Simulation of quantum-classical dynamics by surface-hopping trajectories

2007 ◽  
pp. 131-143
Author(s):  
Hyojoon Kim ◽  
Raymond Kapral
Keyword(s):  
Classical Dynamics ◽  
Surface Hopping

scholarly journals Study of the Vibrational Predissociation of the NeBr2 Complex by Computational Simulation Using the Trajectory Surface Hopping Method

Mathematics ◽  
2020 ◽  
Vol 8 (11) ◽  
pp. 2029
Author(s):  
Ernesto García-Alfonso ◽  
Maykel Márquez-Mijares ◽  
Jesús Rubayo-Soneira ◽  
Nadine Halberstadt ◽  
Kenneth C. Janda ◽  
...  
Keyword(s):  
Energy Surface ◽  
Computational Simulation ◽  
Kinetic Mechanism ◽  
Experimental Methods ◽  
Classical Dynamics ◽  
Vibrational States ◽  
Surface Hopping ◽  
Vibrational Predissociation ◽  
New Information ◽  
Rotational Distribution

The vibrational predissociation of NeBr2 has been studied using a variety of theoretical and experimental methods, producing a large number of results. It is therefore a useful system for comparing different theoretical methods. Here, we apply the trajectory surface hopping (TSH) method that consists of propagating the dynamics of the system on a potential energy surface (PES) corresponding to quantum molecular vibrational states with possibility of hopping towards other surfaces until the van der Waals bond dissociates. This allows quantum vibrational effects to be added to a classical dynamics approach. We have also incorporated the kinetic mechanism for a better compression of the evolution of the complex. The novelty of this work is that it allows us to incorporate all the surfaces for (v=16,17,…,29) into the dynamics of the system. The calculated lifetimes are similar to those previously reported experimentally and theoretically. The rotational distribution, the rotational energy and jmax are in agreement with other works, providing new information for this complex.

Global Flux Surface Hopping Approach for Mixed Quantum-Classical Dynamics

2014 ◽  
Vol 10 (9) ◽  
pp. 3598-3605 ◽  
Author(s):  
Linjun Wang ◽  
Dhara Trivedi ◽  
Oleg V. Prezhdo
Keyword(s):  
Classical Dynamics ◽  
Surface Hopping ◽  
Flux Surface

scholarly journals Simulation of Excitation by Sunlight in Mixed Quantum-Classical Dynamics

2020 ◽  
Author(s):  
Mario Barbatti
Keyword(s):  
Solar Radiation ◽  
Initial Conditions ◽  
Solar Irradiation ◽  
Test Case ◽  
Classical Dynamics ◽  
Nonadiabatic Dynamics ◽  
Ensemble Averaging ◽  
Surface Hopping ◽  
Thermal Light ◽  
Long Timescales

This paper proposes a method to simulate nonadiabatic dynamics initiated by thermal light, including solar radiation, in the frame of mixed quantum-classical (MQC) methods, like surface hopping. The method is based on the Chenu-Brumer approach, which treats the thermal radiation as an ensemble of coherent pulses. It is composed of three steps, 1) sampling initial conditions from a broad blackbody spectrum, 2) propagation of the dynamics using conventional methods, and 3) ensemble averaging considering the field and realization time of the pulses. The application of MQC dynamics with pulse ensemble (MQC-PE) to a model system of nucleic acid photophysics showed the emergence of a stationary excited-state population. In another test case, modeling retinal isomerization, MQC-PE revealed that even when the underlying photophysics occurs within 200 fs, it may take tens of microseconds of continuous solar irradiation to activate a molecule photochemically. Such emergent long timescales may impact our understanding of biological and technological phenomena occurring under solar radiation.

Mixed quantum-classical dynamics for charge transport in organics

2015 ◽  
Vol 17 (19) ◽  
pp. 12395-12406 ◽  
Author(s):  
Linjun Wang ◽  
Oleg V. Prezhdo ◽  
David Beljonne
Keyword(s):  
Charge Transport ◽  
Mean Field ◽  
Classical Dynamics ◽  
Surface Hopping

This perspective summaries recent progresses of using mean field and surface hopping mixed quantum-classical dynamics for charge transport in organics.

scholarly journals Simulation of Excitation by Sunlight in Mixed Quantum-Classical Dynamics

2020 ◽  
Author(s):  
Mario Barbatti
Keyword(s):  
Solar Radiation ◽  
Initial Conditions ◽  
Solar Irradiation ◽  
Test Case ◽  
Classical Dynamics ◽  
Nonadiabatic Dynamics ◽  
Ensemble Averaging ◽  
Surface Hopping ◽  
Thermal Light ◽  
Long Timescales

