Quantum simulations of excited states with active-space downfolded Hamiltonians

Bauman, Nicholas P.; Low, Guang Hao; Kowalski, Karol

doi:10.1063/1.5128103

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

Journal Article · 18 December 2019 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.5128103 · OSTI ID:1579996

; Low, Guang Hao;

Many-body techniques based on the double unitary coupled cluster (DUCC) ansatz 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 phase estimation (PE) algorithms for quantum computers 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 PE 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 PE algorithms 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 correlated molecular systems, characterized by small energy gaps and high density of quasidegenerate states around the Fermi level.

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Sponsoring Organization:: USDOE

OSTI ID:: 1579996

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 23 Vol. 151; ISSN 0021-9606

Publisher:: American Institute of PhysicsCopyright Statement

Country of Publication:: United States

Language:: English

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