Abstract
Practical ultraviolet nonlinear optical (NLO) crystals are indispensable in modern scientific equipment and solar‐blind communication systems. Herein, a new hydroisocyanurate NLO crystal, Cs3Na(H2C3N3O3)4·3H2O (1), was grown by a facile aqueous solution method. It features a two‐dimensional layered structure composed of coplanar large π‐conjugated 2∞[H2C3N3O3]– isocyanurate ribbons. More importantly, it exhibits concurrently short ultraviolet phase‐matching capability (λpm ≈ 227 nm) and considerable second‐harmonic‐generation response (deff ≈ 2/3 KDP) resulting from the π‐conjugated (H2C3N3O3)– six‐membered ring units. First principles calculations were employed to elaborate its delocalized π‐bonds and strong interaction between the Cs+ cations and (H2C3N3O3)– anionic groups. Consequently, 1 will be a promising ultraviolet NLO material for the fourth harmonic generation of Nd‐based lasers. Successful synthesis of the title compound also provides a new roadmap to discover new ultraviolet linear optical or NLO materials in metal hydroisocyanurates.
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