Record-high near-band-edge optical nonlinearities and two-level model correction of poled polymers by spectroscopic electromodulation and ellipsometry

摘要

The determination of nonlinearities near the band edge of organic and polymeric electro-optic(EO)materials is important from the viewpoint of molecular nonlinear optics(NLO)and photonic device applications.Based on transmission-mode Stark effect electromodulation(EM)spectroscopy,we study the electric-field-induced changes in optical absorption and refraction of newly developed EO polymers from the visible to near-infrared(NIR)wavelengths and report record-high near-band-edge complex EO effects from poled thin films.Values ofΔn andΔk up to 10^(-3) and 10^(-2) are found at an applied electric field of 2.0×10^(5)-3.0×10^(5)V/cm.The study of linear optical properties of poled films by spectroscopic ellipsometry shows large polinginduced birefringence and a nearly two-fold increase in the extinction coefficients at the extraordinary polarization.Through the Kramers-Kronig analysis,we obtained the real and imaginary second-order nonlinear coefficients up to~3,500 and~5,600 pm/V,respectively,which are believed to be the highest NLO coefficients of poled polymers through the resonance enhancement.Our approach goes beyond the previous works,applicable only to several discrete wavelengths,to a full-spectral analysis with independent verification of slab waveguide measurements.By considering both the electroabsorption and electrorefraction effects,our study overcomes the limitation of the classic qualitative two-level model and provides a quantitative understanding of near-resonance optical nonlinearities of organic EO materials.It can inspire the exploration of high-speed,absorptive,or phase-shifting light-modulators using EO polymers for on-chip applications.