skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Theory of torsional control for G 16-type molecules

Abstract

Here, we introduce a four-dimensional quantum model for describing the torsional control with moderately strong, non-resonant laser pulses of G 16-type molecules in the electronic ground state, based on the symmetry-adapted variational method. We define conditions for which lower-dimensional models, commonly used to simulate the strong-field control of molecular torsions, are reliable approximations to a four-dimensional treatment. In particular, we study the role of different types of rotational-torsional couplings—the field-free coupling and the field-induced coupling—and show that the conclusions recently drawn on the role of rotational-torsional couplings in the process of torsional alignment are not correct in general. Furthermore, we demonstrate how important an adequate description of the molecular polarizability is for reliably predicting the torsional alignment.

Authors:
ORCiD logo [1];  [2];  [3]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Freie Univ., Berlin (Germany). Inst. fur Chemie und Biochemie
  2. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  3. Leibniz Univ. Hannover, Hannover (Germany). Inst. fur Theoretische Physik; Christian-Albrechts-Univ.t Kiel, Kiel (Germany). Inst. fur Physikalische Chemie
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1540120
Alternate Identifier(s):
OSTI ID: 1423508
Grant/Contract Number:  
FG02-04ER15612
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 148; Journal Issue: 9; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Physics

Citation Formats

Grohmann, Thomas, Seideman, Tamar, and Leibscher, Monika. Theory of torsional control for G16-type molecules. United States: N. p., 2018. Web. doi:10.1063/1.4997462.
Grohmann, Thomas, Seideman, Tamar, & Leibscher, Monika. Theory of torsional control for G16-type molecules. United States. doi:10.1063/1.4997462.
Grohmann, Thomas, Seideman, Tamar, and Leibscher, Monika. Fri . "Theory of torsional control for G16-type molecules". United States. doi:10.1063/1.4997462. https://www.osti.gov/servlets/purl/1540120.
@article{osti_1540120,
title = {Theory of torsional control for G16-type molecules},
author = {Grohmann, Thomas and Seideman, Tamar and Leibscher, Monika},
abstractNote = {Here, we introduce a four-dimensional quantum model for describing the torsional control with moderately strong, non-resonant laser pulses of G16-type molecules in the electronic ground state, based on the symmetry-adapted variational method. We define conditions for which lower-dimensional models, commonly used to simulate the strong-field control of molecular torsions, are reliable approximations to a four-dimensional treatment. In particular, we study the role of different types of rotational-torsional couplings—the field-free coupling and the field-induced coupling—and show that the conclusions recently drawn on the role of rotational-torsional couplings in the process of torsional alignment are not correct in general. Furthermore, we demonstrate how important an adequate description of the molecular polarizability is for reliably predicting the torsional alignment.},
doi = {10.1063/1.4997462},
journal = {Journal of Chemical Physics},
number = 9,
volume = 148,
place = {United States},
year = {2018},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Biologically inspired molecular machines driven by light. Optimal control of a unidirectional rotor
journal, July 2010


Laser-Controlled Torsions: Four-Dimensional Theory and the Validity of Reduced Dimensionality Models
journal, May 2017


Control and femtosecond time-resolved imaging of torsion in a chiral molecule
journal, May 2012

  • Hansen, Jonas L.; Nielsen, Jens H.; Madsen, Christian Bruun
  • The Journal of Chemical Physics, Vol. 136, Issue 20
  • DOI: 10.1063/1.4719816

Simulating strong field control of axial chirality using optimal control theory
journal, August 2012


Dissipative dynamics of laser induced nonadiabatic molecular alignment
journal, January 2006

  • Ramakrishna, S.; Seideman, Tamar
  • The Journal of Chemical Physics, Vol. 124, Issue 3
  • DOI: 10.1063/1.2130708

On the Asymmetrical Top in Quantum Mechanics
journal, July 1929


Selective preparation of enantiomers by laser pulses: quantum model simulation for H2POSH
journal, June 1999


Coherent control of molecular torsion
journal, December 2011

  • Parker, Shane M.; Ratner, Mark A.; Seideman, Tamar
  • The Journal of Chemical Physics, Vol. 135, Issue 22
  • DOI: 10.1063/1.3663710

Dissipative Dynamics of Laser-Induced Torsional Coherences
journal, June 2013

  • Ashwell, Benjamin A.; Ramakrishna, S.; Seideman, Tamar
  • The Journal of Physical Chemistry C, Vol. 117, Issue 43
  • DOI: 10.1021/jp403090u

On the possibility of orienting rotationally cooled polar molecules in an electric field
journal, June 1991

  • Friedrich, B.; Herschbach, D. R.
  • Zeitschrift f�r Physik D Atoms, Molecules and Clusters, Vol. 18, Issue 2
  • DOI: 10.1007/bf01437441

