TY - JOUR
T1 - Laser-Controlled Torsions
T2 - Four-Dimensional Theory and the Validity of Reduced Dimensionality Models
AU - Grohmann, Thomas
AU - Leibscher, Monika
AU - Seideman, Tamar
N1 - Funding Information:
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.
Publisher Copyright:
© 2017 American Physical Society.
PY - 2017/5/17
Y1 - 2017/5/17
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85019959966&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85019959966&partnerID=8YFLogxK
U2 - 10.1103/PhysRevLett.118.203201
DO - 10.1103/PhysRevLett.118.203201
M3 - Article
C2 - 28581807
AN - SCOPUS:85019959966
SN - 0031-9007
VL - 118
JO - Physical Review Letters
JF - Physical Review Letters
IS - 20
M1 - 203201
ER -