Qi Xin, Helland Sarah, Lowe Christopher D, Larson Helen, Cui Jianming, Zheng Renyu, Monahan Madison, Chen Chun-Long, De Yoreo James, Pfaendtner Jim, Cossairt Brandi
Department of Chemistry, Dartmouth College,Hanover, New Hampshire 03755, United States.
Department of Chemistry, University of Washington, Seattle, Washington 98195, United States.
Nano Lett. 2025 Mar 12;25(10):3989-3996. doi: 10.1021/acs.nanolett.5c00024. Epub 2025 Feb 25.
Combining the advantages of structural programmability in sequence-defined biomimetic molecules and the controllable packing geometry in nanoparticle superlattices, we demonstrate a self-assembled organic-inorganic superlattice whose structure can be altered with the slightest change in the sequence of the organic counterpart. Here, oleate-coated CdS quantum dots (QDs) form a square-packed superlattice with a 1:1 molar equivalence of a diblock amphiphilic peptoid (NbrpeDig) in chloroform. In contrast, no apparent structure is observed in the organic solvent alone. Based on theoretical evidence, we show that the assembly is a binary superlattice where both the CdS QDs and the peptoids serve as building blocks and further predict a correlation between the superlattice structure and the peptoid sequence. The computationally guided prediction is validated by experiments where superlattice transformation is observed with modified peptoids. The mechanism identified in our work inspires new ways to control and tune organic-inorganic hybrid nanomaterial self-assembly.
结合序列定义的仿生分子的结构可编程性和纳米粒子超晶格中可控的堆积几何结构的优点，我们展示了一种自组装的有机-无机超晶格，其结构会随着有机对应物序列的微小变化而改变。在这里，油酸包覆的硫化镉量子点（QDs）与二嵌段两亲性类肽（NbrpeDig）在氯仿中以1:1的摩尔当量形成方形堆积的超晶格。相比之下，单独在有机溶剂中未观察到明显的结构。基于理论证据，我们表明该组装是一种二元超晶格，其中硫化镉量子点和类肽均作为构建块，并进一步预测了超晶格结构与类肽序列之间的相关性。通过使用修饰类肽观察到超晶格转变的实验验证了计算指导的预测。我们工作中确定的机制激发了控制和调节有机-无机杂化纳米材料自组装的新方法。
