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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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Bounce-averaged theory in arbitrary multi-well plasmas: solution domains and the graph structure of their connections

Bounce-averaged theories provide a framework for simulating relatively slow processes, such as collisional transport and quasilinear diffusion, by averaging these processes over the fast periodic motions of a particle on a closed orbit. This procedure dramatically increases the characteristic time scale and reduces the dimensionality of the modelled system. The natural coordinates for such calculations are the constants of motion (COM) of the fast particle motion, which by definition do not change during an orbit. However, for sufficiently complicated fields – particularly in the presence of local maxima of the electric potential and magnetic field – the COM are not sufficient to specify the particle trajectory. In such cases, multiple domains in COM space must be used to solve the problem, with boundary conditions enforced between the domains to ensure continuity and particle conservation. Previously, these domains have been imposed by hand, or by recognising local maxima in the fields, limiting the flexibility of bounce-averaged simulations. Here, we present a general set of conditions for identifying consistent domains and the boundary condition connections between the domains, allowing the application of bounce-averaged theories in arbitrarily complicated and dynamically evolving electromagnetic field geometries. We also show how the connections between the domains can be represented by a directed graph, which can help to succinctly represent the trajectory bifurcation structure.

fusion plasma↗
DOE OSTI2024

A review of fluids under nanoconfinement: Reactivity, geomechanics, phase transitions, and flow

Due to its many industrial applications, the physics associated with the nanoconfinement of fluids has garnered great attention from the scientific community in roughly the last fifteen years. One pioneer of that research has been the Multi-Scale Fluid-Solid Interactions in Architected and Natural Materials (MUSE) Energy Frontier Research Center, which produced more than 50 journal articles from 2018 to 2023. We structure the findings of MUSE into four categories and contextualize the work with the broader literature. Here, the four categories are (1) the dependence of chemical reactions on the degree of confinement, which given the lower freedom of motion of molecules yet improved availability of reaction sites generally lead to enhancement from bulk reactions; (2) the mechanical properties of the porous matrix, which are dependent on the heterogeneity of the system in terms of both composition and structure; (3) the phase transitions under nanoconfinement, which are influenced by the pore size and morphology, surface chemistry, and substrate composition; and (4) the physical controls of slip flow, which demonstrate the importance of several factors, such as wettability. These aspects of nanoconfinement are becoming clearer, but there are other elements such as mathematical theory that are still being developed.

58 GEOSCIENCES↗
DOE OSTI2025

Seismic response of vertical dry storage casks under three-dimensional earthquake motions

Ensuring the long-term seismic safety of dry storage casks (DSCs) is becoming increasingly critical as these systems evolve from temporary to de facto permanent repositories for spent nuclear fuels. Traditional seismic soil–structure interaction (SSI) assessment methods use one-dimensional deconvolution or simplified boundary conditions to model incident waves. Although computationally appealing, simplifying assumptions may alter the seismic risk by neglecting the full complexity of three-dimensional (3D) wave propagation effects. To address this challenge, this paper introduces a novel high-fidelity computational framework that leverages the Domain Reduction Method (DRM) with perfectly matched layers (PML) to accurately transfer complex, 3D seismic wavefields from regional-scale fault-rupture simulations into local-scale finite element models of DSCs. Using broadband, physics-based ground motions from a generic M w 7.0 strike-slip event, both single-cask and multi-cask configurations were investigated under near- and far-field conditions. Emphasis is placed on capturing complex SSI, spatial variability in the ground motion, and nonlinear phenomena such as cask rocking and sliding. Numerical results demonstrate that near-field conditions, where forward directivity and fling-step effects dominate, lead to significantly higher DSC rocking and sliding. Far-field cases, by contrast, generally exhibit modest responses. Incorporating SSI tends to amplify or alter DSC response spectra and introduce response variability, which underscores the need for site-specific evaluations and robust modeling approaches to ensure the seismic integrity of DSCs in interim spent fuel storage installations.

