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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 163 records · Page 9
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DOE OSTI2024

Multiparticle cumulant mapping for Coulomb explosion imaging: Calculations and algorithm

We present a versatile cumulant mapping algorithm for analyzing correlated particle emission, offering insights into complex electronic and nuclear dynamics. Recently, we have demonstrated the use of cumulant mapping to extract information-rich correlations between the momenta of multiple fragments produced in Coulomb explosion imaging experiments [C. Cheng et al., Phys. Rev. Lett. 130, 093001 (2023)]. We define cumulant mapping in terms of histograms, enabling fast computation of linear (additive) observables. However, applying the same algorithm to nonlinear (nonadditive) observables poses challenges, as the computation time of conventional estimators scales nonlinearly with data size. To overcome this, we develop estimators and an accompanying algorithm to enable computationally efficient estimation of the cumulant of interest. Comparisons of computation times and signal-to-noise ratios reveal the superior performance of our approach. This method is demonstrated on the (D+, D+, C+, O+) dissociation channel of CD 2 ⁢O 4+ produced in a strong-field ionization experiment. Additionally, Poisson statistics are used to simulate the two methods and provide insights into the efficiency of our algorithm. The proposed methodology unlocks efficient computation of cumulant mapping for a broader range of complex systems and observables, such as the laser pulse dependence of ionization dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Autoionizing polaritons with the Jaynes-Cummings model

Intense laser pulses have the capability to couple resonances in the continuum, leading to the formation of a split pair of autoionizing polaritons. These polaritons can exhibit extended lifetimes due to interference between radiative and Auger decay channels. In this work we show how an extension of the Jaynes-Cummings model to autoionizing states quantitatively reproduces the observed phenomenology. Furthermore, this extended model allows us to study how the dressing laser parameters can be tuned to control the ionization rate of the polariton multiplet.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Local distortion driven magnetic phase switching in pyrochlore Yb 2 ( Ti 1 - x Sn x ) 2 O 7

While it is commonly accepted that the disorder induced by magnetic ion doping in quantum magnets usually generates a rugged free-energy landscape resulting in slow or glassy spin dynamics, the disorder/distortion effects associated with nonmagnetic ion sites doping are still illusive. Here, using AC susceptibility measurements, we show that the mixture of Sn/Ti on the nonmagnetic ion sites of pyrochlore Yb 2 ⁢(Ti 1-x⁢ Sn x ) 2⁢ O 7 induces an antiferromagnetic ground state despite both parent compounds, Yb 2 ⁢Ti 2 ⁢O 7 and Yb 2 ⁢Sn 2⁢ O 7 , order ferromagnetically. Local structure studies through neutron total scattering reveals the local distortion in the nonmagnetic ion sites and its strong correlation with the magnetic phase switching. Further, our study demonstrates the local distortion as induced by the nonmagnetic ion site mixture could be a new path to achieve magnetic phase switching, which has been traditionally obtained by external stimuli such as temperature, magnetic field, pressure, strain, light, etc.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Effect of interfacial vibrational coupling on surface wettability and water transport

Here, we report that the atomic-scale vibrational coupling at the solid-fluid interface can substantially alter the interfacial properties such as wettability and fluid slip. The wettability of water droplets on substrates subjected to various vibrational frequencies is studied using molecular dynamics simulation. The contact angle increases (i.e., becomes more hydrophobic) when the oscillation frequency of the substrate matches the intermolecular bending frequency of liquid water. We investigate the underlying mechanism by examining the dynamics of water molecules at the interface and find that the temporal contact between the solid and fluid is shorter when the frequencies match, resulting in weak solid-fluid adsorption. We further report that the vibrational match at the interface reduces wall-fluid friction and enhances water transport through the nanopore. Our findings demonstrate the importance of the atomic-scale vibrational coupling at the solid-fluid interface on the physicochemical behavior of nanodevices and biological nanochannels.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Autoionizing Polaritons in Attosecond Atomic Ionization

