Negative Zero-Point-Energy Parameter in the Meyer–Miller Mapping Model for Nonadiabatic Dynamics

He, Xin; Gong, Zhihao; Wu, Baihua; Liu, J.

doi:10.1021/acs.jpclett.1c00232

Cited by 23 publications

(107 citation statements)

References 48 publications

(112 reference statements)

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“…• Classical molecular dynamics 67 • Molecular dynamics with electronic friction (MDEF) 43,44 • Ehrenfest molecular dynamics [7][8][9] • Fewest-switches surface hopping 49 • Ring polymer molecular dynamics (RPMD) 74,75 • Nonadiabatic RPMD (NRPMD) [35][36][37][38] • Centroid ring polymer surface hopping (RPSH) 14,15 • Centroid ring polymer Ehrenfest dynamics 76 • Extended classical mapping model (eCMM) 30,77 • Generalized spin mapping approach 78,79 C. Defining the Hamiltonian with NQCModels.jl…”

Section: B Performing Dynamicsmentioning

confidence: 99%

“…From the unified framework, the extended classical mapping model 30,77,122 uses the Meyer-Miller Hamiltonian:…”

Section: Extended Classical Mapping Model (Ecmm)mentioning

confidence: 99%

“…30 A recent investigation into the value of γ suggests the effect is minimal for reasonable values. 77 For the ring polymer simulations, 50 beads were used to obtain converged results. However, for the ring polymer Ehrenfest and RPSH, using only a single bead was capable of reproducing the same population dynamics.…”

Section: Simulation Detailsmentioning

confidence: 99%

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NQCDynamics.jl: A Julia Package for Nonadiabatic Quantum Classical Molecular Dynamics in the Condensed Phase

Gardner,

Douglas-Gallardo,

Stark

et al. 2022

Preprint

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Accurate and efficient methods to simulate nonadiabatic and quantum nuclear effects in high-dimensional and dissipative systems are crucial for the prediction of chemical dynamics in condensed phase. To facilitate effective development, code sharing and uptake of newly developed dynamics methods, it is important that software implementations can be easily accessed and built upon. Using the Julia programming language, we have developed the NQCDynamics.jl package which provides a framework for established and emerging methods for performing semiclassical and mixed quantum-classical dynamics in condensed phase. The code provides several interfaces to existing atomistic simulation frameworks, electronic structure codes, and machine learning representations. In addition to the existing methods, the package provides infrastructure for developing and deploying new dynamics methods which we hope will benefit reproducibility and code sharing in the field of condensed phase quantum dynamics. Herein, we present our code design choices and the specific Julia programming features from which they benefit. We further demonstrate the capabilities of the package on two examples of chemical dynamics in condensed phase: the population dynamics of the spin-boson model as described by a wide variety of semi-classical and mixed quantum-classical nonadiabatic methods and the reactive scattering of H 2 on Ag(111) using the Molecular Dynamics with Electronic Friction method. Together, they exemplify the broad scope of the package to study effective model Hamiltonians and realistic atomistic systems. Methods FSSH NRPMD Ehrenfest MDEF Classical Langevin eCMM Simulation Parameters Atoms Elements Masses Models Analytic model ASE calculator ML model Keywords Simulation cell Temperature Method extras Simulation Method (atoms , model; kwargs¡ ) { } FIG. 1. The user inputs required to define the parameters for a simulation. This diagram along with Figs. 2 and 3 was created using the Excalidraw 65 online tool.

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Section: B Performing Dynamicsmentioning

confidence: 99%

“…From the unified framework, the extended classical mapping model 30,77,122 uses the Meyer-Miller Hamiltonian:…”

Section: Extended Classical Mapping Model (Ecmm)mentioning

confidence: 99%

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NQCDynamics.jl: A Julia Package for Nonadiabatic Quantum Classical Molecular Dynamics in the Condensed Phase

Gardner,

Douglas-Gallardo,

Stark

et al. 2022

Preprint

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“…In the MMST mapping formalism, this parameter is viewed as the zero-point energy (ZPE) parameter. 23,54,55 In the su(N ) mapping formalism, it is the parameter related to the choice of r s . Nevertheless, Eq.…”

Section: Connections With the Mmst Mapping Formalismmentioning

confidence: 99%

“…The constraint of the radius r s ∈ (0, ∞) leads to a corresponding constraint for the ZPE parameter, γ ∈ (− 2 N , ∞). The negative values of the ZPE parameter has been proposed in the MMST framework, 55 and simply correspond to…”

Section: Connections With the Mmst Mapping Formalismmentioning

confidence: 99%

Non-adiabatic Dynamics using the Generators of the su(N) Lie Algebra

Bossion

Chowdhury

Huo

2022

Preprint

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We present the rigorous theoretical framework of the generalized spin mapping representation for non- adiabatic dynamics. This formalism is based on the generators of the su(N) Lie algebra to represent N discrete electronic states, thus preserving the size of the original Hilbert space in the state representation. We use the generalized spin coherent states representation and the Stratonovich-Weyl transform to describe these electronic spin-mapping variables in the continuous variables space. Wigner representation is used to de- scribe the nuclear degrees of freedom. Using the above representations, we derived an exact expression of the time-correlation function as well as the exact quantum Liouvillian. Making the linearization approximation, this exact Liouvillian is reduced to the Liouvillian of the recently proposed spin-Linearized Semi-Classical (spin-LSC) dynamics. These expressions lead to a self-consistent trajectory-based method to simulate non- adiabatic dynamics, which is based entirely on the generalized spin mapping formalism to treat the electronic states without the necessity of converting back to the cartesian mapping variables of the bosonic DOF (which are commonly referred to as the Meyer-Miller-Stock-Thoss mapping variables). The accuracy of this approach is tested with several challenging non-adiabatic model systems.

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New phase space formulations and quantum dynamics approaches

Shang

et al. 2022

WIREs Comput Mol Sci

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We report recent progress on the phase space formulation of quantum mechanics with coordinate-momentum variables, focusing more on new theory of (weighted) constraint coordinate-momentum phase space for discretevariable quantum systems. This leads to a general coordinate-momentum phase space formulation of composite quantum systems, where conventional representations on infinite phase space are employed for continuous variables. It is convenient to utilize (weighted) constraint coordinate-momentum phase space for representing the quantum state and describing nonclassical features. Various numerical tests demonstrate that new trajectorybased quantum dynamics approaches derived from the (weighted) constraint phase space representation are useful and practical for describing dynamical processes of composite quantum systems in gas phase as well as in condensed phase.

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Negative Zero-Point-Energy Parameter in the Meyer–Miller Mapping Model for Nonadiabatic Dynamics

Cited by 23 publications

References 48 publications

NQCDynamics.jl: A Julia Package for Nonadiabatic Quantum Classical Molecular Dynamics in the Condensed Phase

NQCDynamics.jl: A Julia Package for Nonadiabatic Quantum Classical Molecular Dynamics in the Condensed Phase

Non-adiabatic Dynamics using the Generators of the su(N) Lie Algebra

New phase space formulations and quantum dynamics approaches

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