Efficient calculation of level alignment at weakly coupled molecule-metal interfaces using substrate screening within the GW approach

ORAL

Abstract

The physics of level alignment at molecule-metal interfaces can often be accurately captured by the ab initio GW approach. However, the computational cost for such GW calculations for typical interfaces is significant, given their large system size and chemical complexity. In the past, approximate self-energy corrections constructed from image-charge models have been used to compute level alignment with good accuracy. However, this approach neglects dynamical effects of the polarizability and requires the definition of an image plane. In this work, we propose a new approximation for GW calculations of molecule-metal interfaces, where we greatly simplify the evaluation of the polarizability of the combined system. This is done by first computing the polarizability of each individual system in smaller cells, followed by unfolding and interpolation techniques to efficiently combine these quantities. Overall, this approach greatly reduces the computational cost for GW calculations of level alignment without sacrificing the accuracy. Moreover, this approach captures both dynamical and nonlocal polarization effects without the need to invoke a classical image charge expression. We benchmark our approximation for the case of a benzene molecule physisorbed on Al(111) surface.

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Presenters

  • Zhenfei Liu

    • Department of Chemistry, Wayne State University

Authors

  • Zhenfei Liu

    • Department of Chemistry, Wayne State University

  • Felipe Da Jornada

    • Department of Physics, University of California, Berkeley
    • Department of Physics, University of California at Berkeley and Materials Sciences Division, Lawrence Berkeley National Laboratory
    • Physics, University of California at Berkeley
    • Lawrence Berkeley National Laboratory
    • University of California at Berkeley and Lawrence Berkeley National Laboratory
    • Physics, University of California, Berkeley
    • UC Berkeley and Lawrence Berkeley National Lab
    • Lawrence Berkeley National Lab
    • Lawrence Berkeley National Lab and University of California, Berkeley

  • Steven G. Louie

    • Physics, UC Berkeley
    • University of California, Berkeley
    • Department of Physics, University of California, Berkeley
    • Physics Department, UC Berkeley and Lawrence Berkeley National Lab
    • Department of Physics, University of California at Berkeley and Materials Sciences Division, Lawrence Berkeley National Laboratory
    • Physics, University of California at Berkeley
    • University of California at Berkeley and Lawrence Berkeley National Lab
    • University of California at Berkeley and Lawrence Berkeley National Laboratory
    • Physics, University of California, Berkeley
    • UC Berkeley and Lawrence Berkeley National Lab
    • Physics, University of California - Berkeley
    • Physics and Materials Sciences, University of California at Berkeley and Lawrence Berkeley National Laboratory
    • Lawrence Berkeley National Lab and University of California, Berkeley
    • University of California - Berkeley, Lawrence Berkeley National Laboratory

  • Jeffrey B Neaton

    • Molecular Foundry, Lawrence Berkeley National Lab
    • University of California, Berkeley
    • Lawrence Berkeley National Laboratory
    • Molecular Foundry, Lawrence Berkeley National Laboratory
    • Department of Physics, University of California, Berkeley
    • UC Berkeley/Lawrence Berkeley Natl Lab
    • Lawrence Berkeley National Lab, Berkeley, CA
    • Physics, University of California, Berkeley
    • Molecular Foundry, LBNL; UC Berkeley; Kavli ENSI
    • Lawrence Berkeley National Laboratory, University of California - Berkeley, Kavli Energy NanoSciences Institute at Berkeley