Tracking Conical Intersections with Nonlinear X-ray Raman Spectroscopy
Research Article|Updated:2024-10-22
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Tracking Conical Intersections with Nonlinear X-ray Raman Spectroscopy
超快科学(英文)2022年2卷第6期
Affiliations:
a Department of Physics, Stockholm University, Albanova University Centre,- Stockholm,SE,Sweden,106 91
Author bio:
Funds:
Support from the Swedish Research Council (grant no. VR 2018-05346) is acknowledged. This project has receivedfunding from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement no. 860553. The authors declare no competing interests.
Deependra Jadoun, Markus Kowalewski. 2022: Tracking Conical Intersections with Nonlinear X-ray Raman Spectroscopy. 超快科学, 2022(6).
Deependra Jadoun, Markus Kowalewski, . 2022: Tracking Conical Intersections with Nonlinear X-ray Raman Spectroscopy. Ultrafast Science, 2022(6).
Deependra Jadoun, Markus Kowalewski. 2022: Tracking Conical Intersections with Nonlinear X-ray Raman Spectroscopy. 超快科学, 2022(6). DOI: 10.34133/ultrafastscience.0003
Deependra Jadoun, Markus Kowalewski, . 2022: Tracking Conical Intersections with Nonlinear X-ray Raman Spectroscopy. Ultrafast Science, 2022(6). DOI: 10.34133/ultrafastscience.0003
Tracking Conical Intersections with Nonlinear X-ray Raman Spectroscopy
摘要
Conical intersections are formed when 2 or more electronic states become degenerate and give rise to ultrafast nonadiabatic processes such as radiation-less decay channels and geometric phase effects. The branching of nuclear wave packets near a conical intersection creates a coherent superposition of electronic states
which carries information about the energy difference of the involved states. X-ray Raman techniques have been proposed to observe the coherent superposition of the electronic states and to monitor the evolving electronic state separation. However
these techniques rely on the coherence generated as the wave packet passes through the conical intersection
and the electronic energy gap before the wave packet passes through the conical intersection is not tracked. In this paper
we theoretically demonstrate how a nonlinear Raman detection scheme can be used to gain further insight into the nonadiabatic dynamics in the vicinity of the conical intersection.We employ a combination of a resonant visible/infrared pulse and an off-resonant x-ray Raman probe to map the electronic state separation around the conical intersection. We demonstrate that this technique can achieve high contrast and is able to selectively probe the narrow electronic state separation around the conical intersection.
Abstract
Conical intersections are formed when 2 or more electronic states become degenerate and give rise to ultrafast nonadiabatic processes such as radiation-less decay channels and geometric phase effects. The branching of nuclear wave packets near a conical intersection creates a coherent superposition of electronic states
which carries information about the energy difference of the involved states. X-ray Raman techniques have been proposed to observe the coherent superposition of the electronic states and to monitor the evolving electronic state separation. However
these techniques rely on the coherence generated as the wave packet passes through the conical intersection
and the electronic energy gap before the wave packet passes through the conical intersection is not tracked. In this paper
we theoretically demonstrate how a nonlinear Raman detection scheme can be used to gain further insight into the nonadiabatic dynamics in the vicinity of the conical intersection.We employ a combination of a resonant visible/infrared pulse and an off-resonant x-ray Raman probe to map the electronic state separation around the conical intersection. We demonstrate that this technique can achieve high contrast and is able to selectively probe the narrow electronic state separation around the conical intersection.
a State Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University, Changchun 130012, Chinab Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japanc CAS Center for Excellence in Ultra-Intense Laser Science