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Chemical Physics Letters

Optical dephasing of small and large molecules: coherent oscillations of emitting molecules

Thomas E. Orlowski, K. E. Jones, Ahmed H. Zewail

Published Aug 1, 1977• 18 citations
Publisher
DOI
10.1016/0009-2614(77)80677-5

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The evolution of a small spherical system of many harmonic oscillators, initially in a coherent superradiant state, is considered. The dipole oscillators interact via their mutual fields, both longitudinal and transverse, including both radiation- and near-zone contributions. In principle, this interaction can dephase the vibration of oscillators and thereby decrease or eliminate the coherent superradiant contribution to the emitted radiation. It is shown, however, that if the system is sufficiently small, this dephasing makes only small corrections to the decay of the initial state. Thus the emission of a superradiant pulse and cooperative radiative decay are major processes in the system.
Free induction decay is the coherent emission of light that follows the excitation of a medium by a short pulse. During the coherence time of the medium (T2), all atoms/molecules oscillate ’in unison’, forming a macroscopic dipole that emits light as a large coherent antenna, ’broadcasting’ information on the quantum state of the atoms/molecules and its dynamical evolution. We present an optical oscillator, where the coherent dipole emission from a dynamical wave-packet, is amplified beyond the lasing threshold. By placing a molecular medium in an optical cavity that is synchronously pumped by a frequency comb laser, emission from the excitation of one pump pulse can return to the medium with subsequent pump pulses, allowing stimulated amplification. When threshold is crossed, a broadband coherent oscillation is achieved, bearing information on the coherent wave-packet dynamics inside the medium. We analyze theoretically this coherent Raman oscillator and simulate thoroughly it’s dynamics under most realistic conditions for a model system of Alkali dimers (Li2,K2) in a hot gas cell (100−300 ◦ C), showing that the oscillation condition is well within reach. If realized, this coherent Raman oscillator can open avenues for precise measurement of vibrational dynamics in molecules.
We discuss the Rabi splitting and Rabi oscillation of excitons in semiconductor quantum dots and clarify the fundamental physics and new characteristic features. These coherent optical phenomena are not restricted to semiconductor quantum dots and the predicted features would be observed also in atoms and molecules. The universality of the phenomena ensures the possibility for application to quantum state control and quantum information processing by optical means. We discuss briefly the mechanisms of exciton dephasing in semiconductor quantum dots in conjunction with recent observations of the lifetime-limited exciton dephasing time and show that the pure dephasing rate is very small but is not vanishing even at zero Kelvin.