Quantum Trajectory Mean-Field Method for Nonadiabatic Dynamics in Photochemistry

Shen, Lin; Tang, Diandong; Xie, Binbin; Fang, Wei‐Hai

doi:10.1021/acs.jpca.9b03480

Cited by 13 publications

(8 citation statements)

References 126 publications

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“…46 However, the gradient of energy that includes the SOC interaction, which is required in the adiabatic representation, is a nontrivial problem and still unavailable in most quantum chemistry programs. On the basis of our recent work in QTMF-FSSH, 41 a generalized QTMF method to deal with both the IC and ISC processes is under development now.…”

Section: Role Of Ms-mei In Photochemistry Uncoveredmentioning

confidence: 99%

“…The decoherence effect should be considered at least approximately to address this issue. Recently we developed a quantum trajectory mean-field (QTMF) method to overcome the limitation of the original EMF scheme. − Inspired by the quantum measurement, the damping and random terms are introduced to the equation of motion of electronic density ρ( t ) The first term on the right-hand side is the same as that in the original EMF and TSH schemes, in which where d IJ is the derivative nonadiabatic coupling between state I and J as Ψ I and Ψ J are the electronic wave functions of the relevant states. The second term on the right-hand side of eq is a damping term that describes the decoherence effect using the Lindblad superoperator D as where The third one is a random term that accounts for the back-action effect of the nuclear motion to the electrons using the superoperator H as Here Γ IJ , γ IJ F , and rγ IJ ′ denote different types of decoherence rates and ξ IJ denotes white noise.…”

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confidence: 99%

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Role of Multistate Intersections in Photochemistry

Shen

Xie

et al. 2020

J. Phys. Chem. Lett.

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It has been generally accepted that the intersection of potential energy surfaces can facilitate nonadiabatic transitions and plays a crucial role in photochemistry. Although most previous studies have focused on the conical intersection of two electronic states, multistate intersections are common in polyatomic molecules, and their key roles in photochemistry have been uncovered by electronic structure calculations and nonadiabatic dynamics simulations. In this Perspective, the algorithms for searching two- or three-state intersections are first examined with an emphasis on the latest development in a general algorithm for location of multistate intersections. Then, we focus on intersystem crossing (ISC) that occurs in the region of multistate intersection, paying more attention to how the state-specific spin–orbit coupling interaction influences nonadiabatic ISC processes. Finally, the interweaving of nonadiabatic dynamics simulation and electronic structure calculation has been recognized as a correct way to ascertain the vital roles of multistate intersections in photochemical reactions.

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Section: Role Of Ms-mei In Photochemistry Uncoveredmentioning

confidence: 99%

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confidence: 99%

Role of Multistate Intersections in Photochemistry

Shen

Xie

et al. 2020

J. Phys. Chem. Lett.

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“…With the continuous social and economic development, the studies on quantum mechanics have become more and more in-depth gradually [ 1 – 5 ]. Quantum entanglement is a unique property of quantum mechanics and its essential application in the field of quantum information science, which has attracted the increasing attention of humans [ 6 – 8 ].…”

Section: Introductionmentioning

confidence: 99%

Quantum Decoherence Technique for Two Two-level Interacting Atomic Engineering in Dissipative Field

Shu

2022

Computational Intelligence and Neuroscience

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In order to improve the in-depth understanding and research on the dissipative field of atomic engineering, the research object of this paper is the dissipative field of atomic engineering. Through the engineering of two two-level interacting atoms as the background, an in-depth study of two two-level atoms is carried out, so the decoherence factor of two two-level atoms is obtained. In this paper, the numerical simulation calculation experiment of the dissipative field of atomic engineering is carried out, and the evolution of the quantum coherent oscillation of the dissipative field to the quantum decoherence is discussed. The results indicate that the dissipation coefficient and strength of the atom-light field interaction not only affect the oscillation of the quantum coherent evolution of atomic states but also the periodicity of the evolution. All preliminary results throw light on the nature of two-level interacting atoms in the dissipative field of atomic engineering, which also provides a reference value for related researchers.

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“…Note that apart from these strategies, a variety of other formalisms has been developed to describe non-Born-Oppenheimer dynamics, such as semiclassical approaches [40][41][42], including e.g. mapping approaches [43][44][45][46][47], quantum-classical Liouville methods [48][49][50], Bohmian dynamics [51][52][53][54] or quantum trajectory mean-field dynamics [55].…”

Section: Introductionmentioning

confidence: 99%

Excited-state dynamics of molecules with classically driven trajectories and Gaussians

2019

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Simulating the dynamics of a molecule initiated in an excited electronic state constitutes a rather challenging task for theoretical and computational chemistry, as such dynamics leads to a strong coupling between nuclear motion and electronic states, that is, a breakdown of the Born-Oppenheimer approximation. This New Views article proposes a brief overview on recent theoretical developments aiming at simulating the excited-state dynamics of molecules-nonadiabatic molecular dynamics-focusing in particular on strategies employing travelling basis functions to portray the dynamics of nuclear wavefunctions. We start by discussing the central equations for nonadiabatic molecular dynamics in a Born-Huang representation. We then propose a comparison between two commonly employed strategies to simulate the excited-state dynamics of molecular systems in their full configuration space, Ab Initio Multiple Spawning (AIMS) and Trajectory Surface Hopping (TSH). The equations of motion for the two techniques are compared and used to contrast their respective description of phenomena involving the decoherence of nuclear wavepackets. Some recent works and developments of the AIMS method are then summarised. This New Views article ends with a highlight on the Exact Factorisation of the molecular wavefunction and how this approach contrasts with the more conventional Born-Huang picture when it comes to the description of photophysical and photochemical processes.

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Quantum Trajectory Mean-Field Method for Nonadiabatic Dynamics in Photochemistry

Cited by 13 publications

References 126 publications

Role of Multistate Intersections in Photochemistry

Role of Multistate Intersections in Photochemistry

Quantum Decoherence Technique for Two Two-level Interacting Atomic Engineering in Dissipative Field

Excited-state dynamics of molecules with classically driven trajectories and Gaussians

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