Сибирский федеральный университет

Тип публикации: статья из журнала

Год издания: 2022

Идентификатор DOI: 10.1039/d1cp05000a

Аннотация: 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. 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. © 2022 the Owner Societies.

Журнал: PHYSICAL CHEMISTRY CHEMICAL PHYSICS

Выпуск журнала: Vol. 24, Is. 11

Номера страниц: 6627-6638

ISSN журнала: 14639076

Место издания: CAMBRIDGE

Издатель: ROYAL SOC CHEMISTRY

• Liu Ji-Cai (North China Elect Power Univ, Dept Math & Phys, Beijing 102206, Peoples R China)
• Ignatova Nina (Siberian Fed Univ, Int Res Ctr Spect & Quantum Chem IRC SQC, Krasnoyarsk 660041, Russia)
• Kimberg Victor (Siberian Fed Univ, Int Res Ctr Spect & Quantum Chem IRC SQC, Krasnoyarsk 660041, Russia; KTH Royal Inst Technol, Dept Theoret Chem & Biol, S-10691 Stockholm, Sweden)
• Krasnov Pavel (Siberian Fed Univ, Int Res Ctr Spect & Quantum Chem IRC SQC, Krasnoyarsk 660041, Russia)
• Foehlisch Alexander (Helmholtz Zentrum Berlin Mat & Energie, Inst Methods & Instrumentat Synchrotron Radiat Re, FG ISRR, Albert Einstein Str 15, D-12489 Berlin, Germany; Univ Potsdam, Inst Phys & Astron, Karl Liebknecht Str 24-25, D-14476 Potsdam, Germany)
• Simon Marc (Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, LCPMR, CNRS, F-75005 Paris, France)
• Gel'mukhanov Faris (Siberian Fed Univ, Int Res Ctr Spect & Quantum Chem IRC SQC, Krasnoyarsk 660041, Russia; KTH Royal Inst Technol, Dept Theoret Chem & Biol, S-10691 Stockholm, Sweden; Helmholtz Zentrum Berlin Mat & Energie, Inst Methods & Instrumentat Synchrotron Radiat Re, FG ISRR, Albert Einstein Str 15, D-12489 Berlin, Germany)

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