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Title: Quantum simulations of excited states with active-space downfolded Hamiltonians

Abstract

Many-body techniques based on the double unitary coupled cluster ansatz (DUCC) can be used to downfold electronic Hamiltonians into low-dimensional active spaces. It can be shown that the resulting dimensionality reduced Hamiltonians are amenable for quantum computing. Recent studies performed for several benchmark systems using quantum phase estimation (QPE) algorithms demonstrated that these formulations can recover a significant portion of ground-state dynamical correlation effects that stem from the electron excitations outside of the active space. These results have also been confirmed in studies of ground-state potential energy surfaces using quantum simulators. In this letter, we study the effectiveness of the DUCC formalism in describing excited states. We also emphasize the role of the QPE formalism and its stochastic nature in discovering/identifying excited states or excited-state processes in situations when the knowledge about the true configurational structure of a sought after excited state is limited or postulated (due to the specific physics driving excited-state processes of interest). In this context, we can view the QPE algorithm as an engine for verifying various hypotheses for excited-state processes and providing statistically meaningful results that correspond to the electronic state(s) with the largest overlap with a postulated configurational structure. We illustrate these ideas onmore » examples of strongly cor- related molecular systems, characterized by small energy gaps and high density of quasi-degenerate states around the Fermi level.« less

Authors:
 [1];  [2];  [1]
+ Show Author Affiliations
  1. BATTELLE (PACIFIC NW LAB)
  2. MICROSOFT
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1581619
Report Number(s):
PNNL-SA-146959
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 23
Country of Publication:
United States
Language:
English
Subject:
quantum chemistry, quantum computing, computational chemistry, electronic structure methods

Citation Formats

Bauman, Nicholas P., Low, Guang Hao, and Kowalski, Karol. Quantum simulations of excited states with active-space downfolded Hamiltonians. United States: N. p., 2019. Web. doi:10.1063/1.5128103.
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Bauman, Nicholas P., Low, Guang Hao, & Kowalski, Karol. Quantum simulations of excited states with active-space downfolded Hamiltonians. United States. doi:10.1063/1.5128103.
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Bauman, Nicholas P., Low, Guang Hao, and Kowalski, Karol. Sat . "Quantum simulations of excited states with active-space downfolded Hamiltonians". United States. doi:10.1063/1.5128103.
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@article{osti_1581619,
title = {Quantum simulations of excited states with active-space downfolded Hamiltonians},
author = {Bauman, Nicholas P. and Low, Guang Hao and Kowalski, Karol},
abstractNote = {Many-body techniques based on the double unitary coupled cluster ansatz (DUCC) can be used to downfold electronic Hamiltonians into low-dimensional active spaces. It can be shown that the resulting dimensionality reduced Hamiltonians are amenable for quantum computing. Recent studies performed for several benchmark systems using quantum phase estimation (QPE) algorithms demonstrated that these formulations can recover a significant portion of ground-state dynamical correlation effects that stem from the electron excitations outside of the active space. These results have also been confirmed in studies of ground-state potential energy surfaces using quantum simulators. In this letter, we study the effectiveness of the DUCC formalism in describing excited states. We also emphasize the role of the QPE formalism and its stochastic nature in discovering/identifying excited states or excited-state processes in situations when the knowledge about the true configurational structure of a sought after excited state is limited or postulated (due to the specific physics driving excited-state processes of interest). In this context, we can view the QPE algorithm as an engine for verifying various hypotheses for excited-state processes and providing statistically meaningful results that correspond to the electronic state(s) with the largest overlap with a postulated configurational structure. We illustrate these ideas on examples of strongly cor- related molecular systems, characterized by small energy gaps and high density of quasi-degenerate states around the Fermi level.},
doi = {10.1063/1.5128103},
journal = {Journal of Chemical Physics},
number = 23,
volume = 151,
place = {United States},
year = {2019},
month = {12}
}
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Journal Article:
DOI:  10.1063/1.5128103
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