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Efficient photoredox chemical transformations are essential to the development of novel, cost-effective, and environmentally friendly synthetic methodologies. The concept of the entatic state in bioinorganic catalysis proposes that a preorganized structural configuration can reduce the energy barriers associated with chemical reactions. This concept provides one of the guiding principles to enhance catalytic efficiency by maintaining high-energy conformations close to the reaction's transition state. Copper(I)-based photocatalysts, recognized for their low toxicity and highly negative oxidation potentials, are of particular interest in entasis studies. In this study, we explore the impact of entasis caused by stress induced by the surrounding lattice on the excited state dynamics of a prototypical copper(I)-based photocatalyst in a single crystal form. Using femtosecond broadband transient absorption spectroscopy, we show that triplet state formation from the entactic state is faster (∼3.9 ps) in crystals compared with solution (∼11.3 ps). The observed faster intersystem crossing in crystals hints toward the possible existence of distorted square planar geometry with higher spin-orbit coupling at the minima of the S
Tiwari et al. (Wed,) studied this question.