This paper proposes a method to simulate nonadiabatic dynamics initiated by thermal light, including solar radiation, in the frame of mixed quantum-classical (MQC) methods, like surface hopping. The method is based on the Chenu-Brumer approach, which treats the thermal radiation as an ensemble of coherent pulses. It is composed of three steps, 1) sampling initial conditions from a broad blackbody spectrum, 2) dynamics propagation using conventional methods, and 3) ensemble averaging considering the field and realization time of the pulses. The application of MQC dynamics with pulse ensemble (MQC-PE) to a model system of nucleic acid photophysics showed the emergence of a steady excited-state population. In another test case, modeling retinal photophysics, MQC-PE predicted that although the photoisomerization occurs within 200 fs, it may take tens of microseconds of continuous solar irradiation to photoactivate a single retinal. Such emergent long timescales may impact our understanding of biological and technological phenomena occurring under solar radiation.

scholarly journals Simulation of Excitation by Sunlight in Mixed Quantum-Classical Dynamics

2020 ◽  
Author(s):  
Mario Barbatti
Keyword(s):  
Solar Radiation ◽  
Initial Conditions ◽  
Solar Irradiation ◽  
Test Case ◽  
Classical Dynamics ◽  
Nonadiabatic Dynamics ◽  
Ensemble Averaging ◽  
Surface Hopping ◽  
Thermal Light ◽  
Long Timescales

<div>This paper proposes a method to simulate nonadiabatic dynamics initiated by thermal light, including solar radiation, in the frame of mixed quantum-classical (MQC) methods, like surface hopping. The method is based on the Chenu-Brumer approach, which treats the thermal radiation as an ensemble of coherent pulses. It is composed of three steps, 1) sampling initial conditions from a broad blackbody spectrum, 2) dynamics propagation using conventional methods, and 3) ensemble averaging considering the field and realization time of the pulses. The application of MQC dynamics with pulse ensemble (MQC-PE) to a model system of nucleic acid photophysics showed the emergence of a steady excited-state population. In another test case, modeling retinal photophysics, MQC-PE predicted that although the photoisomerization occurs within 200 fs, it may take tens of microseconds of continuous solar irradiation to photoactivate a single retinal. Such emergent long timescales may impact our understanding of biological and technological phenomena occurring under solar radiation.</div><div><br></div><div>Final version at JCTC, DOI: <a href="https://doi.org/10.1021/acs.jctc.0c00501" rel="noopener noreferrer" target="_blank">10.1021/acs.jctc.0c00501</a></div>

Quantum simulations

2017 ◽  
Author(s):  
Michael P. Allen ◽  
Dominic J. Tildesley
Keyword(s):  
Ab Initio ◽  
Quantum Monte Carlo ◽  
Degrees Of Freedom ◽  
Small Region ◽  
Time Correlation ◽  
Ab Initio Molecular Dynamics ◽  
Classical Dynamics ◽  
Integral Methods ◽  
Quantum Time ◽  
Low Mass

This chapter covers the introduction of quantum mechanics into computer simulation methods. The chapter begins by explaining how electronic degrees of freedom may be handled in an ab initio fashion and how the resulting forces are included in the classical dynamics of the nuclei. The technique for combining the ab initio molecular dynamics of a small region, with classical dynamics or molecular mechanics applied to the surrounding environment, is explained. There is a section on handling quantum degrees of freedom, such as low-mass nuclei, by discretized path integral methods, complete with practical code examples. The problem of calculating quantum time correlation functions is addressed. Ground-state quantum Monte Carlo methods are explained, and the chapter concludes with a forward look to the future development of such techniques particularly to systems that include excited electronic states.

Nonadiabatic molecular dynamics simulation for the ultrafast photoisomerization of dMe-OMe-NAIP based on TDDFT on-the-fly potential energy surfaces

2021 ◽  
Vol 23 (9) ◽  
pp. 5236-5243
Author(s):  
Ying Hu ◽  
Chao Xu ◽  
Linfeng Ye ◽  
Feng Long Gu ◽  
Chaoyuan Zhu
Keyword(s):  
Molecular Dynamics ◽  
Molecular Dynamics Simulation ◽  
Potential Energy ◽  
Potential Energy Surfaces ◽  
Dynamics Simulation ◽  
Surface Hopping ◽  
Nonadiabatic Molecular Dynamics ◽  
Energy Surfaces

Global switching on-the-fly trajectory surface hopping molecular dynamics simulation was performed on the accurate TD-B3LYP/6-31G* potential energy surfaces for E-to-Z and Z-to-E photoisomerization of dMe-OMe-NAIP up to S1(ππ*) excitation.

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