Non-adiabatic dynamics of molecules in optical cavities

Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul

doi:10.1063/1.4941053

Title: Non-adiabatic dynamics of molecules in optical cavities

Journal Article · Sun Feb 07 00:00:00 EST 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4941053· OSTI ID:22493720

Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul ^[1]

Department of Chemistry, University of California, Irvine, California 92697-2025 (United States)

Strong coupling of molecules to the vacuum field of micro cavities can modify the potential energy surfaces thereby opening new photophysical and photochemical reaction pathways. While the influence of laser fields is usually described in terms of classical field, coupling to the vacuum state of a cavity has to be described in terms of dressed photon-matter states (polaritons) which require quantized fields. We present a derivation of the non-adiabatic couplings for single molecules in the strong coupling regime suitable for the calculation of the dressed state dynamics. The formalism allows to use quantities readily accessible from quantum chemistry codes like the adiabatic potential energy surfaces and dipole moments to carry out wave packet simulations in the dressed basis. The implications for photochemistry are demonstrated for a set of model systems representing typical situations found in molecules.

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OSTI ID:: 22493720

Journal Information:: Journal of Chemical Physics, Vol. 144, Issue 5; Other Information: (c) 2016 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606

Country of Publication:: United States

Language:: English

References (27)

Modifying Chemical Landscapes by Coupling to Vacuum Fields Hutchison, James A.; Schwartz, Tal; Genet, Cyriaque Angewandte Chemie International Edition, Vol. 51, Issue 7 https://doi.org/10.1002/anie.201107033	journal	January 2012
Numerical integration of the time-dependent Schrödinger equation for laser-driven helium Smyth, Edward S.; Parker, Jonathan S.; Taylor, K. T. Computer Physics Communications, Vol. 114, Issue 1-3 https://doi.org/10.1016/s0010-4655(98)00083-6	journal	November 1998
Squeezing Photons into a Point-Like Space Kim, Myung-Ki; Sim, Hongchul; Yoon, Seung Ju Nano Letters, Vol. 15, Issue 6 https://doi.org/10.1021/acs.nanolett.5b01204	journal	May 2015
Control of 1,3-Cyclohexadiene Photoisomerization Using Light-Induced Conical Intersections Kim, Jaehee; Tao, Hongli; White, James L. The Journal of Physical Chemistry A, Vol. 116, Issue 11 https://doi.org/10.1021/jp208384b	journal	December 2011
Molecular Collision Dynamics on Several Electronic States Martínez, T. J.; Ben-Nun, M.; Levine, R. D. The Journal of Physical Chemistry A, Vol. 101, Issue 36 https://doi.org/10.1021/jp970842t	journal	September 1997
Ab Initio Multiple Spawning: Photochemistry from First Principles Quantum Molecular Dynamics Ben-Nun, M.; Quenneville, Jason; Martínez, Todd J. The Journal of Physical Chemistry A, Vol. 104, Issue 22 https://doi.org/10.1021/jp994174i	journal	June 2000
Chemoselective quantum control of carbonyl bonds in Grignard reactions using shaped laser pulses Gollub, Caroline; Kowalewski, Markus; Thallmair, Sebastian Physical Chemistry Chemical Physics, Vol. 12, Issue 48 https://doi.org/10.1039/c0cp01657h	journal	January 2010
Searching for pathways involving dressed states in optimal control theory von den Hoff, Philipp; Kowalewski, Markus; de Vivie-Riedle, Regina Faraday Discussions, Vol. 153 https://doi.org/10.1039/c1fd00031d	journal	January 2011
A perfectly matched layer applied to a reactive scattering problem Nissen, Anna; Karlsson, Hans O.; Kreiss, Gunilla The Journal of Chemical Physics, Vol. 133, Issue 5 https://doi.org/10.1063/1.3458888	journal	August 2010
Proton transfer in solution: Molecular dynamics with quantum transitions Hammes‐Schiffer, Sharon; Tully, John C. The Journal of Chemical Physics, Vol. 101, Issue 6 https://doi.org/10.1063/1.467455	journal	September 1994
Light-induced conical intersections in polyatomic molecules: General theory, strategies of exploitation, and application Demekhin, Philipp V.; Cederbaum, Lorenz S. The Journal of Chemical Physics, Vol. 139, Issue 15 https://doi.org/10.1063/1.4826172	journal	October 2013
