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.
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Presenters
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Carlos Mejuto Zaera
University of California, Berkeley, Lawrence Berkeley National Laboratory
Authors
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Carlos Mejuto Zaera
University of California, Berkeley, Lawrence Berkeley National Laboratory
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Guorong Weng
University of California, Santa Barbara
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Mariya Romanova
University of California, Santa Barbara
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Stephen J. Cotton
NASA Ames, NASA Ames Research Center, Quantum Artificial Intelligence Laboratory (QuAIL), KBR; NASA Ames Research Center
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Birgitta K Whaley
University of California, Berkeley, Chemistry, University of California, Berkeley
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Norm Tubman
NASA Ames Research Center, NASA Ames, Quantum Artificial Intelligence Laboratory (QuAIL), NASA Ames Research Center
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Vojtech Vlcek
University of California, Santa Barbara