Issue 11, 2022

Time-resolved study of recoil-induced rotation by X-ray pump – X-ray probe spectroscopy

Abstract

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 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.

Graphical abstract: Time-resolved study of recoil-induced rotation by X-ray pump – X-ray probe spectroscopy

Supplementary files

Article information

Article type
Paper
Submitted
02 11 2021
Accepted
21 2 2022
First published
24 2 2022
This article is Open Access
Creative Commons BY license

Phys. Chem. Chem. Phys., 2022,24, 6627-6638

Time-resolved study of recoil-induced rotation by X-ray pump – X-ray probe spectroscopy

J. Liu, N. Ignatova, V. Kimberg, P. Krasnov, A. Föhlisch, M. Simon and F. Gel'mukhanov, Phys. Chem. Chem. Phys., 2022, 24, 6627 DOI: 10.1039/D1CP05000A

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