Quantum dynamics of solid Ne upon photo-excitation of a NO impurity: A Gaussian wave packet approach

Unn-Toc, Wesley; Uranga-Piña, Ll.; Meier, Christoph; Halberstadt, Nadine; Rubayo‐Soneira, J.

doi:10.1063/1.4739754

Cited by 2 publications

(1 citation statement)

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“…Other alternatives have been employed to generate a trajectory representation of the dynamics (in an effective phase space) from the time-dependent Schrödinger equation, usually based on the Dirac–Frenkel variational principle (for instance, the Gaussian Wave-Packet method, , or the Quantized Hamiltonian Dynamics − ). Conversely to the QCT method, the latter approaches allow one to partially incorporate quantum effects into the dynamical evolution of the system.…”

Section: Introductionmentioning

confidence: 99%

Effective Phase Space Representation of the Quantum Dynamics of Vibrational Predissociation of the ArBr₂(B,ν =16···25) Complex

et al. 2022

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We perform trajectory-based simulations of the vibrational predissociation of the ArBr2(B,ν=16···25) van der Waals triatomic complex, constrained to the T-shape geometry. To this aim, we employ a 2-fold mapping of the quantum dynamics into classical-like dynamics in an extended phase space. The effective phase space comprises two distinct sets of degrees of freedom, namely a collection of coupled harmonic oscillators and an ensemble of quantum trajectories. The time evolution of these variables represent bound and unbound motions of the quantum system, respectively. Quantum trajectories are propagated within the interacting trajectory representation. The comparison between the lifetimes of the predissociating complexes computed using the trajectory-based approach and the experimental results available for the target systems indicates that the present method is competitive with wavepacket propagation techniques. The competition between several simultaneous vibrational relaxation pathways was found to have a direct impact on the time scales of vibrational predissociation. Likewise, the analysis of the time evolution of the trajectories reveals the existence of regions in the effective phase space where transitions to vibrational states of higher energy are more likely to occur. The size and location of these regions influence the transient vibrational distributions and therefore the computed lifetimes. Furthermore, the mechanisms of energy redistribution along the dissociation coordinate are analyzed.

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Section: Introductionmentioning

confidence: 99%

Effective Phase Space Representation of the Quantum Dynamics of Vibrational Predissociation of the ArBr₂(B,ν =16···25) Complex

et al. 2022

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Variational mixed quantum/semiclassical simulation of dihalogen guest and rare-gas solid host dynamics

Cina

2014

The Journal of Chemical Physics

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A variational mixed quantum-semiclassical theory for the internal nuclear dynamics of a small molecule and the induced small-amplitude coherent motion of a low-temperature host medium is developed, tested, and used to simulate the temporal evolution of nonstationary states of the internal molecular and surrounding medium degrees of freedom. In this theory, termed the Fixed Vibrational Basis/Gaussian Bath (FVB/GB) method, the system is treated fully quantum mechanically while Gaussian wave packets are used for the bath degrees of freedom. An approximate time-dependent wave function of the entire model is obtained instead of just a reduced system density matrix, so the theory enables the analysis of the entangled system and bath dynamics that ensues following initial displacement of the internal-molecular (system) coordinate from its equilibrium position. The norm- and energy-conserving properties of the propagation of our trial wave function are natural consequences of the Dirac-Frenkel-McLachlan variational principle. The variational approach also stabilizes the time evolution in comparison to the same ansatz propagated under a previously employed locally quadratic approximation to the bath potential and system-bath interaction terms in the bath-parameter equations of motion. Dynamics calculations are carried out for molecular iodine in a 2D krypton lattice that reveal both the time-course of vibrational decoherence and the details of host-atom motion accompanying energy dissipation and dephasing. This work sets the stage for the comprehensive simulation of ultrafast time-resolved optical experiments on small molecules in low-temperature solids.

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Quantum dynamics of solid Ne upon photo-excitation of a NO impurity: A Gaussian wave packet approach

Cited by 2 publications

References 55 publications

Effective Phase Space Representation of the Quantum Dynamics of Vibrational Predissociation of the ArBr₂(B,ν =16···25) Complex

Effective Phase Space Representation of the Quantum Dynamics of Vibrational Predissociation of the ArBr₂(B,ν =16···25) Complex

Variational mixed quantum/semiclassical simulation of dihalogen guest and rare-gas solid host dynamics

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Quantum dynamics of solid Ne upon photo-excitation of a NO impurity: A Gaussian wave packet approach

Cited by 2 publications

References 55 publications

Effective Phase Space Representation of the Quantum Dynamics of Vibrational Predissociation of the ArBr2(B,ν =16···25) Complex

Effective Phase Space Representation of the Quantum Dynamics of Vibrational Predissociation of the ArBr2(B,ν =16···25) Complex

Variational mixed quantum/semiclassical simulation of dihalogen guest and rare-gas solid host dynamics

Contact Info

Product

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About

Effective Phase Space Representation of the Quantum Dynamics of Vibrational Predissociation of the ArBr₂(B,ν =16···25) Complex

Effective Phase Space Representation of the Quantum Dynamics of Vibrational Predissociation of the ArBr₂(B,ν =16···25) Complex