Issue 5, 2022

Circularly polarized light-induced potentials and the demise of excited states

Abstract

In the presence of strong electric fields, the excited states of single-electron molecules and molecules with large transient dipoles become unstable because of anti-alignment, the rotation of the molecular axis perpendicular to the field vector, where bond hardening is not possible. We show how to overcome this problem by using circularly polarized electromagnetic fields. Using a full quantum description of the electronic, vibrational, and rotational degrees of freedom, we characterize the excited electronic state dressed by the field and analyze its dependence on the bond length and angle and the stability of its vibro-rotational eigenstates. Although the dynamics is metastable, most of the population remains trapped in this excited state for hundreds of femtoseconds, allowing quantum control. Contrary to what happens with linearly polarized fields, the photodissociation occurs along the initial molecular axis, not perpendicular to it.

Graphical abstract: Circularly polarized light-induced potentials and the demise of excited states

Article information

Article type
Paper
Submitted
03 okt 2021
Accepted
28 dek 2021
First published
29 dek 2021

Phys. Chem. Chem. Phys., 2022,24, 2966-2973

Author version available

Circularly polarized light-induced potentials and the demise of excited states

S. Carrasco, J. Rogan, J. A. Valdivia, B. Y. Chang, V. S. Malinovsky and I. R. Sola, Phys. Chem. Chem. Phys., 2022, 24, 2966 DOI: 10.1039/D1CP04523G

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