Journal ArticleDOI
Molecular dynamics with electronic transitions
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In this article, a method for carrying out molecular dynamics simulations of processes that involve electronic transitions is proposed, where the time dependent electronic Schrodinger equation is solved self-consistently with the classical mechanical equations of motion of the atoms.Abstract:
A method is proposed for carrying out molecular dynamics simulations of processes that involve electronic transitions. The time dependent electronic Schrodinger equation is solved self‐consistently with the classical mechanical equations of motion of the atoms. At each integration time step a decision is made whether to switch electronic states, according to probabilistic ‘‘fewest switches’’ algorithm. If a switch occurs, the component of velocity in the direction of the nonadiabatic coupling vector is adjusted to conserve energy. The procedure allows electronic transitions to occur anywhere among any number of coupled states, governed by the quantum mechanical probabilities. The method is tested against accurate quantal calculations for three one‐dimensional, two‐state models, two of which have been specifically designed to challenge any such mixed classical–quantal dynamical theory. Although there are some discrepancies, initial indications are encouraging. The model should be applicable to a wide variety of gas‐phase and condensed‐phase phenomena occurring even down to thermal energies.read more
Citations
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Journal ArticleDOI
Quantum-classical Liouville description of multidimensional nonadiabatic molecular dynamics
TL;DR: In this article, an efficient Monte Carlo implementation of the quantum-classical Liouville equation is proposed to describe multidimensional nonadiabatic processes in complex molecular systems.
Journal ArticleDOI
Nonradiative Electron--Hole Recombination Rate Is Greatly Reduced by Defects in Monolayer Black Phosphorus: Ab Initio Time Domain Study.
TL;DR: The reduced electron-phonon coupling and increased bandgap in MBP-DV rationalize slower recombination in this material, suggesting that electron- phonon energy losses inMBP can be minimized by creating suitable defects in semiconductor device material.
Journal ArticleDOI
Nonadiabatic Molecular Dynamics for Thousand Atom Systems: A Tight-Binding Approach toward PYXAID.
TL;DR: An efficient approach for simulating nonadiabatic molecular dynamics of large systems in the framework of the self-consistent charge density functional tight binding (SCC-DFTB) method, capable of treating accurately and efficiently excitation dynamics in large, realistic nanoscale materials, employing modest computational resources.
Journal ArticleDOI
Unravelling the details of vitamin D photosynthesis by non-adiabatic molecular dynamics simulations
TL;DR: The results show that LR-TDDFT-SH is a highly valuable tool for studying the photochemistry of moderately large systems, even though challenges remain in the vicinity of conical intersections.
Journal ArticleDOI
The treatment of classically forbidden electronic transitions in semiclassical trajectory surface hopping calculations
TL;DR: In this article, a family of four weakly coupled electronically nonadiabatic bimolecular model photochemical systems is presented, and the quantum probabilities for electronic non-deexcitation and non-reactive deexcitation events are found to be highly classically forbidden for these systems.
References
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Journal ArticleDOI
Trajectory Surface Hopping Approach to Nonadiabatic Molecular Collisions: The Reaction of H+ with D2
John C. Tully,Richard K. Preston +1 more
TL;DR: In this article, an extension of the classical trajectory approach is proposed that may be useful in treating many types of nonadiabatic molecular collisions, where nuclei are assumed to move classically on a single potential energy surface until an avoided surface crossing or other region of large NDE coupling is reached.
Journal ArticleDOI
A fourier method solution for the time dependent Schrödinger equation as a tool in molecular dynamics
Dan Kosloff,Ronnie Kosloff +1 more
TL;DR: In this paper, a new method is presented for the solution of the time dependent SchrBdinger equation in its application to physical and chemical molecular phenomena, which is based on discretizing space and time on a grid, and using the Fourier method to produce both spatial derivatives, and second order differencing for time derivatives.
Book
Mathematical methods for digital computers
TL;DR: This is the book that many people in the world waiting for to publish, mathematical methods for digital computers, and the book lovers are really curious to see how this book is actually.
BookDOI
Dynamics of Molecular Collisions
TL;DR: In this paper, the potential energy surfaces and their effect on collision processes are discussed. But the authors focus on the nonadiabatic processes in collision theory and not on the classical trajectories of trajectories.
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