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

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 ^[2]; Ho, Tak-San ^[2]; ^[2]

Princeton Univ., NJ (United States); DOE/OSTI
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.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: FG02-02ER15344; FG02-97ER25308

OSTI ID:: 1609378

Alternate ID(s):: OSTI ID: 1508434

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

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

Country of Publication:: United States

Language:: English

References (57)

Quantum Computation using Arrays of N Polar Molecules in Pendular States Wei, Qi; Cao, Yudong; Kais, Sabre ChemPhysChem, Vol. 17, Issue 22 https://doi.org/10.1002/cphc.201600781	journal	October 2016
Dissociation dynamics of Ar3 in the time-dependent self-consistent field (TDSCF) approximation Buch, V.; Gerber, R. B.; Ratner, M. A. Chemical Physics Letters, Vol. 101, Issue 1 https://doi.org/10.1016/0009-2614(83)80302-9	journal	October 1983
A semi-classical implementation of quantum control using Gaussian wave packet dynamics Messina, Michael; Wilson, Kent R. Chemical Physics Letters, Vol. 241, Issue 5-6 https://doi.org/10.1016/0009-2614(95)00656-o	journal	August 1995
Dynamics of metal electron excitation in atom-surface collisions: A quantum wave packet approach Kirson, Z.; Gerber, R. B.; Nitzan, A. Surface Science, Vol. 137, Issue 2-3 https://doi.org/10.1016/0039-6028(84)90528-4	journal	February 1984
Dynamics of metal electron excitation in atom-surface collisions: A quantum wave packet approach Kirson, Z.; Gerber, R. B.; Nitzan, A. Surface Science Letters, Vol. 137, Issue 2-3 https://doi.org/10.1016/0167-2584(84)90886-7	journal	February 1984
On self-consistent and stochastic treatments of V—T energy transfer in collinear atom-diatom collisions Schatz, George C. Chemical Physics, Vol. 24, Issue 2 https://doi.org/10.1016/0301-0104(77)85233-6	journal	September 1977
Control of molecular orientation with combined near-single-cycle THz and optimally designed non-resonant laser pulses: Carrier-envelope phase effects Yoshida, Masataka; Ohtsuki, Yukiyoshi Chemical Physics Letters, Vol. 633 https://doi.org/10.1016/j.cplett.2015.05.041	journal	July 2015
Photonic generation of microwave arbitrary waveforms Yao, Jianping Optics Communications, Vol. 284, Issue 15 https://doi.org/10.1016/j.optcom.2011.02.069	journal	July 2011
Control of unimolecular reactions using coherent light Brumer, Paul; Shapiro, Moshe Chemical Physics Letters, Vol. 126, Issue 6 https://doi.org/10.1016/s0009-2614(86)80171-3	journal	May 1986
Time-dependent methods to study the dissociation dynamics of tri- and tetra-atomic clusters Hernández, M. I.; García-Vela, A.; Campos-Martínez, J. Computer Physics Communications, Vol. 145, Issue 1 https://doi.org/10.1016/s0010-4655(02)00149-2	journal	May 2002
Quantum control of alignment and orientation of molecules by optimized laser pulses Hoki, K.; Fujimura, Y. Chemical Physics, Vol. 267, Issue 1-3 https://doi.org/10.1016/s0301-0104(01)00255-5	journal	June 2001
Note on Exchange Phenomena in the Thomas Atom Dirac, P. A. M. Mathematical Proceedings of the Cambridge Philosophical Society, Vol. 26, Issue 3 https://doi.org/10.1017/s0305004100016108	journal	July 1930
Condensed Matter Theory of Dipolar Quantum Gases Baranov, M. A.; Dalmonte, M.; Pupillo, G. Chemical Reviews, Vol. 112, Issue 9 https://doi.org/10.1021/cr2003568	journal	April 2012
Quantum Molecular Dynamics of Ultrafast Processes in Large Polyatomic Systems Jungwirth, Pavel; Gerber, R. Benny Chemical Reviews, Vol. 99, Issue 6 https://doi.org/10.1021/cr9800210	journal	June 1999
Quantum error correction in a solid-state hybrid spin register Waldherr, G.; Wang, Y.; Zaiser, S. Nature, Vol. 506, Issue 7487 https://doi.org/10.1038/nature12919	journal	February 2014
High-fidelity spin entanglement using optimal control Dolde, Florian; Bergholm, Ville; Wang, Ya Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4371	journal	February 2014
Laser control of chemical reactions Henriksen, Niels E. Chemical Society Reviews, Vol. 31, Issue 1, p. 37-42 https://doi.org/10.1039/b100111f	journal	January 2002
