The present disclosure is directed, in general, to (1) nonlinear optical (NLO) chromophores containing 3-aminocyclohex-2-en-1-one based donor groups, including (2) compositions/materials/resistive layers comprising NLO chromophores containing 3-aminocyclohex-2-en-1-one based donor groups, and the methods of making the compositions/materials/resistive layers comprising NLO chromophores containing 3-aminocyclohex-2-en-1-one based donor groups (e.g., methods of drying and/or poling, and the like), (3) uses of NLO chromophores containing 3-aminocyclohex-2-en-1-one based donor groups in electro-optic devices (e.g., EOMs).