Coupled wave-packets for non-adiabatic molecular dynamics: a generalization of Gaussian wave-packet dynamics to multiple potential energy surfaces

White, Alexander James; Tretiak, Sergei; Mozyrsky, Dima V.

doi:10.1039/C6SC01319H

Title: Coupled wave-packets for non-adiabatic molecular dynamics: a generalization of Gaussian wave-packet dynamics to multiple potential energy surfaces

Journal Article · Mon Apr 25 00:00:00 EDT 2016 · Chemical Science

DOI:https://doi.org/10.1039/C6SC01319H· OSTI ID:1338745

White, Alexander James ^[1]; Tretiak, Sergei ^[2]; Mozyrsky, Dima V. ^[3]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division, Center for Nonlinear Studies
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division, Center for Nonlinear Studies and Center for Integrated Nanotechnologies
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division

Accurate simulation of the non-adiabatic dynamics of molecules in excited electronic states is key to understanding molecular photo-physical processes. Here we present a novel method, based on a semiclassical approximation, that is as efficient as the commonly used mean field Ehrenfest or ad hoc surface hopping methods and properly accounts for interference and decoherence effects. This novel method is an extension of Heller's thawed Gaussian wave-packet dynamics that includes coupling between potential energy surfaces. By studying several standard test problems we demonstrate that the accuracy of the method can be systematically improved while maintaining high efficiency. The method is suitable for investigating the role of quantum coherence in the non-adiabatic dynamics of many-atom molecules.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1338745

Report Number(s):: LA-UR-16-20319

Journal Information:: Chemical Science, Vol. 7, Issue 8; ISSN 2041-6520

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 17 works

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References (74)

