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Title: Inception of electronic damage of matter by photon-driven post-ionization mechanisms

Journal Article · · Structural Dynamics
DOI: https://doi.org/10.1063/1.5090332 · OSTI ID:1625001

“Probe-before-destroy” methodology permitted diffraction and imaging measurements of intact specimens using ultrabright but highly destructive X-ray free-electron laser (XFEL) pulses. The methodology takes advantage of XFEL pulses ultrashort duration to outrun the destructive nature of the X-rays. Atomic movement, generally on the order of >50 fs, regulates the maximum pulse duration for intact specimen measurements. In this contribution, we report the electronic structure damage of a molecule with ultrashort X-ray pulses under preservation of the atoms’ positions. A detailed investigation of the X-ray induced processes revealed that X-ray absorption events in the solvent produce a significant number of solvated electrons within attosecond and femtosecond timescales that are capable of coulombic interactions with the probed molecules. The presented findings show a strong influence on the experimental spectra coming from ionization of the probed atoms’ surroundings leading to electronic structure modification much faster than direct absorption of photons. This work calls for consideration of this phenomenon in cases focused on samples embedded in, e.g., solutions or in matrices, which in fact concerns most of the experimental studies.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Ministry of Science and Higher Education; National Science Centre of Poland (NCN); Knut and Alice Wallenberg Foundation
Grant/Contract Number:
AC02-76SF00515; 2015/19/B/ST2/00931; KAW-2013.0020
OSTI ID:
1625001
Alternate ID(s):
OSTI ID: 1505255
Journal Information:
Structural Dynamics, Vol. 6, Issue 2; ISSN 2329-7778
Publisher:
American Crystallographic Association/AIPCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 8 works
Citation information provided by
Web of Science

References (57)

