The vast majority of quantum chemical studies of catalytic processes use the Born-Oppenheimer approximation, which assumes that the electrons are always in their ground state. Although these calculations often have strong explanatory power, it is unclear when the Born-Oppenheimer approximation may break down. Here, we explore the possibility that processes on catalytic surfaces may induce electronic excitations, which are not captured by simulations using the Born-Oppenheimer approximation. Since metal surfaces have no band gap, electronic excitations are easily induced, and we hence focus on these surfaces.
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