6533b7dafe1ef96bd126e01f

RESEARCH PRODUCT

Nonlinear optical susceptibilities of polysilanes: exciton effect

Wu-pei SuMichael SchreiberS. Abe

subject

chemistry.chemical_classificationCondensed matter physicsAbsorption spectroscopyChemistryExcitonGeneral Physics and AstronomyPolymerCondensed Matter::Mesoscopic Systems and Quantum Hall EffectMolecular physicsNonlinear opticalchemistry.chemical_compoundCoulombPolysilanePhysical and Theoretical ChemistryAbsorption (electromagnetic radiation)

description

Abstract Third-order nonlinear optical susceptibilities of σ-conjugated one-dimensional polymers have been calculated in a tight-binding model by taking account of the formation of excitons due to long-range Coulomb interactions. The spectrum of third-harmonic generation (THG) exhibits peaks due to excitons as well as unbound electron—hole states, in contrast to the linear absorption spectrum which is dominated by the lowest exciton state. The results are in excellent agreement with recent experiments in polysilanes not only for THG but also for linear absorption, two-photon absorption, and electroabsorption in a mutually consistent way.

https://doi.org/10.1016/0009-2614(92)85493-t