Integration of Variational Quantum Algorithms into Atomistic Simulation Workflows

TL;DR

This paper integrates variational quantum algorithms into atomistic simulation workflows, enabling quantum-classical hybrid calculations for molecular properties and dynamics with promising accuracy and stability.

Contribution

It introduces a novel coupling of Qiskit Nature's quantum chemistry solvers with ASE, allowing for hybrid workflows that include geometry optimization and molecular dynamics.

Findings

ADAPT-VQE achieves results close to classical CCSD calculations.

The integrated workflow produces stable, chemically meaningful forces.

Demonstrates feasibility of quantum algorithms in atomistic simulations.

Abstract

In this work, we present the integration of Qiskit Nature's quantum chemistry solvers into the Atomic Simulation Environment (ASE), enabling hybrid quantum-classical workflows for force-driven atomistic simulations. This coupling allows the use of the Variational Quantum Eigensolver (VQE) and its adaptive variant (ADAPT-VQE) not only for ground-state energy calculations, but also for geometry optimisation, vibrational frequency analysis, strain evaluation, and molecular dynamics, all managed through ASE's calculator interface. By applying ADAPT-VQE to multi-electron systems such as BeH2, we obtain vibrational and structural properties in close agreement with high-level classical CCSD calculations within the same minimal basis. These results demonstrate that adaptive variational quantum algorithms can deliver stable and chemically meaningful forces within an atomistic modelling workflow, enabling downstream applications such as molecular dynamics and active-learning accelerated simulations.