Ab Initio Molecular Dynamics Marx, Dominik; Hutter, Jurg https://doi.org/10.1017/CBO9780511609633	book	January 2009
Unified Approach for Molecular Dynamics and Density-Functional Theory Car, R.; Parrinello, M. Physical Review Letters, Vol. 55, Issue 22 https://doi.org/10.1103/PhysRevLett.55.2471	journal	November 1985
Solution of the Schrödinger equation by a spectral method Feit, M. D.; Fleck, J. A.; Steiger, A. Journal of Computational Physics, Vol. 47, Issue 3 https://doi.org/10.1016/0021-9991(82)90091-2	journal	September 1982
An accurate and efficient scheme for propagating the time dependent Schrödinger equation Tal‐Ezer, H.; Kosloff, R. The Journal of Chemical Physics, Vol. 81, Issue 9 https://doi.org/10.1063/1.448136	journal	November 1984
Unitary quantum time evolution by iterative Lanczos reduction Park, Tae Jun; Light, J. C. The Journal of Chemical Physics, Vol. 85, Issue 10 https://doi.org/10.1063/1.451548	journal	November 1986
Propagation Methods for Quantum Molecular Dynamics Kosloff, R. Annual Review of Physical Chemistry, Vol. 45, Issue 1 https://doi.org/10.1146/annurev.pc.45.100194.001045	journal	October 1994
Fully quantal initial‐state‐selected reaction probabilities ( J =0) for a four‐atom system: H ₂ ( v =0, 1, j =0)+OH( v =0,1, j =0)→H+H ₂ O Neuhauser, Daniel The Journal of Chemical Physics, Vol. 100, Issue 12 https://doi.org/10.1063/1.466681	journal	June 1994
Full-Dimensional Quantum State-to-State Nonadiabatic Dynamics for Photodissociation of Ammonia in its A -Band Xie, Changjian; Ma, Jianyi; Zhu, Xiaolei The Journal of Physical Chemistry Letters, Vol. 5, Issue 7 https://doi.org/10.1021/jz500227d	journal	March 2014
Dynamics of Water Dissociative Chemisorption on Ni(111): Effects of Impact Sites and Incident Angles Jiang, Bin; Guo, Hua Physical Review Letters, Vol. 114, Issue 16 https://doi.org/10.1103/PhysRevLett.114.166101	journal	April 2015
Zur Quantentheorie der Molekeln Born, M.; Oppenheimer, R. Annalen der Physik, Vol. 389, Issue 20 https://doi.org/10.1002/andp.19273892002	journal	January 1927
Collisions between atoms and molecules at ordinary temperatures Massey, H. S. W. Reports on Progress in Physics, Vol. 12, Issue 1 https://doi.org/10.1088/0034-4885/12/1/311	journal	January 1949
Bemerkung �ber die angen�herte G�ltigkeit der klassischen Mechanik innerhalb der Quantenmechanik Ehrenfest, P. Zeitschrift f�r Physik, Vol. 45, Issue 7-8 https://doi.org/10.1007/BF01329203	journal	July 1927
Mean-trajectory approximation for charge- and energy-transfer processes at surfaces Sawada, Shin-Ichi; Nitzan, Abraham; Metiu, Horia Physical Review B, Vol. 32, Issue 2 https://doi.org/10.1103/PhysRevB.32.851	journal	July 1985
Trajectory Surface Hopping Approach to Nonadiabatic Molecular Collisions: The Reaction of H ⁺ with D ₂ Tully, John C.; Preston, Richard K. The Journal of Chemical Physics, Vol. 55, Issue 2 https://doi.org/10.1063/1.1675788	journal	July 1971
Molecular dynamics with electronic transitions Tully, John C. The Journal of Chemical Physics, Vol. 93, Issue 2 https://doi.org/10.1063/1.459170	journal	July 1990
Augmented Ehrenfest dynamics yields a rate for surface hopping Subotnik, Joseph E. The Journal of Chemical Physics, Vol. 132, Issue 13 https://doi.org/10.1063/1.3314248	journal	April 2010
Fewest-Switches Surface Hopping and Decoherence in Multiple Dimensions Subotnik, Joseph E. The Journal of Physical Chemistry A, Vol. 115, Issue 44 https://doi.org/10.1021/jp206557h	journal	November 2011
Breaking the Phonon Bottleneck in PbSe and CdSe Quantum Dots: Time-Domain Density Functional Theory of Charge Carrier Relaxation Kilina, Svetlana V.; Kilin, Dmitri S.; Prezhdo, Oleg V. ACS Nano, Vol. 3, Issue 1 https://doi.org/10.1021/nn800674n	journal	December 2008
On-the-fly ab initio molecular dynamics with multiconfigurational Ehrenfest method Saita, Kenichiro; Shalashilin, Dmitrii V. The Journal of Chemical Physics, Vol. 137, Issue 22 https://doi.org/10.1063/1.4734313	journal	December 2012
Nonadiabatic Excited-State Molecular Dynamics: Modeling Photophysics in Organic Conjugated Materials Nelson, Tammie; Fernandez-Alberti, Sebastian; Roitberg, Adrian E. Accounts of Chemical Research, Vol. 47, Issue 4 https://doi.org/10.1021/ar400263p	journal	February 2014
