Calibrating TDDFT Calculations of the X-ray Emission Spectrum of Liquid Water: The Effects of Hartree–Fock Exchange DOI Creative Commons
Thomas Fransson, Lars G. M. Pettersson

Journal of Chemical Theory and Computation, Journal Year: 2023, Volume and Issue: 19(20), P. 7333 - 7342

Published: Oct. 3, 2023

The structure and dynamics of liquid water continue to be debated, with insight provided by, among others, X-ray emission spectroscopy (XES), which shows a split in the high-energy 1b1 feature. This is yet reproduced by theory, it remains unclear if these difficulties are related inaccuracies simulations, spectrum calculations, or both. We investigate performance different methods for calculating XES water, focusing on ability time-dependent density functional theory (TDDFT) reproduce reference spectra obtained high-level coupled cluster algebraic-diagrammatic construction scheme calculations. A metric evaluating agreement between theoretical termed integrated absolute difference (IAD), considers integral shifted spectra, introduced used exchange-correlation functionals. find that computed symmetric asymmetric model structures strongly differently influenced amount Hartree-Fock exchange, best ∼40-50%. Lower percentages tend yield high contributing states, resulting too broad features. method here useful also other particular where ensembles evaluated.

Language: Английский

Resonant inelastic X-ray scattering DOI
Frank M. F. de Groot, M. W. Haverkort, Hebatalla Elnaggar

et al.

Nature Reviews Methods Primers, Journal Year: 2024, Volume and Issue: 4(1)

Published: July 4, 2024

Language: Английский

Citations

12
Rebuilding the vibrational wavepacket in TRAS using attosecond X-ray pulses DOI Creative Commons
Chao Wang, Maomao Gong, Xi Zhao

et al.

Communications Physics, Journal Year: 2024, Volume and Issue: 7(1)

Published: Jan. 2, 2024

Abstract Time-resolved X-ray photoelectron spectroscopy (TXPS) is a well-established technique to probe coherent nuclear wavepacket dynamics using both table-top and free-electron-based ultrafast lasers. Energy resolution, however, becomes compromised for very short pulse duration in the sub-femtosecond range. By resonantly tuning core-excited states undergoing Auger decay, this drawback of TXPS can be mitigated. While resonant Auger-electron (RAS) recover vibrational structures not hidden by broadband excitation, full reconstruction standing challenge. Here, we theoretically demonstrate how complete information wavepacket, i.e., populations relative phases constituting retrieved from time-resolved RAS (TRAS) measurements. Thus, TRAS offers key insights into coupled electronic complex systems on ultrashort timescales, providing an alternative leverage femtosecond attosecond pulses.

Language: Английский

Citations

11
Exploring Quantum Materials with Resonant Inelastic X-Ray Scattering DOI Creative Commons
Matteo Mitrano, Steven Johnston, Young‐June Kim

et al.

Physical Review X, Journal Year: 2024, Volume and Issue: 14(4)

Published: Dec. 13, 2024

Understanding quantum materials—solids in which interactions among constituent electrons yield a great variety of novel emergent phenomena—is forefront challenge modern condensed matter physics. This goal has driven the invention and refinement several experimental methods, can spectroscopically determine elementary excitations correlation functions that material properties. Here we focus on future theoretical trends resonant inelastic x-ray scattering (RIXS), is remarkably versatile rapidly growing technique for probing different charge, lattice, spin, orbital materials. We provide forward-looking introduction to RIXS outline how this poised deepen our insight into nature materials their electronic phenomena. Published by American Physical Society 2024

Language: Английский

Citations

6
Parity violation in resonant inelastic soft x-ray scattering at entangled core holes DOI Creative Commons
Johan Söderström, Anirudha Ghosh, Ludvig Kjellsson

et al.

Science Advances, Journal Year: 2024, Volume and Issue: 10(7)

Published: Feb. 14, 2024

Resonant inelastic x-ray scattering (RIXS) is a major method for investigation of electronic structure and dynamics, with applications ranging from basic atomic physics to materials science. In RIXS applied inversion-symmetric systems, it has generally been accepted that strict parity selectivity applies in the sub–kilo–electron volt region. contrast, we show selection rule violated spectra free homonuclear diatomic O 2 molecule. By analyzing spectral dependence on angle, demonstrate violation due phase difference coherent at two sites, analogy Young’s double-slit experiment. The result also implies interpretation absorption inversion symmetric molecules this energy range must be revised.

