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arXiv:physics/0507061

Quantum control of optical four-wave mixing with femtosecond w-3w laser pulses: coherent ac Stark nonlinear spectroscopy

Carles Serrat

Published Jul 7, 2005• 0 citations
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Abstract

The four-wave mixing produced with two ultrashort phase-locked w-3w laser pulses propagating coherently in a two-level system in the infrared spectral region is shown to depend on the pulses relative phase. The Maxwell-Bloch equations are solved beyond the rotating-wave approximation to account for field frequencies which are largely detuned from the atomic resonance. The relative phase dominating the efficiency of the coupling to the 5w anti-Stokes Raman component is determined by sign of the total ac Stark shift induced in the system, in such a way that the phase influence disappears precisely where the ac Stark effect due to both pulses is compensated. This fundamental quantum interference effect can be the basis for nonlinear ultrafast optical spectroscopy techniques.

DOI
10.48550/arxiv.physics/0507061

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The four-wave mixing produced with two ultrashort phase-locked w-3w laser pulses propagating coherently in a two-level system in the infrared spectral region is shown to depend on the pulses relative phase. The Maxwell-Bloch equations are solved beyond the rotating-wave approximation to account for field frequencies which are largely detuned from the atomic resonance. The relative phase dominating the efficiency of the coupling to the 5w anti-Stokes Raman component is determined by sign of the total ac Stark shift induced in the system, in such a way that the phase influence disappears precisely where the ac Stark effect due to both pulses is compensated. This fundamental quantum interference effect can be the basis for nonlinear ultrafast optical spectroscopy techniques.
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Coherent Stark nonlinear spectroscopy (CSNS) is a spectroscopic tool based on the cancellation of the phase sensitivity at frequency $5\ensuremath{\omega}$ in the ultrafast four-wave mixing (FWM) of two-color pulses with frequencies $\ensuremath{\omega}$ and $3\ensuremath{\omega}$. We develop a theory for CSNS in three-level V-type systems, and reveal that the mechanism for the phase sensitivity at $5\ensuremath{\omega}$ is the quantum interference between the two primary paths in the FWM of the $\ensuremath{\omega}$ and $3\ensuremath{\omega}$ fields. We find that the cancellation phenomenon occurs when the probability amplitude of one of these two primary pathways becomes equal to zero due to the competition effect between the two allowed transitions in the V-type system. The analytical expressions that describe the phase-sensitivity phenomenon and the conditions for its cancellation have been derived on the basis of perturbation theory, and are confirmed by numerical integration of the density matrix and Maxwell equations. We argue that CSNS can be utilized, in particular, for the investigation of optically dense media.