Conjugated Polycyanines: A New Class of Materials with Large Third‐Order Optical Nonlinearities

Abstract

A fully conjugated polycyanine (AJMPC02) showing a very large Re(γ) value of −9.0 × 10−57 mks at 1.3 μm is synthesized. It is used as a host polymer for anionic TCF‐cyanines for creating a complementary polymeric cyanine salt complex, which exhibits a Re(γ) value of −5.6 × 10−57 mks at 1.3 μm. A good optical quality thin film based on AJMPC02‐TCF gives a Re(γ) value of −2.1 × 10−18 mks at 1.3 μm and −8.5 × 10−19 mks at 1.55 μm, which are among the highest values reported for molecular materials, and much higher than those derived from silicon.

Synthesis, optical and electrochemical properties of a series of push-pull dyes based on the 2-(3-cyano-4,5,5-trimethylfuran-2(5H)-ylidene)malononitrile (TCF) acceptor

“…It has to be noticed that TCF6 possesses the most red-shifted absorption of the series with a non-negligible contribution in the near-infrared region. Such an absorption at long wavelength is relatively unusual for push-pull dyes comprising TCF as the electron acceptor and an absorption in this region was only reported for polymethine dyes [70][71][72] or indolizinebased dyes in the literature. [73] Based on their chemical structures, indolizine-based dyes are the most similar dyes compared to the TCF-based dyes examined in this work due to their donor-spacer-acceptor structures and the absorption maximum reported for one of the indolizine-based dyes at 758 nm (AH25) is directly related to the use of an extended electron donor, as in the case of TCF6.…”

Systematic study on the optimization of a bis(N,N-diethyl)aniline based NLO chromophore via a stronger electron acceptor, extended π-conjugation and isolation groups

“…As in a reference reported earlier, b tot has been calculated at the 6-31+G* level under vacuum. 29 From this, the scalar quantity of b tot can be computed from the x, y, and z components according to the following equation:…”

Temporal and polarization dependence of the nonlinear optical response of solvents

“…9(a) and 9(b), respectively, have been extensively studied in our previous work using the dual-arm Z-scan technique [63,64]. A large and negative NLR along with a relatively small two-photon absorption is measured at wavelengths approaching their linear absorption edge, making them possible candidate materials for organic all-optical switching application [63,[65][66][67]. To explore the physical origins of this large and negative NLR, we make two solution samples by dissolving AJBC3701 and YZ-V-69 into DMF and CCl 4 , respectively, and perform BD measurements on them to resolve the temporal dynamics of the NLR.…”