Molecular attochemistry: correlated electron dynamics driven by light
- Modern laser technology and ultrafast spectroscopies have pushed the timescales for detecting and manipulating dynamical processes in molecules from the picosecond over femtosecond domains, to the attosecond regime (1 as = 10(-18) s). This way, real-time dynamics of electrons after their photoexcitation can be probed and manipulated. In particular, experiments are moving more and more from atomic and solid state systems to molecules, opening the fields of "molecular electron dynamics" and "attosecond chemistry." Also on the theory side, powerful quantum dynamical tools have been developed to rationalize experiments on ultrafast electron dynamics in molecular species. <br /> In this contribution, we concentrate on theoretical aspects of ultrafast electron dynamics in molecules, mostly driven by lasers. The dynamics will be described with the help of wavefunction-based ab initio methods such as time-dependent configuration interaction (TD-CI) or the multiconfigurational time-dependent Hartree-Fock (MCTDHF) methods. Besides a survey ofModern laser technology and ultrafast spectroscopies have pushed the timescales for detecting and manipulating dynamical processes in molecules from the picosecond over femtosecond domains, to the attosecond regime (1 as = 10(-18) s). This way, real-time dynamics of electrons after their photoexcitation can be probed and manipulated. In particular, experiments are moving more and more from atomic and solid state systems to molecules, opening the fields of "molecular electron dynamics" and "attosecond chemistry." Also on the theory side, powerful quantum dynamical tools have been developed to rationalize experiments on ultrafast electron dynamics in molecular species. <br /> In this contribution, we concentrate on theoretical aspects of ultrafast electron dynamics in molecules, mostly driven by lasers. The dynamics will be described with the help of wavefunction-based ab initio methods such as time-dependent configuration interaction (TD-CI) or the multiconfigurational time-dependent Hartree-Fock (MCTDHF) methods. Besides a survey of the methods and their extensions toward, e.g., treatment of ionization, laser pulse optimization, and open quantum systems, two specific examples of applications will be considered: The creation and/or dynamical fate of electronic wavepackets, and the nonlinear optical response to laser pulse excitation in molecules by high harmonic generation (HHG).…
Author details: | Peter SaalfrankORCiDGND, Florian Bedurke, Chiara Heide, Tillmann KlamrothORCiDGND, Stefan KlinkuschGND, Pascal Krause, Mathias NestGND, Jean Christophe TremblayORCiDGND |
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DOI: | https://doi.org/10.1016/bs.aiq.2020.03.001 |
ISBN: | 978-0-12-819757-8 |
ISSN: | 0065-3276 |
Title of parent work (English): | Advances in quantum chemistry |
Publisher: | Elsevier |
Place of publishing: | Amsterdam [u.a.] |
Editor(s): | Kenneth Ruud, Erkki J. Brändas |
Publication type: | Part of a Book |
Language: | English |
Date of first publication: | 2020/09/17 |
Publication year: | 2020 |
Release date: | 2023/11/13 |
Tag: | dipole approximation; electron dynamics; electronic wavepackets; high harmonic generation; ionization; optimal control theory; time-dependent Schrödinger equation |
Volume: | 81 |
Number of pages: | 36 |
First page: | 15 |
Last Page: | 50 |
Funding institution: | Deutsche Forschungsgemeinschaft (DFG)German Research Foundation (DFG); [Sa 547/15-1, Kl 1387/5-1] |
Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
DDC classification: | 5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften |
Peer review: | Referiert |