skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Observing Femtosecond Fragmentation Using Ultrafast X-ray-Induced Auger Spectra

Journal Article · · Applied Sciences
DOI:https://doi.org/10.3390/app7070681· OSTI ID:1390703
 [1];  [2];  [3];  [4];  [5];  [6];  [7];  [1];  [1];  [1];  [8];  [7];  [1];  [9];  [10];  [11];  [3];  [12]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Synchrotron SOLEIL (France); Univ. of Wurzburg (Germany)
  3. Univ. of Wurzburg (Germany)
  4. Univ. of Connecticut, Storrs, CT (United States)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
  6. Synchrotron SOLEIL (France); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
  8. Univ. of Gothenburg (Sweden)
  9. Uppsala Univ. (Sweden)
  10. Synchrotron SOLEIL (France); Lund Univ. (Sweden)
  11. Univ. of Perugia (Italy)
  12. SLAC National Accelerator Lab., Menlo Park, CA (United States); Univ. of Potsdam (Germany)

Molecules often fragment after photoionization in the gas phase. Usually, this process can only be investigated spectroscopically as long as there exists electron correlation between the photofragments. Important parameters, like their kinetic energy after separation, cannot be investigated. We are reporting on a femtosecond time-resolved Auger electron spectroscopy study concerning the photofragmentation dynamics of thymine. We observe the appearance of clearly distinguishable signatures from thymine's neutral photofragment isocyanic acid. Furthermore, we observe a time-dependent shift of its spectrum, which we can attribute to the influence of the charged fragment on the Auger electron. This allows us to map our time-dependent dataset onto the fragmentation coordinate. The time dependence of the shift supports efficient transformation of the excess energy gained from photoionization into kinetic energy of the fragments. Our method is broadly applicable to the investigation of photofragmentation processes.

Research Organization:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1390703
Journal Information:
Applied Sciences, Vol. 7, Issue 7; ISSN 2076-3417
Publisher:
MDPICopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 17 works
Citation information provided by
Web of Science

References (34)

Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction journal June 2015
Operation of a free-electron laser from the extreme ultraviolet to the water window journal June 2007
A compact X-ray free-electron laser emitting in the sub-ångström region journal June 2012
Understanding the modulation mechanism in resonance-enhanced multiphoton probing of molecular dynamics journal March 2015
Astrochemistry of dust, ice and gas: introduction and overview journal January 2014
First lasing and operation of an ångstrom-wavelength free-electron laser journal August 2010
Higher-order approximations for the particle-particle propagator journal October 1984
Radical cations of DNA bases: some insights on structure and fragmentation patterns by density functional methods journal July 2000
Ultrafast X-ray Auger probing of photoexcited molecular dynamics journal June 2014
Free-Electron Lasers: New Avenues in Molecular Physics and Photochemistry journal May 2012
The Auger spectroscopy of pyrimidine and halogen-substituted pyrimidines journal October 2008
Experimental strategies for optical pump – soft x-ray probe experiments at the LCLS journal April 2014
X-ray–optical cross-correlator for gas-phase experiments at the Linac Coherent Light Source free-electron laser journal March 2012
AMO instrumentation for the LCLS X-ray FEL journal March 2009
Ultrafast isomerization initiated by X-ray core ionization journal September 2015
Electron affinities of the first‐row atoms revisited. Systematic basis sets and wave functions journal May 1992
Imaging charge transfer in iodomethane upon x-ray photoabsorption journal July 2014
The Atomic, Molecular and Optical Science instrument at the Linac Coherent Light Source journal April 2015
Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses journal April 2016
A multi purpose source chamber at the PLEIADES beamline at SOLEIL for spectroscopic studies of isolated species: Cold molecules, clusters, and nanoparticles journal November 2013
Highly coherent and stable pulses from the FERMI seeded free-electron laser in the extreme ultraviolet journal September 2012
Photoion mass spectrometry of adenine, thymine and uracil in the 6–22eV photon energy range journal July 2005
Synthesis, Properties and Dimerization Study of Isocyanic Acid journal January 2002
The calculation of molecular double ionization spectra by Green’s functions journal October 2006
Self-Referenced Coherent Diffraction X-Ray Movie of Ångstrom- and Femtosecond-Scale Atomic Motion journal October 2016
Probing ultrafast ππ*/nπ* internal conversion in organic chromophores via K-edge resonant absorption journal June 2017
Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules journal October 2016
Double-core-hole spectroscopy for chemical analysis with an intense X-ray femtosecond laser journal October 2011
Ultralong-range energy transfer by interatomic Coulombic decay in an extreme quantum system journal June 2010
Determination of the K—LL Auger Spectra of N 2 , O 2 , CO, NO, H 2 O, and CO 2 journal September 1971
Discerning vibronic molecular dynamics using time-resolved photoelectron spectroscopy journal September 1999
Ultrafast Electron Diffraction (UED): A New Development for the 4D Determination of Transient Molecular Structures journal June 2003
Femtochemistry: Atomic-Scale Dynamics of the Chemical Bond Using Ultrafast Lasers (Nobel Lecture) journal August 2000
A core-level photoionization study of furan journal October 2002

Cited By (4)

Computing the Ultrafast and Radiationless Electronic Excited State Decay of Cytosine and 5‐methyl‐cytosine Cations: Uncovering the Role of Dynamic Electron Correlation journal May 2019
Modeling multidimensional spectral lineshapes from first principles: application to water-solvated adenine journal January 2020
Normal and resonant Auger spectroscopy of isocyanic acid, HNCO journal July 2018
Photochemical pathways in nucleobases measured with an X-ray FEL
  • Wolf, Thomas J. A.; Gühr, Markus
  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145 https://doi.org/10.1098/rsta.2017.0473
journal April 2019

Similar Records

Femtosecond probing of sodium cluster ion Na sub n sup + fragmentation
Journal Article · Mon Sep 07 00:00:00 EDT 1992 · Physical Review Letters; (United States) · OSTI ID:1390703

Laser control over the ultrafast Coulomb explosion of N22+ after Auger decay: A quantum-dynamics investigation
Journal Article · Mon Apr 24 00:00:00 EDT 2017 · Physical Review A · OSTI ID:1390703

Transient resonant Auger–Meitner spectra of photoexcited thymine
Journal Article · Wed Nov 18 00:00:00 EST 2020 · Faraday Discussions · OSTI ID:1390703