The application of extended permutation-inversion groups to internal rotation of a symmetric rotor top in a symmetric or asymmetric rotor molecule
journal, April 1983


Controlling the sense of molecular rotation
journal, October 2009


Molecular vibrational and rotational motion in static and dynamic electric fields
journal, April 1990


Laser-driven torsional coherences
journal, January 2013

  • Ashwell, Benjamin A.; Ramakrishna, S.; Seideman, Tamar
  • The Journal of Chemical Physics, Vol. 138, Issue 4
  • DOI: 10.1063/1.4773009

Advances in molecular quantum chemistry contained in the Q-Chem 4 program package
journal, September 2014


Selective control of molecular rotation
journal, March 2008

  • Fleischer, Sharly; Averbukh, I. Sh; Prior, Yehiam
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 41, Issue 7
  • DOI: 10.1088/0953-4075/41/7/074018

Theory and applications of atomic and ionic polarizabilities
journal, October 2010

  • Mitroy, J.; Safronova, M. S.; Clark, Charles W.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 43, Issue 20
  • DOI: 10.1088/0953-4075/43/20/202001

Intense Laser Alignment in Dissipative Media as a Route to Solvent Dynamics
journal, September 2005


Laser-induced selective alignment of water spin isomers
journal, December 2008


Alignment of symmetric top molecules by short laser pulses
journal, October 2005


Laser-operated chiral molecular switch: quantum simulations for the controlled transformation between achiral and chiral atropisomers
journal, January 2007

  • Kröner, Dominik; Klaumünzer, Bastian
  • Physical Chemistry Chemical Physics, Vol. 9, Issue 36
  • DOI: 10.1039/b705974d

Symmetry considerations for internal rotation in ethylene-like molecules
journal, September 1973


Nuclear spin selective laser control of rotational and torsional dynamics
journal, February 2012

  • Floß, J.; Grohmann, T.; Leibscher, M.
  • The Journal of Chemical Physics, Vol. 136, Issue 8
  • DOI: 10.1063/1.3687343

Quantum separation of para- and ortho-fulvene with coherent light: The influence of the conical intersection
journal, September 2007


Theoretical description of adiabatic laser alignment and mixed-field orientation: the need for a non-adiabatic model
journal, January 2011

  • Omiste, J. J.; Gärttner, M.; Schmelcher, P.
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 42
  • DOI: 10.1039/c1cp21195a

Frequency dependent nonlinear optical properties of molecules
journal, July 1986

  • Sekino, Hideo; Bartlett, Rodney J.
  • The Journal of Chemical Physics, Vol. 85, Issue 2
  • DOI: 10.1063/1.451255

Symmetry Analysis of Molecules Consisting of Two Coaxial Rotors Using the Extended Permutation–Inversion Groups
journal, December 1996


Selective Alignment of Molecular Spin Isomers
journal, August 2007


Cross sections for rotational decoherence of perturbed nitrogen measured via decay of laser-induced alignment
journal, July 2010

  • Owschimikow, N.; Königsmann, F.; Maurer, J.
  • The Journal of Chemical Physics, Vol. 133, Issue 4
  • DOI: 10.1063/1.3464487

Nuclear spin selective alignment of ethylene and analogues
journal, May 2011

  • Grohmann, Thomas; Leibscher, Monika
  • The Journal of Chemical Physics, Vol. 134, Issue 20
  • DOI: 10.1063/1.3595133

Spinning molecules selectively: laser control of isotopes and nuclear spin isomers
journal, November 2007

  • Fleischer, Sharly; Averbukh, Ilya S. H.; Prior, Yehiam
  • Journal of Modern Optics, Vol. 54, Issue 16-17
  • DOI: 10.1080/09500340701553014

Torsional and rotational couplings in nonrigid molecules
journal, February 2017


A combined experimental and theoretical study on realizing and using laser controlled torsion of molecules
journal, June 2009

  • Madsen, C. B.; Madsen, L. B.; Viftrup, S. S.
  • The Journal of Chemical Physics, Vol. 130, Issue 23
  • DOI: 10.1063/1.3149789

Making the Best of Mixed-Field Orientation of Polar Molecules: A Recipe for Achieving Adiabatic Dynamics in an Electrostatic Field Combined with Laser Pulses
journal, May 2012


Optimal control of rotational motions in dissipative media
journal, October 2008

  • Pelzer, Adam; Ramakrishna, S.; Seideman, Tamar
  • The Journal of Chemical Physics, Vol. 129, Issue 13
  • DOI: 10.1063/1.2973633

Nonadiabatic effects in long-pulse mixed-field orientation of a linear polar molecule
journal, October 2012