Orbital optimized unitary coupled cluster theory for quantum computer

TL;DR

This paper introduces an orbital optimized unitary coupled cluster method within the VQE framework for quantum computers, enabling efficient molecular structure optimization with reduced quantum resources.

Contribution

It presents a fully variational orbital optimized UCC approach that improves efficiency and accuracy in quantum chemistry calculations on quantum computers.

Findings

Achieves geometry optimization of water and ammonia molecules.

Requires smaller active space and shallower circuits than traditional UCC.

Demonstrates effectiveness using quantum simulators.

Abstract

We propose an orbital optimized method for unitary coupled cluster theory (OO-UCC) within the variational quantum eigensolver (VQE) framework for quantum computers. OO-UCC variationally determines the coupled cluster amplitudes and also molecular orbital coefficients. Owing to its fully variational nature, first-order properties are readily available. This feature allows the optimization of molecular structures in VQE without solving any additional equations. Furthermore, the method requires smaller active space and shallower quantum circuit than UCC to achieve the same accuracy. We present numerical examples of OO-UCC using quantum simulators, which include the geometry optimization of the water and ammonia molecules using analytical first derivatives of the VQE.