Language: Английский

Citations

4
Elementary excitations of single-photon emitters in hexagonal boron nitride DOI
Jonathan Pelliciari, Enrique Mejía‐Ospino, John M. Woods

et al.

Nature Materials, Journal Year: 2024, Volume and Issue: 23(9), P. 1230 - 1236

Published: April 23, 2024

Language: Английский

Citations

4
Stimulated resonant inelastic X-ray scattering in a solid DOI Creative Commons
Daniel J. Higley, Zhao Chen, Martin Beye

et al.

Communications Physics, Journal Year: 2022, Volume and Issue: 5(1)

Published: April 6, 2022

Abstract When materials are exposed to X-ray pulses with sufficiently high intensity, various nonlinear effects can occur. The most fundamental one consists of stimulated electronic decays after resonant absorption X-rays. Such enhance the number emitted photons and emission direction is confined that stimulating incident which clone themselves in process. Here we report observation elastic (REXS) inelastic (RIXS) scattering near cobalt L 3 edge solid Co/Pd multilayer samples. We observe an enhancement order 10 6 over conventional spontaneous RIXS signal into small acceptance angle spectrometer. also find solids both REXS spectra contain contributions from electron processes, even for ultrashort 5 fs pulses. Our results reveal potential caveats development condensed matter.

Language: Английский

Citations

17
Imaging temperature and thickness of thin planar liquid water jets in vacuum DOI Creative Commons
Tillmann Buttersack, Henrik Haak, Hendrik Bluhm

et al.

Structural Dynamics, Journal Year: 2023, Volume and Issue: 10(3)

Published: May 1, 2023

We present spatially resolved measurements of the temperature a flat liquid water microjet for varying ambient pressures, from vacuum to 100% relative humidity. The entire jet surface is probed in single shot by high-resolution infrared camera. Obtained 2D images are substantially influenced apparatus on opposite side camera; protocol correct thermal background radiation presented. In vacuum, we observe cooling rates due evaporation order 10

Language: Английский

Citations

10
A Combined Experimental and Computational Study on the Broadening Mechanism of the Luminescence in Narrow-Band Eu2+-Doped Phosphors DOI Creative Commons
Rami Shafei, Philipp Strobel, Peter J. Schmidt

et al.

The Journal of Physical Chemistry C, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

In this work, we present a comprehensive study of the luminescence relaxation mechanism and associated spectral broadening in series Eu2+-doped narrow-band phosphors. It is highlighted that commonly used full-width at half-maximum (fwhm) no longer sensitive measure for quantifying emission bandwidth these materials. A thorough understanding factors contributing to narrow requires an explicit treatment magnetic structure ground emissive excited state manifolds. This incorporating spin–orbit coupling effects using wave function-based methods such as complete active space self-consistent field combined with second-order N-electron valence perturbation theory (CASSCF/NEVPT2). addition, dynamics calculations, one needs consider vibronic interactions on basis Franck–Condon (FC), Herzberg–Teller (HT), and, when necessary, pseudo Jahn–Teller (PJT) effects. Our analysis underscores controlling synergistic roles "static" "dynamic" are essential accurately assessing band systems. We show results can, principle, be generalized arbitrary set phosphor candidates can potentially aid experimental efforts toward developing novel phosphors enhanced luminescent properties.

Language: Английский

Citations

0
Quasimolecular electronic structure of the trimer iridate Ba4NbIr3O12 DOI
M. Magnaterra, Anna Sandberg,

Harold K. Schilling

et al.

Physical review. B./Physical review. B, Journal Year: 2025, Volume and Issue: 111(8)

Published: Feb. 10, 2025

Citations

0
Universality of extreme-broadening mechanisms in some near-edge x-ray spectra DOI

Terrence Jach,

John Vinson, Michael Woodcox

et al.

Physical review. B./Physical review. B, Journal Year: 2025, Volume and Issue: 111(12)

Published: March 5, 2025

Extreme broadening previously observed in certain N x-ray fluorescence lines excited near the K edge nitrates has been S L sodium sulfate, ${\mathrm{Na}}_{2}{\mathrm{SO}}_{4}$. It is explained as a large imaginary self-energy corresponding to an anomalously short lifetime of quasiparticles one valence bands these compounds. Our latest measurement and many-body theory indicate that this general effect not specific nitrates.

Language: Английский

Citations

0