Taming Disulfide Bonds with Laser Fields. Nonadiabatic Surface-Hopping Simulations in a Ruthenium Complex

[Image: see text] Laser control of chemical reactions is a challenging field of research. In particular, the theoretical description of coupled electronic and nuclear motion in the presence of laser fields is not a trivial task and simulations are mostly restricted to small systems or molecules treated within reduced dimensionality. Here, we demonstrate how the excited state dynamics of [Ru((S–S)bpy)(bpy)(2)](2+) can be controlled using explicit laser fields in the context of fewest-switches surface hopping. In particular, the transient properties along the excited state dynamics leading to population of the T(1) minimum energy structure are exploited to define simple laser fields capable of slowing and even completely stopping the onset of S–S bond dissociation. The use of a linear vibronic coupling model to parametrize the potential energy surfaces showcases the strength of the surface-hopping methodology to study systems including explicit laser fields using many nuclear degrees of freedom and a large amount of close-lying electronic excited states.