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 »
- Authors:
-
- 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}
}
Web of Science
Works referenced in this record:
Toward scalable information processing with ultracold polar molecules in an electric field: A numerical investigation
journal, December 2010
- Bomble, Laëtitia; Pellegrini, Philippe; Ghesquière, Pierre
- Physical Review A, Vol. 82, Issue 6
A semi-classical implementation of quantum control using Gaussian wave packet dynamics
journal, August 1995
- Messina, Michael; Wilson, Kent R.
- Chemical Physics Letters, Vol. 241, Issue 5-6
One-dimensional nuclear dynamics in the time-dependent Hartree-Fock approximation
journal, March 1976
- Bonche, P.; Koonin, S.; Negele, J. W.
- Physical Review C, Vol. 13, Issue 3
Singularity-free quantum tracking control of molecular rotor orientation
journal, October 2018
- Magann, Alicia; Ho, Tak-San; Rabitz, Herschel
- Physical Review A, Vol. 98, Issue 4
Quantum control of I2 wave packet localization in solid argon matrix
journal, February 2000
- Guiang, Chona S.; Wyatt, Robert E.
- The Journal of Chemical Physics, Vol. 112, Issue 8
Quantum error correction in a solid-state hybrid spin register
journal, February 2014
- Waldherr, G.; Wang, Y.; Zaiser, S.
- Nature, Vol. 506, Issue 7487
High-harmonic spectroscopy of oriented OCS molecules: emission of even and odd harmonics
text, January 2012
- Kraus, Peter M.; Rupenyan-Vasileva, Alisa Bohos; Wörner, Hans Jakob
- ETH Zurich
Condensed Matter Theory of Dipolar Quantum Gases
journal, April 2012
- Baranov, M. A.; Dalmonte, M.; Pupillo, G.
- Chemical Reviews, Vol. 112, Issue 9
Dissociation dynamics of Ar3 in the time-dependent self-consistent field (TDSCF) approximation
journal, October 1983
- Buch, V.; Gerber, R. B.; Ratner, M. A.
- Chemical Physics Letters, Vol. 101, Issue 1
Optimal control of orientation and entanglement for two dipole–dipole coupled quantum planar rotors
journal, January 2018
- Yu, Hongling; Ho, Tak-San; Rabitz, Herschel
- Physical Chemistry Chemical Physics, Vol. 20, Issue 18
Quantum Computation using Arrays of N Polar Molecules in Pendular States
journal, October 2016
- Wei, Qi; Cao, Yudong; Kais, Sabre
- ChemPhysChem, Vol. 17, Issue 22
Optimal control of interacting particles: a multi-configuration time-dependent Hartree–Fock approach
journal, October 2009
- Mundt, Michael; Tannor, David J.
- New Journal of Physics, Vol. 11, Issue 10
Molecular Dipole Moments and Stark Effects. II. Stark Effects in OCS
journal, February 1950
- Shulman, R. G.; Townes, C. H.
- Physical Review, Vol. 77, Issue 4
Quantum control of alignment and orientation of molecules by optimized laser pulses
journal, June 2001
- Hoki, K.; Fujimura, Y.
- Chemical Physics, Vol. 267, Issue 1-3
Two-pulse coherent control of electronic branching in Li2 photodissociation
journal, March 1998
- Abrashkevich, Dmitri G.; Shapiro, Moshe; Brumer, Paul
- The Journal of Chemical Physics, Vol. 108, Issue 9
Dynamics of metal electron excitation in atom-surface collisions: A quantum wave packet approach
journal, February 1984
- Kirson, Z.; Gerber, R. B.; Nitzan, A.
- Surface Science Letters, Vol. 137, Issue 2-3
Photonic generation of microwave arbitrary waveforms
journal, July 2011
- Yao, Jianping
- Optics Communications, Vol. 284, Issue 15
Quantum observable homotopy tracking control
journal, October 2005
- Rothman, Adam; Ho, Tak-San; Rabitz, Herschel
- The Journal of Chemical Physics, Vol. 123, Issue 13
Dynamics of metal electron excitation in atom-surface collisions: A quantum wave packet approach
journal, February 1984
- Kirson, Z.; Gerber, R. B.; Nitzan, A.
