Leveraging small scale quantum computers with unitarily downfolded Hamiltonians

Abstract: In this work, we propose a quantum unitary downfolding formalism based on the driven similarity renormalization group (QDSRG) that may be combined with quantum algorithms for both noisy and fault-tolerant hardware. The QDSRG is a classical polynomially-scaling downfolding method that avoids the evaluation of costly three- and higher-body reduced density matrices while retaining the accuracy of classical multireference many-body theories. We calibrate and test the QDSRG on several challenging chemical problems and propose a strategy for avoiding classical exponential-scaling steps in the QDSRG scheme. We report QDSRG computations of two chemical systems using the variational quantum eigensolver on IBM quantum devices: i) the dissociation curve of H$_2$ using a quintuple-$\zeta$ basis and ii) the bicyclobutane isomerization reaction to $trans$-butadiene, demonstrating the reduction of problems that require several hundred qubits to a single qubit. Our work shows that the QDSRG is a viable approach to leverage near-term quantum devices for the accurate estimation of molecular properties.