Two novel compounds KZn4SbO7 (1) and KZn4Sb3O12 (2) having quasi-white light emission and second-harmonic generation are prepared, and their single-crystal structures are characterized as P63mc and R3 space groups, respectively. The crystal structure transition from high symmetry P63mc of 1 to low symmetry R3 of 2 arises from the large contents of Sb5+ diluter in wurtzite-type ZnO crystals (ionic ratio of Sb5+/Zn2+ = 1/4 and 3/4 for crystals 1 and 2). The lifetime and quantum efficiency of luminescence are measured, and the density of states and frequency doubling coefficients are calculated for the two compounds. The strong charge transfers from O2− to Sb5+, and blue-shifts of absorption edge and emission bands originate from a large Sb5+ ion content for compound 2. Further, large charge transfer from O2− to Sb5+ lead to high quantum efficiency and low lifetime, and weak second-harmonic generation intensity for compound 2.
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