Revealing fingerprints of valence excitons in x-ray absorption spectra with the Bethe-Salpeter equation DOI
Nasrin Farahani, Daria Popova-Gorelova

Physical review. B./Physical review. B, Journal Year: 2024, Volume and Issue: 110(23)

Published: Dec. 10, 2024

The Bethe-Salpeter equation (BSE) is a powerful theoretical approach that capable to accurately treat electron-hole interactions in materials an excited state. We developed ab initio framework based on the BSE describe pump-probe experiment, which x-ray pulse probes solid-state valence excitons by means of absorption spectroscopy. Our relevance for accurate modeling experiments photoexcited utilize novel capabilities offered science.

Language: Английский

Solvatochromism Observed in the X-ray Absorption Spectrum of Indole Dissolved in Water DOI
Shota Tsuru, Masanari Nagasaka

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

Published: March 21, 2025

Current developments in X-ray absorption spectroscopy (XAS) for liquid samples the water window demand a rigorous understanding of interactions between molecules or solute–solvent observed spectra. Meanwhile, theoretical description such effects, addition to inner-shell excitations, remains controversial. The controversy is mainly over whether orbitals should be optimized final states orbital optimizations can expressed by dynamic electron correlation. In present work, we measured XAS spectra indole aqueous solution at carbon and nitrogen K-edges compare them with those gas phase. Obvious solvatochromism was only spectrum K-edge. We then interpreted simulating both ΔSCF, where were states, algebraic-diagrammatic construction through second order [ADC(2)], molecular ground state used throughout. results indicate that covalent interactions, as hydrogen bonds, are dominant causes solvation effects simulations ΔSCF ADC(2), some other reports, highlight importance optimizing excited general calculations predictive accuracy.

Language: Английский

Citations

0
Laboratory soft X-ray setup for transient absorption experiments in the liquid phase using a laser-produced plasma source DOI Creative Commons
Richard Gnewkow, H. Stiel, Adrian Jonas

et al.

Optica, Journal Year: 2024, Volume and Issue: 11(6), P. 744 - 744

Published: April 8, 2024

With time-resolved soft X-ray spectroscopy, the element-specific dynamics of electronic structure disordered systems can be investigated. Measurements species in dilute liquid solutions are particularly challenging and require high photon flux combined with low experimental noise. This mostly limited these experiments to large-scale facilities, especially for energies above water window (533 eV). Based on a laser-produced plasma source, our system enables, best knowledge, first static transient phase performed laboratory up 1400 eV time resolution 500 ps. We benchmark investigations [Ni(CN) 4 ] 2− widely used model complex [Fe(bpy) 3 2+ , both an aqueous solution. The introduced self-referencing concept ensures that measurements noise limited. Our results form basis further liquid-phase investigating diluted solutions.

Language: Английский

Citations

2
Perspective: towards real-time extreme ultraviolet to x-ray imaging and spectroscopy of laser-driven materials DOI Creative Commons
Daria Popova-Gorelova

Journal of Physics B Atomic Molecular and Optical Physics, Journal Year: 2024, Volume and Issue: 57(17), P. 172501 - 172501

Published: July 5, 2024

Abstract Optical manipulation of light is a highly relevant concept in modern solid-state physics and its microscopic mechanisms are widely investigated. From this perspective, we discuss how x-ray extreme ultraviolet pulses that probe material during the time it driven by optical can deliver valuable details about electron dynamics.

Language: Английский

Citations

2
Few-femtosecond soft X-ray transient absorption spectroscopy with tuneable DUV-Vis pump pulses DOI Creative Commons

Jacob P. Lee,

Timur Avni, Oliver Alexander

et al.