Temperature- and pressure-induced spin-state transitions in LaCoO 3 journal January 2006
Calculations of electron inelastic mean free paths. XI. Data for liquid water for energies from 50 eV to 30 keV: Calculations of electron inelastic mean free paths journal August 2016
Femtosecond X-ray Absorption Spectroscopy at a Hard X-ray Free Electron Laser: Application to Spin Crossover Dynamics journal January 2013
Disentangling Transient Charge Density and Metal–Ligand Covalency in Photoexcited Ferricyanide with Femtosecond Resonant Inelastic Soft X-ray Scattering journal June 2018
Disentangling Transient Charge Density and Metal–Ligand Covalency in Photoexcited Ferricyanide with Femtosecond Resonant Inelastic Soft X-ray Scattering text January 2018
Room temperature femtosecond X-ray diffraction of photosystem II microcrystals journal June 2012
Indefinitely stable iron(IV) cage complexes formed in water by air oxidation journal January 2017
Influence of the core hole on K β emission following photoionization or orbital electron capture: A comparison using MnO and 55 Fe 2 O 3 journal July 2001
Direct Determination of Metal Complexes’ Interaction with DNA by Atomic Telemetry and Multiscale Molecular Dynamics journal January 2017
Tracking excited-state charge and spin dynamics in iron coordination complexes journal May 2014
X-ray emission spectroscopy journal August 2009
The hydrated electron journal January 1967
X-ray pump optical probe cross-correlation study of GaAs journal January 2012
CSPAD-140k: A versatile detector for LCLS experiments
  • Herrmann, Sven; Boutet, Sébastien; Duda, Brian
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 718 https://doi.org/10.1016/j.nima.2013.01.057
journal August 2013
The CTM4XAS program for EELS and XAS spectral shape analysis of transition metal L edges journal October 2010
Femtosecond X-ray protein nanocrystallography journal February 2011
Femtosecond electronic response of atoms to ultra-intense X-rays journal July 2010
Feasibility of Valence-to-Core X-ray Emission Spectroscopy for Tracking Transient Species journal February 2015
Cryocooling and radiation damage in macromolecular crystallography journal December 2005
The Hydrated Electron journal December 1964
X-ray Emission Spectroscopy at X-ray Free Electron Lasers: Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis text January 2019
A von Hamos x-ray spectrometer based on a segmented-type diffraction crystal for single-shot x-ray emission spectroscopy and time-resolved resonant inelastic x-ray scattering studies journal October 2012
Femtosecond response of polyatomic molecules to ultra-intense hard X-rays journal May 2017
Empirical formula for cross section of direct electron-impact ionization of ions journal October 2000
Calculations of Electron Inelastic Mean Free Paths. XI. Data for Liquid Water for Energies from 50 eV to 30 keV text January 2020
Real Time Determination of the Electronic Structure of Unstable Reaction Intermediates during Au 2 O 3 Reduction journal December 2013
The Hydrated Electron journal May 2017
Atomic inner-shell X-ray laser at 1.46 nanometres pumped by an X-ray free-electron laser journal January 2012
Rational design of oxynitride materials: From theory to experiment journal January 2013
X-ray atomic scattering factors of low- Z ions with a core hole journal October 2007
X-ray Emission Spectroscopy at X-ray Free Electron Lasers: Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis journal December 2018
Generation of 1020 W cm−2 hard X-ray laser pulses with two-stage reflective focusing system journal April 2014
Fe L-Edge XAS Studies of K 4 [Fe(CN) 6 ] and K 3 [Fe(CN) 6 ]:  A Direct Probe of Back-Bonding journal August 2006
The xraylib library for X-ray–matter interactions. Recent developments journal November 2011
Determining electronic damage to biomolecular structures in x-ray free-electron-laser imaging experiments journal May 2013
Photoelectron spectroscopy of liquid water, some alcohols, and pure nonane in free micro jets journal June 1997
X-ray atomic scattering factors of low- Z ions with a core hole text January 2007
The CTM4XAS program for EELS and XAS spectral shape analysis of transition metal L edges journal October 2010
CSPAD-140k: A versatile detector for LCLS experiments
  • Herrmann, Sven; Boutet, Sébastien; Duda, Brian
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 718 https://doi.org/10.1016/j.nima.2013.01.057
journal August 2013
The xraylib library for X-ray–matter interactions. Recent developments journal November 2011
Direct Determination of Metal Complexes’ Interaction with DNA by Atomic Telemetry and Multiscale Molecular Dynamics journal January 2017
X-ray Emission Spectroscopy at X-ray Free Electron Lasers: Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis journal December 2018
Fe L-Edge XAS Studies of K 4 [Fe(CN) 6 ] and K 3 [Fe(CN) 6 ]:  A Direct Probe of Back-Bonding journal August 2006
Femtosecond X-ray Absorption Spectroscopy at a Hard X-ray Free Electron Laser: Application to Spin Crossover Dynamics journal January 2013
Feasibility of Valence-to-Core X-ray Emission Spectroscopy for Tracking Transient Species journal February 2015
Femtosecond electronic response of atoms to ultra-intense X-rays journal July 2010
Femtosecond X-ray protein nanocrystallography journal February 2011
Tracking excited-state charge and spin dynamics in iron coordination complexes journal May 2014
Femtosecond response of polyatomic molecules to ultra-intense hard X-rays journal May 2017
Indefinitely stable iron(IV) cage complexes formed in water by air oxidation journal January 2017
X-ray pump optical probe cross-correlation study of GaAs journal January 2012
Rational design of oxynitride materials: From theory to experiment journal January 2013
The hydrated electron journal January 1967
Photoelectron spectroscopy of liquid water, some alcohols, and pure nonane in free micro jets journal June 1997
A von Hamos x-ray spectrometer based on a segmented-type diffraction crystal for single-shot x-ray emission spectroscopy and time-resolved resonant inelastic x-ray scattering studies journal October 2012
Room temperature femtosecond X-ray diffraction of photosystem II microcrystals journal June 2012
Disentangling Transient Charge Density and Metal–Ligand Covalency in Photoexcited Ferricyanide with Femtosecond Resonant Inelastic Soft X-ray Scattering text January 2018

Cited By (1)

Femtosecond electronic structure response to high intensity XFEL pulses probed by iron X-ray emission spectroscopy journal October 2020

Figures / Tables (5)