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Title: Resource-Efficient Chemistry on Quantum Computers with the Variational Quantum Eigensolver and the Double Unitary Coupled-Cluster Approach

Abstract

Applications of quantum simulation algorithms to obtain electronic energies of molecules on noisy intermediate-scale quantum (NISQ) devices require careful consideration of resources describing the complex electron correlation effects. In modeling second-quantized problems, the biggest challenge confronted is that the number of qubits scales linearly with the size of the molecular basis. This poses a significant limitation on the size of the basis sets and the number of correlated electrons included in quantum simulations of chemical processes. To address this issue and enable more realistic simulations on NISQ computers, we employ the double unitary coupled-cluster (DUCC) method to effectively downfold correlation effects into the reduced-size orbital space, commonly referred to as the active space. Using downfolding techniques, we demonstrate that properly constructed effective Hamiltonians can capture the effect of the whole orbital space in small-size active spaces. Combining the downfolding preprocessing technique with the variational quantum eigensolver, we solve for the ground-state energy of H2, Li2, and BeH2 in the cc-pVTZ basis using the DUCC-reduced active spaces. Finally, we compare these results to full configuration-interaction and high-level coupled-cluster reference calculations.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1616985
Grant/Contract Number:  
AC02-05CH11231; AC06-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Theory and Computation
Additional Journal Information:
Journal Volume: 16; Journal Issue: 10; Journal ID: ISSN 1549-9618
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
97 MATHEMATICS AND COMPUTING; Algorithms; Energy; Mathematical methods; Circuits; Hamiltonians

Citation Formats

Metcalf, Mekena, Bauman, Nicholas P., Kowalski, Karol, and de Jong, Wibe A. Resource-Efficient Chemistry on Quantum Computers with the Variational Quantum Eigensolver and the Double Unitary Coupled-Cluster Approach. United States: N. p., 2020. Web. doi:10.1021/acs.jctc.0c00421.
Metcalf, Mekena, Bauman, Nicholas P., Kowalski, Karol, & de Jong, Wibe A. Resource-Efficient Chemistry on Quantum Computers with the Variational Quantum Eigensolver and the Double Unitary Coupled-Cluster Approach. United States. https://doi.org/10.1021/acs.jctc.0c00421
Metcalf, Mekena, Bauman, Nicholas P., Kowalski, Karol, and de Jong, Wibe A. Fri . "Resource-Efficient Chemistry on Quantum Computers with the Variational Quantum Eigensolver and the Double Unitary Coupled-Cluster Approach". United States. https://doi.org/10.1021/acs.jctc.0c00421. https://www.osti.gov/servlets/purl/1616985.
@article{osti_1616985,
title = {Resource-Efficient Chemistry on Quantum Computers with the Variational Quantum Eigensolver and the Double Unitary Coupled-Cluster Approach},
author = {Metcalf, Mekena and Bauman, Nicholas P. and Kowalski, Karol and de Jong, Wibe A.},
abstractNote = {Applications of quantum simulation algorithms to obtain electronic energies of molecules on noisy intermediate-scale quantum (NISQ) devices require careful consideration of resources describing the complex electron correlation effects. In modeling second-quantized problems, the biggest challenge confronted is that the number of qubits scales linearly with the size of the molecular basis. This poses a significant limitation on the size of the basis sets and the number of correlated electrons included in quantum simulations of chemical processes. To address this issue and enable more realistic simulations on NISQ computers, we employ the double unitary coupled-cluster (DUCC) method to effectively downfold correlation effects into the reduced-size orbital space, commonly referred to as the active space. Using downfolding techniques, we demonstrate that properly constructed effective Hamiltonians can capture the effect of the whole orbital space in small-size active spaces. Combining the downfolding preprocessing technique with the variational quantum eigensolver, we solve for the ground-state energy of H2, Li2, and BeH2 in the cc-pVTZ basis using the DUCC-reduced active spaces. Finally, we compare these results to full configuration-interaction and high-level coupled-cluster reference calculations.},
doi = {10.1021/acs.jctc.0c00421},
journal = {Journal of Chemical Theory and Computation},
number = 10,
volume = 16,
place = {United States},
year = {2020},
month = {9}
}

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