中央研究院 原子與分子科學研究所

Analytical Chemistry, 94, 5752 (2022)

A novel spectrometer has been developed based on synchronized two-color time-resolved dual-comb spectroscopy (TRDCS), enabling high-resolution hyperspectral measurements. The proposed approach with TRDCS exhibits great potential in quantitative diagnostics of multispecies and opens opportunities to decipher key reaction mechanisms in atmospheric chemistry. In this work, we perform simultaneous measurements in two distinct molecular fingerprint regions near 2.9 and 7.8 μm by employing the new approach with synchronized two-color TRDCS. Upon flash photolysis of CH₂I₂/O₂/N₂ gas mixtures, multiple reaction species, involving the simplest Criegee intermediates (CH₂OO), formaldehyde (CH₂O), hydroxyl (OH) and hydroperoxy (HO₂) radicals are simultaneously detected with microsecond time resolution. The concentration of each molecule can be determined based on high-resolution rovibrational absorption spectroscopy. With quantitative detection and simulation of temporal concentration profiles of the targeted molecules at various conditions, the underlying reaction mechanisms and pathways related to the formation of the HO_x radicals, which can be generated from decomposition of initially energized and vibrationally excited Criegee intermediates, are explored.