Das, Tonmoy↗
DOE OSTI2024

Tailoring Ion Transport in Li 3‐3y Ho 1+y Cl 6‐x Br x via Transition‐Metal Free Structural Planes and Charge Carrier Distribution

Abstract Localized atomistic disorder in halide‐based solid electrolytes (SEs) can be leveraged to boost Li + mobility. In this study, Li + transport in structurally modified Li 3 HoCl 6 , via Br − introduction and Li + deficiency, is explored. The optimized Li 3‐3 y Ho 1+ y Cl 6‐ x Br x achieves an ionic conductivity of 3.8 mS cm −1 at 25 °C, the highest reported for holmium halide materials. 6,7 Li nuclear magnetic resonance and relaxometry investigations unveil enhanced ion dynamics with bromination, attaining a Li + motional rate neighboring 116 MHz. X‐ray diffraction analyses reveal mixed‐anion‐induced phase transitions with disproportionate octahedral expansions and distortions, creating Ho‐free planes with favorable energetics for Li + migration. Bond valence site energy analysis highlights preferred Li + transport pathways, particularly in structural planes devoid of Ho 3+ blocking effects. Molecular dynamics simulations corroborate enhanced Li + diffusion with Br − introduction into Li 3 HoCl 6 . Li‐Ho electrostatic repulsions in the (001) plane presumably drive Li + diffusion into the Ho‐free (002) layer, enabling rapid intraplanar Li + motion and exchange between the 2d and 4h sites. Li 3‐3 y Ho 1+ y Cl 6‐ x Br x also demonstrates good battery cycling stability. These findings offer valuable insights into the intricate correlations between structure and ion transport and will help guide the design of high‐performance fast ion conductors for all‐solid‐state batteries.

Chemistry↗
DOE OSTI2026

Environmental Contributions to Proton Sharing in Protein Low-Barrier Hydrogen Bonds

Hydrogen bonds (H-bonds) are central to biomolecular structure and dynamics. Although H-bonds are typically characterized by well-defined proton positions, proton delocalization has been proposed to play a role in facilitating enzyme catalysis and allostery in some systems. Experimentally locating protons is difficult, hampering the study of proton mobility in H-bonds. We used neutron crystallography, atomic resolution X-ray bond length analysis, and large quantum mechanics/molecular mechanics-Born–Oppenheimer molecular dynamics (QM/MM-BOMD) simulations to comprehensively characterize the shared proton/deuteron in a Glu–Asp low-barrier hydrogen bond (LBHB) in the bacterial protein YajL that is a conventional H-bond in the homologous disease-associated human protein DJ-1. X-ray bond length analysis of protiated and perdeuterated DJ-1 and YajL shows no significant effect of deuteron substitution on these carboxylic acid-carboxylate H-bonds but does reveal an effect at the active site glutamic acid near a cysteine thiolate. Residues in an H-bonded network that might favor LBHB formation in YajL were interrogated by the mutation of homologous residues in DJ-1. A distal DJ-1 substitution increases proton delocalization in the Glu–Asp H-bond, demonstrating that mutations within extended H-bond networks can modulate proton transfer barriers in carboxylic acid-carboxylate H-bonds. In addition, proton mobility in the H-bond is correlated with dimer-spanning motions in the QM/MM-BOMD simulations of YajL and DJ-1. Our results show that proton delocalization can be tuned using combined bioinformatic, structural, and computational information, opening the possibility of using engineered proton delocalization as a probe of H-bonding environments and as a tool to test hypotheses about LBHB function.

Lin, Jiusheng [University of Nebraska, Lincoln, NE↗
DOE OSTI2024

Performance evaluation of the USGS velocity model for the San Francisco Bay Area

In this study, we evaluated the performance of the United States Geological Survey velocity model developed for the San Francisco Bay Area (SFBA), version 21.1. The evaluation was performed through high-resolution three-dimensional physics-based ground motion simulations of seven small-magnitude earthquakes (ranging from magnitude 3.8 to 4.4) that occurred on the eastern side of the San Francisco Bay. The simulations were performed in the frequency range from 0 to 5 Hz with a minimum shear-wave velocity of 250 m/s, which allowed the capture of wave propagation effects of the near-surface soft materials that characterize local basins. Based on the direct comparison of Fourier amplitude spectra between recorded and simulated ground motions for more than 250 stations, we found that the velocity model generally performs well in the frequency range of 0.2–5 Hz. The median value of the Fourier amplitude residuals was found to be near zero for all seven earthquakes. The slight over-prediction of 0.2 log-natural units at frequencies above 3 Hz in our simulations was attributed to the potentially inaccurate representation of the source radiation pattern by a double-couple point source model, and simple representation of shallow small-scale underground structural complexity in the velocity model. Maps of spectral amplitude differences between the simulated and recorded data were used to identify areas responsible for systematic ground motion over-predictions or under-predictions. For example, while some sub-domains over soft sediments show over-prediction patterns, the block east of the Hayward fault is prone to exhibit patterns of under-prediction. These maps can be used to guide future refinements of the SFBA velocity model. Since our simulation methodology allows for the decoupling of the source and wave propagation effects, the ground motion data generated by our simulations can also be used to quantify the epistemic uncertainty due to the velocity model, in empirically based ground motion estimates for the SFBA.

