By a simple cross-substitution of A-site Li/Na in tetragonal tungsten bronze (TTB) structures, we successfully synthesized a new niobate compound, Pb2.15(Li0.25Na0.75)0.7Nb5O15, with a superstructure. This compound exhibits a strong second harmonic generation (SHG) up to ∼47 × KDP. The large SHG response is related to strengthened local distortion, manifesting cross-substitution as a possibly general route to improve the NLO effect in stiff and low symmetric structures.
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