- Surface Science, Vol. 137, Issue 2-3
Time-dependent methods to study the dissociation dynamics of tri- and tetra-atomic clusters
journal, May 2002
- Hernández, M. I.; García-Vela, A.; Campos-Martínez, J.
- Computer Physics Communications, Vol. 145, Issue 1
New formulations of monotonically convergent quantum control algorithms
journal, May 2003
- Maday, Yvon; Turinici, Gabriel
- The Journal of Chemical Physics, Vol. 118, Issue 18
Quantum control of multidimensional systems Implementation within the time‐dependent Hartree approximation
journal, January 1996
- Messina, Michael; Wilson, Kent R.; Krause, Jeffrey L.
- The Journal of Chemical Physics, Vol. 104, Issue 1, p. 173-182
Control of selectivity of chemical reaction via control of wave packet evolution
journal, November 1985
- Tannor, David J.; Rice, Stuart A.
- The Journal of Chemical Physics, Vol. 83, Issue 10, p. 5013-5018
Pair-eigenstates and mutual alignment of coupled molecular rotors in a magnetic field
journal, January 2016
- Sharma, Ketan; Friedrich, Bretislav
- Physical Chemistry Chemical Physics, Vol. 18, Issue 19
Control of molecular orientation with combined near-single-cycle THz and optimally designed non-resonant laser pulses: Carrier-envelope phase effects
journal, July 2015
- Yoshida, Masataka; Ohtsuki, Yukiyoshi
- Chemical Physics Letters, Vol. 633
Photonic synthesis of broadband microwave arbitrary waveforms applicable to ultra-wideband communication
journal, April 2005
- Lin, I. S.; McKinney, J. D.; Weiner, A. M.
- IEEE Microwave and Wireless Components Letters, Vol. 15, Issue 4
Chopped random-basis quantum optimization
journal, August 2011
- Caneva, Tommaso; Calarco, Tommaso; Montangero, Simone
- Physical Review A, Vol. 84, Issue 2
Directional Dynamics in the Photodissociation of Oriented Molecules
journal, March 2004
- Rakitzis, T. P.
- Science, Vol. 303, Issue 5665
Note on Exchange Phenomena in the Thomas Atom
journal, July 1930
- Dirac, P. A. M.
- Mathematical Proceedings of the Cambridge Philosophical Society, Vol. 26, Issue 3
Laser Control of Chemical Reactions
journal, March 1998
- Zare, Richard N.
- Science, Vol. 279, Issue 5358, p. 1875-1879
Time-dependent mean-field approximation for nuclear dynamical problems
journal, April 1980
- Levit, S.
- Physical Review C, Vol. 21, Issue 4
High-Harmonic Spectroscopy of Oriented OCS Molecules: Emission of Even and Odd Harmonics
journal, December 2012
- Kraus, P. M.; Rupenyan, A.; Wörner, H. J.
- Physical Review Letters, Vol. 109, Issue 23
Femtosecond laser pulse control of multidimensional vibrational dynamics: Computational studies on the pyrazine molecule
journal, July 2006
- Wang, Luxia; Meyer, Hans-Dieter; May, Volkhard
- The Journal of Chemical Physics, Vol. 125, Issue 1
Multi-polarization quantum control of rotational motion through dipole coupling
journal, February 2010
- Turinici, Gabriel; Rabitz, Herschel
- Journal of Physics A: Mathematical and Theoretical, Vol. 43, Issue 10
Optimal molecular alignment and orientation through rotational ladder climbing
journal, October 2005
- Salomon, Julien; Dion, Claude M.; Turinici, Gabriel
- The Journal of Chemical Physics, Vol. 123, Issue 14
Vibrational eigenvalues and eigenfunctions for planar acetylene by wave-packet propagation, and its mode-selective infrared excitation
journal, September 1997
- Liu, Li; Muckerman, James T.