Implementation of an iterative algorithm for optimal control of molecular dynamics into MCTDH Schröder, Markus; Carreón-Macedo, José-Luis; Brown, Alex Phys. Chem. Chem. Phys., Vol. 10, Issue 6 https://doi.org/10.1039/b714821f	journal	January 2008
Pair-eigenstates and mutual alignment of coupled molecular rotors in a magnetic field Sharma, Ketan; Friedrich, Bretislav Physical Chemistry Chemical Physics, Vol. 18, Issue 19 https://doi.org/10.1039/c6cp00390g	journal	January 2016
Optimal control of orientation and entanglement for two dipole–dipole coupled quantum planar rotors Yu, Hongling; Ho, Tak-San; Rabitz, Herschel Physical Chemistry Chemical Physics, Vol. 20, Issue 18 https://doi.org/10.1039/c8cp00231b	journal	January 2018
New formulations of monotonically convergent quantum control algorithms Maday, Yvon; Turinici, Gabriel The Journal of Chemical Physics, Vol. 118, Issue 18 https://doi.org/10.1063/1.1564043	journal	May 2003
Quantum observable homotopy tracking control Rothman, Adam; Ho, Tak-San; Rabitz, Herschel The Journal of Chemical Physics, Vol. 123, Issue 13 https://doi.org/10.1063/1.2042456	journal	October 2005
Optimal molecular alignment and orientation through rotational ladder climbing Salomon, Julien; Dion, Claude M.; Turinici, Gabriel The Journal of Chemical Physics, Vol. 123, Issue 14 https://doi.org/10.1063/1.2049270	journal	October 2005
Femtosecond laser pulse control of multidimensional vibrational dynamics: Computational studies on the pyrazine molecule Wang, Luxia; Meyer, Hans-Dieter; May, Volkhard The Journal of Chemical Physics, Vol. 125, Issue 1 https://doi.org/10.1063/1.2208611	journal	July 2006
Microwave Spectra of Molecules of Astrophysical Interest VI. Carbonyl Sulfide and Hydrogen Cyanide Maki, Arthur G. Journal of Physical and Chemical Reference Data, Vol. 3, Issue 1 https://doi.org/10.1063/1.3253139	journal	January 1974
Control of selectivity of chemical reaction via control of wave packet evolution Tannor, David J.; Rice, Stuart A. The Journal of Chemical Physics, Vol. 83, Issue 10, p. 5013-5018 https://doi.org/10.1063/1.449767	journal	November 1985
Quantum control of multidimensional systems Implementation within the time‐dependent Hartree approximation Messina, Michael; Wilson, Kent R.; Krause, Jeffrey L. The Journal of Chemical Physics, Vol. 104, Issue 1, p. 173-182 https://doi.org/10.1063/1.470887	journal	January 1996
Vibrational eigenvalues and eigenfunctions for planar acetylene by wave-packet propagation, and its mode-selective infrared excitation Liu, Li; Muckerman, James T. The Journal of Chemical Physics, Vol. 107, Issue 9 https://doi.org/10.1063/1.474714	journal	September 1997
Two-pulse coherent control of electronic branching in Li2 photodissociation Abrashkevich, Dmitri G.; Shapiro, Moshe; Brumer, Paul The Journal of Chemical Physics, Vol. 108, Issue 9 https://doi.org/10.1063/1.475785	journal	March 1998
A rapid monotonically convergent iteration algorithm for quantum optimal control over the expectation value of a positive definite operator Zhu, Wusheng; Rabitz, Herschel The Journal of Chemical Physics, Vol. 109, Issue 2 https://doi.org/10.1063/1.476575	journal	July 1998
Quantum control of I2 wave packet localization in solid argon matrix Guiang, Chona S.; Wyatt, Robert E. The Journal of Chemical Physics, Vol. 112, Issue 8 https://doi.org/10.1063/1.480935	journal	February 2000
Quantum phases of dipolar rotors on two-dimensional lattices Abolins, B. P.; Zillich, R. E.; Whaley, K. B. The Journal of Chemical Physics, Vol. 148, Issue 10 https://doi.org/10.1063/1.5005522	journal	March 2018
Optimal control of interacting particles: a multi-configuration time-dependent Hartree–Fock approach Mundt, Michael; Tannor, David J. New Journal of Physics, Vol. 11, Issue 10 https://doi.org/10.1088/1367-2630/11/10/105038	journal	October 2009
Multi-polarization quantum control of rotational motion through dipole coupling Turinici, Gabriel; Rabitz, Herschel Journal of Physics A: Mathematical and Theoretical, Vol. 43, Issue 10 https://doi.org/10.1088/1751-8113/43/10/105303	journal	February 2010
Molecular Dipole Moments and Stark Effects. II. Stark Effects in OCS Shulman, R. G.; Townes, C. H. Physical Review, Vol. 77, Issue 4 https://doi.org/10.1103/physrev.77.500	journal	February 1950
