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Observing femtosecond fragmentation using ultrafast X-ray-induced auger spectra

Wolf, Thomas J.A.; Holzmeier, Fabian; Wagner, Isabella; Berrah, Nora; Bostedt, Christoph; Bozek, John; Bucksbaum, Phil; Coffee, Ryan; Cryan, James and Farrell, Joe, et al. (2017) In Applied Sciences (Switzerland) 7(7).
Abstract

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 thymine0s 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... (More)

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 thymine0s 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.

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publication status
published
subject
keywords
Auger electron spectroscopy, Photochemistry, Photofragmentation, Ultrafast dynamics
in
Applied Sciences (Switzerland)
volume
7
issue
7
external identifiers
  • scopus:85021624051
  • wos:000407700400038
DOI
10.3390/app7070681
language
English
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yes
id
8c23f1bb-0294-47b5-acca-4617eb24f53c
date added to LUP
2017-07-18 14:59:40
date last changed
2017-09-18 11:38:36
@article{8c23f1bb-0294-47b5-acca-4617eb24f53c,
  abstract     = {<p>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 thymine0s 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.</p>},
  articleno    = {681},
  author       = {Wolf, Thomas J.A. and Holzmeier, Fabian and Wagner, Isabella and Berrah, Nora and Bostedt, Christoph and Bozek, John and Bucksbaum, Phil and Coffee, Ryan and Cryan, James and Farrell, Joe and Feifel, Raimund and Martinez, Todd J. and McFarland, Brian and Mucke, Melanie and Nandi, Saikat and Tarantelli, Francesco and Fischer, Ingo and Gühr, Markus},
  keyword      = {Auger electron spectroscopy,Photochemistry,Photofragmentation,Ultrafast dynamics},
  language     = {eng},
  month        = {07},
  number       = {7},
  series       = {Applied Sciences (Switzerland)},
  title        = {Observing femtosecond fragmentation using ultrafast X-ray-induced auger spectra},
  url          = {http://dx.doi.org/10.3390/app7070681},
  volume       = {7},
  year         = {2017},
}