Transient measurement of phononic states with covariance-based stochastic spectroscopy
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
Journal
Book Volume: 11
Article Number: 44
Journal Issue: 1
DOI: 10.1038/s41377-022-00727-6
Abstract
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.
Authors with CRIS profile
Involved external institutions
Università degli Studi di Trieste
Italy (IT)
University of California Irvine
United States (USA) (US)
Swinburne University of Technology
Australia (AU)
Italy (IT)
University of California Irvine
United States (USA) (US)
Swinburne University of Technology
Australia (AU)
How to cite
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://dx.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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