Abstract
Deep-UV, (wavelength λ<200nm) nonlinear-optical (NLO) silicate crystals have long been troubled by weak second-harmonic-generation (SHG) effect and common non-phase-matchability, leading to the stagnation of silicate research, despite abundant reserves of silicates on the earth. Representative and simple α-SiO2 is an ideal structural prototype toward improving silicate NLO performance by exploring efficient strategies. Herein, through two-step structural modulations based on fundamental "distortion and superposition" principles of NLO response, two deep-UV NLO crystals taking α-SiO2 as a structural template, Na2BeSiO4 and Li2BeSiO4, are synthesized successively. By providing flexible coordination BeO4 tetrahedra for rigid tetrahedral SiO4 that induces distortion of SiO4, Na2BeSiO4 achieves significant enhancement of phase-matchable SHG effect of 15×α-SiO2. Further, by introducing a low coordination number of Li+ cations that stimulates uniform orientation of SiO4, Li2BeSiO4 exhibits the strongest phase-matchable SHG effect as large as 40×α-SiO2 among the universal SiO4-governed NLO silicates. Also, computational investigations support the rationality of the structural modulations well. Such efficient structural modulations can greatly promote the exploration and rational design of NLO silicates.
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