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タイトル: Conical-intersection dynamics and ground-state chemistry probed by extreme-ultraviolet time-resolved photoelectron spectroscopy
著者: von Conta, A.
Tehlar, A.
Schletter, A.
Arasaki, Y.
Takatsuka, K.
Wörner, H. J.
著者名の別形: 新崎, 康樹
高塚, 和夫
発行日: 8-Aug-2018
出版者: Springer Nature America, Inc
誌名: Nature Communications
巻: 9
論文番号: 3162
抄録: Time-resolved photoelectron spectroscopy (TRPES) is a useful approach to elucidate the coupled electronic-nuclear quantum dynamics underlying chemical processes, but has remained limited by the use of low photon energies. Here, we demonstrate the general advantages of XUV-TRPES through an application to NO₂, one of the simplest species displaying the complexity of a non-adiabatic photochemical process. The high photon energy enables ionization from the entire geometrical configuration space, giving access to the true dynamics of the system. Specifically, the technique reveals dynamics through a conical intersection, large-amplitude motion and photodissociation in the electronic ground state. XUV-TRPES simultaneously projects the excited-state wave packet onto many final states, offering a multi-dimensional view of the coupled electronic and nuclear dynamics. Our interpretations are supported by ab initio wavepacket calculations on new global potential-energy surfaces. The presented results contribute to establish XUV-TRPES as a powerful technique providing a complete picture of ultrafast chemical dynamics from photoexcitation to the final products.
著作権等: © The Author(s) 2018. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
URI: http://hdl.handle.net/2433/234181
DOI(出版社版): 10.1038/s41467-018-05292-4
PubMed ID: 30089780
出現コレクション:学術雑誌掲載論文等

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