Molecular & Materials Modelling, DATA61 CSIRO, Door 34 Goods Shed, Village St, Docklands VIC, Australia 3008, Australia.
Nanoscale. 2017 Aug 31;9(34):12698-12708. doi: 10.1039/c7nr03472e.
Many applications of silver nanoparticles are moderated by the electron charge transfer properties, such as the ionization potential, electron affinity and Fermi energy, which may be tuned by controlling the size and shape of individual particles. However, since producing samples of silver nanoparticles that are perfectly monodispersed in terms of both size and shape can be prohibitive, it is important to understand how these properties are impacted by polydispersivity, and ideally be able to predict the tolerance for variation of different geometric features. In this study, we use straightforward statistical methods, together with electronic structure simulations, to predict the electron charge transfer properties of different types of ensembles of silver nanoparticles and how restricting the structural diversity in different ways can improve or retard performance. In agreement with previous reports, we confirm that restricting the shape distribution will tune the charge transfer properties toward specific reactions, but by including the quality factors for each case we go beyond this assessment and show how targeting specific classes of morphologies and restricting the distribution of size can impact sensitivity.
许多银纳米粒子的应用都受到电子电荷转移性质的调节，如电离势、电子亲和能和费米能，这些性质可以通过控制单个粒子的尺寸和形状来调节。然而，由于要生产出在尺寸和形状上都完全单分散的银纳米粒子样品可能会受到限制，因此了解这些性质如何受到多分散性的影响，以及理想情况下能够预测不同几何特征的变化容限是很重要的。在这项研究中，我们使用简单的统计方法，结合电子结构模拟，来预测不同类型的银纳米粒子集合的电子电荷转移性质，以及以不同方式限制结构多样性如何改善或阻碍性能。与之前的报告一致，我们证实限制形状分布将使电荷转移性质向特定反应进行调谐，但通过包括每种情况下的质量因素，我们超越了这种评估，并展示了如何针对特定形态类和限制尺寸分布来影响灵敏度。
