Quasiparticle energy level alignment of a PTCDA-MoS<sub>2</sub> bilayer from first-principles GW calculations

ORAL

Abstract

Two-dimensional (2D) transition metal dichalcogenide (TMD) semiconductor crystals are highly sensitive to their environments, and molecular adsorbates decorating the 2D material surfaces constitute a route to tuning their electronic and optical properties. Here, we use a first-principles GW approach to compute the quasiparticle (QP) energies and energy level alignment at an interface formed by an atomically-flat molecular PTCDA monolayer and a MoS2 monolayer. To reduce the computational cost, we use the substrate screening GW approach which reduces the expense associated with computing the interface polarizability by using smaller supercells. We show that the respective band gaps of the molecular PTCDA and MoS2 substrate are both modified upon interface formation and we explore the QP energy level alignment at the interface. We also discuss how a molecular monolayer may controllably alter the photophysics of a TMD monolayer.

*This work is supported by the Center for Computational Study of Excited-state Phenomena in Energy Materials (C2SEPEM), funded by the US Department of Energy (DOE). AC acknowledges the support from Wallonie Bruxelles International. Computational resources are provided by NERSC.

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Presenters

  • Aurelie Champagne

    • Lawrence Berkeley National Laboratory

Authors

  • Aurelie Champagne

    • Lawrence Berkeley National Laboratory

  • Olugbenga M Adeniran

    • Wayne State University

  • Jonah B Haber

    • University of California, Berkeley
    • University of California, Berkeley; Lawrence Berkeley National Laboratory
    • Department of Physics, University of California, Berkeley
    • Department of Physics, University of California, Berkeley, CA 94720; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720.

  • Fauzia Mujid

    • University of Chicago
    • Department of Chemistry, University of Chicago
    • The University of Chicago

  • Jiwoong Park

    • University of Chicago
    • Department of Chemistry, University of Chicago

  • Zhenfei Liu

    • Wayne State University

  • Jeffrey B Neaton

    • Lawrence Berkeley National Laboratory
    • University of California, Berkeley; Lawrence Berkeley National Laboratory; Kavli Energy NanoSciences Institute at Berkeley
    • Department of Physics, University of California, Berkeley; Materials Sciences Division, Lawrence Berkeley National Laboratory; Kavli Energy NanoScience Institute at Berkeley
    • Department of Physics, University of California, Berkeley, CA 94720; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720; Kavli Energy Nano