Quantum Algorithm for Vibronic Dynamics: Case Study on Singlet Fission Solar Cell Design

Vibronic interactions between nuclear motion and electronic states are critical for the accurate modeling of photochemistry. However, accurate simulations of fully quantum non-adiabatic dynamics are often prohibitively expensive for classical methods beyond small systems. In this work, we present a quantum algorithm based on product formulas for simulating time evolution under a general vibronic Hamiltonian in real space, capable of handling an arbitrary number of electronic states and vibrational modes. We develop the first trotterization scheme for vibronic Hamiltonians beyond two electronic states and introduce an array of optimization techniques for the exponentiation of each fragment in the product formula, resulting in a remarkably low cost of implementation. To demonstrate practical relevance, we outline a proof-of-principle integration of our algorithm into a materials discovery pipeline for designing more efficient singlet fission-based organic solar cells. Based on commutator bounds, we estimate that a 100 femtosecond evolution using a second-order Trotter product formula of a 4-state model of an anthracene-fullerene interface requires 117 qubits and 1.5 × 10 7 Toffoli gates in a reduced dimensionality of 11 modes. In its full dimensionality of 246 modes, it requires 1065 qubits and 2.7 × 10 9 Toffoli gates.