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Time-gated pre-resonant femtosecond stimulated Raman spectroscopy of diethylthiatricarbocyanine iodide
- Time-gated pre-resonant femtosecond stimulated Raman spectroscopy of diethylthiatricarbocyanine iodide
- Kim, Hyung Min; Kim, Hyunmin; Yang, Ilseung; Jin, Seung Min; Suh, Yung Doug
- DGIST Authors
- Kim, Hyunmin
- Issue Date
- Physical Chemistry Chemical Physics, 16(11), 5312-5318
- Article Type
- Carbocyanine; Carbocyanines; Chemistry; Diethylthiotricarbocyanine Iodide; Methodology; Raman Spectrometry; Spectrum Analysis, Raman
- We present time-gated femtosecond stimulated Raman spectroscopy (fSRS) under the pre-resonance Raman conditions of diethylthiatricarbocyanine (DTTC) iodide. A 'pseudo emission-free' condition is achieved by delivering the probe beam ahead of the pump beam. Regeneratively amplified pulse trains are employed to create an angle-geometry (non-collimated) mixing between the pump and probe beams, leading to highly sensitive measurement of the stimulated Raman gain. Time-integrated spectroscopy allows for a more quantitative distinction between the contributions of stimulated Raman scattering and stimulated emission. We successfully obtain a highly sensitive (signal-to-noise ratio >100) stimulated Raman spectrum under the optimized conditions, which compares favourably to results obtained using two-dimensional correlation spectroscopy (2DCOS). Given the optical pre-resonance of ∼0.1 eV, the background signals mostly originate from the stimulated emission of excited electrons and are significantly reduced by partial overlapping of the pump and probe beams; a genuine fSRS spectral profile is obtained for a temporal delay of ∼0.2 ps between the two beams. © 2014 the Owner Societies.
- Royal Society of Chemistry
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