Quantum many-body time correlations from semiclassical molecular dynamics

Mikhael Ovchinnikov; Vartkess Ara Apkarian

doi:10.1117/12.306134

24 April 1998 Quantum many-body time correlations from semiclassical molecular dynamics

Mikhael Ovchinnikov, Vartkess Ara Apkarian

Proceedings Volume 3273, Laser Techniques for Condensed-Phase and Biological Systems; (1998) https://doi.org/10.1117/12.306134
Event: Optoelectronics and High-Power Lasers and Applications, 1998, San Jose, CA, United States

Abstract

The mixed-order semiclassical molecular dynamics method is used for the calculation of quantum time correlation functions in extended systems. The method allows the consistent treatment of a selected number of degrees of freedom to second-order in the stationary phase approximation through the Herman and Kluk propagator, while the rest of the system is treated to zeroth-order, using frozen Gaussians. The formulation is applied to calculate the absorption spectrum, of the B $IMP X transition of Cl₂ isolated in solid Ar, a spectrum that shows zero-phonon lines and phonon sidebands with relative intensities that depend on the excited state vibrational level. The explicit simulation of quantum time correlation functions of the system consisting of 321 degrees of freedom, reproduces the spectrum and allows its interpretation in terms of the underlying molecular motions.IN order to extend the semiclassical methods to longer timescale a new extension of Herman-Kluk propagator is developed, which combines classical propagation of trajectories for length where the initial value propagator remains accurate, followed by Monte-Carlo regeneration of the ensemble of trajectories and continuation of propagation. This new method is tested for the calculation of long time dynamics in a 1D Morse oscillator.

Citation Download Citation

Mikhael Ovchinnikov and Vartkess Ara Apkarian "Quantum many-body time correlations from semiclassical molecular dynamics", Proc. SPIE 3273, Laser Techniques for Condensed-Phase and Biological Systems, (24 April 1998); https://doi.org/10.1117/12.306134

ACCESS THE FULL ARTICLE

INSTITUTIONAL
Select your institution to access the SPIE Digital Library.

SELECT YOUR INSTITUTION

PERSONAL
Sign in with your SPIE account to access your personal subscriptions or to use specific features such as save to my library, sign up for alerts, save searches, etc.

PERSONAL SIGN IN

No SPIE Account? Create one

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