Sparapassi G, Cavaletto SM, Tollerud J, Montanaro A, Glerean F, Marciniak A, Giusti F, Mukamel S, Fausti D (2022)
Publication Type: Journal article
Publication year: 2022
Book Volume: 11
Article Number: 44
Journal Issue: 1
DOI: 10.1038/s41377-022-00727-6
We present a novel approach to transient Raman spectroscopy, which combines stochastic probe pulses and a covariance-based detection to measure stimulated Raman signals in alpha-quartz. A coherent broadband pump is used to simultaneously impulsively excite a range of different phonon modes, and the phase, amplitude, and energy of each mode are independently recovered as a function of the pump–probe delay by a noisy-probe and covariance-based analysis. Our experimental results and the associated theoretical description demonstrate the feasibility of 2D-Raman experiments based on the stochastic-probe schemes, with new capabilities not available in equivalent mean-value-based 2D-Raman techniques. This work unlocks the gate for nonlinear spectroscopies to capitalize on the information hidden within the noise and overlooked by a mean-value analysis.
APA:
Sparapassi, G., Cavaletto, S.M., Tollerud, J., Montanaro, A., Glerean, F., Marciniak, A.,... Fausti, D. (2022). Transient measurement of phononic states with covariance-based stochastic spectroscopy. Light: Science & Applications, 11(1). https://doi.org/10.1038/s41377-022-00727-6
MLA:
Sparapassi, Giorgia, et al. "Transient measurement of phononic states with covariance-based stochastic spectroscopy." Light: Science & Applications 11.1 (2022).
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