Non-centrosymmetric arrangement in the solid state is a prerequisite for a molecule to exhibit second harmonic generation (SHG), yet the majority of achiral molecules crystallize in centrosymmetric lattices. Despite advances in circumventing the molecular preference for centrosymmetric structures, current screening methods of discovering SHG active materials need large quantities of parent material. Here, we present a function-based screening method that is designed to consume small quantities of parent material for screening a large pool of coformers that enhance the probability of discovering SHG active materials. With this method, ∼30 mg of a non-linear optical (NLO) chromophore, N-(2-aminoethyl)-4-nitro-2-ansidine (1), was sufficient for screening 50 coformers, resulting in five SHG active compounds. Crystal-structure analysis revealed that non-covalent interactions influence the disposition of NLO-phore dipoles and thus affect the bulk SHG properties. Quantum chemical calculations highlighted the coformer contribution toward the second-order susceptibility coefficients, providing a deeper understanding of the structure-property relationships in these SHG materials.

固态的非中心对称排列是分子表现出二次谐波生成（SHG）的先决条件，但大多数非手性分子在中心对称晶格中结晶。尽管在绕开中心对称结构的分子偏好方面取得了进展，但是发现SHG活性材料的当前筛选方法仍需要大量的母体材料。在这里，我们提出了一种基于功能的筛选方法，该方法旨在消耗少量的母体材料来筛选大量的共形成者，从而增加发现SHG活性物质的可能性。用这种方法，可得到约30 mg的非线性光学（NLO）生色团N-（2-氨基乙基）-4-硝基-2-ans啶（1）足以筛查50种共形成物，从而产生5种SHG活性化合物。晶体结构分析表明，非共价相互作用会影响NLO-phore偶极子的排列，从而影响整体SHG性质。量子化学计算突显了共成峰剂对二阶磁化系数的贡献，从而提供了对这些SHG材料中结构-性质关系的更深入了解。