Deep-UV, (wavelength λ < 200 nm) 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-SiO 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-SiO as a structural template, NaBeSiO and LiBeSiO, are synthesized successively. By providing flexible coordination BeO tetrahedra for rigid tetrahedral SiO that induces distortion of SiO, NaBeSiO achieves significant enhancement of phase-matchable SHG effect of 15 × α-SiO. Further, by introducing a low coordination number of Li cations that stimulates uniform orientation of SiO, LiBeSiO exhibits the strongest phase-matchable SHG effect as large as 40 × α-SiO among the universal SiO-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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http://dx.doi.org/10.1002/smll.202408360 | DOI Listing |
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