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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Impact of atomic substitution on core-hole relaxation dynamics: A study of Br 2 and IBr

Understanding inner-shell decay processes in heavy-element molecules is essential for unraveling x-ray-induced photodynamics and advancing molecular imaging techniques. Here, in this study, we investigate the influence of atomic substitution on core-hole relaxation dynamics and molecular fragmentation in Br 2 and IBr, initiated by x-ray ionization absorption at the Br K-edge. Using a combination of x-ray/ion coincidence measurements and Monte Carlo/molecular dynamics simulations, we track the charge distribution and the kinetic energy release (KER) of fragment ions with a total charge from 2+ to 8+. For both molecules, the simulated KER values show good agreement with experiment across different fragmentation channels. Our comparison reveals that substituting Br with the heavier I atom in IBr has a minimal impact on the inner-shell electronic decay process but significantly influences nuclear motion, leading to slower dissociation and thus a KER close to the Coulomb limit—an effect attributed to the atomic mass. These findings highlight the interplay between electronic and nuclear effects in molecular fragmentation, particularly in heavy-element species, and provide new insights into medical therapies, structural biology, and astrophysics.

Bhat, Nivedita [Argonne National Laboratory (ANL),↗
DOE OSTI2024

AI-NERD: Elucidation of relaxation dynamics beyond equilibrium through AI-informed X-ray photon correlation spectroscopy

Abstract Understanding and interpreting dynamics of functional materials in situ is a grand challenge in physics and materials science due to the difficulty of experimentally probing materials at varied length and time scales. X-ray photon correlation spectroscopy (XPCS) is uniquely well-suited for characterizing materials dynamics over wide-ranging time scales. However, spatial and temporal heterogeneity in material behavior can make interpretation of experimental XPCS data difficult. In this work, we have developed an unsupervised deep learning (DL) framework for automated classification of relaxation dynamics from experimental data without requiring any prior physical knowledge of the system. We demonstrate how this method can be used to accelerate exploration of large datasets to identify samples of interest, and we apply this approach to directly correlate microscopic dynamics with macroscopic properties of a model system. Importantly, this DL framework is material and process agnostic, marking a concrete step towards autonomous materials discovery.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Electronic relaxation dynamics in [Au 25 (SR) 18 ] -1 (R = CH 3 , C 2 H 5 , C 3 H 7 , MPA, PET) thiolate-protected nanoclusters

Here we investigate the excited electron dynamics in [Au 25 (SR) 18 ] -1 (R = CH3, C 2 H 5 , C 3 H 7 , MPA, PET) [MPA = mercaptopropanoic acid, PET = phenylethylthiol] nanoparticles to understand how different ligands affect the excited state dynamics in this system. The population dynamics of the core and higher excited states lying in the energy range 0.00–2.20 eV are studied using a surface hopping method with decoherence correction in a real-time DFT approach. All of the ligated clusters follow a similar trend in decay for the core states (S 1 –S 6 ). The observed time constants are on the picosecond time scale (2–19 ps), which agrees with the experimental time scale, and this study confirms that the time constants observed experimentally could originate from core-to-core transitions and not from core-to-semiring transitions. In the presence of higher excited states, R = H, CH 3 , C 2 H 5 , C 3 H 7 , and PET demonstrate similar relaxations trends whereas R = MPA shows slightly different relaxation of the core states due to a smaller gap between the LUMO+1 and LUMO+2 gap in its electronic structure. The S 1 (HOMO → LUMO) state gives the slowest decay in all ligated clusters, while S 7 has a relatively long decay. Furthermore, separate electron and hole relaxations were performed on the [Au 25 (SCH 3 ) 18 ] -1 nanocluster to understand how independent electron and hole relaxations contribute to the overall relaxation dynamics.

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

The Concentration–Mass relation of massive, dynamically relaxed galaxy clusters: agreement between observations and ΛCDM simulations

