Transcending the Trade-off in Refractive Index and Abbe Number for Highly Refractive Polymers: Synergistic Effect of Polarizable Skeletons and Robust Hydrogen Bonds

[Image: see text] High-refractive-index polymers (HRIPs) are attractive materials for the development of optical devices with high performances. However, because practical components and structures for HRIPs are limited from the viewpoint of synthetic techniques, it has proved difficult using traditional strategies to enhance the refractive index (RI) of HRIPs to more than a certain degree (over 1.8) while maintaining their visible transparency. Here, we found that poly(phenylene sulfide) (PPS) derivatives featuring both methylthio and hydroxy groups can simultaneously exhibit balanced properties of an ultrahigh RI of n(D) = 1.85 and Abbe number of ν(D) = 20 owing to the synergistic effect of high molar refraction and dense intermolecular hydrogen bonds (H-bonds). This brand new strategy is anticipated to contribute to the development of HRIPs displaying ultrahigh RI with adequate Abbe numbers beyond the empirical n(D)–ν(D) threshold, which has not been achieved to date.