Photocontrol and optical switching of birefringence (Δn) in a poly(methacrylate) copolymer liquid crystal films substituted with 4-methoxyazobenzene and 4(4-methoxycinnamoyloxy)biphenyl side groups are described. Irradiating with linearly polarized 365 nm light and subsequently annealing generated uniaxial in-plane orientation of the films. Adjusting the exposure doses of nonpolarized (NP) 405 nm light regulated the generated Δn of 0.26–0.13, and after reannealing the initial value is completely restored. Optical control of the birefringence with response times of 50 ms is demonstrated when the films are exposed to NP 405 nm light at elevated temperatures.

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