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International Conference on Ultrafast Phenomena

Ac Stark-mediated quantum control with two-color pulses in Two- and Three-Level Systems

Carles Serrat, Yurii V. Loiko

Published Jan 1, 2006• 0 citations
Publisher

Abstract

The optical Stark shift of two-color pulses propagating in two- and three-level media is critical for the phase-sensitivity of four-wave mixing. We present a coherent control scheme for potential ultrafast nonlinear optical spectroscopy techniques.
DOI
10.1364/up.2006.tug15

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A critical dependence of the quantum interference on the optical Stark spectral shift produced when two-color laser pulses interact with a two-level medium is observed. The four-wave mixing of two ultrashort phase-locked $\ensuremath{\omega}\text{\ensuremath{-}}3\ensuremath{\omega}$ laser pulses propagating coherently in a two-level system depends on the pulses' relative phase. The phase dominating the efficiency of the coupling to the anti-Stokes Raman component is found to be determined by the sign of the total ac Stark shift induced in the system, in such a way that the phase sensitivity disappears precisely where the ac Stark effect due to both pulses is compensated. A coherent control scheme based on this phenomenon can be contemplated as the basis for nonlinear optical spectroscopy techniques.
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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.
Quantum control of the four-wave mixing produced by two-color $\ensuremath{\omega}\text{\ensuremath{-}}3\ensuremath{\omega}$ femtosecond laser pulses propagating in a two-level system is accomplished by varying the relative phase between the two laser pulses. The phase sensitivity of the spectral $5\ensuremath{\omega}$ anti-Stokes component is cancelled when the ac Stark shift produced by the $\ensuremath{\omega}$ and $3\ensuremath{\omega}$ pulses is compensated. We apply perturbation theory and provide simple analytical formulas for the phase-sensitivity cancellation in the $5\ensuremath{\omega}$ anti-Stokes component. We demonstrate that this quantum interference effect is robust against chirping of the pulses and show that asymmetric chirping results in phase-sensitive shaping of the four-wave mixing spectra.