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Title: Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

Journal Article · · Nature Communications
 [1];  [1];  [2];  [3];  [4];  [4];  [5];  [6];  [7];  [8];  [1];  [7];  [4];  [4];  [1];  [1];  [1];  [4];  [4];  [1] more »;  [1];  [9];  [1];  [1];  [1] « less
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
  3. Kansas State Univ., Manhattan, KS (United States)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. Kansas State Univ., Manhattan, KS (United States); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  6. Univ. of Connecticut, Storrs, CT (United States)
  7. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  8. Argonne National Lab. (ANL), Argonne, IL (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  9. SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Specifically, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. In this paper, we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF2 molecules following X-ray absorption at the Xe site.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1272409
Journal Information:
Nature Communications, Vol. 7; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 61 works
Citation information provided by
Web of Science

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Biomolecular imaging and electronic damage using X-ray free-electron lasers text January 2010
When X-rays modify the protein structure: radiation damage at work journal April 2005
Potential for biomolecular imaging with femtosecond X-ray pulses journal August 2000
Selecting core-hole localization or delocalization in CS2 by photofragmentation dynamics journal January 2015
Ultrafast isomerization initiated by X-ray core ionization journal September 2015
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Observation of femtosecond X-ray interactions with matter using an X-ray–X-ray pump–probe scheme journal January 2016
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Cited By (32)

Generation of two-color terahertz radiation using Smith–Purcell emitter and periodic dielectric layers journal February 2019
Accurate prediction of X-ray pulse properties from a free-electron laser using machine learning journal June 2017
Symmetry breakdown of electron emission in extreme ultraviolet photoionization of argon journal November 2018
Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following X-ray multiphoton ionization journal September 2019
Shot-by-shot characterization of focused X-ray free electron laser pulses journal January 2018
Probing memristive switching in nanoionic devices journal May 2018
Alignment, orientation, and Coulomb explosion of difluoroiodobenzene studied with the pixel imaging mass spectrometry (PImMS) camera journal July 2017
Photodissociation of aligned CH 3 I and C 6 H 3 F 2 I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization journal January 2018
Development of a hard X-ray split-and-delay line and performance simulations for two-color pump-probe experiments at the European XFEL journal June 2018
Detecting coherent core-hole wave-packet dynamics in N 2 by time- and angle-resolved inner-shell photoelectron spectroscopy journal August 2019
Density matrix-based time-dependent configuration interaction approach to ultrafast spin-flip dynamics journal December 2016
Roadmap of ultrafast x-ray atomic and molecular physics journal January 2018
Quantum modeling of ultrafast photoinduced charge separation journal December 2017
Nonlinear resonant Auger spectroscopy in CO using an x-ray pump-control scheme journal December 2016
Control of the Lasing Slice by Transverse Mismatch in an X-Ray Free-Electron Laser journal August 2018
The LAMP instrument at the Linac Coherent Light Source free-electron laser text January 2018
Ultrashort Free-Electron Laser X-ray Pulses journal September 2017
Time-Resolved X-ray Absorption Spectroscopy in (Photo)Electrochemistry journal December 2018
The LAMP instrument at the Linac Coherent Light Source free-electron laser journal March 2018
Development of a hard X-ray split-and-delay line and performance simulations for two-color pump-probe experiments at the European XFEL text January 2018
Roadmap of ultrafast x-ray atomic and molecular physics text January 2019
Ultrashort Free-Electron Laser X-ray Pulses text January 2017
Accurate prediction of X-ray pulse properties from a free-electron laser using machine learning text January 2017
Symmetry breakdown of electron emission in extreme ultraviolet photoionization of argon text January 2018
Detecting coherent core-hole wave-packet dynamics in N$_2$ by time- and angle-resolved inner-shell photoelectron spectroscopy text January 2019
Density matrix-based time-dependent configuration interaction approach to ultrafast spin-flip dynamics text January 2017
Ultrafast x-ray-induced nuclear dynamics in diatomic molecules using femtosecond x-ray-pump–x-ray-probe spectroscopy text January 2016
Density matrix-based time-dependent configuration interaction approach to ultrafast spin-flip dynamics text January 2017
Roadmap of ultrafast x-ray atomic and molecular physics text January 2018
Shot-by-shot characterization of focused X-ray free electron laser pulses journal January 2018
Ultrashort Free-Electron Laser X-ray Pulses text January 2017
Symmetry breakdown of electron emission in extreme ultraviolet photoionization of argon text January 2018

Figures / Tables (4)