Advanced Capabilities of the PYXAID Program: Integration Schemes, Decoherence Effects, Multiexcitonic States, and Field-Matter Interaction Akimov, Alexey V.; Prezhdo, Oleg V. Journal of Chemical Theory and Computation, Vol. 10, Issue 2 https://doi.org/10.1021/ct400934c	journal	January 2014
Time-Domain Ab Initio Modeling of Photoinduced Dynamics at Nanoscale Interfaces Wang, Linjun; Long, Run; Prezhdo, Oleg V. Annual Review of Physical Chemistry, Vol. 66, Issue 1 https://doi.org/10.1146/annurev-physchem-040214-121359	journal	April 2015
Ehrenfest approach to open double-well dynamics Choi, Stephen; Onofrio, Roberto; Sundaram, Bala Physical Review E, Vol. 92, Issue 4 https://doi.org/10.1103/PhysRevE.92.042907	journal	October 2015
Nonadiabatic Dynamics of Photoinduced Proton-Coupled Electron Transfer in a Solvated Phenol–Amine Complex Goyal, Puja; Schwerdtfeger, Christine A.; Soudackov, Alexander V. The Journal of Physical Chemistry B, Vol. 119, Issue 6 https://doi.org/10.1021/jp5126969	journal	August 2014
Appraisal of Surface Hopping as a Tool for Modeling Condensed Phase Linear Absorption Spectra Petit, Andrew S.; Subotnik, Joseph E. Journal of Chemical Theory and Computation, Vol. 11, Issue 9 https://doi.org/10.1021/acs.jctc.5b00510	journal	August 2015
An On-the-Fly Surface-Hopping Program JADE for Nonadiabatic Molecular Dynamics of Polyatomic Systems: Implementation and Applications Du, Likai; Lan, Zhenggang Journal of Chemical Theory and Computation, Vol. 11, Issue 4 https://doi.org/10.1021/ct501106d	journal	March 2015
Surface hopping with a manifold of electronic states. I. Incorporating surface-leaking to capture lifetimes Ouyang, Wenjun; Dou, Wenjie; Subotnik, Joseph E. The Journal of Chemical Physics, Vol. 142, Issue 8 https://doi.org/10.1063/1.4908032	journal	February 2015
Surface hopping with a manifold of electronic states. II. Application to the many-body Anderson-Holstein model Dou, Wenjie; Nitzan, Abraham; Subotnik, Joseph E. The Journal of Chemical Physics, Vol. 142, Issue 8 https://doi.org/10.1063/1.4908034	journal	February 2015
Surface hopping with a manifold of electronic states. III. Transients, broadening, and the Marcus picture Dou, Wenjie; Nitzan, Abraham; Subotnik, Joseph E. The Journal of Chemical Physics, Vol. 142, Issue 23 https://doi.org/10.1063/1.4922513	journal	June 2015
Nuclear Dynamics at Molecule–Metal Interfaces: A Pseudoparticle Perspective Galperin, Michael; Nitzan, Abraham The Journal of Physical Chemistry Letters, Vol. 6, Issue 24 https://doi.org/10.1021/acs.jpclett.5b02331	journal	November 2015
Quantum decoherence in mixed quantum‐classical systems: Nonadiabatic processes Bittner, Eric R.; Rossky, Peter J. The Journal of Chemical Physics, Vol. 103, Issue 18 https://doi.org/10.1063/1.470177	journal	November 1995
Coherent switching with decay of mixing: An improved treatment of electronic coherence for non-Born–Oppenheimer trajectories Zhu, Chaoyuan; Nangia, Shikha; Jasper, Ahren W. The Journal of Chemical Physics, Vol. 121, Issue 16 https://doi.org/10.1063/1.1793991	journal	January 2004
Mean-field dynamics with stochastic decoherence (MF-SD): A new algorithm for nonadiabatic mixed quantum/classical molecular-dynamics simulations with nuclear-induced decoherence Bedard-Hearn, Michael J.; Larsen, Ross E.; Schwartz, Benjamin J. The Journal of Chemical Physics, Vol. 123, Issue 23 https://doi.org/10.1063/1.2131056	journal	December 2005
Nonadiabatic excited-state molecular dynamics: Treatment of electronic decoherence Nelson, Tammie; Fernandez-Alberti, Sebastian; Roitberg, Adrian E. The Journal of Chemical Physics, Vol. 138, Issue 22 https://doi.org/10.1063/1.4809568	journal	June 2013
Second-Quantized Surface Hopping Akimov, Alexey V.; Prezhdo, Oleg V. Physical Review Letters, Vol. 113, Issue 15 https://doi.org/10.1103/PhysRevLett.113.153003	journal	October 2014
A Simple Solution to the Trivial Crossing Problem in Surface Hopping Wang, Linjun; Prezhdo, Oleg V. The Journal of Physical Chemistry Letters, Vol. 5, Issue 4 https://doi.org/10.1021/jz500025c	journal	January 2014
