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Hydrogen-bonding effectively constructs polar chains in UV nonlinear optical materials, indicating a novel design approach.
Non-centrosymmetric (NCS) materials underpin a host of emerging technologies-from high-power lasers to optical communications and sensors-yet their targeted design remains a formidable challenge. Herein, we introduce a "Hydrogen-Bond-Directed Modular Assembly" strategy for the rational construction of ultraviolet (UV) nonlinear optical (NLO) crystals. In this strategy, programmable hydrogen-bonding schemes serve as a predictive handle to propagate local asymmetry into a macroscopic polar network. Using an explicit modular design algorithm, we selected three building units-C3H3O4 -, C4H5O4 -, and C(NH2)3 +-and assembled them into two one-dimensional polar chain modules, [C(NH2)3C3H3O4]∞ and [C(NH2)3C4H5O4]∞. These modules crystallize as two new UV NLO materials, C(NH2)3C3H3O4 and C(NH2)3C4H5O4, which exhibit excellent linear and nonlinear optical properties. By shifting the synthetic focus from serendipitous screening to hydrogen-bond-guided, module-level engineering, our strategy establishes a predictive framework for the a priori design of NCS structures with tailored properties.
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Wu et al. (2025) studied this question.
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