Trotter Simulation of Vibrational Hamiltonians on a Quantum Computer.

Abstract

Simulating vibrational dynamics is essential for understanding molecular structure, unlocking useful applications such as vibrational spectroscopy for high-fidelity chemical detection. Quantum algorithms for vibrational dynamics are emerging as a promising alternative to resource-demanding classical approaches, but this domain is largely underdeveloped compared with quantum simulations of electronic structure. In this work, we describe in detail three distinct forms of the vibrational Hamiltonian: canonical bosonic quantization, real space representation, and the Christiansen second-quantized form. Leveraging the Lie algebraic properties of each, we develop efficient fragmentation schemes to enable the use of Trotter product formulas for simulating time evolution. We introduce circuits required to implement time evolution in each form and highlight factors that contribute to the simulation cost, including the choice of vibrational coordinates. Using a perturbative approach for the Trotter error, we obtain tight estimates of the T gate cost for the simulation of time evolution in each form, enabling their quantitative comparison. Combining tight Trotter error estimates and efficient fragmentation schemes, we find that for the CH4 molecule with 9 vibrational modes, time evolution for approximately 1.8 ps may be simulated using as few as 36 qubits and approximately 3 × 108 T gates─an order-of-magnitude speedup over state-of-the-art algorithms. Finally, we present calculations of vibrational spectra using each form to demonstrate the fidelity of our algorithms. This work presents a unified and highly optimized framework that makes simulating vibrational dynamics an attractive use case for quantum computers.