Depletion Driven Assembly of Ultrasmall Metal Nanoclusters: From Kinetically Arrested Assemblies to Thermodynamically Stable, Spherical Superclusters,The Journal of Physical Chemistry Letters

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Depletion Driven Assembly of Ultrasmall Metal Nanoclusters: From Kinetically Arrested Assemblies to Thermodynamically Stable, Spherical Superclusters
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2022-10-03 , DOI: 10.1021/acs.jpclett.2c02420
Debkumar Bera _{1,

2} , Mousumi Baruah ₃ , Asish K Dehury _{1,

2} , Animesh Samanta ₃ , Yatendra S Chaudhary _{1,

2} , Nirmal Goswami _{1,

2}

Affiliation

Nanoscale assembly of ultrasmall metal nanoclusters (MNCs) by means of molecular forces has proven to be a powerful strategy to engineer their molecule-like properties in multiscale dimensions. By leveraging depletion attraction as the guiding force, herein, we demonstrate the formation of kinetically trapped NCs assemblies with enhanced photoluminescence (PL) and excited state lifetimes and extend the principle to cluster impregnated cationic nanogels, nonluminescent Au(I)–thiolate complexes, and weakly luminescent CuNCs. We further demonstrate a thermal energy driven kinetic barrier breaking process to isolate these assemblies. These isolated assemblies are thermodynamically stable, built from a strong network among several discrete, ultrasmall AuNCs and exhibit several unusual properties such as high stability in various pH, strong PL, microsecond lifetimes, large Stocks shifts, and higher accumulation in the lysosome of cancer cells. We anticipate our strategy may find wider use in creating a large variety of MNC-based assemblies with many unforeseen arrangements, properties, and applications.

中文翻译：

超小型金属纳米团簇的耗尽驱动组装：从动力学停滞的组装到热力学稳定的球形超团簇

事实证明，通过分子力对超小金属纳米团簇 (MNC) 进行纳米级组装是一种在多尺度维度上设计其类分子特性的有力策略。通过利用耗尽吸引力作为引导力，在此，我们展示了具有增强的光致发光 (PL) 和激发态寿命的动力学捕获的 NCs 组件的形成，并将该原理扩展到簇浸渍的阳离子纳米凝胶、不发光的 Au(I)-硫醇盐配合物，以及弱发光的CuNCs。我们进一步展示了一种热能驱动的动能屏障破坏过程来隔离这些组件。这些孤立的组件在热力学上是稳定的，由几个离散的超小型 AuNC 之间的强大网络构建而成，并表现出一些不寻常的特性，例如在各种 pH 值下的高稳定性、强 PL、微秒的寿命、大的库存变化和癌细胞溶酶体中的更高积累。我们预计我们的策略可能会在创建具有许多不可预见的安排、属性和应用程序的大量基于 MNC 的组件时得到更广泛的应用。

更新日期：2022-10-03

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