58 GEOSCIENCES↗
DOE OSTI2024

Control-inspired design and power optimization of an active mechanical motion rectifier based power takeoff for wave energy converters

Ocean waves have high energy density and are persistent and predictable. Yet, converting wave energy to a useable form remains challenging. A significant hurdle is the oscillatory nature of waves resulting in the alternating loads, which necessitate the use of rectification at some stage of the energy conversion. This research effort presents a novel design of active mechanical motion rectifier (AMMR) for the power takeoff (PTO), which provides enhanced controllability and better power performance when compared to passive mechanical motion rectifiers (MMR). Inspired by transistors used in synchronous electrical rectifiers, the proposed design uses controllable electromagnetic clutches in the mechanical transmission to allow active engagement-disengagement control; thus, rectifying the oscillatory motion into a unidirectional rotation for high energy conversion efficiency and allowing the generator in unidirectional rotation to control the bidirectional wave capture structure for maximizing the power output. A semi-analytical computational approach is developed to efficiently evaluate the optimal power achieved using the proposed AMMR-based PTO and active control. It is found that the AMMR-based PTO design yields a higher optimal power than the previous passive MMR design across the wave spectrum. The influences of generator inertia and reactive power are discussed. Furthermore, the effects of control parameters on the power output and the optimal trajectories are analyzed. Wave tank tests with the AMMR prototype demonstrated the effectiveness of AMMR based PTO design and validated the numerical analysis.

16 TIDAL AND WAVE POWER↗
DOE OSTI2024

Elucidating Anomalous Intensity Ratios in Chlorine L-Edge X-ray Absorption Spectroscopy: Multiplet Effects and Core Rydberg Transitions

A relativistic core–valence-separated equation-of-motion coupled cluster (CVS-EOM-CC) study of chlorine L 2,3 -edge X-ray absorption near-edge structure (XANES) spectra using CH 3 Cl and CH 2 ICl as representative molecules is reported. The nearly identical intensity for the main features in the L 2 - and L 3 -edge XANES spectra is attributed to multiplet effects and the overlap between core–valence and core Rydberg transitions. The multiplet effects originating from the interaction between the core hole and the C–Cl σ* orbitals account for around half of the deviation of the L 3 and L 2 intensity ratio from the 2:1 ratio of the numbers of 2p 3/2 and 2p 1/2 electrons. The 2p 3/2 → 4s core Rydberg transitions are shown to overlap with the 2p 1/2 → σ* transitions and contribute to the other half of the intensity anomaly. Here, we demonstrate that triple excitations in CVS-EOM-CC calculations play important roles in accurate simulation of the overlap between the 2p 1/2 → σ* and 2p 3/2 → 4s transitions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Deciphering Charge Transfer Processes in Transition Metal Complexes from the Perspective of Ultrafast Electronic and Nuclear Motions

Chemical transformations in charge transfer states result from the interplay between electronic dynamics and nuclear reorganization along excited-state trajectories. Here, in this study, we investigate the ultrafast structural dynamics following photoinduced electron transfer from the metal-metal-to-ligand charge transfer state of an electron donor, a Pt dimer complex, to a covalently linked electron acceptor group using ultrafast time-resolved wide-angle X-ray scattering and optical transient absorption spectroscopy methods to disentangle the interdependence of the excited-state electronic and nuclear dynamics. Following photoexcitation, Pt-Pt bond formation and contraction takes up to 1 ps, much slower than the corresponding process in analogous complexes without electron acceptor groups. Because the Pt-Pt distance change is slow with respect to excited-state electron transfer, it can affect the rate of electron transfer. These results have potential impacts on controlling electron transfer rates via structural alterations to the electron donor group, tuning the charge transfer driving force.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Supramolecular Motion Enables Chondrogenic Bioactivity of a Cyclic Peptide Mimetic of Transforming Growth Factor-β1