Light-induced states and Autler-Townes splitting of laser-coupled states are common features in the photoionization spectra of laser-dressed atoms. The entangled light-matter character of metastable Autler-Townes multiplets, which makes them autoionizing polaritons, however, is still largely unexplored. We employ attosecond transient-absorption spectroscopy in argon to study the formation of polariton multiplets between the 3s –1 4p and several light-induced states. We measure a controllable stabilization of the polaritons against ionization, in excellent agreement with ab initio theory. Using an extension of the Jaynes-Cummings model to autoionizing states, we show that this stabilization is due to the destructive interference between the Auger decay and the radiative ionization of the polaritonic components. Furthermore, these results give new insights into the optical control of electronic structure in the continuum and unlock the door to applications of radiative stabilization in metastable polyelectronic systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Raman Interferometry between Autoionizing States to Probe Ultrafast Wave-Packet Dynamics with High Spectral Resolution

Photoelectron interferometry with femtosecond and attosecond light pulses is a powerful probe of the fast electron wave-packet dynamics, albeit it has practical limitations on the energy resolution. We show that one can simultaneously obtain both high temporal and spectral resolution by stimulating Raman interferences with one light pulse and monitoring the modification of the electron yield in a separate step. Applying this spectroscopic approach to the autoionizing states of argon, we experimentally resolved its electronic composition and time evolution in exquisite detail. Theoretical calculations show remarkable agreement with the observations and shed light on the light-matter interaction parameters. Using appropriate Raman probing and delayed detection steps, this technique enables highly sensitive probing and control of electron dynamics in complex systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Two-Center Interference in the Photoionization Delays of Kr 2

Herein we present the experimental observation of two-center interference in the ionization time delays of Kr 2 . Using attosecond electron-ion-coincidence spectroscopy, we simultaneously measure the photoionization delays of krypton monomer and dimer. The relative time delay is found to oscillate as a function of the electron kinetic energy, an effect that is traced back to constructive and destructive interference of the photoelectron wave packets that are emitted or scattered from the two atomic centers. Our interpretation of the experimental results is supported by solving the time-independent Schrödinger equation of a 1D double-well potential, as well as coupled-channel multiconfigurational quantum-scattering calculations of Kr 2 . This work opens the door to the study of a broad class of quantum-interference effects in photoionization delays and demonstrates the potential of attosecond coincidence spectroscopy for studying weakly bound systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

Close-coupling approach to electron scattering with multielectron targets

Momentum-space close coupling calculations of electron scattering require removal of spurious and unphysical solutions. Here, we demonstrate here that removal of these solutions involve regulator operators that enforce Pauli exclusion selection rules in addition to removing spurious solutions. The form of a regular operator for e-H scattering has already been established, but a general extension to the multielectron case has been elusive. Here we present a general method for scattering on multielectron targets, atoms, or molecules, ensuring that the scattering solutions obey Pauli-exclusion selection rules. The regulator operator is obtained by finding the null space vectors of the 𝑁+1 electrons of the projectile and target atom scattering system. We demonstrate that this general procedure reduces to the e-H result and provide examples for He- and Li-like targets as well as guidance for implementation.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

New correlated numerical methods for attosecond molecular single and double ionization

This project resulted in the development of ASTRA, a new molecular ionization code capable of describing single and double ionization processes in polyatomic molecules with correlated electrons and time-dependent fields. Key achievements include: (i) the development of the PRISM hybrid-integral library enabling core-ionization and high-angular-momentum convergence; (ii) implementation of time-dependent Schrödinger equation solvers for pump–probe spectroscopies; (iii) validation against experimental and theoretical benchmarks for atoms and molecules; and (iv) extension to two-photon double ionization using the finite-pulse virtual-sequential model. These developments establish ASTRA as a versatile platform for attosecond molecular dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1991

The physical properties of giant molecular cloud complexes in the outer Galaxy - Implications for the ratio of H2 column density to (C-12)O intensity

The physical properties of 35 giant molecular cloud complexes in the outer Galaxy were derived from the Goddard-Columbia surveys of the Galactic plane region (Dame et al., 1987). The spatial and radial velocity boundaries for the individual cloud complexes were estimated by analyzing the spatial and velocity structure of emission features in the (C-12)O surveys, and the distance to each cmplex was determined kinematically on the assumption of a flat rotation curve. The ratio of the H2 column density to the (C-12)O intensity for the outer Galaxy complexes was found to be about 6.0 x 10 to the 20th molecules/sq cm K per km/sec, which is by a factor of 2-3 greater than the value derived by other auhtors for the inner Galaxy complexes. This increase in the H2 column density/(C-12)O intensity with the distance from with the Galactic center is consistent with predictions of the optically thick cloudlet model of giant molecular cloud complexes.

