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Optics Letters

High-contrast interferometry based on anti-Stokes stimulated Raman scattering with broadband and narrow-band quasi-continuous-wave laser light

Darin J. Ulness, Michael J. Stimson, A. C. Albrecht

Published Apr 1, 1997• 3 citations
Publisher

Abstract

Two versions of an anti-Stokes stimulated Raman scattering (SRS) experiment are presented, one with narrow-band light, the other with broadband light. The interferograms exhibit, at optical periods, alternation between complete signal extinction and high signal intensity with much higher contrast than seen in ordinary linear interferometry. Furthermore, for broadband excitation, the envelope of the high-contrast SRS interferogram is limited to an ultrashort time period. Possible applications of such signals for use as switches or logic gates are discussed.

DOI
10.1364/ol.22.000433

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Annual Meeting Optical Society of America•Jan 1, 1988•0 citations
Two versions of an anti-Stokes stimulated Raman scattering (SRS) experiment are presented, one with narrow-band light, the other with broadband light. The interferograms exhibit, at optical periods, alternation between complete signal extinction and high signal intensity with much higher contrast than seen in ordinary linear interferometry. Furthermore, for broadband excitation, the envelope of the high-contrast SRS interferogram is limited to an ultrashort time period. Possible applications of such signals for use as switches or logic gates are discussed.
In the coherent anti-Stokes Raman scattering process, the spectrum of the generated optical phonon depends on the degree of temporal correlation between the pump laser field and the Stokes field. When the two fields are strongly correlated, such as when the Stokes field is generated with stimulated Raman scattering (SRS), the spectral shape of the optical phonon is found experimentally and theoretically to be the same as the gain-narrowed Raman line shape because the laser phase fluctuations cancel out totally, leaving only the collisional noise in the SRS process. When the two fields are uncorrelated, the shape of the optical-phonon spectrum is found to be the same as the Raman line shape without gain narrowing. When two fields are partially correlated, then the two spectral components appear together. We provide a method to measure the degree of correlation between two optical fields that have different central frequencies. The theory developed to interpret the experimental results is an extension of the quantum theory of SRS to include anti-Stokes scattering. We show that only in the high-gain limit can the quantum fluctuations be thought of as arising from a classical noise process.
Stimulated Raman scattering (SRS) produces Stokes light pulses that originate from quantum noise and exhibit macroscopic amplitude and phase fluctuations from one shot to another.1 By using transient stimulated Raman scattering, we generated light pulses with macroscopic energy and temporal coherence times that were long compared to their duration. Stokes pulses were generated independently in each arm of an interferometer and were interfered together at the output. The position, modulation depth, and brightness of the interference fringes fluctuated randomly from one shot to the next. We obtained both the ensemble-averaged intensity and the fourth-order intensity correlation function of the interfered Stokes light. The average has a smooth envelope and shows no modulation, whereas the intensity correlation function has a depth of modulation of 0.35 for Stokes generation in the unsaturated (thermal-like) regime and 0.46 in the saturated (laser-like) regime. This is in agreement with predicted values of 0.33 and 0.5.2
We present a theoretical investigation of stimulated emission pumping to achieve sub-diffraction-limited spatial resolution in coherent anti-Stokes Raman scattering (CARS) microscopy. A pair of control light fields is used to prepopulate the Raman state involved in the CARS process prior to the CARS signal generation. Efficient prepopulation is achieved by employing a path via an electronic or vibrational state. Thereby, the buildup of a coherence between the ground and Raman state during irradiation by the light fields for CARS signal generation is prevented, resulting in the suppression of the CARS intensity by more than 99.8%. Two-dimensional spatial excitation profiles have been calculated using donut-shaped spatial profiles for the control light fields, thus, an intensity-dependent narrowing of the CARS excitation profiles below the diffraction limit. Using computer-generated test images we demonstrate a resolution beyond the diffraction limit for CARS microscopy, which is scalable by the control light field intensity, similar to stimulated emission depletion microscopy.
It is shown that transient anti-Stokes stimulated Raman scattering (SRS) acts as a vacuum field fluctuations amplifier at Stokes frequency, the fluctuations being amplified up to macroscopic values. This makes their investigation possible by studying macroscopic energy fluctuations of transient SRS anti-Stokes pulses. The proposed theory also gives a quantitative description of angular distribution of self-generated anti-Stokes emission around the exact phase-matching angle recently observed by Duncan et al. ( Opt. Lett. , 11 (1986) 803) in the transient regime.
We theoretically demonstrate the achievement of narrow-band coherent anti-Stokes Raman scattering (CARS) signal by manipulating broad-band probe spectrum. The narrowing of the CARS signal depends on the spectrum bandwidth of the probe beam, and thus high-resolution CARS signal for a complicated quantum system can be obtained by the simple spectrum manipulation. Furthermore, the energy-level diagram for the complicated quantum system can also be labelled by measuring the CARS signal at a given frequency.
The degree of phase cross correlation between a fluctuating pump wave and the Stokes wave, which is generated by stimulated Raman scattering, can be determined by observing the spectrum of anti-Stokes light generated by coherent anti-Stokes Raman scattering (CARS). The spectrum of the anti-Stokes light has two distinct features: one that arises from scattering through an off-resonant virtual level and one that arises from resonant scattering through the real level. This provides a method to measure the phase cross correlation between two optical fields of different color. The intensity of the anti-Stokes signal strongly depends on the degree of cross correlation. Depending on the detuning from Raman resonance in the CARS process, the anti-Stokes intensity can be either enhanced or suppressed with respect to the case of uncorrelated fields.1