2023/09/17 by Jianhua Ren, Ren, Jianhua, Zhedong Zhang +1
Computer Science · Physics and Astronomy · #FOS: Physical sciences #Mechanical and Optical Resonators #Quantum Information and Cryptography #Quantum Physics (quant-ph) #Spectroscopy and Quantum Chemical Studies
paper · pdf · doi:10.48550/arxiv.2309.09289
openalex publication_date 2023/09/17 · openalex created_date 2023/09/20 · openalex updated_date 2026/07/28
We have developed a femtosecond ultra-voilet (UV) stimulated Raman spectroscopy (UV-FSRS) for N molecules in optical cavities. The scheme enables a real-time monitoring of collective dynamics of molecular polaritons and their coupling to vibrations, along with a crosstalk between polariton and dark states. Through multidimensional projections of the UV-FSRS signal, we identify clear signature of the dark states, e.g., pathways and timescales that used to be invisible in resonant technique. A microscopic theory is developed for the UV-FSRS, so as to reveal the polaritonic population and coherence dynamics that interplay with each other. The resulting signal makes the dark states visible, thereby providing a new technique for probing dark state dynamics and their correlation with polariton modes.