Quantum simulations of molecular systems with intrinsic atomic orbitals

Quantum simulations of molecular systems on quantum computers often employ minimal basis sets of Gaussian orbitals. In comparison with more realistic basis sets, quantum simulations employing minimal basis sets require fewer qubits and quantum gates, but yield results of lower accuracy. A natural strategy to achieve more accurate results is to increase the basis set size, which in turn requires increasing the number of qubits and quantum gates. Here we explore the use of intrinsic atomic orbitals (IAOs) in quantum simulations of molecules, to improve the accuracy of energies and properties at the same computational cost required by a minimal basis. We investigate ground-state energies and one- and two-body density operators in the framework of the variational quantum eigensolver, employing and comparing different Ans\"{a}tze. We also demonstrate the use of this approach in the calculation of ground- and excited-states energies of small molecules by a combination of quantum algorithms, using IBM Quantum computers.
Comment: 14 pages, 14 figures. Published in Physical Review A