ABSTRACT The relationship linking a galaxy cluster’s total mass with the concentration of its mass profile and its redshift is a fundamental prediction of the Cold Dark Matter (CDM) paradigm of cosmic structure formation. However, confronting those predictions with observations is complicated by the fact that simulated clusters are not representative of observed samples where detailed mass profile constraints are possible. In this work, we calculate the symmetry-peakiness-alignment (SPA) morphology metrics for maps of X-ray emissivity from the three hundred project hydrodynamical simulations of galaxy clusters at four redshifts, and thereby select a sample of morphologically relaxed, simulated clusters, using observational criteria. These clusters have on average earlier formation times than the full sample, confirming that they are both morphologically and dynamically more relaxed than typical. We constrain the concentration–mass–redshift relation of both the relaxed and complete sample of simulated clusters, assuming power-law dependences on mass (κm) and 1 + z (κζ), finding κm = −0.12 ± 0.07 and κζ = −0.27 ± 0.19 for the relaxed subsample. From an equivalently selected sample of massive, relaxed clusters observed with Chandra, we find κm = −0.12 ± 0.08 and κζ = −0.48 ± 0.19, in good agreement with the simulation predictions. The simulated and observed samples also agree well on the average concentration at a pivot mass and redshift providing further validation of the ΛCDM paradigm in the properties of the largest gravitationally collapsed structures observed. This also represents the first clear detection of decreasing concentration with redshift, a longstanding prediction of simulations in data.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Q-dependent collective relaxation dynamics of glass-forming liquid Ca0.4K0.6(NO3)1.4 investigated by wide-angle neutron spin-echo

Abstract The relaxation behavior of glass formers exhibits spatial heterogeneity and dramatically changes upon cooling towards the glass transition. However, the underlying mechanisms of the dynamics at different microscopic length scales are not fully understood. Employing the recently developed wide-angle neutron spin-echo spectroscopy technique, we measured the Q -dependent coherent intermediate scattering function of a prototypical ionic glass former Ca 0.4 K 0.6 (NO 3 ) 1.4 , in the highly viscous liquid state. In contrast to the structure modulated dynamics for Q < 2.4 Å −1 , i.e., at and below the structure factor main peak, for Q > 2.4 Å −1 , beyond the first minimum above the structure factor main peak, the stretching exponent exhibits no temperature dependence and concomitantly the relaxation time shows smaller deviations from Arrhenius behavior. This finding indicates a change in the dominant relaxation mechanisms around a characteristic length of 2π/(2.4 Å −1 ) ≈ 2.6 Å, below which the relaxation process exhibits a temperature independent distribution and more Arrhenius-like behavior.

42 ENGINEERING↗
DOE OSTI2023

The critical role of ultra-low-energy vibrations in the relaxation dynamics of molecular qubits

Improving the performance of molecular qubits is a fundamental milestone towards unleashing the power of molecular magnetism in the second quantum revolution. Taming spin relaxation and decoherence due to vibrations is crucial to reach this milestone, but this is hindered by our lack of understanding on the nature of vibrations and their coupling to spins. Here we propose a synergistic approach to study a prototypical molecular qubit. It combines inelastic X-ray scattering to measure phonon dispersions along the main symmetry directions of the crystal and spin dynamics simulations based on DFT. We show that the canonical Debye picture of lattice dynamics breaks down and that intra-molecular vibrations with very-low energies of 1-2 meV are largely responsible for spin relaxation up to ambient temperature. We identify the origin of these modes, thus providing a rationale for improving spin coherence. The power and flexibility of our approach open new avenues for the investigation of magnetic molecules with the potential of removing roadblocks toward their use in quantum devices.

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

Relaxation dynamics of water in the vicinity of cellulose nanocrystals

Water molecules near cellulose nanocrystals (CNCs; produced via the sulfuric acid-catalyzed hydrolysis of wood pulp) are believed to relax slower than those in the bulk liquid, which may result in unique properties of CNC aqueous dispersions. Herein this study analyzed the polarization behavior of water molecules in CNC aqueous dispersions and other reference samples using a dielectric relaxation spectroscopy (DRS) technique in the microwave frequency range (0.2–20 GHz). As the CNC concentration increases, two slow relaxation components become prominent. The comparison with DRS data of aqueous dispersions of nanoporous silica, polyvinyl alcohol (PVA), and hairy CNC (HCNC) with amorphous chains protruding from both ends suggested that these slow relaxation modes of water near CNC surfaces cannot be attributed to direct hydrogen bonding interactions with the hydroxyl (OH) groups exposed and immobilized at the solid surface. Instead, they are similar to the water molecules interacting with OH groups attached to flexible polymer chains. Molecular dynamics (MD) simulations of the polarization behavior of water near the (110) facet of cellulose Iβ crystals confirmed that the interactions of water molecules with the cellulose crystal surface do not cause slower relaxations in the frequency range studied via the DRS. These results indicated that the CNC surface cannot be depicted with the crystallographic facets of cellulose Iβ; instead, it resembles a polymer-brush surface on which the short glucan residues or fragments of the strong acid-catalyzed hydrolysis process are swollen and extended into the aqueous phase.

