Transient measurement of phononic states with covariance-based stochastic spectroscopy

• 作者: Giorgia Sparapassi Stefano M.Cavaletto Jonathan Tollerud Angela Montanaro Filippo Glerean Alexandre Marciniak Fancesca Giusti Shaul Mukamel Daniele Fausti
• 来源期刊: 光：科学与应用（英文版）
• 年，卷（期）: 2022,（3）
• 所属期刊栏目: Articles
• 页码范围: 357-364
• 页数: 8页
• 语种: 英文

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.