Qian Yiwen, da Silva Alessandra, Yu Emmy, Anderson Christopher L, Liu Yi, Theis Wolfgang, Ercius Peter, Xu Ting
Department of Materials Science and Engineering, University of California, Berkeley, CA, USA.
Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
Nat Commun. 2021 May 13;12(1):2767. doi: 10.1038/s41467-021-22950-2.
Orthogonal to guided growth of nanoparticle (NP) crystals using DNA or supramolecules, a trace amount of polymeric impurities (<0.1 wt.%) leads to reproducible, rapid growth of 3D NP crystals in solution and on patterned substrates with high yield. When polymers preferentially precipitate on the NP surfaces, small NP clusters form and serve as nuclei for NP crystal growth in dilute solutions. This precipitation-induced NP crystallization process is applicable for a range of polymers, and the resultant 3-D NP crystals are tunable by varying polymeric additives loading, solvent evaporation rate, and NP size. The present study elucidates how to balance cohesive energy density and NP diffusivity to simultaneously favor nuclei formation energetically and kinetic growth in dilute solutions to rapidly crystalize NPs over multiple length scales. Furthermore, the amount of impurities needed to grow NP crystals (<0.1%) reminds us the importance of fine details to interpret experimental observations in nanoscience.
与使用DNA或超分子引导纳米颗粒（NP）晶体生长不同，痕量的聚合物杂质（<0.1 wt.%）能使溶液中和图案化衬底上的三维NP晶体以高产率实现可重复的快速生长。当聚合物优先沉淀在NP表面时，会形成小的NP簇，并在稀溶液中作为NP晶体生长的晶核。这种沉淀诱导的NP结晶过程适用于多种聚合物，通过改变聚合物添加剂负载量、溶剂蒸发速率和NP尺寸，可以调节所得的三维NP晶体。本研究阐明了如何平衡内聚能密度和NP扩散率，以在稀溶液中同时在能量上有利于晶核形成和动力学生长，从而在多个长度尺度上快速使NP结晶。此外，生长NP晶体所需的杂质量（<0.1%）提醒我们，在纳米科学中解释实验观察结果时，细微细节非常重要。
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