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Two new diamond-like (DL) chalcogenides, Li 2 MgGeSe 4 and Li 2 MgSnSe 4 , have been successfully synthesized using a conventional high-temperature solid-state method. The two compounds crystallize in the non-centrosymmetric space group Pmn 2 1 with a = 8.402 (14) Å, b = 7.181 (12) Å, c = 6.728 (11) Å, Z = 2 for Li 2 MgSnSe 4 , and a = 8.2961 (7) Å, b = 7.0069 (5) Å, c = 6.6116 (6) Å, Z = 2 for Li 2 MgGeSe 4 . The calculated results show that the second harmonic generation (SHG) coefficients of Li 2 MgSnSe 4 ( d  33 = 12.19 pm/v) and Li 2 MgGeSe 4 ( d  33 = -14.77 pm/v), mainly deriving from the [MSe 4 ] (M = Ge, Sn) tetrahedral units, are close to the one in the benchmark AgGaS 2 ( d  14 = 13.7 pm/V). The calculated band gaps for Li 2 MgSnSe 4 and Li 2 MgGeSe 4 are 2.42 and 2.44 eV, respectively. Moreover, the two compounds are the first series of alkali and alkaline-earth metal DL compounds in the I 2 -II-IV-VI 4 family, enriching the structural diversity of DL compounds.

Syntheses, Structures and Properties of Alkali and Alkaline Earth Metal Diamond-Like Compounds Li2MgMSe4 (M = Ge, Sn)