Critical Limitations in Quantum-Selected Configuration Interaction Methods

TL;DR

This paper critically analyzes Quantum Selected Configuration Interaction methods, revealing significant limitations in their efficiency and practicality for quantum chemistry, especially in high-accuracy scenarios, compared to classical approaches.

Contribution

The study provides a detailed numerical analysis showing the practical limitations of QSCI methods in generating compact, accurate CI expansions for complex molecules.

Findings

QSCI struggles with inefficiency in sampling new determinants

QSCI produces less compact CI expansions than classical heuristics

Sampling inefficiencies hinder QSCI's practical utility in chemistry

Abstract

Quantum Selected Configuration Interaction (QSCI) methods (also known as Sample-based Quantum Diagonalization, SQD) have emerged as promising near-term approaches to solving the electronic Schr{\"o}dinger equation with quantum computers. In this work, we perform numerical analysis to show that QSCI methods face critical limitations that severely hinder their practical applicability in chemistry. Using the nitrogen molecule and the iron-sulfur cluster [2Fe-2S] as examples, we demonstrate that while QSCI can, in principle, yield high-quality configuration interaction (CI) expansions similar to classical SCI heuristics in some cases, the method struggles with inefficiencies in finding new determinants as sampling repeatedly selects already seen configurations. This inefficiency becomes especially pronounced when targeting high-accuracy results or sampling from an approximate ansatz. In cases where the sampling problem is not present, the resulting CI expansions are less compact than those generated from classical heuristics, rendering QSCI an overall more expensive method. Our findings suggest a significant drawback in QSCI methods when sampling from the ground-state distribution as the inescapable trade-off between finding sufficiently many determinants and generating compact, accurate CI expansions. This ultimately hinders utility in quantum chemistry applications, as QSCI falls behind more efficient classical counterparts.