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Chemical Physics Letters

Density matrix approach to optical dephasing in solids: Nonperturbative theory for dephasing processes

Игорь Сергеевич Осадько

Published Apr 1, 1990• 2 citations
Publisher
DOI
10.1016/0009-2614(90)85022-5

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A nonperturbative density-matrix formalism is used for the analysis of strong-field four-wave mixing, allowing the treatment of relaxation processes, including lifetime as well as dephasing. The combined role of proper dephasing and level saturation in the generation of extra resonances is studied. It is shown that, whereas in the absence of proper dephasing there is no pressure-induced resonance, there is always a nonzero contribution to the field-induced resonance. For increasing field intensity, a characteristic double saturation is predicted as a function of the field strength. The dependence on the various parameters is investigated, and the conditions under which these effects should be observable are identified.
An optical coherence phenomenon–power- dependent optical line narrowing—is reported for the first known time. The effect is observed in a low-temperature impurity- ion solid, Pr3+:LaF3, using a coherent transient technique for which saturation conditions prevail. Current theories of saturation, based on the optical Bloch equations or on rate equations, fail to explain our experimental results. We have therefore developed a microscopic coherence theory that introduces dephasing into the density-matrix equations of motion in a manner equally valid at low and high power and that agrees closely with our experimental results. This work thus represents the first reported observation of the failure of the optical Bloch equations in a low-temperature impurity-ion solid.