Time dependence of collisionally induced coherent signals (A)

M. Dagenais

M. Dagenais

It is demonstrated that, in the presence of collisions and for nonresonant lasers, it is energetically possible to access resonantly excited states and induce a coherence between the states. This situation cannot arise in the absence of collisions if the starting state does not decay. This explains why, when collisions are introduced, a new signal can be generated in a wave-mixing type of experiment. The collisionally induced generation of a coherent signal is intimately related to the process of collisional redistribution. It is shown that all the collisionally induced coherent signals that have been reported up to now involve putting real populations in the excited states. This fact has not always been fully appreciated. No resonance between unpopulated states can exist. The time dependence of these new coherent signals is briefly discussed. In the case of a Raman resonance between equally populated states, it is pointed out that new coherent pathways of equal importance should be considered for explaining the experimental results. A new pressure-induced signal in four-wave mixing is also discussed. It is called "collisionally triggered two-photon quasiresonant coherent signal."

H. Tran, Frédéric Chaussard, N. Le Cong +3 more

In this paper, we present measurements and modeling of femtosecond time resolved coherent anti-Stokes Raman spectroscopy (CARS) signal in H(2)-N(2) mixtures at low densities. Three approaches have been used to model the CARS response. The first is the usual sum of Voigt profiles. In the second approach, the speed dependent Voigt profile is used. In the last approach, a model of the temporal CARS signal is developed, which takes into account the velocity changes induced by collisions and the speed dependence of the collisional parameters. The velocity changes are modeled using the Keilson and Storer memory function; the radiator speed dependences of the collisional parameters are determined from their temperature dependences. The results obtained are consistent with previous studies in the frequency domain, showing that the changes of the velocity have important effects for the H(2)/N(2) system in the Dicke narrowing density regime.

Yehiam Prior

Xihua, Yang Yang

Ruwang Sung