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Complete Active Space Methods for NISQ Devices: The Importance of Canonical Orbital Optimization for Accuracy and Noise Resilience
Department of Microtechnology and Nanoscience - MC2, Chalmers University of Technology, SE-412 96 Gothenburg, Sweden.ORCID iD: 0000-0002-7563-8944
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Theoretical Chemistry and Biology. Division of Theoretical Chemistry, Department of Chemistry, Lund University, SE-223 62 Lund, Sweden.ORCID iD: 0000-0001-9883-3569
Department of Microtechnology and Nanoscience - MC2, Chalmers University of Technology, SE-412 96 Gothenburg, Sweden.
2023 (English)In: Journal of Chemical Theory and Computation, ISSN 1549-9618, E-ISSN 1549-9626, Vol. 19, no 10, p. 2863-2872Article in journal (Refereed) Published
Abstract [en]

To avoid the scaling of the number of qubits with the size of the basis set, one can divide the molecular space into active and inactive regions, which is also known as complete active space methods. However, selecting the active space alone is not enough to accurately describe quantum mechanical effects such as correlation. This study emphasizes the importance of optimizing the active space orbitals to describe correlation and improve the basis-dependent Hartree-Fock energies. We will explore classical and quantum computation methods for orbital optimization and compare the chemically inspired ansatz, UCCSD, with the classical full CI approach for describing the active space in both weakly and strongly correlated molecules. Finally, we will investigate the practical implementation of a quantum CASSCF, where hardware-efficient circuits must be used and noise can interfere with accuracy and convergence. Additionally, we will examine the impact of using canonical and noncanonical active orbitals on the convergence of the quantum CASSCF routine in the presence of noise.

Place, publisher, year, edition, pages
American Chemical Society (ACS) , 2023. Vol. 19, no 10, p. 2863-2872
National Category
Theoretical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-331590DOI: 10.1021/acs.jctc.3c00123ISI: 000982455000001PubMedID: 37103120Scopus ID: 2-s2.0-85156259803OAI: oai:DiVA.org:kth-331590DiVA, id: diva2:1782267
Note

QC 20230713

Available from: 2023-07-13 Created: 2023-07-13 Last updated: 2024-03-15Bibliographically approved

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De Gracia Triviño, Juan AngelDelcey, Mickael G

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