H. Tang et al., A GENERALIZED-APPROACH TO THE CONTROL OF THE EVOLUTION OF A MOLECULAR-SYSTEM, The Journal of chemical physics, 104(14), 1996, pp. 5457-5471
The theory of active control of molecular motion by use of shaped lase
r pulses is developed emphasizing the role of interference and using t
hermodynamic analogies. Attention is focused on the control of the dyn
amics in a system with n states coupled by radiation, and the phase re
lations which generate particular control schemes are derived. Among t
he new results reported is an optimal control scheme which constrains
the value of the phase. The n-state model can be considered to represe
nt a molecule with n electronic potential energy surfaces and an arbit
rary number of degrees of freedom or as the skeleton spectrum of syste
m where each level in the spectrum can be associated with a specific s
et of quantum numbers for all of the degrees of freedom. We show how t
he control of the dynamics of an n-state molecule can be represented i
n terms of the control of the dynamics of a precisely defined surrogat
e fewer state system. This reduction is illustrated by use of a surrog
ate two state system to describe the dynamics of population transfer i
n a three state system. (C) 1996 American Institute of Physics.