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Title: Quantum-classical hybrid algorithm for the simulation of all-electron correlation

Journal Article · · Journal of Chemical Physics
DOI: https://doi.org/10.1063/5.0074842 · OSTI ID:1871654
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]
  1. Univ. of Chicago, IL (United States); Department of Chemistry and The James Franck Institute, The University of Chicago, Chicago, IL (United States).
  2. Univ. of Chicago, IL (United States)
+ Show Author Affiliations

While chemical systems containing hundreds to thousands of electrons remain beyond the reach of quantum devices, hybrid quantum-classical algorithms present a promising pathway toward a quantum advantage. Hybrid algorithms treat the exponentially scaling part of the calculation-the static correlation-on the quantum computer and the non-exponentially scaling part-the dynamic correlation-on the classical computer. While a variety of algorithms have been proposed, the dependence of many methods on the total wave function limits the development of easy-to-use classical post-processing implementations. Here, we present a novel combination of quantum and classical algorithms, which computes the all-electron energy of a strongly correlated molecular system on the classical computer from the 2-electron reduced density matrix (2-RDM) evaluated on the quantum device. Significantly, we circumvent the wave function in the all-electron calculations by using density matrix methods that only require input of the statically correlated 2-RDM. Although the algorithm is completely general, we test it with two classical density matrix methods, the anti-Hermitian contracted Schrödinger equation (ACSE) and multiconfiguration pair-density functional theories, using the recently developed quantum ACSE method for simulating the statically correlated 2-RDM. Furthermore, we obtain experimental accuracy for the relative energies of all three benzyne isomers and thereby demonstrate the ability of the developed algorithm to achieve chemically relevant and accurate results on noisy intermediate-scale quantum devices.

Research Organization:
Univ. of Chicago, IL (United States)
Sponsoring Organization:
National Science Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
SC0019215
OSTI ID:
1871654
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 24 Vol. 155; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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