Ab initio molecular design of third-order nonlinear optical susceptibilities of polysilanes

Tomoyuki Hamada

doi:10.1117/12.305437

17 April 1998 Ab initio molecular design of third-order nonlinear optical susceptibilities of polysilanes

Tomoyuki Hamada

Proceedings Volume 3281, Polymer Photonic Devices; (1998) https://doi.org/10.1117/12.305437
Event: Optoelectronics and High-Power Lasers and Applications, 1998, San Jose, CA, United States

Abstract

Third-order nonlinear optical susceptibilities (chi) ⁽³) of polysilanes were estimated both at molecular and crystalline levels, in order to establish a molecular design strategy of (chi) ⁽³) of polysilanes, by using an ab initio coupled perturbed Hartree-Fock (CPHF) method and the oriented-gas approximation. Molecular calculation results showed the main chain conformation of polysilanes directly affects second hyperpolarizabilities (gamma) of polysilane oligomers, and the trans planar oligomers have larger (gamma) than the 7/3 helical or alternating trans gauche (TGTG') oligomers, due to a stronger (sigma) -electron delocalization in their trans planar main chain. On the other hand, it was found that crystalline (chi) ⁽³) of polysilanes are influenced not only by the main chain confirmation, but also by the molecular weight of polysilane repeating unit M_Si. Based on those molecular and crystalline results, a strategy of molecular design of polysilane (chi) ⁽³) was proposed which predicts trans planar poly[dimetylsilane] may have the largest (chi) ⁽³) among polysilanes investigated so far, owing to its trans planar main chain and smallest M_Si.

Citation Download Citation

Tomoyuki Hamada "Ab initio molecular design of third-order nonlinear optical susceptibilities of polysilanes", Proc. SPIE 3281, Polymer Photonic Devices, (17 April 1998); https://doi.org/10.1117/12.305437

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