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Issue 11, 2014
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Time-gated pre-resonant femtosecond stimulated Raman spectroscopy of diethylthiatricarbocyanine iodide

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Abstract

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.

Graphical abstract: Time-gated pre-resonant femtosecond stimulated Raman spectroscopy of diethylthiatricarbocyanine iodide

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Publication details

The article was received on 19 Nov 2013, accepted on 22 Jan 2014 and first published on 23 Jan 2014


Article type: Paper
DOI: 10.1039/C3CP54870H
Author version available: Download Author version (PDF)
Citation: Phys. Chem. Chem. Phys., 2014,16, 5312-5318
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    Time-gated pre-resonant femtosecond stimulated Raman spectroscopy of diethylthiatricarbocyanine iodide

    H. M. Kim, H. Kim, I. Yang, S. M. Jin and Y. D. Suh, Phys. Chem. Chem. Phys., 2014, 16, 5312
    DOI: 10.1039/C3CP54870H

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