Transient measurement of phononic states with covariance-based stochastic spectroscopy

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

作者机构：Physics DepartmentUniversity of TriesteTriesteItaly Elettra-Sincrotrone Trieste S.C.p.A.TriesteItaly Department of Chemistry and Department of Physics&AstronomyUniversity of CaliforniaIrvineCAUSA Optical Sciences CentreSwinburne UniversityMelbourneAustralia 

出 版 物：《Light(Science & Applications)》 (光（科学与应用)（英文版）)

年 卷 期：2022年第11卷第3期

页      面：68-75页

核心收录：

学科分类：070207[理学-光学] 07[理学] 0702[理学-物理学] 

基　　金：This work was supported by the European Commission through the European Research Council(ERC)Starting Grant Project“Inhomogenieties and Fluctuations in Quantum Coherent Matter Phases by Ultrafast Optical Tomography(INCEPT)”(Grant#677488) DF aknowledges the support of ERC Proof of Concept grant COBRAS(Grant#860365) This work has been performed using the LEGEND laser source made available by the Nanoscience Foundry and Fine Analysis(NFFA-MIUR Italy Progetti Internazionali)facility S.M.C.gratefully acknowledges the support of the Alexander von Humboldt foundation through the Feodor Lynen program S.M.C.and S.M.gratefully acknowledge the support of the National Science Foundation(Grant CHE1953045). 

主　　题：stochastic spectroscopy coherent 

摘      要：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.