Multiscale Simmulations for Catalysis at Strongly Ionized Nanoparticle Surfaces

Surface charges and the large electric fields they can produce play a fundamental in dictating the catalytic properties of nanomaterials. Recently, strong-field excitation of dielectric nanoparticles has emerged as an avenue for studying catalysis in highly ionized environments producing extreme electric fields. While the dynamics of laser-driven surface electron-ion emission has been extensively explored, understanding the molecular dynamics leading to fragmentation has remained elusive. Here we employ a multiscale approach performing non-adiabatic quantum molecular dynamics (NAQMD) simulations on hydrogenated silica surfaces in both bare and wetted environments under field conditions mimicking those of an ionized nanoparticle. We find that hole localization drives fragmentation dynamics, leading to surface silanol dissociation within 50 femtoseconds and charge transfer-induced water splitting in wetted environments within 150 femtoseconds. Overall, our results indicate on demand metallization of dielectric nanoparticles through strong field ionization allowing for development of time resolved experiments of ultrafast catalytic processes.