear quantum effects (NQEs) are important. In contrast to existing PIMD simulation software, MixPI enables the implementation of mixed quantum–classical path integral simulations where only a subset of system degrees of freedom (dofs) are treated quantum mechanically in an extended phase space while the remaining dofs are described classically. We expect this software to be particularly useful for simulations of electron and proton transfer in condensed phase systems, as well as for the study of biological and material systems where only a handful of dofs contribute significantly to the observed NQEs. We demonstrate the use of MixPI in two different systems. The first is a simple water model where we implement a set of mixed quantum–classical simulations to compute average energy and radial distribution functions. We use these simulations to benchmark the effectiveness of MixPI and to demonstrate how it enables systematic investigation into the origin of observed NQEs. We then compute radial distribution functions for a system where MixPI is essential: a solvated metal (M 2+ ) cation described using an explicit quantized electron localized on an M 3+ ion in water.

chemical physics↗
DOE OSTI2024

Self-diffusion of liquid deuterium hydride and liquid tritium

Here, we present a quasi-elastic neutron scattering study of liquid deuterium hydride carried out using the Disk Chopper Spectrometer at the National Institute of Standards and Technology. Under saturated vapor pressure, the self-diffusion constant of deuterium hydride obeys an Arrhenius law D = D 0 exp(-E A /k B T), where the prefactor D 0 is given by D 0 = 9.5 ± 1.2 Å 2 /ps and the activation energy is given by E A = 58 ± 2 K. We apply the quantum law of corresponding states to the known diffusion constants of the hydrogen isotopologues. From this application, we estimate that D 0 ≈ 9.1 Å 2 /ps and E A ≈ 75 K in liquid tritium. Young’s theory of quantum-mechanical effects in van der Waals fluids is shown to apply to the diffusion constants of the liquid hydrogens. Our results underscore the importance of nuclear quantum effects in shaping the properties and behavior of the hydrogen isotopologues.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Quantum stabilization and flat hydrogen-based bands of nitrogen-doped lutetium hydride

We explore the electronic and structural properties of Lu-H-N structures with specific N,H ordering due to their remarkably narrow hydrogen-based bands at the Fermi level. Although exhibits a classical instability persisting up to 17 GPa, it is anharmonically stable near ambient pressure when accounting for quantum nuclear effects. The presence of flat bands near is understood to arise from destructive quantum interference between and surrounding orbitals, with certain types of defects leaving the flat bands unaffected. The results suggest that if this system is superconducting, there is an optimal pressure near ambient where the superconducting is maximized by anharmonically stabilized low-frequency and nonadiabatically coupled high-frequency hydrogen modes. Despite the metastability of this structure, its dynamical stability when modeled beyond a classical harmonic approach suggests the narrow bands near do not cause structural distortions in certain Lu-H-N stoichiometries.

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

Thermophysical Properties of Liquid Tritium: A Path Integral Monte Carlo Study

Here, we present worm-algorithm, path integral Monte Carlo simulations of bulk liquid tritium. The simulations are benchmarked against empirically known thermophysical properties of liquid deuterium and liquid tritium. Results for the pair correlation function, chemical potential, isothermal compressibility, isochoric heat capacity, and single-particle momentum distributions are reported. Given the benchmark comparisons, our predictions of liquid tritium properties are expected to be accurate to within a few percent. Our simulations unambiguously demonstrate the significance of nuclear quantum effects to the properties of liquid tritium. In particular, under saturated vapor pressure, the average molecular kinetic energy of the liquid is found to be more than 60% higher than the value expected from the classical equipartition theorem.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Energy conservation in real-time nuclear–electronic orbital Ehrenfest dynamics

Real-time nuclear–electronic orbital Ehrenfest (RT-NEO-Ehrenfest) dynamics methods provide a first-principles approach for describing nonadiabatic molecular processes with nuclear quantum effects. For an efficient description of proton transfer within RT-NEO-Ehrenfest dynamics, the basis function center associated with the quantum proton can be allowed to move classically. Here, this traveling proton basis (TPB) approach effectively captures proton quantum dynamics, although its energy conservation behavior is not yet fully satisfactory. Two recently proposed TPB approaches, in principle, conserve the extended energy, which includes both the system energy and the kinetic energy associated with the proton basis function center. Herein, a thermostatted TPB approach is proposed to improve the conservation of the system energy, excluding the kinetic energy associated with the proton basis function center. In this approach, the quantum proton dynamics are modulated by dynamically rescaling the proton momentum operator to maintain the system energy conservation. With the excited-state intramolecular proton transfer of o-hydroxybenzaldehyde as an example, this approach is shown to significantly improve the system energy conservation while preserving the accuracy of the quantum proton dynamics as achieved in the original TPB approach.