Mixed quantum-classical equilibrium in global flux surface hopping Sifain, Andrew E.; Wang, Linjun; Prezhdo, Oleg V. The Journal of Chemical Physics, Vol. 142, Issue 22 https://doi.org/10.1063/1.4922162	journal	June 2015
Fewest Switches Surface Hopping in Liouville Space Wang, Linjun; Sifain, Andrew E.; Prezhdo, Oleg V. The Journal of Physical Chemistry Letters, Vol. 6, Issue 19 https://doi.org/10.1021/acs.jpclett.5b01502	journal	September 2015
Decoherence Allows Model Reduction in Nonadiabatic Dynamics Simulations Trivedi, Dhara J.; Prezhdo, Oleg V. The Journal of Physical Chemistry A, Vol. 119, Issue 33 https://doi.org/10.1021/acs.jpca.5b05869	journal	August 2015
A classical analog for electronic degrees of freedom in nonadiabatic collision processes Meyera), Hans‐Dieter; Miller, William H. The Journal of Chemical Physics, Vol. 70, Issue 7 https://doi.org/10.1063/1.437910	journal	April 1979
Mapping approach to the semiclassical description of nonadiabatic quantum dynamics Thoss, Michael; Stock, Gerhard Physical Review A, Vol. 59, Issue 1 https://doi.org/10.1103/PhysRevA.59.64	journal	January 1999
Progress in the Theory of Mixed Quantum-Classical Dynamics Kapral, Raymond Annual Review of Physical Chemistry, Vol. 57, Issue 1 https://doi.org/10.1146/annurev.physchem.57.032905.104702	journal	May 2006
Matching-pursuit/split-operator-Fourier-transform simulations of excited-state nonadiabatic quantum dynamics in pyrazine Chen, Xin; Batista, Victor S. The Journal of Chemical Physics, Vol. 125, Issue 12 https://doi.org/10.1063/1.2356477	journal	September 2006
Electronically Nonadiabatic Dynamics via Semiclassical Initial Value Methods Miller, William H. The Journal of Physical Chemistry A, Vol. 113, Issue 8 https://doi.org/10.1021/jp809907p	journal	February 2009
Semiclassical nonadiabatic dynamics with quantum trajectories Rassolov, Vitaly A.; Garashchuk, Sophya Physical Review A, Vol. 71, Issue 3 https://doi.org/10.1103/PhysRevA.71.032511	journal	March 2005
Non-adiabatic molecular dynamics with complex quantum trajectories. II. The adiabatic representation Zamstein, Noa; Tannor, David J. The Journal of Chemical Physics, Vol. 137, Issue 22 https://doi.org/10.1063/1.4739846	journal	December 2012
Semiclassical Monte-Carlo approach for modelling non-adiabatic dynamics in extended molecules Gorshkov, Vyacheslav N.; Tretiak, Sergei; Mozyrsky, Dmitry Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3144	journal	July 2013
Kinetically constrained ring-polymer molecular dynamics for non-adiabatic chemical reactions Menzeleev, Artur R.; Bell, Franziska; Miller, Thomas F. The Journal of Chemical Physics, Vol. 140, Issue 6 https://doi.org/10.1063/1.4863919	journal	February 2014
Semiclassical Monte Carlo: A first principles approach to non-adiabatic molecular dynamics White, Alexander J.; Gorshkov, Vyacheslav N.; Wang, Ruixi The Journal of Chemical Physics, Vol. 141, Issue 18 https://doi.org/10.1063/1.4900988	journal	November 2014
Quantum-classical path integral: A rigorous approach to condensed phase dynamics Makri, Nancy International Journal of Quantum Chemistry, Vol. 115, Issue 18 https://doi.org/10.1002/qua.24975	journal	July 2015
Nonadiabatic Dynamics in Atomistic Environments: Harnessing Quantum-Classical Theory with Generalized Quantum Master Equations Pfalzgraff, William C.; Kelly, Aaron; Markland, Thomas E. The Journal of Physical Chemistry Letters, Vol. 6, Issue 23 https://doi.org/10.1021/acs.jpclett.5b02131	journal	November 2015
Communication: Fully coherent quantum state hopping Martens, Craig C. The Journal of Chemical Physics, Vol. 143, Issue 14 https://doi.org/10.1063/1.4933049	journal	October 2015
Multi-Electronic-State Molecular Dynamics: A Wave Function Approach with Applications Martinez, Todd J.; Ben-Nun, M.; Levine, R. D. The Journal of Physical Chemistry, Vol. 100, Issue 19 https://doi.org/10.1021/jp953105a	journal	January 1996
A semiclasical justification for the use of non-spreading wavepackets in dynamics calculations Herman, Michael F.; Kluk, Edward Chemical Physics, Vol. 91, Issue 1 https://doi.org/10.1016/0301-0104(84)80039-7	journal	November 1984
