Laser-Controlled Torsions: Four-Dimensional Theory and the Validity of Reduced Dimensionality Models

Thomas Grohmann, Monika Leibscher, and Tamar Seideman
Phys. Rev. Lett. 118, 203201 – Published 17 May 2017
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Abstract

A multitude of possible applications along with unique coherence, chirality, and symmetry properties makes the control of molecular torsion with moderately strong, nonresonant laser pulses a fascinating subject. A description of combined rotation and torsion requires at least four angular degrees of freedom, which is challenging for the majority of systems. Lower-dimensional models have been proposed but also questioned. Here, we develop a four-dimensional model for the coupled rotational-torsional motions of molecules consisting of two identical moieties. By comparing four-dimensional calculations with a two-dimensional model, we define conditions under which the lower-dimensional model is valid. In particular, we point to the crucial role of coordinate dependence of the polarizability tensor. Our results do not agree with those of previous four-dimensional calculations but support the conclusions of recent experiments.

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  • Received 16 November 2016

DOI:https://doi.org/10.1103/PhysRevLett.118.203201

© 2017 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

Thomas Grohmann1, Monika Leibscher2,3, and Tamar Seideman1,*

  • 1Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, USA
  • 2Institut für Theoretische Physik, Leibniz Universität Hannover, Appelstraße 2, 30167 Hannover, Germany
  • 3Institut für Physikalische Chemie, Christian-Albrechts-Universität Kiel, Olshausenstraße 40, 24098 Kiel, Germany

  • *Corresponding author. t-seideman@northwestern.edu

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Issue

Vol. 118, Iss. 20 — 19 May 2017

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