First-Principles Studies of the Vibrational Stark Effect in C60

ORAL

Abstract

C60 has played a central role in molecular and organic electronics, where coupling between charge and vibrational degrees of freedom is of paramount importance. Recent surface-enhanced Raman scattering (SERS) studies of C60-Au junctions have reported significant shifts in vibrational mode frequencies with applied bias. Here we compute the magnitude of the vibrational Stark effect in gas-phase C60 and seek to understand and simulate the shifts in Raman mode frequencies observed in these electromigration junction-SERS experiments. Using density functional theory and a finite-difference approach, we calculate trends in the vibrational Stark effect for different modes of gas-phase C60, comparing directly to experiment and assessing the role of substrate-induced charging and external electric fields. This work supported by DOE and computational resources provided by NERSC.

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Authors

  • Peter Doak

    • Department of Chemistry, UC-Berkeley, Molecular Foundry, LBNL

  • Yajing Li

    • Department of Physics and Astronomy, Rice University
    • Department of Physics and Astronomy, MS 61, Rice University

  • Douglas Natelson

    • Department of Physics and Astronomy and Department of Computer and Electrical Engineering, Rice University, 6100 Main St, Houston, TX 77005
    • Department of Physics and Astronomy, Rice University
    • Department of Physics \& Astronomy, Rice University

  • Leeor Kronik

    • Weizmann Institute of Science, Israel
    • Department of Materials and Interfaces, Weizmann Institute of Science

  • Jeffrey Neaton

    • Molecular Foundry, LBNL
    • Lawrence Berkeley National Lab
    • Lawrence Berkeley National Laboratory