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Title: Quantum optimal control of multiple weakly interacting molecular rotors in the time-dependent Hartree approximation

Abstract

In this work we perform quantum optimal control simulations, based on the Time-Dependent Hartree (TDH) approximation, for systems of three to five dipole-dipole coupled OCS rotors. A control electric field is used to steer all of the individual rotors, arranged in chains and regular polygons in a plane, toward either identical or unique objectives. The goal is to explore the utility of the TDH approximation to model the field-induced dynamics of multiple interacting rotors in the weak dipole-dipole coupling regime. A stochastic hill climbing approach is employed to seek an optimal control field that achieves the desired objectives at a specified target time. We first show that multiple rotors in chain and polygon geometries can be identically oriented in the same direction; these cases do not significantly depend on the presence of the dipole-dipole interaction. Additionally, in particular geometrical arrangements, we demonstrate that individual rotors can be uniquely manipulated toward different objectives with the same field. Specifically, it is shown that for a three rotor chain, the two end rotors can be identically oriented in a specific direction while keeping the middle rotor in its ground state, and for an equilateral triangle, two rotors can be identically oriented in amore » specific direction while the third rotor is oriented in the opposite direction. These multirotor unique objective cases exploit the shape of the field in coordination with dipole-dipole coupling between the rotors. Comparisons to numerically exact calculations, utilizing the TDH-determined fields, are given for all optimal control studies involving systems of three rotors.« less

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [1]
  1. Princeton Univ., NJ (United States)
Publication Date:
Research Org.:
Princeton Univ., NJ (United States); Krell Institute, Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); US Army Research Office (ARO)
OSTI Identifier:
1609378
Alternate Identifier(s):
OSTI ID: 1508434
Grant/Contract Number:  
FG02-02ER15344; FG02-97ER25308; ARO W911NF-16-1-0014
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 150; Journal Issue: 16; 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; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Chemistry; Physics; Quantum control theory; Rotational dynamics; Time-dependent Hartree method

Citation Formats

Magann, Alicia, Chen, Linhan, Ho, Tak-San, and Rabitz, Herschel. Quantum optimal control of multiple weakly interacting molecular rotors in the time-dependent Hartree approximation. United States: N. p., 2019. Web. doi:10.1063/1.5091520.
Magann, Alicia, Chen, Linhan, Ho, Tak-San, & Rabitz, Herschel. Quantum optimal control of multiple weakly interacting molecular rotors in the time-dependent Hartree approximation. United States. https://doi.org/10.1063/1.5091520
Magann, Alicia, Chen, Linhan, Ho, Tak-San, and Rabitz, Herschel. Mon . "Quantum optimal control of multiple weakly interacting molecular rotors in the time-dependent Hartree approximation". United States. https://doi.org/10.1063/1.5091520. https://www.osti.gov/servlets/purl/1609378.
@article{osti_1609378,
title = {Quantum optimal control of multiple weakly interacting molecular rotors in the time-dependent Hartree approximation},
author = {Magann, Alicia and Chen, Linhan and Ho, Tak-San and Rabitz, Herschel},
abstractNote = {In this work we perform quantum optimal control simulations, based on the Time-Dependent Hartree (TDH) approximation, for systems of three to five dipole-dipole coupled OCS rotors. A control electric field is used to steer all of the individual rotors, arranged in chains and regular polygons in a plane, toward either identical or unique objectives. The goal is to explore the utility of the TDH approximation to model the field-induced dynamics of multiple interacting rotors in the weak dipole-dipole coupling regime. A stochastic hill climbing approach is employed to seek an optimal control field that achieves the desired objectives at a specified target time. We first show that multiple rotors in chain and polygon geometries can be identically oriented in the same direction; these cases do not significantly depend on the presence of the dipole-dipole interaction. Additionally, in particular geometrical arrangements, we demonstrate that individual rotors can be uniquely manipulated toward different objectives with the same field. Specifically, it is shown that for a three rotor chain, the two end rotors can be identically oriented in a specific direction while keeping the middle rotor in its ground state, and for an equilateral triangle, two rotors can be identically oriented in a specific direction while the third rotor is oriented in the opposite direction. These multirotor unique objective cases exploit the shape of the field in coordination with dipole-dipole coupling between the rotors. Comparisons to numerically exact calculations, utilizing the TDH-determined fields, are given for all optimal control studies involving systems of three rotors.},
doi = {10.1063/1.5091520},
journal = {Journal of Chemical Physics},
number = 16,
volume = 150,
place = {United States},
year = {Mon Apr 22 00:00:00 EDT 2019},
month = {Mon Apr 22 00:00:00 EDT 2019}
}

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