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

Magann, Alicia; Chen, Linhan; Ho, Tak-San; Rabitz, Herschel

doi:10.1063/1.5091520

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

Journal Article · Mon Apr 22 00:00:00 EDT 2019 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5091520· OSTI ID:1609378

^[1]; Chen, Linhan ^[1]; Ho, Tak-San ^[1];

^[1]

Princeton Univ., NJ (United States)

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.

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Research Organization:: Princeton Univ., NJ (United States); Krell Institute, Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC); US Army Research Office (ARO)

Grant/Contract Number:: FG02-02ER15344; FG02-97ER25308; ARO W911NF-16-1-0014

OSTI ID:: 1609378

Alternate ID(s):: OSTI ID: 1508434

Journal Information:: Journal of Chemical Physics, Vol. 150, Issue 16; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 2 works

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