Exploring the Vibrational Stark Effect in Fullerene and Derivatives from First Principles

ORAL

Abstract

Fullerene (C60) and its derivatives have played a central role in molecular and organic electronics, where its electron affinity and high symmetry result in key functionality. Understanding the impact of local fields on C60 properties in situ is of considerable interest, and here we determine how electric fields alter vibrational modes via the vibrational Stark effect. Using density functional theory-based finite-difference approach, we calculate the shifts in mode energy and symmetry in electric fields in gas-phase C60, PCBM, and other derivatives of fullerene. We examine the effect of high and low symmetry electronic field orientations, symmetry breaking functionalization, and doping on the the magnitude and mode-dependence of the vibrational Stark effect. The implications for fullerene-based materials under device conditions is discussed. This work is supported by DOE and computational resources were provided by NERSC.

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Authors

  • Peter Doak

    Department of Chemistry, UC-Berkeley; Molecular Foundry LBNL, Molecular Foundry, Lawrence Berkeley National Laboratory and Department of Chemistry, University of California, Berkeley

  • Yajing Li

    Department of Physics, Rice University, Department of Physics and Astronomy, Rice Univ

  • Douglas Natelson

    Department of Physics \& Astronomy, Rice University, Department of Physics, Rice University, Department of Physics and Astronomy, Rice University, Rice University, Department of Physics and Astronomy, 6100 Main St., Houston, TX 77005, Department of Physics and Astronomy, Rice Univ, Rice U

  • Leeor Kronik

    Department of Materials and Interfaces, Weizmann Institute of Science, Weizmann Institute of Science, Israel, Dept. Materials and Interfaces, Weizmann Institute, Weizmann Institute of Science, Department of Materials and Interfaces, Weizmann Institute of Science, Rehovoth 76100, Israel, Dept. of Materials and Interfaces, Weizmann Institute of Science, Rehovot 7610001, Department of Materials and Interfaces, Weizmann Institute of Science, Israel

  • Jeffery B. Neaton

    Department of Physics, UC-Berkeley; Molecular Foundry, LBNL, Molecular Foundry, LBNL, Department of Physics, UC Berkeley, Molecular Foundry, LBNL and Dept. Physics, UC Berkeley, Molecular Foundry, Lawrence Berkeley National Laboratory and Department of Physics, University of California, Berkeley, UC Berkeley, Dept of Physics; Materials Science Division, LBNL, Molecular Foundry, Lawrence Berkeley National Laboratory; Department of Physics, UC-Berkeley, The Molecular Foundry, LBNL; Dept. of Physics, University of California, Berkeley, Lawrence Berkeley National Laboratory, UC Berkeley Department of Physics, Lawrence Berkeley Natl Lab and Department of Physics, UC-Berkeley, Physics Department, UC Berkeley; Molecular Foundry, Lawrence Berkeley National Lab