Time-resolved study of recoil-induced rotation by X-ray pump - X-ray probe spectroscopy
- Modern stationary X-ray spectroscopy is unable to resolve rotational structure. In the present paper, we propose to use time-resolved two color X-ray pump-probe spectroscopy with picosecond resolution for real-time monitoring of the rotational dynamics induced by the recoil effect. The proposed technique consists of two steps. The first short pump X-ray pulse ionizes the valence electron, which transfers angular momentum to the molecule. The second time-delayed short probe X-ray pulse resonantly excites a 1s electron to the created valence hole. Due to the recoil-induced angular momentum the molecule rotates and changes the orientation of transition dipole moment of core-excitation with respect to the transition dipole moment of the valence ionization, which results in a temporal modulation of the probe X-ray absorption as a function of the delay time between the pulses. We developed an accurate theory of the X-ray pump-probe spectroscopy of the recoil-induced rotation and study how the energy of the photoelectron andModern stationary X-ray spectroscopy is unable to resolve rotational structure. In the present paper, we propose to use time-resolved two color X-ray pump-probe spectroscopy with picosecond resolution for real-time monitoring of the rotational dynamics induced by the recoil effect. The proposed technique consists of two steps. The first short pump X-ray pulse ionizes the valence electron, which transfers angular momentum to the molecule. The second time-delayed short probe X-ray pulse resonantly excites a 1s electron to the created valence hole. Due to the recoil-induced angular momentum the molecule rotates and changes the orientation of transition dipole moment of core-excitation with respect to the transition dipole moment of the valence ionization, which results in a temporal modulation of the probe X-ray absorption as a function of the delay time between the pulses. We developed an accurate theory of the X-ray pump-probe spectroscopy of the recoil-induced rotation and study how the energy of the photoelectron and thermal dephasing affect the structure of the time-dependent X-ray absorption using the CO molecule as a case-study. We also discuss the feasibility of experimental observation of our theoretical findings, opening new perspectives in studies of molecular rotational dynamics.…
Author details: | Ji-Cai LiuORCiD, Nina Ignatova, Victor Kimberg, Pavel Krasnov, Alexander FöhlischORCiDGND, Marc Simon, Faris Gel'mukhanov |
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DOI: | https://doi.org/10.1039/d1cp05000a |
ISSN: | 1463-9076 |
ISSN: | 1463-9084 |
Pubmed ID: | https://pubmed.ncbi.nlm.nih.gov/35234760 |
Title of parent work (English): | Physical chemistry, chemical physics : a journal of European Chemical Societies |
Publisher: | Royal Society of Chemistry |
Place of publishing: | Cambridge |
Publication type: | Article |
Language: | English |
Date of first publication: | 2022/02/24 |
Publication year: | 2022 |
Release date: | 2024/06/17 |
Volume: | 24 |
Issue: | 11 |
Number of pages: | 12 |
First page: | 6627 |
Last Page: | 6638 |
Funding institution: | Russian Science Foundation [21-12-00193]; National Natural Science; Foundation of China [11974108, 11574082]; Fundamental Research Funds for; the Central Universities [2021MS046]; European Research Council through; ERC-ADG-2014 at the University of Potsdam within the Horizon 2020 EU; Framework Programme for Research and Innovation [669531 EDAX];; Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH; Foundation; for the Advancement of Theoretical Physics and Mathematics ``BASIS''; [19-1-4-66-1]; Swedish Research Council [2019-03470] |
Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie |
DDC classification: | 5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik |
Peer review: | Referiert |
Publishing method: | Open Access / Hybrid Open-Access |
License (English): | Creative Commons - Namensnennung 3.0 Unported |