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The coupled quantum dynamics of electrons and protons is ubiquitous in manydynamical processes involving light-matter interaction, such as solar energyconversion in chemical systems and photosynthesis. A first-principlesdescription of such nuclear-electronic quantum dynamics requires not only thetime-dependent treatment of nonequilibrium electron dynamics but also that ofquantum protons. Quantum mechanical correlation between electrons and protonsadds further complexity to such coupled dynamics. Here we extend real-timenuclear-electronic orbital time-dependent density functional theory(RT-NEO-TDDFT) to periodic systems and perform first-principles simulations ofcoupled quantum dynamics of electrons and protons in complex heterogeneoussystems. The process studied is electronically excited state intramolecularproton transfer of o-hydroxybenzaldehyde in water and at a silicon (111)semiconductor-molecule interface. These simulations illustrate how environmentssuch as hydrogen-bonding water molecules and an extended material surfaceimpact the dynamical process on the atomistic level. Depending on how themolecule is chemisorbed on the surface, excited state electron transfer fromthe molecule to the semiconductor surface can inhibit ultrafast proton transferwithin the molecule. This work elucidates how heterogeneous environmentsinfluence the balance between the quantum mechanical proton transfer andexcited electron dynamics. The periodic RT-NEO-TDDFT approach is applicable toa wide range of other photoinduced heterogeneous processes.

First-Principles Approach for Coupled Quantum Dynamics of Electrons and Protons in Heterogeneous Systems