Li Yan, Galli Giulia, Gygi François
Department of Chemistry, University of California, Davis, California 95616, USA.
ACS Nano. 2008 Sep 23;2(9):1896-902. doi: 10.1021/nn800340f.
We present first principles, density functional theory (DFT) calculations of the structural and electronic properties of thiolate-protected gold nanoparticles [Au(102)(MBA)(44) ] that have been recently crystallized and measured by X-ray diffraction. Our calculations yield structural properties in very good agreement with experiment and reveal the impact of thiolate adsorption on both the surface geometry and the electronic structure of the gold core; in particular, within DFT we observe the emergence of an energy gap of about 0.5 eV, upon MBA adsorption. Using a localized orbital analysis, we characterize the electron distribution in the nanoparticle and provide insight into the bonding of thiolates on curved gold surfaces.
我们展示了对硫醇盐保护的金纳米颗粒[Au(102)(MBA)(44)]的结构和电子性质的第一性原理密度泛函理论(DFT)计算，该颗粒最近已通过X射线衍射结晶并测量。我们的计算得出的结构性质与实验结果非常吻合，并揭示了硫醇盐吸附对金核表面几何形状和电子结构的影响；特别是，在DFT范围内，我们观察到在MBA吸附后出现了约0.5 eV的能隙。通过局域轨道分析，我们表征了纳米颗粒中的电子分布，并深入了解了硫醇盐在弯曲金表面上的键合情况。