- The Journal of Chemical Physics, Vol. 107, Issue 9
Colloquium : Optimal control of high-harmonic generation
journal, January 2008
- Winterfeldt, Carsten; Spielmann, Christian; Gerber, Gustav
- Reviews of Modern Physics, Vol. 80, Issue 1
Implementation of an iterative algorithm for optimal control of molecular dynamics into MCTDH
journal, January 2008
- Schröder, Markus; Carreón-Macedo, José-Luis; Brown, Alex
- Phys. Chem. Chem. Phys., Vol. 10, Issue 6
On self-consistent and stochastic treatments of V—T energy transfer in collinear atom-diatom collisions
journal, September 1977
- Schatz, George C.
- Chemical Physics, Vol. 24, Issue 2
Quantum phases of dipolar rotors on two-dimensional lattices
journal, March 2018
- Abolins, B. P.; Zillich, R. E.; Whaley, K. B.
- The Journal of Chemical Physics, Vol. 148, Issue 10
A rapid monotonically convergent iteration algorithm for quantum optimal control over the expectation value of a positive definite operator
journal, July 1998
- Zhu, Wusheng; Rabitz, Herschel
- The Journal of Chemical Physics, Vol. 109, Issue 2
Quantum Computation with Trapped Polar Molecules
journal, January 2002
- DeMille, D.
- Physical Review Letters, Vol. 88, Issue 6
High-fidelity spin entanglement using optimal control
journal, February 2014
- Dolde, Florian; Bergholm, Ville; Wang, Ya
- Nature Communications, Vol. 5, Issue 1
Microwave Spectra of Molecules of Astrophysical Interest VI. Carbonyl Sulfide and Hydrogen Cyanide
journal, January 1974
- Maki, Arthur G.
- Journal of Physical and Chemical Reference Data, Vol. 3, Issue 1
Quantum Molecular Dynamics of Ultrafast Processes in Large Polyatomic Systems
journal, June 1999
- Jungwirth, Pavel; Gerber, R. Benny
- Chemical Reviews, Vol. 99, Issue 6
Chopped random-basis quantum optimization
text, January 2011
- Caneva, Tommaso; Calarco, Tommaso; Montangero, Simone
- arXiv
Condensed Matter Theory of Dipolar Quantum Gases
text, January 2012
- Baranov, M. A.; Dalmonte, M.; Pupillo, G.
- arXiv
Quantum error correction in a solid-state hybrid spin register
text, January 2013
- Waldherr, G.; Wang, Y.; Zaiser, S.
- arXiv
Pair-eigenstates and mutual alignment of coupled molecular rotors in a magnetic field
text, January 2016
- Sharma, Ketan; Friedrich, Bretislav
- arXiv
Quantum computation using arrays of N polar molecules in pendular states
preprint, January 2016
- Wei, Qi; Cao, Yudong; Kais, Sabre
- arXiv
Quantum phases of dipolar rotors on two-dimensional lattices
text, January 2018
- Abolins, Brendan P.; Zillich, Robert E.; Whaley, K. Birgitta
- arXiv
Singularity-free quantum tracking control of molecular rotor orientation
text, January 2018
- Magann, Alicia; Ho, Tak-San; Rabitz, Herschel
- arXiv
Optimal molecular alignment and orientation through rotational ladder climbing
text, January 2005
- Salomon, Julien; Dion, Claude M.; Turinici, Gabriel
- arXiv
Works referencing / citing this record:
Implementation of three-qubit quantum computation with pendular states of polar molecules by optimal control
journal, January 2020
- Zhang, Zuo-Yuan; Liu, Jin-Ming; Hu, Zhengfeng
- The Journal of Chemical Physics, Vol. 152, Issue 4