Quantum State‐Resolved Photodissociation Dynamics Study of Transition‐Metal Carbonyl and Nitrosyl

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.