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Record-high near-band-edge optical nonlinearities and two-level model correction of poled polymers by spectroscopic electromodulation and ellipsometry
作者姓名:Taili Liu  Di Zhang  Md Rashedul Huqe  Wen Wang  Juan Antonio Zapien  Sai-Wing Tsang  Jingdong Luo
作者单位:Shenzhen Research Institute;Department of Chemistry;Department of Materials Science and Engineering;Center of Super-Diamond and Advanced Films(COSDAF)
基金项目:supported by the Fundamental Research Project Funding from Shenzhen Science & Technology Innovation Committee (JCYJ20180507181718203);the National Natural Science Foundation of China (21975213);the Research Grants Council (RGC) of Hong Kong (11306320, 11303618, 11210218);the City University of Hong Kong (9610389, 9680263, 9610454);the Innovation and Technology Commission of Hong Kong (ITS/461/18)。
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 2.0×105-3.0×105V/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.

关 键 词:poled  polymers  ELECTROABSORPTION  electro-optic  effect  second-order  nonlinear  susceptibilities

Record-high near-band-edge optical nonlinearities and two-level model correction of poled polymers by spectroscopic electromodulation and ellipsometry
Taili Liu,Di Zhang,Md Rashedul Huqe,Wen Wang,Juan Antonio Zapien,Sai-Wing Tsang,Jingdong Luo.Record-high near-band-edge optical nonlinearities and two-level model correction of poled polymers by spectroscopic electromodulation and ellipsometry[J].中国科学 化学(英文版),2022,65(3):584-593.
Authors:Liu  Taili  Zhang  Di  Huqe  Md Rashedul  Wang  Wen  Zapien  Juan Antonio  Tsang  Sai-Wing  Luo  Jingdong
Institution:1.Shenzhen Research Institute, City University of Hong Kong, Shenzhen, 518057, China
;2.Department of Chemistry, City University of Hong Kong, Hong Kong SAR, China
;3.Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR, China
;4.Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Hong Kong SAR, China
;
Abstract:Science China Chemistry - 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...
Keywords:
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