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Abstract
A review of direct dynamics methods is given, focusing on their application to nonadiabatic photochemistryi.e. systems in which a conical intersection plays an important role. Direct dynamics simulations use electronic structure calculations to obtain the potential energy surface only as it is required 'onthefly'. This is in contrast to traditional methods that require the surface to be globally known as an analytic function before a simulation can be performed. The properties and abilities, with descriptions of calculations made, of the three main methods are compared: trajectory surface hopping (TSH), ab initio multiple spawning (AIMS), and variational multiconfiguration Gaussian wavepackets (vMCG). TSH is the closest to classical dynamics, is the simplest to implement, but is hard to converge, and even then not always accurate. AIMS solves the timedependent Schrodinger more rigorously, but as its basis functions follow classical trajectories again suffers from poor convergence. vMCG is harder to implement, but its basis functions do not follow classical trajectories and it converges much faster.
Original language  English 

Pages (fromto)  20772091 
Number of pages  15 
Journal  Molecular Physics 
Volume  106 
Issue number  1618 
DOIs  
Publication status  Published  1 Jan 2008 
Keywords
 quantum dynamics simulations
 nonadiabatic population transfer
 conical intersections
 direct dynamics
 theoretical photochemistry
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Dive into the research topics of 'Solving the timedependent Schrodinger equation for nuclear motion in one step: direct dynamics of nonadiabatic systems'. Together they form a unique fingerprint.Projects
 1 Finished

Development of a General Strategy of Optimal Control of Photochemical Reactions
Worth, G.
Engineering & Physical Science Research Council
1/05/08 → 30/04/10
Project: Research Councils