Transforming growth factor (TGF)-β1 is a multifunctional protein that is essential in many cellular processes that include fibrosis, inflammation, chondrogenesis, and cartilage repair. In particular, cartilage repair is important to avoid physical disability since this tissue does not have the inherent capacity to regenerate beyond full development. We report here on supramolecular coassemblies of two peptide amphiphile molecules, one containing a TGF-β1 mimetic peptide, and another which is one of two constitutional isomers lacking bioactivity. Using human articular chondrocytes, we investigated the bioactivity of the supramolecular copolymers of each isomer displaying either the previously reported linear form of the mimetic peptide or a novel cyclic analogue. Based on fluorescence depolarization and 1 H NMR spin–lattice relaxation times, we found that coassemblies containing the cyclic compound and the most dynamic isomer exhibited the highest intracellular TGF-β1 signaling and gene expression of cartilage extracellular matrix components. Here, we conclude that control of supramolecular motion is emerging as an important factor in the binding of synthetic molecules to receptors that can be tuned through chemical structure.

Antigens↗
DOE OSTI2025

Understanding plasma turbulence through exact coherent structures

Plasma turbulence is a key challenge in understanding transport phenomena in magnetically confined plasmas. This work presents a generalized framework to analyze plasma turbulence that utilizes periodic orbit theory. In periodic orbit theory, doubly periodic solutions (coherent structures) of the governing equation(s) serve as building blocks of the considered turbulent dynamics. To illustrate the concept and method, the particularly simple Kuramoto–Sivashinsky (referred to here as LMRT for the original authors: LaQuey, Mahajan, Rutherford, and Tang) trapped-ion mode toy model is used. By applying numerical optimization techniques to the LMRT equation, we extract coherent spacetime patterns that represent the library of allowable fundamental structures of the equation. These structures provide a framework to systematically describe turbulence as a composition of recurrent solutions, revealing an underlying order within chaotic plasma motion. Although illustrated here using the simplified LMRT model for clarity, this framework provides a general strategy that can be extended to more complex and realistic models of plasma turbulence, including gyrokinetic systems. This offers a new method for predicting and potentially controlling transport processes in fusion plasmas by providing a bridge between nonlinear dynamical systems theory and plasma physics in the form of a generalized framework with which to analyze and understand spatially extended nonlinear partial differential equations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2026

Recurrent convolutional neural networks for modeling nonadiabatic dynamics of quantum-classical systems

Recurrent neural networks (RNNs) have recently been extensively applied to model the time evolution in fluid dynamics, weather predictions, and even chaotic systems due to their ability to capture temporal dependencies and sequential patterns in data. Here we present an RNN model based on convolutional neural networks for modeling the nonlinear nonadiabatic dynamics of hybrid quantum-classical systems. The dynamical evolution of the hybrid systems is governed by equations of motion for classical degrees of freedom and von Neumann equation for electrons. The Physics-Aware Recurrent Convolution (PARC) neural network structure incorporates a differentiator-integrator architecture that inductively models the spatiotemporal dynamics of generic physical systems. Here, we apply our RNN approach to learn the space-time evolution of a one-dimensional semiclassical Holstein model after an interaction quench. For shallow quenches (small changes in electron-lattice coupling), the deterministic dynamics can be accurately captured using a single-CNN-based recurrent network. In contrast, deep quenches induce chaotic evolution, making long-term trajectory prediction significantly more challenging. Nonetheless, we demonstrate that the PARC-CNN architecture can effectively learn the statistical climate of the Holstein model under deep-quench conditions.

