Ultrafast dynamics of 2-thiouracil investigated by time-resolved Auger spectroscopy

Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review

Autorschaft

  • F. Lever
  • D. Mayer
  • D. Picconi
  • J. Metje
  • S. Alisauskas
  • F. Calegari
  • S. Düsterer
  • C. Ehlert
  • R. Feifel
  • M. Niebuhr
  • B. Manschwetus
  • M. Kuhlmann
  • T. Mazza
  • M. S. Robinson
  • R. J. Squibb
  • A. Trabattoni
  • M. Wallner
  • P. Saalfrank
  • T. J.A. Wolf
  • M. Gühr

Externe Organisationen

  • Universität Potsdam
  • Deutsches Elektronen-Synchrotron (DESY)
  • Universität Hamburg
  • Heidelberger Institut für Theoretische Studien (HITS gGmbH)
  • Göteborgs Universitet
  • European X-Ray Free-Electron Laser Facility GmbH (XFEL)
  • Stanford University
Forschungs-netzwerk anzeigen

Details

OriginalspracheEnglisch
Aufsatznummer014002
FachzeitschriftJournal of Physics B: Atomic, Molecular and Optical Physics
Jahrgang54
Ausgabenummer1
PublikationsstatusVeröffentlicht - 17 Dez. 2020
Extern publiziertJa

Abstract

We present time-resolved ultraviolet-pump X-ray probe Auger spectra of 2-thiouracil. An ultraviolet induced shift towards higher kinetic energies is observed in the sulfur 2p Auger decay. The difference Auger spectra of pumped and unpumped molecules exhibit ultrafast dynamics in the shift amplitude, in which three phases can be recognized. In the first 100 fs, a shift towards higher kinetic energies is observed, followed by a 400 fs shift back to lower kinetic energies and a 1 ps shift again to higher kinetic energies. We use a simple Coulomb-model, aided by quantum chemical calculations of potential energy states, to deduce a C-S bond expansion within the first 100 fs. The bond elongation triggers internal conversion from the photoexcited S2 to the S1 state. Based on timescales, the subsequent dynamics can be interpreted in terms of S1 nuclear relaxation and S1-triplet internal conversion.

ASJC Scopus Sachgebiete

Zitieren

Ultrafast dynamics of 2-thiouracil investigated by time-resolved Auger spectroscopy. / Lever, F.; Mayer, D.; Picconi, D. et al.
in: Journal of Physics B: Atomic, Molecular and Optical Physics, Jahrgang 54, Nr. 1, 014002, 17.12.2020.

Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review

Lever, F, Mayer, D, Picconi, D, Metje, J, Alisauskas, S, Calegari, F, Düsterer, S, Ehlert, C, Feifel, R, Niebuhr, M, Manschwetus, B, Kuhlmann, M, Mazza, T, Robinson, MS, Squibb, RJ, Trabattoni, A, Wallner, M, Saalfrank, P, Wolf, TJA & Gühr, M 2020, 'Ultrafast dynamics of 2-thiouracil investigated by time-resolved Auger spectroscopy', Journal of Physics B: Atomic, Molecular and Optical Physics, Jg. 54, Nr. 1, 014002. https://doi.org/10.1088/1361-6455/abc9cb
Lever, F., Mayer, D., Picconi, D., Metje, J., Alisauskas, S., Calegari, F., Düsterer, S., Ehlert, C., Feifel, R., Niebuhr, M., Manschwetus, B., Kuhlmann, M., Mazza, T., Robinson, M. S., Squibb, R. J., Trabattoni, A., Wallner, M., Saalfrank, P., Wolf, T. J. A., & Gühr, M. (2020). Ultrafast dynamics of 2-thiouracil investigated by time-resolved Auger spectroscopy. Journal of Physics B: Atomic, Molecular and Optical Physics, 54(1), Artikel 014002. https://doi.org/10.1088/1361-6455/abc9cb
Lever F, Mayer D, Picconi D, Metje J, Alisauskas S, Calegari F et al. Ultrafast dynamics of 2-thiouracil investigated by time-resolved Auger spectroscopy. Journal of Physics B: Atomic, Molecular and Optical Physics. 2020 Dez 17;54(1):014002. doi: 10.1088/1361-6455/abc9cb
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abstract = "We present time-resolved ultraviolet-pump X-ray probe Auger spectra of 2-thiouracil. An ultraviolet induced shift towards higher kinetic energies is observed in the sulfur 2p Auger decay. The difference Auger spectra of pumped and unpumped molecules exhibit ultrafast dynamics in the shift amplitude, in which three phases can be recognized. In the first 100 fs, a shift towards higher kinetic energies is observed, followed by a 400 fs shift back to lower kinetic energies and a 1 ps shift again to higher kinetic energies. We use a simple Coulomb-model, aided by quantum chemical calculations of potential energy states, to deduce a C-S bond expansion within the first 100 fs. The bond elongation triggers internal conversion from the photoexcited S2 to the S1 state. Based on timescales, the subsequent dynamics can be interpreted in terms of S1 nuclear relaxation and S1-triplet internal conversion.",
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T1 - Ultrafast dynamics of 2-thiouracil investigated by time-resolved Auger spectroscopy

AU - Lever, F.

AU - Mayer, D.

AU - Picconi, D.

AU - Metje, J.

AU - Alisauskas, S.

AU - Calegari, F.

AU - Düsterer, S.

AU - Ehlert, C.

AU - Feifel, R.

AU - Niebuhr, M.

AU - Manschwetus, B.

AU - Kuhlmann, M.

AU - Mazza, T.

AU - Robinson, M. S.

AU - Squibb, R. J.

AU - Trabattoni, A.

AU - Wallner, M.

AU - Saalfrank, P.

AU - Wolf, T. J.A.

AU - Gühr, M.

PY - 2020/12/17

Y1 - 2020/12/17

N2 - We present time-resolved ultraviolet-pump X-ray probe Auger spectra of 2-thiouracil. An ultraviolet induced shift towards higher kinetic energies is observed in the sulfur 2p Auger decay. The difference Auger spectra of pumped and unpumped molecules exhibit ultrafast dynamics in the shift amplitude, in which three phases can be recognized. In the first 100 fs, a shift towards higher kinetic energies is observed, followed by a 400 fs shift back to lower kinetic energies and a 1 ps shift again to higher kinetic energies. We use a simple Coulomb-model, aided by quantum chemical calculations of potential energy states, to deduce a C-S bond expansion within the first 100 fs. The bond elongation triggers internal conversion from the photoexcited S2 to the S1 state. Based on timescales, the subsequent dynamics can be interpreted in terms of S1 nuclear relaxation and S1-triplet internal conversion.

AB - We present time-resolved ultraviolet-pump X-ray probe Auger spectra of 2-thiouracil. An ultraviolet induced shift towards higher kinetic energies is observed in the sulfur 2p Auger decay. The difference Auger spectra of pumped and unpumped molecules exhibit ultrafast dynamics in the shift amplitude, in which three phases can be recognized. In the first 100 fs, a shift towards higher kinetic energies is observed, followed by a 400 fs shift back to lower kinetic energies and a 1 ps shift again to higher kinetic energies. We use a simple Coulomb-model, aided by quantum chemical calculations of potential energy states, to deduce a C-S bond expansion within the first 100 fs. The bond elongation triggers internal conversion from the photoexcited S2 to the S1 state. Based on timescales, the subsequent dynamics can be interpreted in terms of S1 nuclear relaxation and S1-triplet internal conversion.

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