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.
| Original language | English (US) |
|---|---|
| Article number | 203201 |
| Journal | Physical review letters |
| Volume | 118 |
| Issue number | 20 |
| DOIs | |
| State | Published - May 17 2017 |
Funding
We acknowledge support by the U.S. Department of Energy (Award No. DE-FG02-04ER15612) and the Deutsche Forschungsgemeinschaft (Projects No. LE 2138/2-1 and No. GR 4508/1-1). This research was supported in part through the computational resources and staff contributions provided for the Quest high performance computing facility at Northwestern University, which is jointly supported by the Office of the Provost, the Office for Research, and Northwestern University Information Technology.
ASJC Scopus subject areas
- General Physics and Astronomy