Holstein model↗
DOE OSTI2024

Mitigating Band Tailing in Kesterite Solar Absorbers: Ab Initio Quantum Dynamics

Open-circuit voltage deficits are limiting factors in kesterite solar cells. Addressing this issue by suppressing band tailing and nonradiative charge recombination is essential for enhancing the performance. We employ ab initio nonadiabatic molecular dynamics to elucidate the origin of band tailing and charge losses and propose a mitigation strategy. The simulations show that Cu–Zn disorder, associated with antisite defect clusters [Cu Zn +Zn Cu ], is a significant source of band tailing in kesterites, as evidenced by the much larger Urbach energy in disordered than ordered kesterites. Cu–Zn disorder gives rise to new sulfur-centered coordination polyhedra, increases structural inhomogeneity, changes electrostatic potential at sulfur centers, and shifts the S(3p) orbital energy. Differences in the S(3p)/Cu(3d) and S(3p)/Sn(5s) hybridization strengths and the S(3p) orbital energy shift reduce the band gap by 0.37 eV. Furthermore, Cu–Zn disorder enhances vibrational motion of sulfur anions and surrounding cations, increasing band gap fluctuations by 15 meV. The stronger electron–phonon interactions reduce charge carrier lifetimes and limit the kesterite solar cell efficiency. Partial substitution of Zn with Cd facilitates structural ordering and significantly suppresses band tailing, particularly in disordered systems. The improvement can be attributed to the larger atomic radius and mass of Cd, which weakens bonding around the anion, suppresses S-related vibrations within the covalent tetrahedra, and reduces nonadiabatic coupling, thereby increasing charge carrier lifetimes. The reported results establish the key influence of cation disorder on band tailing and reduced charge carrier lifetimes in kesterites and highlight cation disorder engineering as a strategy to achieve high-efficiency kesterite solar cells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Solvent-Dependent Dynamics of Cellulose Nanocrystals in Process-Relevant Flow Fields

Flow-assisted alignment of anisotropic nanoparticles is a promising route for the bottom-up assembly of advanced materials with tunable properties. While aligning processes could be optimized by controlling factors such as solvent viscosity, flow deformation, and the structure of the particles themselves, it is necessary to understand the relationship between these factors and their effect on the final orientation. In this study, we investigated the flow of surface-charged cellulose nanocrystals (CNCs) with the shape of a rigid rod dispersed in water and propylene glycol (PG) in an isotropic tactoid state. In situ scanning small-angle X-ray scattering (SAXS) and rheo-optical flow-stop experiments were used to quantify the dynamics, orientation, and structure of the assigned system at the nanometer scale. The effects of both shear and extensional flow fields were revealed in a single experiment by using a flow-focusing channel geometry, which was used as a model flow for nanomaterial assembly. Due to the higher solvent viscosity, CNCs in PG showed much slower Brownian dynamics than CNCs in water and thus could be aligned at lower deformation rates. Moreover, CNCs in PG also formed a characteristic tactoid structure but with less ordering than CNCs in water owing to weaker electrostatic interactions. The results indicate that CNCs in water stay assembled in the mesoscale structure at moderate deformation rates but are broken up at higher flow rates, enhancing rotary diffusion and leading to lower overall alignment. Albeit being a study of cellulose nanoparticles, the fundamental interplay between imposed flow fields, Brownian motion, and electrostatic interactions likely apply to many other anisotropic colloidal systems.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Highly Anisotropic Quasi‐Direct Organic Metal Halide Hybrids: A Platform for Polarization‐Sensitive Optoelectronics

Low-dimensional organic–inorganic metal halide hybrids (OMHHs) exhibit remarkable optical properties and enhanced environmental stability. We investigate a 1D OMHH with formula C 4 N 2 H 14 PbBr 4 , consisting of Pb–Br chains separated by organic cations, which shows a large Stokes shift (0.83 eV) and broadband emission. Through first-principles calculations and polarized Raman spectroscopy, we characterize the material's vibrational properties and identify the specific phonon modes that drive exciton self-trapping. Our novel GW/Bethe-Salpeter equation force formalism reveals that low-frequency phonons (∼ 100 cm −1 , primarily involving Pb–Br motions) couple strongly with excitons, with a remarkably high Huang-Rhys factor of 137 ± 4, and gives a pathway for ultrafast structural analysis during the absorption process. This phonon-exciton coupling mechanism explains the material's broadband emission and provides a pathway for controlling optical properties through vibrations and for tuning vibrations through optical excitations. The material also exhibits highly anisotropic optical properties and electronic transport, with bands that are dispersive along the Pb–Br chains but nearly flat in perpendicular directions, resulting in direction-dependent electrical conductivity that is calculated to be an order of magnitude higher along the chain direction and consistent with measurements. These combined properties make this system an excellent platform for polarization-sensitive optoelectronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Unravelling the dynamics of the maturation protein in MS2 bacteriophage via molecular simulations

