Simulating Photoexcitation With A Laser Pulse Beyond The Perturbative Limit

Dey, Diptesh

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https://hdl.handle.net/2142/116622 Copy

Description

Title

Simulating Photoexcitation With A Laser Pulse Beyond The Perturbative Limit

Author(s)

Dey, Diptesh

Contributor(s)

Worth, Graham

Issue Date

2022-06-21

Keyword(s)

Mini-symposium: Spectroscopy meets Chemical Dynamics

Abstract

The advent of ultrashort laser pulses in the femtosecond to attosecond regime allows the study of ultrafast molecular dynamics with unprecedented time resolution [1,2]. These powerful modern light sources can result in the ionization of matter and thereby trigger electronic and nuclear dynamics [3,4]. In my talk, I will give an overview of the ongoing research efforts in the Worth group at UCL addressing the following fundamental questions: (i) Can we control photochemical processes by creating/manipulating a quantum superposition state with a laser pulse? (ii) Can we understand the coupled electron-nuclear motion and the associated ultrafast decoherence? (iii) Can we design laser pulses in a simple way to make use of the quantum interference pathways? (iv) Can we simulate an experimental photoelectron spectrum by developing simple theoretical models? These elementary aspects of laser-matter interactions are governed by quantum mechanics and therefore we solve the time-dependent Schrödinger equation using state-of-the-art quantum dynamics method, MCTDH [5], in combination with vibronic coupling Hamiltonian [6]. This further allows us to deal with the non-adiabatic coupling between the electrons and the nuclei [6]. The ionized electron is modeled explicitly by incorporating the continuum of free-electron states [7]. The QUANTICS suite of programs are used to run the dynamical simulations [8]. References [1] M. Nisoli, P. Decleva, F. Calegari, A. Palacios and F. Martín, Chem. Rev. 117, 10760 (2017). [2] H. H. Fielding and G. A. Worth, Chem. Soc. Rev. 47, 309 (2018). [3] V. Despré, N. V. Golubev and A. I. Kuleff, Phys. Rev. Lett. 121, 203002 (2018). [4] A. Henley, J. W. Riley, B. Wang and H. H. Fielding, Faraday Discuss. 221, 202 (2020). [5] M. H. Beck, A. Jäckle, G. A. Worth and H.-D. Meyer, Phys. Rep. 324, 1 (2000). [6] G. A. Worth and L. S. Cederbaum, Annu. Rev. Phys. Chem. 55, 127 (2004). [7] M. Seel and W. Domcke, J. Chem. Phys. 95, 7806 (1991). [8] QUANTICS, http://www2.chem.ucl.ac.uk/quantics/doc/index.html

Publisher

International Symposium on Molecular Spectroscopy

Type of Resource

text

Language

eng

Handle URL

https://hdl.handle.net/2142/116622&&

DOI

https://doi.org/10.15278/isms.2022.TA09

Copyright and License Information

Copyright 2022 held by the authors

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