Theory and simulation of condensed-phase ultrafast dynamics

Arnaldo Donoso; Craig C. Martens

doi:10.1117/12.306126

Abstract

In this paper, we describe a new approach to simulating many-body molecular dynamics on coupled electronic surfaces. The method is based on a semiclassical limit of the quantum Louisville equation, which yields equations of motion for classical-like distribution functions describing both nuclear probability densities on the coupled surfaces and the coherences between the electronic states. The Hamiltonian dynamics underlying the evolution of these distributions is augmented by nonclassical source and sink terms, which allow the flow of probability between the coupled surfaces and the corresponding formation and decay of electronic coherences. We show that this approach reproduces the familiar Landau-Zehnder transition probability in the limit of weak electronic coupling. In addition, we describe a trajectory-based implementation in the context of a conventional molecular dynamics simulation.

Citation Download Citation

Arnaldo Donoso, Arnaldo Donoso, Craig C. Martens, Craig C. Martens, } "Theory and simulation of condensed-phase ultrafast dynamics", Proc. SPIE 3273, Laser Techniques for Condensed-Phase and Biological Systems, (24 April 1998); doi: 10.1117/12.306126; https://doi.org/10.1117/12.306126

ACCESS THE FULL ARTICLE

PERSONAL SIGN IN
Full access may be available with your subscription

Email or Username Forgot your username?

Password Forgot your password?

Show

Remember Email/Username on this computer

Remember Password

No SPIE account? Create an account
or Institutional Sign In via Shibboleth

PURCHASE THIS CONTENT

SUBSCRIBE TO DIGITAL LIBRARY

50 downloads per 1-year subscription

Members: $195

Non-members: $335 ADD TO CART

25 downloads per 1 - year subscription

Members: $145

Non-members: $250 ADD TO CART

PURCHASE SINGLE ARTICLE

Includes PDF, HTML & Video, when available

Members: $14.40

Non-members: $18.00 ADD TO CART

Show All Keywords

Keywords/Phrases

Search In:

Publication Years