Acentric lattice electro-optic materials by rational design

Abstract

Quantum and statistical mechanical calculations have been used to guide the improvement of the macroscopic electro-optic activity of organic thin film materials to values greater than 300 pm/V at telecommunication wavelengths. Various quantum mechanical methods (Hartree-Fock, INDO, and density functional theory) have been benchmarked and shown to be reliable for estimating trends in molecular first hyperpolarizability, β, for simple variation of donor, bridge, and acceptor structures of charge-transfer (dipolar) chromophores. β values have been increased significantly over the past five years and quantum mechanical calculations suggest that they can be further significantly improved. Statistical mechanical calculations, including pseudo-atomistic Monte Carlo calculations, have guided the design of the super/supramolecular structures of chromophores so that they assemble, under the influence of electric field poling, into macroscopic lattices with high degrees of acentric order. Indeed, during the past year, chromophores doped into single- and multi-chromophore-containing dendrimer materials to form binary glasses have yielded thin films that exhibit electro-optic activities at telecommunication wavelengths of greater than 300 pm/V. Such materials may be viewed as intermediate between chromophore/polymer composites and crystalline organic chromophore materials. Theory suggests that further improvements of electro-optic activity are possible. Auxiliary properties of these materials, including optical loss, thermal and photochemical stability, and processability are discussed. Such organic electro-optic materials have been incorporated into silicon photonic circuitry for active wavelength division multiplexing, reconfigurable optical add/drop multiplexing, and high bandwidth optical rectification. A variety of all-organic devices, including stripline, cascaded prism, Fabry-Perot etalon, and ring microresonator devices, have been fabricated and evaluated.