Journal ArticleDOI
Molecular dynamics with electronic transitions
Reads0
Chats0
TLDR
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
More filters
Journal ArticleDOI
On the dynamics of coupled Bohmian and phase-space variables: a new hybrid quantum-classical approach.
Irene Burghardt,Gérard Parlant +1 more
TL;DR: Partial hydrodynamic moments are introduced, the dynamics of which is determined by a hierarchy of equations derived from the quantum Liouville equation, and a trajectory representation in a hybrid hydrod dynamic-Liouvillian phase space is introduced.
Journal ArticleDOI
Quasi-diabatic representations of adiabatic potential energy surfaces coupled by conical intersections including bond breaking: a more general construction procedure and an analysis of the diabatic representation.
Xiaolei Zhu,David R. Yarkony +1 more
TL;DR: Extensions of a promising method for representing the nuclear coordinate dependence of the energies, energy gradients, and derivative couplings of N(state) adiabatic electronic states coupled by conical intersections are described and analyzed.
Journal ArticleDOI
Nonadiabatic Ab Initio Molecular Dynamics with the Floating Occupation Molecular Orbital-Complete Active Space Configuration Interaction Method
Daniel Hollas,Lukáš Šištík,Edward G. Hohenstein,Edward G. Hohenstein,Todd J. Martínez,Todd J. Martínez,Petr Slavíček +6 more
TL;DR: In this article, the floating occupation molecular orbital complete active space configuration interaction (FOMO-CASCI) method is used to simulate photodynamics of three archetypal molecules in photodynamics.
Journal ArticleDOI
Modeling ultrafast exciton deactivation in oligothiophenes via nonadiabatic dynamics.
TL;DR: These data agree with the self-localization mechanism observed for poly(3-hexylthiophene) (P3HT) and shed light on the complex exciton relaxation dynamics occurring in π-conjugated oligomers of potential interest for optoelectronic applications.
Journal ArticleDOI
Semiclassical Tunneling Rates from Ab Initio Molecular Dynamics
M. Ben-Nun,Todd J. Martínez +1 more
TL;DR: In this article, a new ab initio semiclassical technique for investigating tunneling effects is proposed, which incorporates tunneling effect into first principles molecular dynamics and applies it to the intramolecular proton transfer in malonaldehyde.
References
More filters
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.
Related Papers (5)
Proton transfer in solution: Molecular dynamics with quantum transitions
Trajectory Surface Hopping Approach to Nonadiabatic Molecular Collisions: The Reaction of H+ with D2
John C. Tully,Richard K. Preston +1 more