State-resolved scattering methods based on laser spectroscopy and ion-imaging have been used to probe nuclear motion in chemical reaction systems. While for successful applications to many small molecular systems at the quantum state level of detail, transition-metal complexes have not been investigated using state-resolved scattering measurements because of their photochemical character, such as their high photoabsorbance. In this Personal Account, we address the challenges by examining the electronic and bonding natures of transition-metal carbonyl and nitrosyl complexes that hinder state-selective measurements. Our approaches to overcoming these limitations are presented alongside the results of photodissociation dynamics studies of Fe(CO)5, CpCo(CO)2, and Co(CO)3NO. Our findings highlight the advantage of the approach for exploring nonstatistical behavior and well-defined nuclear motion, even in systems with intricate potential energy surface structures.
Nagamori et al. (Thu,) studied this question.