Efficient poling and thermal crosslinking of randomly bonded main-chain polymers for stable second-order nonlinearities

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Abstract
We report our second‐harmonic generation study of a new crosslinked main‐chain polymer system for second‐order nonlinear optics (NLO). In this unique polymer system, the rigid second‐order NLO chromophores are randomly bonded in the main chain with flexible links between the rigid chromophores to allow electric poling at or above the glass transition temperature. A thermal crosslinker is added to crosslink the polymer backbone during electric poling. The combination of the flexible chain segments and crosslinking allows us to achieve a high degree of alignment (〈cos3θ〉≊0.34) and long‐term (≳2500 h) temporal stability of the nonlinearities.