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Charge redistribution and polarization energy of organic molecular crystals

2001/06/05 by E. V. Tsiper, Z. G. Soos · 2 citations
Chemistry · Materials Science · Physics and Astronomy · #Chemical Thermodynamics and Molecular Structure #Nonlinear Optical Materials Research #Photochemistry and Electron Transfer Studies #cond-mat

paper · pdf · doi:10.1103/physrevb.64.195124

12 pages, 5 figures inlined

arxiv created 2001/06/05 · openalex publication_date 2001/10/22 · arxiv updated 2009/11/30 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28

Abstract

We present an approach to electronic polarization in molecular solids treated as a set of quantum systems interacting classically. Individual molecules are dealt with rigorously as quantum-mechanical systems subject to classical external fields created by all other molecules and, possibly, external sources. Self-consistent equations are derived for induced dipoles and for atomic charges whose redistribution in external fields is given explicitly by an atom-atom polarizability tensor. Electronic polarization is studied in two representative organic molecular crystals, anthracene and perylenetetracarboxylic acid dianhydride, and contrasted to previous results for systems of polarizable points. The stabilization energies of the neutral lattice, of isolated anions and cations, and of cation-anion pairs are found. Charge redistribution on ions is included. The dielectric tensors of crystals are successfully related to gas-phase properties and provide consistency checks on polarization energies. The procedure is generally applicable to organic crystals in the limit of no intermolecular overlap.

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