Reduced density matrix formulation of quantum linear response

TL;DR

This paper introduces a reduced density matrix approach to quantum linear response theory, enabling more efficient spectral property calculations for larger molecules on quantum computers.

Contribution

It develops and implements a RDM-driven method for quantum linear response, reducing classical computational costs and expanding feasible molecular sizes.

Findings

Successful application to benzene and R-methyloxirane with cc-pVTZ basis

Analysis of shot noise effects on water's absorption spectra

Enhanced capability for spectral calculations on larger molecules

Abstract

The prediction of spectral properties via linear response (LR) theory is an important tool in quantum chemistry for understanding photo-induced processes in molecular systems. With the advances of quantum computing, we recently adapted this method for near-term quantum hardware using a truncated active space approximation with orbital rotation, named quantum linear response (qLR). In an effort to reduce the classic cost of this hybrid approach, we here derive and implement a reduced density matrix (RDM) driven approach of qLR. This allows for the calculation of spectral properties of moderately sized molecules with much larger basis sets than so far possible. We report qLR results for benzene and $R$-methyloxirane with a cc-pVTZ basis set and study the effect of shot noise on the valence and oxygen K-edge absorption spectra of H$_2$O in the cc-pVTZ basis.