Toward scalable information processing with ultracold polar molecules in an electric field: A numerical investigation Bomble, Laëtitia; Pellegrini, Philippe; Ghesquière, Pierre Physical Review A, Vol. 82, Issue 6 https://doi.org/10.1103/physreva.82.062323	journal	December 2010
Chopped random-basis quantum optimization Caneva, Tommaso; Calarco, Tommaso; Montangero, Simone Physical Review A, Vol. 84, Issue 2 https://doi.org/10.1103/physreva.84.022326	journal	August 2011
Singularity-free quantum tracking control of molecular rotor orientation Magann, Alicia; Ho, Tak-San; Rabitz, Herschel Physical Review A, Vol. 98, Issue 4 https://doi.org/10.1103/physreva.98.043429	journal	October 2018
One-dimensional nuclear dynamics in the time-dependent Hartree-Fock approximation Bonche, P.; Koonin, S.; Negele, J. W. Physical Review C, Vol. 13, Issue 3 https://doi.org/10.1103/physrevc.13.1226	journal	March 1976
Time-dependent mean-field approximation for nuclear dynamical problems Levit, S. Physical Review C, Vol. 21, Issue 4 https://doi.org/10.1103/physrevc.21.1594	journal	April 1980
High-Harmonic Spectroscopy of Oriented OCS Molecules: Emission of Even and Odd Harmonics Kraus, P. M.; Rupenyan, A.; Wörner, H. J. Physical Review Letters, Vol. 109, Issue 23 https://doi.org/10.1103/physrevlett.109.233903	journal	December 2012
Quantum Computation with Trapped Polar Molecules DeMille, D. Physical Review Letters, Vol. 88, Issue 6 https://doi.org/10.1103/physrevlett.88.067901	journal	January 2002
*Colloquium* : Optimal control of high-harmonic generation Winterfeldt, Carsten; Spielmann, Christian; Gerber, Gustav Reviews of Modern Physics, Vol. 80, Issue 1 https://doi.org/10.1103/revmodphys.80.117	journal	January 2008
Photonic synthesis of broadband microwave arbitrary waveforms applicable to ultra-wideband communication Lin, I. S.; McKinney, J. D.; Weiner, A. M. IEEE Microwave and Wireless Components Letters, Vol. 15, Issue 4 https://doi.org/10.1109/lmwc.2005.845698	journal	April 2005
Directional Dynamics in the Photodissociation of Oriented Molecules Rakitzis, T. P. Science, Vol. 303, Issue 5665 https://doi.org/10.1126/science.1094186	journal	March 2004
Reactions of Oriented Molecules Brooks, P. R. Science, Vol. 193, Issue 4247 https://doi.org/10.1126/science.193.4247.11	journal	July 1976
Laser Control of Chemical Reactions Zare, Richard N. Science, Vol. 279, Issue 5358, p. 1875-1879 https://doi.org/10.1126/science.279.5358.1875	journal	March 1998
High-harmonic spectroscopy of oriented OCS molecules: emission of even and odd harmonics Kraus, Peter M.; Rupenyan-Vasileva, Alisa Bohos; Wörner, Hans Jakob ETH Zurich https://doi.org/10.3929/ethz-a-010780595	text	January 2012
Chopped random-basis quantum optimization Caneva, Tommaso; Calarco, Tommaso; Montangero, Simone arXiv https://doi.org/10.48550/arxiv.1103.0855	text	January 2011
Condensed Matter Theory of Dipolar Quantum Gases Baranov, M. A.; Dalmonte, M.; Pupillo, G. arXiv https://doi.org/10.48550/arxiv.1207.1914	text	January 2012
Quantum error correction in a solid-state hybrid spin register Waldherr, G.; Wang, Y.; Zaiser, S. arXiv https://doi.org/10.48550/arxiv.1309.6424	text	January 2013
Pair-eigenstates and mutual alignment of coupled molecular rotors in a magnetic field Sharma, Ketan; Friedrich, Bretislav arXiv https://doi.org/10.48550/arxiv.1601.04860	text	January 2016
Quantum computation using arrays of N polar molecules in pendular states Wei, Qi; Cao, Yudong; Kais, Sabre arXiv https://doi.org/10.48550/arxiv.1607.04959	preprint	January 2016
Quantum phases of dipolar rotors on two-dimensional lattices Abolins, Brendan P.; Zillich, Robert E.; Whaley, K. Birgitta arXiv https://doi.org/10.48550/arxiv.1803.02512	text	January 2018
Singularity-free quantum tracking control of molecular rotor orientation Magann, Alicia; Ho, Tak-San; Rabitz, Herschel arXiv https://doi.org/10.48550/arxiv.1809.06349	text	January 2018
Optimal molecular alignment and orientation through rotational ladder climbing Salomon, Julien; Dion, Claude M.; Turinici, Gabriel arXiv https://doi.org/10.48550/arxiv.physics/0506179	text	January 2005
Quantum computation with trapped polar molecules DeMille, D. arXiv https://doi.org/10.48550/arxiv.quant-ph/0109083	text	January 2001

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