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Optics Communications

The generation of stimulated resonance Raman scattering using external dye fluorescence

H.‐J. Weigmann, M. Pfeiffer, A. Lau, Kurt Lenz

Published Nov 1, 1974• 7 citations
Publisher
DOI
10.1016/0030-4018(74)90002-9

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Summary form only given. Sub-diffraction limited imaging schemes have become widely used in fluorescence microscopy [1]. Howaever, the need for labeling with fluorescent dyes remains a major downside of fluorescence microscopy. The size, availability, toxicity as well as photo-bleaching of the used dyes can complicate measurements [2]. In contrast, Raman imaging is inherently label-free. Unfortunately, the super-resolution schemes used in fluorescence microscopy are currently not transferable to Raman microscopy. This paper presents the development of a scheme for the suppression of coherent Raman scattering through the depletion of probe photons, inspired by the work of M. Cho et al. [3, 4], who showed the suppression of coherent Raman scattering using laser pulses at three different wavelengths and two Raman resonances. In our case, probe depletion is achieved through saturated stimulated Raman scattering in a three-beam setup with only two colors involved. Fig. 1 (a) describes the working principle: in the unsuppressed case, the combination of pump and probe pulse induces stimulated Raman scattering at the Raman resonances, leading to stimulated Raman loss (SRL) of the probe and and stimulated Raman gain (SRG) of the pump. The Raman spectrum then results from the difference between two spectra, recorded with pump on and off, respectively. In the suppressed case a second strong pump pulse, working as a depletion pulse, depletes the probe pulse via stimulated Raman scattering (SRLD) and induces a shortage of the probe photons at the Raman resonances, saturating the stimulated Raman scattering. Thus, only a small amount of additional SRLSup is induced by the original pump. If SRL is detected in addition to the spectral change, induced by the depletion pulse, the SRL will be reduced resulting in SRLSup<; SRL.

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Relationship between stimulated fluorescence and stimulated resonance Raman scattering of dyes in a resonator

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An investigation was made of the visibility of stimulated Raman lines under conditions of molecular resonance. A cell containing the medium under study was placed inside a resonator whose parameters were varied by changing the reflection coefficients of the mirrors or altering the length. The observed deterioration in the visibility of the Raman lines when the resonator Q factor was increased and its length was decreased could be explained qualitatively by a decrease in the nonlinear transmission of the dye for the pump radiation.

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A computational and experimental study of the optical propagation of light in a collisionally broadened three-level Raman amplifier is presented. The Stokes light consists of two distinct spectral components: of resonance stimulated Raman scattering (SRS) and on-resonance stimulated fluorescence (ASE). The intensity dependence of these effects on the buffer gas and on the intensity and detuning of the exciting radiation are calculated. We have carried out the calculation over physically realistic propagation distance. The theoretical model for a description of ASE i SRS signals generation in such a system was developed. The numerical calculations based on the rate equations agree with the experimental results.

AIP conference proceedings•Jan 1, 1997•0 citations
Summary form only given. Sub-diffraction limited imaging schemes have become widely used in fluorescence microscopy [1]. Howaever, the need for labeling with fluorescent dyes remains a major downside of fluorescence microscopy. The size, availability, toxicity as well as photo-bleaching of the used dyes can complicate measurements [2]. In contrast, Raman imaging is inherently label-free. Unfortunately, the super-resolution schemes used in fluorescence microscopy are currently not transferable to Raman microscopy. This paper presents the development of a scheme for the suppression of coherent Raman scattering through the depletion of probe photons, inspired by the work of M. Cho et al. [3, 4], who showed the suppression of coherent Raman scattering using laser pulses at three different wavelengths and two Raman resonances. In our case, probe depletion is achieved through saturated stimulated Raman scattering in a three-beam setup with only two colors involved. Fig. 1 (a) describes the working principle: in the unsuppressed case, the combination of pump and probe pulse induces stimulated Raman scattering at the Raman resonances, leading to stimulated Raman loss (SRL) of the probe and and stimulated Raman gain (SRG) of the pump. The Raman spectrum then results from the difference between two spectra, recorded with pump on and off, respectively. In the suppressed case a second strong pump pulse, working as a depletion pulse, depletes the probe pulse via stimulated Raman scattering (SRLD) and induces a shortage of the probe photons at the Raman resonances, saturating the stimulated Raman scattering. Thus, only a small amount of additional SRLSup is induced by the original pump. If SRL is detected in addition to the spectral change, induced by the depletion pulse, the SRL will be reduced resulting in SRLSup<; SRL.
An investigation was made of the visibility of stimulated Raman lines under conditions of molecular resonance. A cell containing the medium under study was placed inside a resonator whose parameters were varied by changing the reflection coefficients of the mirrors or altering the length. The observed deterioration in the visibility of the Raman lines when the resonator Q factor was increased and its length was decreased could be explained qualitatively by a decrease in the nonlinear transmission of the dye for the pump radiation.
A computational and experimental study of the optical propagation of light in a collisionally broadened three-level Raman amplifier is presented. The Stokes light consists of two distinct spectral components: of resonance stimulated Raman scattering (SRS) and on-resonance stimulated fluorescence (ASE). The intensity dependence of these effects on the buffer gas and on the intensity and detuning of the exciting radiation are calculated. We have carried out the calculation over physically realistic propagation distance. The theoretical model for a description of ASE i SRS signals generation in such a system was developed. The numerical calculations based on the rate equations agree with the experimental results.