
doi: 10.1063/1.441786
The formalism of collective (Dicke-like) states and operators is used to describe the relaxation of the initially prepared state of a material in the presence of a laser field. The material states are shown to be expressible as minimum uncertainty wave packets formed from those special collective states that couple with the radiation field. It is shown that these coherent states of matter exhibit all the features that are usually attributed to ensemble averages of two-level molecules in a conventional statistical picture. However, there are new features in the quantum mechanical model when there are correlations among the molecules in the ensemble. The loss of minimum uncertainty characteristics of the wave packet correspnds to the transverse (T2) relaxation of the statistical model. Different types of T2 processes can be defined corresponding to the decay of different orders of coherence of the wave packet. Only for the case that the system decays in all orders of coherence do the quantum and statistical results coincide. There is expected to be a transverse relaxation that preserves one or more orders of coherence. Experiments are suggested that can test these ideas. A particular case of the formalism of collective states applies to molecular crystals and it provides a quantum mechanical picture of the dephasing of molecular excitons in terms of orders of coherence analogous to the usual manner of describing states of the radiation field.
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