Nanoscale Surface Curvature Effects on Ligand–Nanoparticle Interactions: A Plasmon-Enhanced Spectroscopic Study of Thiolated Ligand Adsorption, Desorption, and Exchange on Gold Nanoparticles,Nano Letters

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Nanoscale Surface Curvature Effects on Ligand–Nanoparticle Interactions: A Plasmon-Enhanced Spectroscopic Study of Thiolated Ligand Adsorption, Desorption, and Exchange on Gold Nanoparticles
Nano Letters ( IF 9.6 ) Pub Date : 2017-06-12 00:00:00 , DOI: 10.1021/acs.nanolett.7b01593
Esteban Villarreal ₁ , Guangfang Grace Li ₁ , Qingfeng Zhang ₁ , Xiaoqi Fu ₁ , Hui Wang ₁

Affiliation

The interfacial adsorption, desorption, and exchange behaviors of thiolated ligands on nanotextured Au nanoparticle surfaces exhibit phenomenal site-to-site variations essentially dictated by the local surface curvatures, resulting in heterogeneous thermodynamic and kinetic profiles remarkably more sophisticated than those associated with the self-assembly of organothiol ligand monolayers on atomically flat Au surfaces. Here we use plasmon-enhanced Raman scattering as a spectroscopic tool combining time-resolving and molecular fingerprinting capabilities to quantitatively correlate the ligand dynamics with detailed molecular structures in real time under a diverse set of ligand adsorption, desorption, and exchange conditions at both equilibrium and nonequilibrium states, which enables us to delineate the effects of nanoscale surface curvature on the binding affinity, cooperativity, structural ordering, and the adsorption/desorption/exchange kinetics of organothiol ligands on colloidal Au nanoparticles. This work provides mechanistic insights on the key thermodynamic, kinetic, and geometric factors underpinning the surface curvature-dependent interfacial ligand behaviors, which serve as a central knowledge framework guiding the site-selective incorporation of desired surface functionalities into individual metallic nanoparticles for specific applications.

中文翻译：

纳米级表面曲率对配体-纳米粒子相互作用的影响：等离子体对金纳米颗粒上硫代配体的吸附，解吸和交换的等离子体光谱研究

纳米结构化的Au纳米粒子表面上硫醇化配体的界面吸附，解吸和交换行为表现出显着的位点间变化，这主要是由局部表面曲率决定的，从而导致异质热力学和动力学特征比与自相关特征更为复杂。在原子平坦的金表面上组装有机硫醇配体单层。在这里，我们使用等离激元增强拉曼散射作为结合时间分辨和分子指纹图谱功能的光谱工具，在平衡态和平衡态下各种不同的配体吸附，解吸和交换条件下，实时定量地将配体动力学与详细的分子结构相关联。非平衡态这使我们能够描述纳米级表面曲率对胶态金纳米颗粒上有机硫醇配体的结合亲和力，协同作用，结构有序性以及吸附/解吸/交换动力学的影响。这项工作提供了对支撑表面曲率依赖的界面配体行为的关键热力学，动力学和几何因素的机械洞察力，这些因素是指导特定应用将所需的表面官能团选择性结合到各个金属纳米颗粒中的中心知识框架。

更新日期：2017-06-28

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