Tailored and Externally Corrected Coupled Cluster with Quantum Inputs

We propose to use wave function overlaps obtained from a quantum computer as inputs for the classical split-amplitude techniques, tailored and externally corrected coupled cluster, to achieve balanced treatment of static and dynamic correlation effects in molecular electronic structure simulations....

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Bibliographic Details
Published in:Journal of chemical theory and computation 2024-06, Vol.20 (12), p.5068-5093
Main Authors: Scheurer, Maximilian, Anselmetti, Gian-Luca R., Oumarou, Oumarou, Gogolin, Christian, Rubin, Nicholas C.
Format: Article
Language:English
Subjects:
Clusters
Correlation
Electronic structure
Molecular structure
Qualitative analysis
Quantum computers
Quantum Electronic Structure
Wave functions
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Summary:We propose to use wave function overlaps obtained from a quantum computer as inputs for the classical split-amplitude techniques, tailored and externally corrected coupled cluster, to achieve balanced treatment of static and dynamic correlation effects in molecular electronic structure simulations. By combining insights from statistical properties of matchgate shadows, which are used to measure quantum trial state overlaps, with classical correlation diagnostics, we can provide quantum resource estimates well into the classically no longer exactly solvable regime. We find that rather imperfect wave functions and remarkably low shot counts are sufficient to cure qualitative failures of plain coupled cluster singles doubles and to obtain chemically precise dynamic correlation energy corrections. We provide insights into which wave function preparation schemes have a chance of yielding quantum advantage, and we test our proposed method using overlaps measured on Google’s Sycamore device.
ISSN:1549-9618
1549-9626
1549-9626
DOI:10.1021/acs.jctc.4c00037