Are multi-quasiparticle interactions important in molecular ionization?

ORAL

Abstract

Understanding multi-quasiparticle (MQP) phenomena is a key step towards the design of quantum materials with tailored opto-electronic properties. Photo-emission spectra (PES) offer an experimental probe for these effects, but accurate theoretical descriptions of the quasiparticle interactions underlying the MQP regime are still lacking. We tackle this challenge by studying the inner valence PES of closed-shell molecules using the fully-correlated adaptive sampling configuration interaction (ASCI) method. Our results show a rich satellite structure, hallmark of MQP physics, even in these deceivingly simple systems. We complement the ASCI spectra with perturbative calculations, namely GW and vertex corrected GWΓ, and conclude that the satellite features originate from correlated quasiparticles. The vertex corrections in GWΓ seem recover the excitonic interactions necessary to qualitatively capture these satellites, improving the GW results.

*Supported by an NSF CAREER award through Grant No.~DMR-1945098, the NSF Quantum Foundry through QAMASE-i program Award No.~DMR-1906325, an Obra Social ``La Caixa'' graduate fellowship (ID 100010434, LCF/BQ/AA16/11580047), as well as the NASA Ames Research Center and the AFRL Information Directorate under Grant No.~F4HBKC4162G001.

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Presenters

  • Carlos Mejuto Zaera

    • University of California, Berkeley
    • Lawrence Berkeley National Laboratory

Authors

  • Carlos Mejuto Zaera

    • University of California, Berkeley
    • Lawrence Berkeley National Laboratory

  • Guorong Weng

    • University of California, Santa Barbara

  • Mariya Romanova

    • University of California, Santa Barbara

  • Stephen J. Cotton

    • NASA Ames
    • NASA Ames Research Center
    • Quantum Artificial Intelligence Laboratory (QuAIL), KBR; NASA Ames Research Center

  • Birgitta K Whaley

    • University of California, Berkeley
    • Chemistry, University of California, Berkeley

  • Norm Tubman

    • NASA Ames Research Center
    • NASA Ames
    • Quantum Artificial Intelligence Laboratory (QuAIL), NASA Ames Research Center

  • Vojtech Vlcek

    • University of California, Santa Barbara