Work

State-correlated reaction dynamics unveiled in full from a single product-image measurement

Year: 2025

Type: article

Abstract: Electron- or photoionization mass spectrometry coupled with product time-of-flight measurement is a universal detection scheme, which has been playing pivotal role in advancing our fundamental understanding of chemical reactions. This powerful detection scheme, however, usually does not provide the product state-specific information. Here, we propose a variant of universal detection with state-resolving capability by leveraging a three-dimensional velocity-map imaging detector with vacuum-ultraviolet photoionization probe. As demonstrated by a crossed-beam reaction of F + CH4 → CH3(vi) + HF(v), both product vibrational branching and state-resolved angular distributions are simultaneously unveiled in a (vi, v) pair-correlated manner from a single product-image measurement, which enables us to gain previously inaccessible insights. Comparisons with a six-dimensionality quantum dynamics calculation show excellent agreements, validating the approach. The proposed method is general and should open a new opportunity to gain deeper insights into many important complex chemical processes that are otherwise difficult to study. A universal detection scheme capable of providing all reaction products and states information at once from a single measurement is demonstrated in F + CH4 → HF + CH3. The results unveil the previously inaccessible underlying reaction mechanism.

Source: Nature Communications

DOI: 10.1038/s41467-025-66587-x

Authors: Huilin Pan, Shu Liu, Pengcheng Wang, Xueming Yang, Dong H. Zhang, Kopin Liu