Quantum self-consistent equation-of-motion method for computing molecular excitation energies, ionization potentials, and electron affinities on a quantum computer

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dc.contributor.authorAsthana, Ayushen
dc.contributor.authorKumar, Ashutoshen
dc.contributor.authorAbraham, Vibinen
dc.contributor.authorGrimsley, Harperen
dc.contributor.authorZhang, Yuen
dc.contributor.authorCincio, Lukaszen
dc.contributor.authorTretiak, Sergeien
dc.contributor.authorDub, Pavel A.en
dc.contributor.authorEconomou, Sophia E.en
dc.contributor.authorBarnes, Edwin Flemingen
dc.contributor.authorMayhall, Nicholas J.en
dc.date.accessioned2023-03-28T13:07:12Zen
dc.date.available2023-03-28T13:07:12Zen
dc.date.issued2023-01-27en
dc.description.abstractNear-term quantum computers are expected to facilitate material and chemical research through accurate molecular simulations. Several developments have already shown that accurate ground-state energies for small molecules can be evaluated on present-day quantum devices. Although electronically excited states play a vital role in chemical processes and applications, the search for a reliable and practical approach for routine excited-state calculations on near-term quantum devices is ongoing. Inspired by excited-state methods developed for the unitary coupled-cluster theory in quantum chemistry, we present an equation-of-motion-based method to compute excitation energies following the variational quantum eigensolver algorithm for ground-state calculations on a quantum computer. We perform numerical simulations on H-2, H-4, H2O, and LiH molecules to test our quantum self-consistent equation-of-motion (q-sc-EOM) method and compare it to other current state-of-the-art methods. q-sc-EOM makes use of self-consistent operators to satisfy the vacuum annihilation condition, a critical property for accurate calculations. It provides real and size-intensive energy differences corresponding to vertical excitation energies, ionization potentials and electron affinities. We also find that q-sc-EOM is more suitable for implementation on NISQ devices as it is expected to be more resilient to noise compared with the currently available methods.en
dc.description.notesThis research was supported by the Department of Energy (DOE). E. B. and N. J. M. acknowledge Award No. DE-SC0019199, and S. E. E. acknowledges support from the NSF, award number 1839136. A. A. would like to thank Dr Luke Bertels for helpful discussions. The authors thank the Advanced Research Computing (ARC) facility at Virginia Tech for the computational infrastructure. A. K., Y. Z., L. C., S. T., and P. A. D. are thankful for the support from the Laboratory Directed Research and Development (LDRD) program of Los Alamos National Laboratory (LANL) under project number 20200056DR. LANL is operated by Triad National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy (contract no. 89233218CNA000001).en
dc.description.sponsorshipDepartment of Energy (DOE) [DE-SC0019199]; NSF [1839136]; Laboratory Directed Research and Development (LDRD) program of Los Alamos National Laboratory (LANL) [20200056DR]; National Nuclear Security Administration of the U.S. Department of Energy [89233218CNA000001]en
dc.description.versionPublished versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.doihttps://doi.org/10.1039/d2sc05371cen
dc.identifier.eissn2041-6539en
dc.identifier.pmid36873839en
dc.identifier.urihttp://hdl.handle.net/10919/114195en
dc.language.isoenen
dc.publisherRoyal Society Chemistryen
dc.rightsCreative Commons Attribution 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/en
dc.subjectCoupled-cluster methoden
dc.subjectexcited-stateen
dc.subjectpropagatoren
dc.subjectconstructionen
dc.subjectchemistryen
dc.titleQuantum self-consistent equation-of-motion method for computing molecular excitation energies, ionization potentials, and electron affinities on a quantum computeren
dc.title.serialChemical Scienceen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten

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