Matching-pursuit∕split-operator Fourier-transform simulations of nonadiabatic quantum dynamics Wu, Yinghua; Herman, Michael F.; Batista, Victor S. The Journal of Chemical Physics, Vol. 122, Issue 11 https://doi.org/10.1063/1.1881132	journal	March 2005
Time‐dependent approach to semiclassical dynamics Heller, Eric J. The Journal of Chemical Physics, Vol. 62, Issue 4 https://doi.org/10.1063/1.430620	journal	February 1975
Frozen Gaussians: A very simple semiclassical approximation Heller, Eric J. The Journal of Chemical Physics, Vol. 75, Issue 6 https://doi.org/10.1063/1.442382	journal	September 1981
Generalized Gaussian wave packet dynamics Huber, Daniel; Heller, Eric J. The Journal of Chemical Physics, Vol. 87, Issue 9 https://doi.org/10.1063/1.453647	journal	November 1987
Multidimensional variational Gaussian wave packet dynamics with application to photodissociation spectroscopy Coalson, Rob D.; Karplus, Martin The Journal of Chemical Physics, Vol. 93, Issue 6 https://doi.org/10.1063/1.458778	journal	September 1990
Gaussian wave-packet dynamics: Semiquantal and semiclassical phase-space formalism Pattanayak, Arjendu K.; Schieve, William C. Physical Review E, Vol. 50, Issue 5 https://doi.org/10.1103/PhysRevE.50.3601	journal	November 1994
Comparison of the propagation of semiclassical frozen Gaussian wave functions with quantum propagation for a highly excited anharmonic oscillator Kluk, Edward; Herman, Michael F.; Davis, Heidi L. The Journal of Chemical Physics, Vol. 84, Issue 1 https://doi.org/10.1063/1.450142	journal	January 1986
Quantum Dynamics with Gaussian Bases Defined by the Quantum Trajectories Gu, Bing; Garashchuk, Sophya The Journal of Physical Chemistry A, Vol. 120, Issue 19 https://doi.org/10.1021/acs.jpca.5b10029	journal	January 2016
Beyond Born-Oppenheimer Baer, Michael John Wiley & Sons, Inc. https://doi.org/10.1002/0471780081	book	January 2006
Path‐integral treatment of multi‐mode vibronic coupling Krempl, Stefan; Winterstetter, Manfred; Plöhn, Heiko The Journal of Chemical Physics, Vol. 100, Issue 2 https://doi.org/10.1063/1.467253	journal	January 1994
A Wavepacket−Path Integral Method for Curve-Crossing Dynamics Coalson, Rob D. The Journal of Physical Chemistry, Vol. 100, Issue 19 https://doi.org/10.1021/jp9531826	journal	January 1996
Nonadiabatic semiclassical scattering. I. Analysis of generalized surface hopping procedures Herman, Michael F. The Journal of Chemical Physics, Vol. 81, Issue 2 https://doi.org/10.1063/1.447708	journal	July 1984
Non-adiabatic molecular dynamics by accelerated semiclassical Monte Carlo White, Alexander J.; Gorshkov, Vyacheslav N.; Tretiak, Sergei The Journal of Chemical Physics, Vol. 143, Issue 1 https://doi.org/10.1063/1.4923473	journal	July 2015
Phase-corrected surface hopping: Correcting the phase evolution of the electronic wavefunction Shenvi, Neil; Subotnik, Joseph E.; Yang, Weitao The Journal of Chemical Physics, Vol. 135, Issue 2 https://doi.org/10.1063/1.3603447	journal	July 2011
Semiclassical Real-Time Tunneling by Multiple Spawning of Classical Trajectories Grossmann, Frank Physical Review Letters, Vol. 85, Issue 5 https://doi.org/10.1103/PhysRevLett.85.903	journal	July 2000
Time-Sliced Thawed Gaussian Propagation Method for Simulations of Quantum Dynamics Kong, Xiangmeng; Markmann, Andreas; Batista, Victor S. The Journal of Physical Chemistry A, Vol. 120, Issue 19 https://doi.org/10.1021/acs.jpca.5b12192	journal	February 2016
Matching-pursuit for simulations of quantum processes Wu, Yinghua; Batista, Victor S. The Journal of Chemical Physics, Vol. 118, Issue 15 https://doi.org/10.1063/1.1560636	journal	April 2003
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
Insights for Light-Driven Molecular Devices from Ab Initio Multiple Spawning Excited-State Dynamics of Organic and Biological Chromophores Martínez, Todd J. Accounts of Chemical Research, Vol. 39, Issue 2 https://doi.org/10.1021/ar040202q	journal	February 2006
Implementation of ab initio multiple spawning in the Molpro quantum chemistry package Levine, Benjamin G.; Coe, Joshua D.; Virshup, Aaron M. Chemical Physics, Vol. 347, Issue 1-3 https://doi.org/10.1016/j.chemphys.2008.01.014	journal	May 2008

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