Details
| Original language | English |
|---|---|
| Article number | 014002 |
| Journal | Journal of Physics B: Atomic, Molecular and Optical Physics |
| Volume | 54 |
| Issue number | 1 |
| Publication status | Published - 17 Dec 2020 |
| Externally published | Yes |
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.
Keywords
- Auger spectroscopy, thionucleobases, time-resolved X-ray spectroscopy
ASJC Scopus subject areas
- Physics and Astronomy(all)
- Atomic and Molecular Physics, and Optics
- Physics and Astronomy(all)
- Condensed Matter Physics
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In: Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 54, No. 1, 014002, 17.12.2020.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
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.
KW - Auger spectroscopy
KW - thionucleobases
KW - time-resolved X-ray spectroscopy
UR - http://www.scopus.com/inward/record.url?scp=85098851670&partnerID=8YFLogxK
U2 - 10.1088/1361-6455/abc9cb
DO - 10.1088/1361-6455/abc9cb
M3 - Article
AN - SCOPUS:85098851670
VL - 54
JO - Journal of Physics B: Atomic, Molecular and Optical Physics
JF - Journal of Physics B: Atomic, Molecular and Optical Physics
SN - 0953-4075
IS - 1
M1 - 014002
ER -