Modeling the Optical Behavior of Complex Organic Media: From Molecules to Materials

    Authors

    P. A. Sullivan; H. L. Rommel; Y. Takimoto; S. R. Hammond; D. H. Bale; B. C. Olbricht; Y. Liao; J. Rehr; B. E. Eichinger; A. K. Y. Jen; P. J. Reid; L. R. Dalton;B. H. Robinson

    Comments

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    Abbreviated Journal Title

    J. Phys. Chem. B

    Keywords

    HYPER-RAYLEIGH SCATTERING; BOND-LENGTH ALTERNATION; ELECTROOPTIC; ACTIVITY; 1ST HYPERPOLARIZABILITY; 2ND-HARMONIC GENERATION; CONJUGATED; MOLECULES; CHROMOPHORES; POLARIZATION; LIQUIDS; POLYMER; Chemistry, Physical

    Abstract

    For the past three decades, a full understanding of the electro-optic (EO) effect in amorphous organic media has remained elusive. Calculating a bulk material property from fundamental molecular properties, intermolecular electrostatic forces, and field-induced net acentric dipolar order has proven to be very challenging. Moreover, there has been a gap between ab initio quantum-mechanical (QM) predictions of molecular properties and their experimental verification at the level of bulk materials and devices. This report unifies QM-based estimates of molecular properties with the statistical mechanical interpretation of the order in solid phases of electric-field-poled, amorphous, organic dipolar chromophore-containing materials. By combining interdependent statistical and quantum mechanical methods, bulk material EO properties are predicted. Dipolar order in bulk, amorphous phases of EO materials can be understood in terms of simple coarse-grained force field models when the dielectric properties of the media are taken into account. Parameters used in the statistical mechanical modeling are not adjusted from the QM-based values, yet the agreement with the experimentally determined electro-optic coefficient is excellent.

    Journal Title

    Journal of Physical Chemistry B

    Volume

    113

    Issue/Number

    47

    Publication Date

    1-1-2009

    Document Type

    Article

    Language

    English

    First Page

    15581

    Last Page

    15588

    WOS Identifier

    WOS:000271826300021

    ISSN

    1520-6106

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