Electronic and optical properties of a metal-organic framework with ab initio many-body perturbation theory

ORAL

Abstract

With their unprecedented surface area, and their structural and chemical tunability, metal-organic frameworks (MOFs) are being thoroughly explored for applications related to gas storage. Less studied are their electronic, excited-state, and optical properties. Here we explored such properties of Mg-MOF-74 using a combination of density functional theory (DFT) and many-body perturbation theory (MBPT) within the GW approximation and the Bethe-Salpeter equation (BSE) approach. The near-gap electronic conduction states were found to fall into two distinct categories: molecular-like and 1d-dispersive. Further, using the BSE approach, we predict a strongly anisotropic absorption spectrum, which we link to the nature of its strongly-bound excitons. Our calculations are found to be in good agreement with experimental absorption spectra, validating our theoretical approach.

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Authors

  • Kristian Berland

    Univ. of Oslo, Dept. Physics, SMN

  • Kyuho Lee

    Lawrence Berkeley National Lab., Molecular Foundry

  • Sahar Sharifzadeh

    Boston University, Dept. of Electrical and Computer Engineering, Boston University

  • Jeffrey Neaton

    Univ of California - Berkeley, Molecular Foundry, Lawrence Berkeley National Laboratory, Physics Department, UC Berkeley \& Molecular Foundry, LBNL \& Kavli Energy NanoSciences Institute at Berkeley, Berkeley, University of California at Berkeley, University of California, Berkeley; Lawrence Berkeley National Laboratory, Dept. of Physics, UC Berkeley, Molecular Foundry, Lawrence Berkeley National Laboratory; Department of Physics, University of California-Berkeley, University of California, Berkeley and Lawrence Berkeley National Lab, Molecular Foundry, Lawrence Berkeley National Laboratory, and Department of Physics, UC-Berkeley, Lawrence Berkeley National Laboratory