Improved algorithms of quantum imaginary time evolution for ground and excited states of molecular systems

Abstract: Quantum imaginary time evolution (QITE) is a recently proposed quantum-classical hybrid algorithm that is guaranteed to reach the lowest state of system. In this study, we present several improvements on QITE, mainly focusing on molecular applications. We analyze the derivation of the underlying QITE equation order-by-order, and suggest a modification that is theoretically well founded. Our results clearly indicate the soundness of the here-derived equation, enabling a better approximation of the imaginary time propagation by a unitary. We also discuss how to accurately estimate the norm of an imaginary-time-evolved state, and applied it to excited state calculations using the quantum Lanczos algorithm. Finally, we propose the folded-spectrum QITE scheme as a straightforward extension of QITE for general excited state simulations. The effectiveness of all these developments is illustrated by noiseless simulations, offering the further insights into quantum algorithms for imaginary time evolution.