Transient measurement of phononic states with covariance-based stochastic spectroscopy

Giorgia Sparapassi; Stefano M. Cavaletto; Jonathan Tollerud; Angela Montanaro; Filippo Glerean; Alexandre Marciniak; Fancesca Giusti; Shaul Mukamel; Daniele Fausti

doi:10.1038/s41377-022-00727-6

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Transient measurement of phononic states with covariance-based stochastic spectroscopy

Articles

- Transient measurement of phononic states with covariance-based stochastic spectroscopy
- Light: Science & Applications Vol. 11, Issue 3, Pages: 357-364(2022)
- Affiliations：
  
  1.Physics Department, University of Trieste, Trieste, Italy
  2.Elettra-Sincrotrone Trieste S.C.p.A., Trieste, Italy
  3.Department of Chemistry and Department of Physics & Astronomy, University of California, Irvine, CA, USA
  4.Optical Sciences Centre, Swinburne University, Melbourne, Australia
- Author bio：
  
  Jonathan Tollerud (jtollerud@swin.edu.au)
  Daniele Fausti (daniele.fausti@elettra.eu)
- Funds：
- DOI：10.1038/s41377-022-00727-6
  CLC：
- Published：31 March 2022，
  
  Published Online：01 March 2022，
  
  Received：16 August 2021，
  
  Revised：17 January 2022，
  
  Accepted：26 January 2022
- Accepted：
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Sparapassi, G. et al. Transient measurement of phononic states with covariance-based stochastic spectroscopy. Light: Science & Applications, 11, 357-364 (2022).
DOI：

Sparapassi, G. et al. Transient measurement of phononic states with covariance-based stochastic spectroscopy. Light: Science & Applications, 11, 357-364 (2022). DOI： 10.1038/s41377-022-00727-6.

摘要

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.

关键词

Keywords

references

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