Ehrenfest dynamics↗
DOE OSTI2025

Constrained nuclear–electronic orbital method for periodic density functional theory: Application to H 2 chemisorption on Si(001) surfaces

The nuclear–electronic orbital (NEO) method provides a powerful computational framework for incorporating nuclear quantum effects (NQE) in electronic structure calculations beyond the Born–Oppenheimer approximation. By incorporating additional constraints to the position operator on quantum particles like protons, the NEO method enables calculation of effective potential that accounts for NQE. Here, in this work, we present a new constrained NEO (cNEO) formulation for density functional theory (cNEO-DFT) calculations in the context of extended periodic systems. Using the nudged elastic band method, we discuss an application of the cNEO-DFT approach to studying the adsorption of a hydrogen molecule on the Si(001) surfaces. The calculation shows how NQE impacts the reaction energetics. The proton density changes are computed along the reaction pathways. This work demonstrates the capability of the new cNEO-DFT method to study a wide range of chemical processes, such as surface reactions where the quantum nature of light atoms like protons is non-negligible.

Chemical processes↗
DOE OSTI2026

Quantum effects on the dynamics and properties of soft materials

The quantum effects of nuclear and electronic motion play an important role in the structure, dynamics, and function of soft materials, yet they are difficult to capture with conventional classical simulations or static electronic–structure methods. In this work several complementary approaches for treating quantum effects in polymeric and soft–matter systems are demonstrated, with a focus being on the hydrogen-bonded networks, ion and charge transport, and photoactive chromophores. The proton transfer, tunneling, and isotope effects are captured within the reduced-dimensionality models by implementing grid-based nuclear quantum dynamics in terms of the discrete variable and Fourier bases. The nuclear quantum dynamics is extended to larger systems by employing the quantum trajectories and quantum–thermal bath schemes combined with on-the-fly electronic structure, enabling the description of high-dimensional polymeric environments at feasible cost. The dynamics in the electronic degrees of freedom, simulating the optical response in large chromophores such as chlorophylls, is performed using the real-time time-dependent density functional theory implemented in the real-space multigrid (RMG) code. These approaches are demonstrated on case studies of the proton and hydroxide transport in hydrated polymer membranes, charge transfer in conjugated polymers, and the optical spectra of chlorophyll chromophores relevant to polymerized chlorophyll materials and chlorophyll–polymer hybrids. The reviewed methods and applications highlight practical routes of including quantum effects in simulations of soft functional materials.

Garashchuk, Sophya [Univ. of South Carolina, Colum↗
DOE OSTI2025

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

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

chemical physics↗
NASA NTRS2001

Integration of the QMSFRG Database into the HZETRN Code

Accurate nuclear interaction data bases are needed for describing the transport of space radiation in matter including space craft structures, atmospheres, and tissues. Transport models support the identification and development of new material concepts for human and electronic part protection. Quantum effects are manifested in nuclear reactions in several ways including interference effects between terms in the multiple scattering series, the many-body nuclear wave functions (for e.g. the roles of shell structure and Fermi momentum) and nuclear clustering. The quantum multiple scattering fragmentation model (QMSFRG) is a comprehensive model for generating nuclear interaction databases for galactic cosmic ray (GCR) transport. Other nuclear databases including the NUCFRG model and Monte-Carlo simulation codes such as FLUKA, LAHET, HETC, and GEANT ignore quantum effects. These codes fail to describe many important features of nuclear reactions and are thus inaccurate for the evaluation of materials for radiation protection. Previously we have shown that quantum effects are manifested through constructive interference in forward production spectra, the effects of Fermi momentum on production spectra, cluster nuclei knockout, and the nuclear response function. Quantum effects are especially important for heavy ions with mass numbers less than 20 that dominate radiation transport in human tissues and for the materials that are expected to be superior in space radiation protection. We describe the integration of the QMSFRG model into the HZETRN transport code. Integration milestones include proper treatment of odd-even charge-mass effects in nuclear fragmentation and the momentum distribution of nucleon production from GCR primary heavy ions. We have also modified the two-body amplitudes in the model to include nuclear medium effects. In order to include a comprehensive description of the GCR isotopic composition in materials, we have described the isotopic composition of the GCR by extending the 59-isotope version of HZETRN to an 120-isotope version. The isotopic composition of most primary GCR elements (including H, He, C, N, O, Ne, Mg, Si, Ar, Ca, Cr, and Fe) are included in the extended model. We discuss results for the high-energy neutron composition inside materials, and the charge and mass distribution for benchmark GCR problems.

Cucinotta, F. A.↗
NASA NTRS2005

Effect of electron-nuclear spin interactions for electron-spin qubits localized in InGaAs self-assembled quantum dots

The effect of electron-nuclear spin interactions on qubit operations is investigated for a qubit represented by the spin of an electron localized in an InGaAs self-assembled quantum dot. The localized electron wave function is evaluated within the atomistic tight-binding model. The electron Zeeman splitting induced by the electron-nuclear spin interaction is estimated in the presence of an inhomogeneous environment characterized by a random nuclear spin configuration, by the dot-size distribution, alloy disorder, and interface disorder. Due to these inhomogeneities, the electron Zeeman splitting varies from one qubit to another by the order of 10(-6), 10(-6), 10(-7), and 10(-9) eV, respectively. Such fluctuations cause errors in exchange operations due to the inequality of the Zeeman splitting between two qubits. However, the error can be made lower than the quantum error threshold if an exchange energy larger than 10(-4) eV is used for the operation. This result shows that the electron-nuclear spin interaction does not hinder quantum-dot based quantum computer architectures from being scalable even in the presence of inhomogeneous environments.

Whaley, K. Birgitta↗