Sodroski, T. J.↗
DOE OSTI2026

Spectral deconvolution without the deconvolution: Extracting temperature from x-ray Thomson scattering spectra without the source-and-instrument function

X-ray Thomson scattering (XRTS) probes the dynamic structure factor of the system, but the measured spectrum is broadened by the combined source-and-instrument function (SIF) of the setup. In order to extract properties such as temperature from an XRTS spectrum, the broadening by the SIF needs to be removed. Recent work [Dornheim et al. Nat. Commun. 13 , 7911 (2022)] has suggested that the SIF may be deconvolved using the two-sided Laplace transform. However, the extracted information can depend strongly on the shape of the input SIF, and the SIF is in practice challenging to measure accurately. Here, we propose an alternative approach: we demonstrate that considering ratios of Laplace-transformed XRTS spectra collected at different scattering angles is equivalent to performing the deconvolution, but without the need for explicit knowledge of the SIF. From these ratios, it is possible to directly extract the temperature from the scattering spectra, when the system is in thermal equilibrium. We find the method to be generally robust to spectral noise and physical differences between the spectrometers, and we explore situations in which the method breaks down. Furthermore, the fact that consistent temperatures can be extracted for systems in thermal equilibrium indicates that non-equilibrium effects could be identified by inconsistent temperatures of a few eV between the ratios of three or more scattering angles.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Opacity on NIF: Anchor 2 Iron (Level 2 Milestone 7118 Report)

In FY2020 we fulfilled the exit criteria of milestone 7118. We fielded iron opacity experiments at higher densities and temperatures approaching anchor 2 conditions and made good progress on overcoming the problems that we found. This report describes in detail the progress that has been made. We presented the results in a LANL seminar on August 10 and we gave two talks on our results to the National Opacity Workshop Series, one on July 9 and the other on September 14. Before discussing the anchor 2 measurements, we present an update of the NIF anchor 1 data. We did a new analysis of the anchor 1 data and compared the results to a series of calculations using the LANL ATOMIC code. Figures 1 and 2 compare the data with the best-fit to calculations. This result is significantly improved over the result published in Atoms. The differences are small for the iron quasi-continuum between 8-9.5 Å and for the Mg Heα and Lyα lines. The opacities near the centers of the iron bound-bound features also match fairly well in the 9.5-12.5 Å range. However, the opacity windows between the large iron bound-bound features are deeper in the Atomic predictions than the measurement. Furthermore, large discrepancies exist for the Mg He β, γ, and δ lines and for the short-wavelength quasicontinuum. The experiment and analysis refinements described below have set the stage for unraveling these discrepancies. Specifically, we can repeat the Anchor 1 experiments using improved backlighter, hohlraum, and spectrometers to obtain reduced backgrounds and better spectral resolution. Exploiting the AlMg calibration experiments and repeating the Anchor 1 measurements multiple times will enable formal and rigorous uncertainty determination. This well-defined path gives us confidence that high quality opacity data can be obtained on NIF.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Applying Bayesian inference and deterministic anisotropy to retrieve the molecular structure ∣Ψ(R)∣2 distribution from gas-phase diffraction experiments

Abstract Currently, our general approach to retrieving molecular structures from ultrafast gas-phase diffraction heavily relies on complex ab initio electronic or vibrational excited state simulations to make conclusive interpretations. Without such simulations, inverting this measurement for the structural probability distribution is typically intractable. This creates a so-called inverse problem. Here we address this inverse problem by developing a broadly applicable method that approximates the molecular frame structure ∣Ψ( R , t )∣ 2 distribution independent of these complex simulations. We retrieve the vibronic ground state ∣Ψ( R )∣ 2 for both simulated stretched NO 2 and measured N 2 O. From measured N 2 O, we observe 40 mÅ coordinate-space resolution from 3.75 Å −1 reciprocal space range and poor signal-to-noise, a 50X improvement over traditional Fourier transform methods. In simulated NO 2 diffraction experiments, typical to high signal-to-noise levels predict 100–1000X resolution improvements, down to 0.1 mÅ. By directly measuring the width of ∣Ψ( R )∣ 2 , we open ultrafast gas-phase diffraction capabilities to measurements beyond current analysis approaches. This method has the potential to effectively turn gas-phase ultrafast diffraction into a discovery-oriented technique to probe systems that are prohibitively difficult to simulate.

74 ATOMIC AND MOLECULAR PHYSICS↗