Quantum--classical break-even in electronic dynamics of macrocyclic molecules

Abstract

Here we demonstrate quantum--classical break-even for chemical dynamics applications, reaching useful accuracy with a quantum-hardware wall-clock time comparable to that estimated for practical classical computing resources. Specifically, we construct a quantum workflow for electronic dynamics based on tensor-network circuit compression leveraging spatial locality, extending circuit compression beyond one-dimensional open-boundary systems. This enables application of the workflow to problems that are hardware-native but classically hard. The workflow targets one-dimensional periodic Hamiltonians: circuits classically optimized only for short-time evolution within a small spatial region can be replicated in both space and time to construct long-time dynamics of the full system without classically simulating the corresponding large-scale evolution. We apply the workflow to cyclic conjugated macrocycles with rotational periodicity, 12-qubit benzene and 120-qubit [60]annulene, by embedding their electronic structure onto loops of IBM quantum processors. For the annulene, the quantum-processing-unit (QPU) wall-clock times for hole-doped nonequilibrium dynamics became comparable to the estimated wall-clock time of two classical methods, Majorana propagation and matrix-product-state time evolution based on the time-dependent variational principle; this corresponds to tens to hundreds of compute nodes depending on the task (36 CPU cores per node), assuming near-ideal parallel scaling, bringing the quantum calculation into a wall-clock-time regime comparable to conventional parallel high-performance-computing resources. We also show a situation in which a hybrid quantum--classical calculation is a reasonable choice in terms of both accuracy and computational time. These results show that quantum hardware can become a realistic computational option for chemically relevant electronic dynamics.