Optica, Journal Year: 2024, Volume and Issue: 11(9), P. 1320 - 1320

Published: Sept. 3, 2024

Achieving few-femtosecond resolution for a pump-probe experiment is crucial to measuring the fastest electron dynamics and creating superpositions of valence states in quantum systems. However, traditional UV-Vis pump pulses cannot achieve few-fs durations usually operate at fixed wavelengths. Here, we present, our knowledge, an unprecedented temporal tuneability UV-Vis-pumped soft X-ray transient absorption spectroscopy. We have combined deep-UV visible tuneable from resonant dispersive wave emission hollow capillary fiber with attosecond probe high harmonic generation. sub-5-fs time resolution, sub-fs interferometric stability, continuous 230 700 nm. demonstrate that can initiate ultrafast photochemical reaction different atomic sites be resolved simultaneously. These capabilities will allow studies electronic large range photochemical, photobiological photovoltaic reactions.

Language: Английский

Citations

2
Preface to Special Topic: The Advent of Ultrafast X-Ray Absorption Spectroscopy DOI Creative Commons
Emiliano Principi

Structural Dynamics, Journal Year: 2024, Volume and Issue: 11(3)

Published: May 1, 2024

Views Icon Article contents Figures & tables Video Audio Supplementary Data Peer Review Share Twitter Facebook Reddit LinkedIn Tools Reprints and Permissions Cite Search Site Citation Emiliano Principi; Preface to Special Topic: The Advent of Ultrafast X-Ray Absorption Spectroscopy. Struct. Dyn. 1 May 2024; 11 (3): 030401. https://doi.org/10.1063/4.0000259 Download citation file: Ris (Zotero) Reference Manager EasyBib Bookends Mendeley Papers EndNote RefWorks BibTex toolbar search Dropdown Menu input auto suggest filter your All ContentAmerican Crystallographic Association IncStructural Dynamics Advanced |Citation

Language: Английский

Citations

0
Role of crystal orientation in attosecond photoinjection dynamics of germanium DOI Creative Commons
Nicola Di Palo, Lyudmyla Adamska, Simone Bonetti

et al.

Structural Dynamics, Journal Year: 2024, Volume and Issue: 11(4)

Published: July 1, 2024

Understanding photoinjection in semiconductors-a fundamental physical process-represents the first step toward devising new opto-electronic devices, capable of operating on unprecedented time scales. Fostered by development few-femtosecond, intense infrared pulses, and attosecond spectroscopy techniques, ultrafast charge injection solids has been subject theoretical experimental investigation. Recent results have shown that while under certain conditions can be ascribed to a single, well-defined phenomenon, realistic multi-band semiconductor like Ge, several competing mechanisms determine sub-cycle interaction an light field with atomic electronic structure matter. In this latter case, it is yet unclear how complex balance between different altered chosen geometry, dictated relative orientation crystal lattice laser electric direction. work, we investigate Ge monocrystalline sample temporal resolution two distinct orientations. Our combined effort suggests determining carrier excitation are largely robust against rotation. Nevertheless, alignment unit cell causes non-negligible changes momentum distribution excited carriers their yield. Further experiments needed clarify whether used tune at these extreme

Language: Английский

Citations

0
Exploring the Influence of Approximations for Simulating Valence Excited X-ray Spectra DOI Creative Commons
Thomas J. Penfold, Basile F. E. Curchod

The Journal of Physical Chemistry A, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 4, 2024

First-principles simulations of excited-state X-ray spectra are becoming increasingly important to interpret the wealth electronic and geometric information contained within femtosecond absorption recorded at Free Electron Lasers (X-FELs). However, because transition dipole matrix elements must be calculated between two excited states (i.e., valence state final core arising from initial state) very different energies, this can challenging time-consuming compute. Herein using molecules, protonated formaldimine cyclobutanone, we assess ability

Language: Английский

Citations

0
Revealing fingerprints of valence excitons in x-ray absorption spectra with the Bethe-Salpeter equation DOI
Nasrin Farahani, Daria Popova-Gorelova

Physical review. B./Physical review. B, Journal Year: 2024, Volume and Issue: 110(23)

Published: Dec. 10, 2024

The Bethe-Salpeter equation (BSE) is a powerful theoretical approach that capable to accurately treat electron-hole interactions in materials an excited state. We developed ab initio framework based on the BSE describe pump-probe experiment, which x-ray pulse probes solid-state valence excitons by means of absorption spectroscopy. Our relevance for accurate modeling experiments photoexcited utilize novel capabilities offered science.

Language: Английский

Citations

0