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 Nov 2021
Accepted
21 Feb 2022
First published
24 Feb 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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