Time-dependent methods of quantum dynamics: from few atoms to condensed matter

Abstract

An overview of theoretical work on quantum molecular dynamics done by our research group at the QTP of the University of Florida is presented. It covers aspects of molecular collisions using time-dependent wavefunctions and scattering propagators, partitioning methods describing resonance scattering and optical potentials, collisional time-correlation functions and related computational procedures for few-atom and many-atom collisions. Applications are mentioned on reactive atom–diatom collisions, atom–polyatomic and atom-surface collisional energy transfer. More recent work has dealt with the spectra and dynamics of many-atom systems in terms of a density operator (DOp) that combines quantal and statistical descriptions. A quantum–classical version of its equation of motion has been developed and applied to photodissociation. Further, work on dissipative dynamics introduces a reduced DOp to describe spectra and dynamics at surfaces and to account for fluctuation and dissipation phenomena, and mentions recent applications to surface photovoltages and photoinduced electron transfer at nanostructured surfaces.

Keywords:

• quantum dynamics
• resonance scattering
• reactive scattering
• Faddeev equations
• atom–diatom
• collisional time-correlation functions
• atom–polyatomic
• density operator
• quantum–classical dynamics
• vibrational relaxation
• photodissociation
• dissipative dynamics
• surfaces
• photovoltages

Acknowledgements

Work over many years at the QTP has been supported mainly by the NSF of the USA, and partly also by the USA NASA and Dreyfus Foundation. Recent computational work has also been partly supported by the High Performance Computation Center of the University of Florida.