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...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.展开更多
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)+2 种基金This work has been performed using the LEGEND laser source made available by the Nanoscience Foundry and Fine Analysis(NFFA-MIUR Italy Progetti Internazionali)facilityS.M.C.gratefully acknowledges the support of the Alexander von Humboldt foundation through the Feodor Lynen programS.M.C.and S.M.gratefully acknowledge the support of the National Science Foundation(Grant CHE1953045).
文摘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.
