由种子动力学控制的核碱基自组装中的组合压缩
Combinatorial Compression in Nucleobase Self-Assembly Governed by Seeding Kinetics
AI总结：
以腺嘌呤、胸腺嘧啶和尿嘧啶的过饱和混合物为模型，研究竞争超分子结晶。发现三元混合物结晶慢且低效，而预形成的晶种可促进其有序生长，此过程为动力学压缩，为选择分子混合物组成途径提供机制。
摘要：
化学复杂混合物的结晶不仅受热力学稳定性控制，还受成核和生长过程中结构相关组分间的动力学竞争影响。本文以腺嘌呤（A）、胸腺嘧啶（T）和尿嘧啶（U）的过饱和水性混合物为竞争性超分子结晶的最小模型进行研究。结果表明三元A+T+U混合物结晶比二元体系更慢且效率更低，预形成的A+T晶种可挽救其有序生长，此过程为动力学压缩，为选择分子混合物组成途径提供了一种机制。
英文摘要：
Crystallization from chemically complex mixtures is governed not only by thermodynamic stability but also by kinetic competition among structurally related components during nucleation and growth. When multiple compatible molecules compete for incorporation into early nuclei, the number of possible local recognition motifs can expand, delaying access to productive crystalline pathways. Here, we investigate this effect using supersaturated aqueous mixtures of the canonical nucleobases adenine (A), thymine (T), and uracil (U) as a minimal model for competitive supramolecular crystallization. Time-resolved turbidity measurements showed that ternary A+T+U mixtures crystallize more slowly and less efficiently than selected binary systems, despite containing individually crystallizable components. This inhibition is consistent with competition-induced kinetic frustration, where structurally similar hydrogen-bonding partners compete during early nucleation, delaying formation of a productive crystalline nucleus. We then show that preformed A+T crystalline seeds rescue ordered growth from the ternary mixture. Seeding sharply reduces the lag time, increases the apparent nucleation/onset rate, and redirects the solid product toward the A+T crystalline pathway, as confirmed by HPLC. Thus, the seed acts not only as a nucleation accelerator but as a selector of molecular composition and assembly trajectory within a multicomponent solution. We describe this process as kinetic compression: the reduction of accessible supramolecular assembly pathways through amplifications of selected productive growth pathways. These findings establish seeded crystallization as a mechanism for selecting compositional pathways in competitive molecular mixtures and suggest a physical route by which ordered molecular subsets can emerge from chemically complex environments.
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