A New Nonlinear Optical Material with N(CN)2− Anion.

Discovering new functional genes and developing high‐performance materials are the goals being pursued by scientists. In this work, we successfully obtained a second‐order nonlinear optical (NLO) material via the aqueous solution method, Y[N(CN)2]4[NH(C2H5)3] ⋅ 3H2O, which is the first NLO material with the anionic group N(CN)2−. Remarkably, this material is not only strongly NLO‐active at 1064 nm with a response of about 2.8 × KH2PO4, but also possesses a short UV absorption edge of 250 nm. In‐depth first‐principles calculations illustrate well that the optical properties are mainly from the strong interaction of N, C and Y atoms. This result indicates that the N(CN)2− anion may be a new NLO functional gene. This work enriches the diversity of NLO functional genes and materials. [ABSTRACT FROM AUTHOR]