59 BASIC BIOLOGICAL SCIENCES↗
NASA NTRS1993

Evolution of planetesimals. I - Dynamics: Relaxation in a thin disk. II - Numerical simulations

The study examines the effects of density inhomogeneity and differential rotation as well as inelastic collisions on the dynamical evolution of planetesimals. Consideration is given to a three-step analysis: the dynamical evolution of the planetesimals, collisions and mass accumulation, and interaction with gas. It is shown that the velocity dispersion of a cold system of planetesimals increases rapidly due to elastic gravitational scattering. When the dispersion in the epicycle amplitude becomes comparable to the planetesimals' Roche radius, energy is transferred from the systematic Keplerian shear to the dispersive motion. With a numerical N-body scheme, gravitational scattering and physical collisions among a system of planetesimals is simulated. It is shown that dynamical equilibrium is attained with a velocity dispersion comparable to the surface escape velocity of those planetesimals which contribute most of the system mass.

Palmer, P. L.↗
DOE OSTI2025

Stretched exponential magnetic relaxation dynamics in artificial square ice revealed through x-ray photon correlation spectroscopy

X-ray photon correlation scattering measurements are undertaken on a thermally active artificial spin ice based on the square lattice, referred to as artificial square ice, to probe the fluctuation timescales as a function of temperature as the system passes through the paramagnetic-antiferromagnetic phase transition, which belongs to the two-dimensional Ising universality class. In the paramagnetic regime, a single exponential timescale is seen, whereas at and below the critical temperature, a stretched exponential decorrelation is observed, with the stretching exponent decreasing from unity down to below one-half as the temperature reduces. This trend is confirmed by kinetic Monte Carlo simulations of a simplified point-dipolar square ice system, and is in agreement with past theoretical work on the kinetic Ising model where stretched exponential relaxation due to equilibrium domain wall dynamics below the critical temperature was found.

36 MATERIALS SCIENCE↗
NASA NTRS1996

Observation of Vibrational Relaxation Dynamics in X(sup 3)Sigma(sup -)(sub g) Oxygen Following Stimulated Raman Excitation to the v=1 Level: Implications for the RELIEF Flow Tagging Technique

The vibrational relaxation of ground-state molecular oxygen (O2, X(sup 3)Sigma(sup -)(sub g)) has been observed, following stimulated Raman excitation to the first excited vibrational level (v=1). Time delayed laser-induced fluorescence probing of the ro-vibrational population distribution was used to examine the temporal relaxation behavior. In the presence of water vapor, the relaxation process is rapid, and is dominated by near-resonant vibrational energy exchange between the v=1 level of O2 and the n2 bending mode of H2O. In the absence of H2O, reequilibration proceeds via homogeneous vibrational energy transfer, in which a collision between two v=1 O2 molecules leaves one molecule in the v=2 state and the other in the v=0 state. Subsequent collisions between molecules in v=1 and v>1 result in continued transfer of population up the vibrational ladder. The implications of these results for the RELIEF flow tagging technique are discussed.

Diskin, Glenn S.↗
DOE OSTI2022

Unconventional non-local relaxation dynamics in a twisted trilayer graphene moiré superlattice

Abstract The electronic and structural properties of atomically thin materials can be controllably tuned by assembling them with an interlayer twist. During this process, constituent layers spontaneously rearrange themselves in search of a lowest energy configuration. Such relaxation phenomena can lead to unexpected and novel material properties. Here, we study twisted double trilayer graphene (TDTG) using nano-optical and tunneling spectroscopy tools. We reveal a surprising optical and electronic contrast, as well as a stacking energy imbalance emerging between the moiré domains. We attribute this contrast to an unconventional form of lattice relaxation in which an entire graphene layer spontaneously shifts position during assembly, resulting in domains of ABABAB and BCBACA stacking. We analyze the energetics of this transition and demonstrate that it is the result of a non-local relaxation process, in which an energy gain in one domain of the moiré lattice is paid for by a relaxation that occurs in the other.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Relaxation Dynamics and Ion Conduction of Poly(Ethylene Carbonate/Ethylene Oxide) Copolymer-Based Electrolytes

