Quantum algorithm for simulating non-adiabatic dynamics at metallic surfaces

TL;DR

This paper introduces a quantum algorithm for simulating complex non-adiabatic dynamics at molecule-metal interfaces, enabling efficient modeling of charge and energy transfer processes relevant to catalysis and solar energy conversion.

Contribution

It generalizes the Anderson-Newns Hamiltonian and develops a resource-efficient quantum algorithm for realistic molecule-metal interface simulations.

Findings

Requires only 271 qubits for models with 100 metal and 8 molecular orbitals.

Needs approximately 79 million Toffoli gates for 1000 Trotter steps.

Demonstrates the feasibility of using early fault-tolerant quantum computers for these simulations.

Abstract

Non-adiabatic dynamics at molecule-metal interfaces govern diverse and technologically important phenomena, from heterogeneous catalysis to dye-sensitized solar energy conversion and charge transport across molecular junctions. Realistic modeling of such dynamics necessitates taking into account various charge and energy transfer channels involving the coupling of nuclear motion with a very large number of electronic states, leading to prohibitive cost using classical computational methods. In this work we introduce a generalization of the Anderson-Newns Hamiltonian and develop a highly optimized quantum algorithm for simulating the non-adiabatic dynamics of realistic molecule-metal interfaces. Using the PennyLane software platform, we perform resource estimations of our algorithm, showing its remarkably low implementation cost for model systems representative of various scientifically and industrially relevant molecule-metal systems. Specifically, we find that time evolution for models including $100$ metal orbitals, $8$ molecular orbitals, and $20$ nuclear degrees of freedom, requires only $271$ qubits and $7.9 \times 10^7$ Toffoli gates for $1000$ Trotter steps, suggesting non-adiabatic molecule-metal dynamics as a fruitful application of first-generation fault-tolerant quantum computers.