Ab initio multiple spawning on laser-dressed states: a study of 1,3-cyclohexadiene photoisomerization via light-induced conical intersections Kim, Jaehee; Tao, Hongli; Martinez, Todd J. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 48, Issue 16 https://doi.org/10.1088/0953-4075/48/16/164003	journal	July 2015
Exploring the Quantum Haroche, Serge; Raimond, Jean-Michel https://doi.org/10.1093/acprof:oso/9780198509141.001.0001	book	January 2006
Cavity sideband cooling of trapped molecules Kowalewski, Markus; Morigi, Giovanna; Pinkse, Pepijn W. H. Physical Review A, Vol. 84, Issue 3 https://doi.org/10.1103/physreva.84.033408	journal	September 2011
Detecting electronic coherence by multidimensional broadband stimulated x-ray Raman signals Dorfman, Konstantin E.; Bennett, Kochise; Mukamel, Shaul Physical Review A, Vol. 92, Issue 2 https://doi.org/10.1103/physreva.92.023826	journal	August 2015
Real-Time Cavity QED with Single Atoms Hood, C. J.; Chapman, M. S.; Lynn, T. W. Physical Review Letters, Vol. 80, Issue 19 https://doi.org/10.1103/physrevlett.80.4157	journal	May 1998
Cavity Cooling of Internal Molecular Motion Morigi, Giovanna; Pinkse, Pepijn W. H.; Kowalewski, Markus Physical Review Letters, Vol. 99, Issue 7 https://doi.org/10.1103/physrevlett.99.073001	journal	August 2007
Dynamic Stark Control of Photochemical Processes Sussman, B. J.; Townsend, D.; Ivanov, M. Yu. Science, Vol. 314, Issue 5797 https://doi.org/10.1126/science.1132289	journal	October 2006
Conical Intersections: Theory, Computation and Experiment Domcke, Wolfgang; Yarkony, David R.; Köppel, Horst Advanced Series in Physical Chemistry https://doi.org/10.1142/7803	book	November 2011
Diamond based photonic crystal microcavities Tomljenovic-Hanic, S.; Steel, M. J.; de Sterke, C. Martijn Optics Express, Vol. 14, Issue 8 https://doi.org/10.1364/oe.14.003556	journal	January 2006
Modifying Chemical Landscapes by Coupling to Vacuum Fields Hutchison, James A.; Schwartz, Tal; Genet, Cyriaque Angewandte Chemie, Vol. 124, Issue 7 https://doi.org/10.1002/ange.201107033	journal	January 2012
Proceedings of the American Physical Society Physical Review, Vol. 83, Issue 4, p. 868-882 https://doi.org/10.1103/physrev.83.868	journal	August 1951
Proceedings of the American Physical Society Cole, A. D. Science, Vol. 42, Issue 1081 https://doi.org/10.1126/science.42.1081.390	journal	September 1915
Proceedings of the American Physical Society Physical Review, Vol. 82, Issue 4, p. 577-577 https://doi.org/10.1103/physrev.82.577	journal	May 1951
Control of 1,3-Cyclohexadiene Photoisomerization Using Light-Induced Conical Intersections Kim, Jaehee; Tao, Hongli; White, James L. arXiv https://doi.org/10.48550/arxiv.1109.5756	text	January 2011
Detecting Electronic Coherence by Multidimensional Broadband Stimulated X-Ray Raman Signals Dorfman, Konstantin E.; Bennett, Kochise; Mukamel, Shaul arXiv https://doi.org/10.48550/arxiv.1506.08226	text	January 2015
Cavity cooling of internal molecular motion Morigi, Giovanna; Pinkse, Pepijn W. H.; Kowalewski, Markus arXiv https://doi.org/10.48550/arxiv.quant-ph/0703157	text	January 2007

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A strong enhancement in electronic current due to conical-intersection Karmakar, Anirban; Gangopadhyay, Gautam Physica Scripta, Vol. 94, Issue 12 https://doi.org/10.1088/1402-4896/ab35ee	journal	September 2019
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Interplay of electron-phonon nonadiabaticity and Raman scattering in the wavepacket dynamics of electron-phonon-photon systems Ishida, Kunio The European Physical Journal D, Vol. 73, Issue 6 https://doi.org/10.1140/epjd/e2019-90485-5	journal	June 2019
Strong light-matter coupling in quantum chemistry and quantum photonics Flick, Johannes; Rivera, Nicholas; Narang, Prineha Nanophotonics, Vol. 7, Issue 9 https://doi.org/10.1515/nanoph-2018-0067	journal	September 2018
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Cavity Casimir-Polder forces and their effects in ground state chemical reactivity Galego, Javier; Climent, Clàudia; Garcia-Vidal, Francisco J. arXiv https://doi.org/10.48550/arxiv.1807.10846	text	January 2018
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Title: Non-adiabatic dynamics of molecules in optical cavities

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