Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy

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Fältnamn	Indikatorer	Metadata
000		03319naa a2200565 4500
001		oai:gup.ub.gu.se/313786
003		SwePub
008		240528s2022 \| \|\|\|\|\|\|\|\|\|\|\|000 \|\|eng\|
024	7	a https://gup.ub.gu.se/publication/3137862 URI
024	7	a https://doi.org/10.1038/s41467-021-27908-y2 DOI
040		a (SwePub)gu
041		a eng
042		9 SwePub
072	7	a ref2 swepub-contenttype
072	7	a art2 swepub-publicationtype
100	1	a Mayer, D.4 aut
245	1 0	a Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy
264		c 2022-01-11
264	1	b Springer Science and Business Media LLC,c 2022
520		a The conversion of photon energy into other energetic forms in molecules is accompanied by charge moving on ultrafast timescales. We directly observe the charge motion at a specific site in an electronically excited molecule using time-resolved x-ray photoelectron spectroscopy (TR-XPS). We extend the concept of static chemical shift from conventional XPS by the excited-state chemical shift (ESCS), which is connected to the charge in the framework of a potential model. This allows us to invert TR-XPS spectra to the dynamic charge at a specific atom. We demonstrate the power of TR-XPS by using sulphur 2p-core-electron-emission probing to study the UV-excited dynamics of 2-thiouracil. The method allows us to discover that a major part of the population relaxes to the molecular ground state within 220–250 fs. In addition, a 250-fs oscillation, visible in the kinetic energy of the TR-XPS, reveals a coherent exchange of population among electronic states. © 2022, The Author(s).
650	7	a NATURVETENSKAPx Fysik0 (SwePub)1032 hsv//swe
650	7	a NATURAL SCIENCESx Physical Sciences0 (SwePub)1032 hsv//eng
653		a chemical composition
653		a kinetic energy
653		a molecular analysis
653		a X-ray spectroscopy
700	1	a Lever, F.4 aut
700	1	a Picconi, D.4 aut
700	1	a Metje, J.4 aut
700	1	a Alisauskas, S.4 aut
700	1	a Calegari, F.4 aut
700	1	a Düsterer, S.4 aut
700	1	a Ehlert, C.4 aut
700	1	a Feifel, Raimundu Gothenburg University,Göteborgs universitet,Institutionen för fysik (GU),Department of Physics (GU)4 aut0 (Swepub:gu)xfeira
700	1	a Niebuhr, M.4 aut
700	1	a Manschwetus, B.4 aut
700	1	a Kuhlmann, M.4 aut
700	1	a Mazza, T.4 aut
700	1	a Robinson, M. S.4 aut
700	1	a Squibb, Richard J.u Gothenburg University,Göteborgs universitet,Institutionen för fysik (GU),Department of Physics (GU)4 aut0 (Swepub:gu)xsquri
700	1	a Trabattoni, A.4 aut
700	1	a Wallner, Måns,d 1992u Gothenburg University,Göteborgs universitet,Institutionen för fysik (GU),Department of Physics (GU)4 aut0 (Swepub:gu)xwaman
700	1	a Saalfrank, P.4 aut
700	1	a Wolf, T. J. A.4 aut
700	1	a Gühr, M.4 aut
710	2	a Göteborgs universitetb Institutionen för fysik (GU)4 org
773	0	t Nature Communicationsd : Springer Science and Business Media LLCg 13:1q 13:1x 2041-1723
856	4	u https://www.nature.com/articles/s41467-021-27908-y.pdf
856	4 8	u https://gup.ub.gu.se/publication/313786
856	4 8	u https://doi.org/10.1038/s41467-021-27908-y

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