TY - JOUR
T1 - Quantum Equation of Motion with Orbital Optimization for Computing Molecular Properties in Near-Term Quantum Computing
AU - Jensen, Phillip W.K.
AU - Kjellgren, Erik Rosendahl
AU - Reinholdt, Peter
AU - Ziems, Karl Michael
AU - Coriani, Sonia
AU - Kongsted, Jacob
AU - Sauer, Stephan P.A.
PY - 2024/5/14
Y1 - 2024/5/14
N2 - Determining the properties of molecules and materials is one of the premier applications of quantum computing. A major question in the field is how to use imperfect near-term quantum computers to solve problems of practical value. Inspired by the recently developed variants of the quantum counterpart of the equation-of-motion (qEOM) approach and the orbital-optimized variational quantum eigensolver (oo-VQE), we present a quantum algorithm (oo-VQE-qEOM) for the calculation of molecular properties by computing expectation values on a quantum computer. We perform noise-free quantum simulations of BeH2 in the series of STO-3G/6-31G/6-31G* basis sets and of H4 and H2O in 6-31G using an active space of four electrons and four spatial orbitals (8 qubits) to evaluate excitation energies, electronic absorption, and, for twisted H4, circular dichroism spectra. We demonstrate that the proposed algorithm can reproduce the results of conventional classical CASSCF calculations for these molecular systems.
AB - Determining the properties of molecules and materials is one of the premier applications of quantum computing. A major question in the field is how to use imperfect near-term quantum computers to solve problems of practical value. Inspired by the recently developed variants of the quantum counterpart of the equation-of-motion (qEOM) approach and the orbital-optimized variational quantum eigensolver (oo-VQE), we present a quantum algorithm (oo-VQE-qEOM) for the calculation of molecular properties by computing expectation values on a quantum computer. We perform noise-free quantum simulations of BeH2 in the series of STO-3G/6-31G/6-31G* basis sets and of H4 and H2O in 6-31G using an active space of four electrons and four spatial orbitals (8 qubits) to evaluate excitation energies, electronic absorption, and, for twisted H4, circular dichroism spectra. We demonstrate that the proposed algorithm can reproduce the results of conventional classical CASSCF calculations for these molecular systems.
U2 - 10.1021/acs.jctc.4c00069
DO - 10.1021/acs.jctc.4c00069
M3 - Journal article
C2 - 38701352
AN - SCOPUS:85192252264
SN - 1549-9618
VL - 20
SP - 3613
EP - 3625
JO - Journal of Chemical theory and Computation
JF - Journal of Chemical theory and Computation
IS - 9
ER -