The MS2 bacteriophage capsid serves as a model system for studying viral structure and function. Mature MS2 virus consists of 178 capsid proteins and a single maturation protein (MP), which is essential for host receptor binding and infection initiation. Despite its critical role, the dynamic behavior of the capsid with the MP remains poorly understood. To address this, we conducted 0.5 µs all-atom molecular dynamics (MD) simulations of the MS2 capsid with and without the MP, revealing key insights into its structural dynamics. Our simulations showed that MP exhibits high flexibility, particularly in the “tip” and “side-loop” regions, which undergo significant motions that likely enhance its ability to engage with the F-pilus receptor. Detailed analysis of MP conformational states revealed that loop rearrangements around H357 enable transient switching between “semi-closed” and “open” conformations, suggesting a conformational selection mechanism for pilus binding. Additionally, ion interaction analyses revealed distinct sodium and chloride binding patterns, where sodium ions were mostly found at the outer capsid shell, while chloride ions interacted with the basic residues on the RNA-facing side. We also found that the presence of the MP enhances salt-bridge interactions, contributing to increased capsid stability, yet it does not significantly alter the pore sizes of pentameric and hexameric units. Together, these findings provide new insights into the functional role of the MP, highlighting its contribution to capsid stability and host receptor engagement. This study offers a foundation for understanding capsid dynamics relevant to viral infectivity and may guide future rational strategies aimed at disrupting host-virus interactions.

Capsid stability↗
DOE OSTI2024

Distorted dislocation cores and asymmetric glide resistances in titanium

The determination of Critical Resolved Shear Stress (CRSS) in titanium for basal, prismatic, and pyramidal slip-planes without empirical constants is presented by combining Density Functional Theory (DFT) and anisotropic elasticity. A new mechanism leading to tension-compression (T-C) asymmetry in the CRSS levels has been revealed for the first time. The conditions for this asymmetry are established, involving a complex interplay between the dislocation core-structure and core-advance behavior. The three conditions for T-C asymmetry that need to be simultaneously satisfied can be summarized as: (1) a medium stacking fault width, d, (3 < d/b F < 10, where b F is the magnitude of the Burgers vector of the full dislocation), (2) an asymmetric core-structure of the extended dislocation (ξ 1 ≠ ξ 2 , where ξ 1 and ξ 2 are the core-widths of the first and second partials, respectively), and (3) intermittent motion of the partials (Δd/b F ≠ 0, where Δd is the magnitude of fluctuation in stacking fault width during intermittent motion). Pyramidal-slip in titanium satisfies all three conditions, resulting in significant T-C asymmetry. The CRSS theory considers a Wigner-Seitz (W-S) cell based domain area assigned to each lattice site for the calculations of core-energies accurately capturing the slip-plane lattice. The W-S based approach is essential due to the lower symmetry of the HCP crystal circumventing potential errors associated with the one-dimensional atomic-row approximation. Dislocation core structures are obtained for all the slip-systems in titanium showing significant distortion of the disregistry profile governing the core-advance behavior. The CRSS values predicted from the theory show agreement with the experimental CRSS levels reported in the literature.

Dislocation core↗
DOE OSTI2026

Interfacial Hydrogen-Bond Dynamics in Transition Metal Compounds

Understanding how water behaves when confined within atomic layers of active transition-metal carbides, nitrides, and carbonitrides is essential for uncovering the fundamental principles needed to engineer solid–liquid interfaces at the atomic scale. Yet, how lattice element chemistry and surface termination groups collectively regulate the structure and mobility of such interlayer water remains poorly understood. Here, we present a composition-controlled investigation of interlayer water dynamics in layered transition-metal nitride, carbide, and carbonitride systems using a systematic integration of quasi-elastic neutron scattering (QENS), ab initio molecular dynamics (AIMD) simulations, and density functional theory (DFT) calculations. QENS measurements show that nitride-rich systems host mobile, translationally diffusing water with thermally activated self-diffusion coefficients on the order of 10 –10 m 2 s –1 , whereas mixed C/N lattices confine water to localized, nontranslational motion that is insensitive to temperature. AIMD and DFT reveal that lattice C/N chemistry and surface functional group composition reshape the first hydration layer by modulating the surface electronic structure and termination-dependent hydrogen-bond networks, leading to pronounced differences in water ordering and thermal resilience. On the other hand, fully carbide systems exhibit intermediate behavior, highlighting that water mobility is not primarily controlled by the hydration level alone but by the coupling between lattice composition and surface chemistry. Overall, this study establishes how surface chemistry and lattice composition jointly control interfacial hydrogen bond dynamics, offering a mechanistic framework for designing transition-metal layered materials with tailored interfacial transport properties.

Hydration↗