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Physical Review Letters

Femtosecond Phase-and-Polarization Control for Background-Free Coherent Anti-Stokes Raman Spectroscopy

Dan Oron, Nirit Dudovich, Yaron R. Silberberg

Published May 30, 2003• 245 citations
Publisher

Abstract

Phase-and-polarization coherent control is applied to control the nonlinear response of a quantum system. We use it to obtain high-resolution background-free single-pulse coherent anti-Stokes Raman spectra. The ability to control both the spectral phase and the spectral polarization enables measurement of a specific off-diagonal susceptibility tensor element while exploiting the different spectral response of the resonant Raman signal and the nonresonant background to achieve maximal background suppression.

DOI
10.1103/physrevlett.90.213902

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Phase-and-polarization coherent control is applied to control the nonlinear response of a quantum system. We use it to obtain high-resolution background-free single-pulse coherent anti-Stokes Raman spectra. The ability to control both the spectral phase and the spectral polarization enables measurement of a specific off-diagonal susceptibility tensor element while exploiting the different spectral response of the resonant Raman signal and the nonresonant background to achieve maximal background suppression.
Spatial symmetries inherent to tight focus optical beams are applied to control the field phase generated at interfaces in nonlinear optical processes. We use these symmetries to obtain a background-free pure Raman spectrum in coherent anti-Stokes Raman scattering spectroscopy from a resonant medium forming a transverse interface with a nonresonant medium. We demonstrate that the nonresonant medium acts as a local oscillator with which the Raman spectrum is measured in heterodyne detection. This method is relevant to remove the nonresonant background in other third-order resonant processes excited with focused beams.
Unlike spontaneous Raman effect, nonlinear Raman scattering generates fields with a well-defined phase, allowing Raman signals from individual scatterers to add up into a highly directional, high-brightness coherent beam. Here, we show that the phase of coherent Raman scattering can be accurately controlled and finely tuned by using spectrally and temporally tailored optical driver fields. In our experiments, performed with spectrally optimized phase-tunable laser pulses, such a phase control is visualized through the interference of the coherent Raman signal with the field resulting from nonresonant four-wave mixing. This interference gives rise to Fano-type profiles in the overall nonlinear response measured as a function of the delay time between the laser pulses, featuring a well-resolved destructive-interference dip on the dark side of the Raman peak. This phase-control strategy is shown to radically enhance the coherent response from weak Raman modes, thus helping confront long-standing challenges in nonlinear Raman imaging and microspectroscopy.
In spectroscopy, the fingerprint of a substance is usually comprised of a sequence of spectral lines with characteristic frequencies and strengths. Identification of substances often involves postprocessing, where the measured spectrum is compared with tabulated fingerprint spectra. Here we suggest a scheme for nonlinear spectroscopy, where, through coherent control of the nonlinear process, the information from the entire spectrum can be practically collected into a single coherent entity. We apply this for all-optical analysis of coherent Raman spectra and demonstrate enhanced detection and effective background suppression using coherent processing.
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.
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.