Poly(ethylene carbonate/ethylene oxide) P(EC/EO) copolymer was synthesized from EC monomer as a new matrix component of solid polymer electrolytes (SPEs), and the correlation between polymer dynamics and ionic conductivity in the P(EC/EO)-based SPEs at various lithium salt weight fractions (w Li ) was investigated by dielectric spectroscopy, rheology, and molecular dynamics (MD) simulations. With the addition of lithium salt, the molecular motions at various scales (i.e., from local to segmental and global motion scales) were found to change as follows: (i) the local motion of P(EC/EO) was slightly accelerated, and at w Li ≥ 0.22, it was separated into two relaxation modes, one faster and the other slower than that of P(EC/EO), (ii) the segmental motion of P(EC/EO) became significantly slower with the addition of lithium salt, and (iii) the global terminal relaxation became slightly slower with the increase of w Li . Thus, the motion of P(EC/EO) at various scales in SPEs changed with different trends with increasing lithium salt. It was also found that the temperature dependence of the ionic conductivity was described by a Vogel–Fulcher–Tammann-type function, which was correlated with the segmental motion, as is known in other SPE systems. Furthermore, from MD simulations, lithium ions are coordinated with the EC units more likely and with a closer distance than EO units in P(EC/EO), and the coordination number of oxygens around one lithium ion was estimated as 6–7 at the distance of 0.30 nm. Here, these results suggest that the coordination structure of the oxygens around the lithium ion is slightly disrupted due to the presence of EC units compared to the chelating structure of pure PEO electrolytes.

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

Subterahertz Spin Relaxation Dynamics of Boron-Vacancy Centers in Hexagonal Boron Nitride

Quantum sensors based on spin defects have become powerful tools for detecting faint magnetic signals, yet their operation remains confined to low magnetic fields and gigahertz frequencies. Extending such sensors into high-field (>0.3 T) and subterahertz regimes would enable quantum metrology across a wide range of electromagnetic phenomena and scientific applications, but has proven challenging. Here, we demonstrate that negatively charged boron vacancies ($V^−_B$) in hexagonal boron nitride can function as relaxation-based quantum sensors operating up to 0.2 terahertz and 7 T fields. Their uniform spin-orientation and persistent spin-contrast at high fields enable measurement of intrinsic spin relaxation across unexplored field regimes. We reveal a crossover in relaxation behavior, initially decreasing at low fields before rising at higher fields, consistent with the emergence of single-phonon-induced resonant noise at subterahertz frequencies. These results establish $V^−_B$ centers as a versatile platform for quantum sensing in the subterahertz, high-field regime.

boron-vacancies↗
DOE OSTI2022

Excited-State-Selective Ultrafast Relaxation Dynamics and Photoisomerization of trans-4,4'-Azopyridine

Here, excited-state dynamics of trans-4,4’-azopyridine in ethanol is studied using femtosecond transient absorption with 30 fs temporal resolution. Exciting the system at three different wavelengths, 460- and 290-(275) nm, to access the S 1 n,π* and S 2 π,π* electronic states, respectively, reveals a 195 cm -1 vibrational coherence, that suggests that the same mode is active in both n,π* and π,π* relaxation channels. Following S 1 -excitation, relaxation proceeds via a nonrotational pathway, where a fraction of the n,π* population is trapped in a planar minimum (lifetime, 2.1 ps), while the remaining population travels further to a second shallow minimum (lifetime, 300 fs) prior to decay into the ground state. Population of the S 2 state leads to 30-fs non-rotational relaxation with a concurrent buildup of n,π* population and nearly simultaneous formation of hot ground state species. An increase in the cis-isomer quantum yield upon π,π* vs. n,π* excitation is observed, which is opposite to trans-azobenzene.

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

Defect Engineering in Large‐Scale CVD‐Grown Hexagonal Boron Nitride: Formation, Spectroscopy, and Spin Relaxation Dynamics

Recently, numerous techniques have been reported for generating optically active defects in exfoliated hexagonal boron nitride (hBN), which hold transformative potential for quantum photonic devices. However, achieving on-demand generation of desirable defect types in scalable hBN films remains a significant challenge. Here, it is demonstrated that formation of negative boron vacancy defects, V B − , in suspended, large-area CVD-grown hBN is strongly dependent on the type of bombarding particles (ions, neutrons, and electrons) and irradiation conditions. In contrast to suspended hBN, defect formation in substrate-supported hBN is more complex due to the uncontrollable generation of secondary particles from the substrate, and the outcome strongly depends on the thickness of the hBN. Different defect types are identified by correlating spectroscopic and optically detected magnetic resonance features, distinguishing boron vacancies (formed by light ions and neutrons and emitting at 800 nm) from other optically active defects emitting at 650 nm assigned to anti-site nitrogen vacancy (N B V N ) and reveal the presence of additional “dark” paramagnetic defects that influence spin-lattice relaxation time (T 1 ) and zero-field splitting parameters, all of which strongly depend on the defect density. These results underscore the potential for precisely engineered defect formation in large-scale CVD-grown hBN, paving the way for the scalable fabrication of quantum photonic devices.

CVD↗