Controlling the Time Evolution of Electron-Nuclei Entanglement for Steering Vibronic Coherences Dynamics Induced by Short 1–2 fs Optical Pulses

Martin Blavier, Natalia Gelfand, R. D. Levine, F. Remacle*

*Corresponding author for this work

Research output: Chapter in Book/Report/Conference proceedingConference contributionpeer-review

1 Scopus citations

Abstract

Atto pulses allow controlling the charge migration and the spatio-temporal beating of the electronic density on a purely electronic time scale by tailoring the parameters of the pump pulse to excite specific electronic coherences. As the nuclei begin to move, the electronic and nuclear motions are entangled and the engineered electronic coherences can be usefully exploited for steering the vibronic density to specific products through the network of non adiabatic interactions. Three recent examples for which we demonstrate such a control by fully quantum dynamical computations are discussed. Two diatomic molecules, LiH and N2 excited by a 2 fs deep UV pulse and the ultrafast structural Jahn-Teller rearrangement in CH4+. The entanglement between electronic and nuclear degrees of freedom arises from the optical excitation and from non adiabatic coupling induced by the nuclear motion. We provide insight of the coherence control mechanism by analyzing the time evolution of the entanglement using a singular valued decomposition (SVD) of the matricized wave function.

Original languageEnglish
Title of host publicationProceedings of the 8th International Conference on Attosecond Science and Technology
EditorsLuca Argenti, Michael Chini, Li Fang
PublisherSpringer Science and Business Media Deutschland GmbH
Pages83-100
Number of pages18
ISBN (Print)9783031479373
DOIs
StatePublished - 2024
Event8th International Conference on Attosecond Science and Technology, ATTO 2023 - Orlando, United States
Duration: 10 Jul 202315 Jul 2023

Publication series

NameSpringer Proceedings in Physics
Volume300
ISSN (Print)0930-8989
ISSN (Electronic)1867-4941

Conference

Conference8th International Conference on Attosecond Science and Technology, ATTO 2023
Country/TerritoryUnited States
CityOrlando
Period10/07/2315/07/23

Bibliographical note

Publisher Copyright:
© The Author(s) 2024.

Keywords

  • Attosecond molecular quantum dynamics
  • Matricization of the wave function
  • Schmidt rank
  • Singular value decomposition
  • Time-resolved electron-nuclei entanglement in molecules

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