摘要： The configurations of core/shell nanowires (NWs) and quantum dots (QDs) decorating NWs have found great applications in forming optoelectronic devices thanks to their superior performances, and the combination of the two configurations would expect to bring more benefits. However, the nanometer-scale electrostatic properties of the QD/buffer layer/NW heterostructures are still un-revealed. In this study, the InAs QDs decorating GaAs/AlAs core/shell NWs are systemically studied both experimentally and theoretically. The layered atomic structures, chemical information, and anisotropic strain conditions are characterized by comprehensive transmission electron microscopy (TEM) techniques. Quantitative electron holography analyses show large number of electrons accumulating in the InAs QD especially at the dot apex, and charges of reversed signs and similar densities are observed to distribute at the sequential interfaces, leaving great amount of holes in the NW core. Theoretical calculations including simulated heterostructural band structures, interfacial charge transfer, and chemical bonding analysis are in good accordance with the experimental results, and prove the important role of AlAs buffer layer in adjusting the heterostructural band structure as well as forming stable InAs QDs on the NW surfaces. These results could be significant for achieving related optoelectronic devices with better stability and higher efficiency.