Abstract
Herewereporta second-order nonlinear optical (NLO) material [C(NH2)3]3C3N3S3(GU3TMT), consisting ofπ-conjugated planar (C3N3S3)3-and triangular [C(NH2)3]+groups. Interestingly, GU3TMT exhibits large NLO response (2.0x KH2PO4) and moderate birefringence 0.067 at550 nm, even though (C3N3S3)3-and [C(NH2)3]＋do not exhibit the most favorable arrangement in the structure of GU3TMT. First-principles calculations suggest that NLO properties mainly originate from the highlyπ-conjugated (C3N3S3)3-rings, and theπ-conjugated [C(NH2)3]＋triangles contribute much less to the overall NLO response. This work will inspire new thoughts with in-depth on the role ofπ-conjugated groups in NLO crystals.
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