“…In 2006, Mercier et al 13 first reported the transformation-induced NLO switchable phenomenon in a molecular-based compound, [{H 3 N(CH 2 ) 2 SS(CH 2 ) 2 NH 3 }PbI 5 ]•H 3 O. Subsequently, a series of molecular-based NLO switchable materials were discovered, such as [α-(H 3 N(CH 2 ) 2 S-S(CH 2 ) 2 NH 3 )BiI 5 , 14 (Hdabco + )(CF 3 COO − ), 15 bis(imidazolium) L -tartrate, 16,17 2-(hydroxymethyl)-2-nitro-1,3-propanediol, 18 (C 4 H 10 N)(CdCl 3 ), 19 dipropylammonium trichloroacetate, 20 (R-CTA) 2 CuCl 4 , 21 and (S-CTA) 2 CuCl 4 . 21 However, despite excellent NLO switchable performance, their bandgaps are relatively narrow on account of π-conjugated electrons, d-d or f-f transition, such as [α-(H 3 N(CH 2 ) 2 S-S(CH 2 ) 2 NH 3 ]BiI 5 (∼1.84 eV), 14 bis(imidazolium) L -tartrate (∼5.21 eV), 17 and dipropylammonium trichloroacetate (∼3.82 eV).…”