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Collisionally induced four-wave mixing in the nonimpact regime

M. Rosenbluh, Nissim Asida

Published May 21, 1990• 0 citations
OpenAlex

Abstract

The relationship between collisional physics and nonlinear optics in the form of four-wave mixing (FWM) is well established.1 The counterintuitive idea that collisions which are coherence destroying processes can nonetheless lead to a nonlinear coherent process such as FWM has been attributed to the destructive interference between, two different quantum pathways leading to the generation of the fourth wave.

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Collisionally Induced Four Wave Mixing: Breakdown of the Impact Approximation

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The relationship between collisional physics and nonlinear optics in the form of four-wave mixing (FWM) is well established.1 The counterintuitive idea that collisions which are coherence destroying processes can nonetheless lead to a nonlinear coherent process such as FWM has been attributed to the destructive interference between, two different quantum pathways leading to the generation of the fourth wave.
Coherent signals induced by fundamentally incoherent phenomena through a four-wave mixing process are among the most intriguing and subtle effects in nonlinear spectroscopy. These effects were initially observed by Bloembergen and his co-workers in the form of pressure-induced extra resonances in four-wave mixing. Using standard perturbance techniques based on the optical Bloch equations, they suggested that these collision induced resonances were the result of a destruction of the destructive interference existent between two alternate time-ordered pathways. Subsequently, Prior et al realised that fluctuations in the incident radiation fields could play essentially the same role as the collisionally induced dephasing. In practice, of course, both collisional dephasing and field fluctuations are present in a typical atomic vapor pulsed four-wave mixing experiment. If the timescales governing these two effects approach one another, one can expect to gain valuable new insight into this fascinating process of incoherently inducing a coherent signal
We analyze a lifetime-broadened four-state four-wave-mixing (FWM) scheme in the ultraslow propagation regime and show that the generated FWM field can acquire the same group velocity and pulse shape as those of an ultraslow pump field. We show that a new type of induced transparency resulted from multiphoton destructive interference that significantly reduced the pump field loss. Such induced transparency based on multphoton destructive interference may have important applications in other nonlinear optical processes.
A unified theory of coherent and incoherent resonance scattering of radiation in gases is presented. Expressions for the scattering rates in collisional redistribution and four-wave mixing (FWM) are obtained, starting from a microscopic formulation based on the Liouville--von Neumann equation. The derivation reemphasizes the point that coherent scattering depends on a product of scattering amplitudes at two separate points in the gas. The theory is extended to the nonimpact domain in which frequency detunings exceed the inverse duration of a single collision, taking into account intracollisional effects. Expressions are given in the so-called quasistatic limit (of semiclassical Franck-Condon transitions) for situations in which one or more radiative transitions occur during the collision. An extension of double-sided diagrams to collision-induced processes is introduced, and is used to illustrate the various phenomena described. Applications are suggested to the study of molecular dynamics, making use of the spectral features of FWM outside the impact domain. Investigations of long-range correlation effects, involving laser fluctuations, or cooperative excitations in dense fluids (utilizing the two-point nature of FWM), are also discussed.