0000000000276031
AUTHOR
Wu-pei Su
Excitons and nonlinear optical spectra in conjugated polymers.
Excitons in conjugated polymers are studied theoretically in the Su-Schrieffer-Heeger model supplemented by long-range Coulomb interactions. The relationship between exciton energies and basic interaction parameters is clarified. Linear and third-order nonlinear optical susceptibilities (two-photon absorption, electroabsorption, and third-harmonic generation) have been calculated, elucidating the significance of singlet and triplet excitons and unbound electron-hole pairs. Using only moderate interaction strength, various experiments in polydiacetylene can be interpreted in a consistent way
Nonlinear optical susceptibilities of polysilanes: exciton effect
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.
Singlet and triplet excitons in conjugated polymers.
Exciton states in conjugated polymers are theoretically studied in the Su-Schrieffer-Heeger model supplemented by long-range Coulomb interactions. The relationship between exciton energies and basic interaction parameters is clarified, demonstrating the special nature of one-dimensional excitons. The binding energies of the lowest singlet and triplet excitons depend sensitively upon the on-site Coulomb energy. Relevant experiments in polydiacetylene can be explained by the present model using moderate interaction strength.
Nonlinear optical spectra of conjugated polymers: Effect of long-range coulomb interactions
Abstract Nonlinear optical spectra of conjugated polymers are theoretically studied in the Su-Schrieffer-Heeger model supplemented by long-range Coulomb interactions. Excitonic correlation for electron-hole excitations in explicitly taken into account by a standard method. Nonlinear susceptibilities χ (3) are calculated numerically with a standard sum-over-states method for finite chains (up to 1000 sites). Using moderate interaction strength, our calculations can reproduce many distinct features observed in the linear and nonlinear spectra (two-photon absorption, third-harmonic generation, and electroabsorption) of polydiacetylenes and some other polymers. Especially, a hump in the spectru…