Nonadiabatic Molecular Quantum Dynamics with Quantum Computers

Abstract

The theoretical investigation of nonadiabatic processes is hampered by the complexity of the coupled electron-nuclear dynamics beyond the Born-Oppenheimer approximation. Classically, the simulation of such reactions is limited by the unfavorable scaling of the computational resources as a function of the system size. While quantum computing exhibits proven quantum advantage for the simulation of real-time dynamics, the study of quantum algorithms for the description of nonadiabatic phenomena is still unexplored. In this Letter, we propose a quantum algorithm for the simulation of fast nonadiabatic chemical processes together with an initialization scheme for quantum hardware calculations. In particular, we introduce a first-quantization method for the time evolution of a wave packet on two coupled harmonic potential energy surfaces (Marcus model). In our approach, the computational resources scale polynomially in the system dimensions, opening up new avenues for the study of photophysical processes that are classically intractable.