Quantum Simulations of Charge and Exciton Transfer in Multi-mode Models using Engineered Reservoirs

Abstract: Quantum simulation offers a route to study open-system molecular dynamics in non-perturbative regimes by programming the interactions among electronic, vibrational, and environmental degrees of freedom on similar energy scales. Trapped-ion systems possess this capability, with their native spins, phonons, and tunable dissipation integrated within a single platform. Here, we demonstrate an open-system quantum simulation of charge and exciton transfer in a multi-mode linear vibronic coupling model (LVCM). Employing tailored spin-phonon interactions alongside reservoir engineering techniques, we emulate a system with two dissipative vibrational modes coupled to donor and acceptor electronic sites and follow its excitation transfer in real time. We continuously drive the system from the charge transfer (CT) regime to the vibrationally assisted exciton transfer (VAET) regime by tuning the vibronic coupling strengths. We find that degenerate modes enhance CT and VAET rates at large energy gaps, while non-degenerate modes activate slow-mode pathways that reduce the energy-gap dependence, thus enlarging the window for efficient transfer. These results show that the presence of just one additional vibration reshapes non-perturbative quantum excitation transfer. Our work also establishes a scalable route to simulating chemically relevant, many-mode vibronic processes with engineered environments, guiding the design of next-generation organic photovoltaics and molecular electronics.