Controlling metallic nanoparticle (NP) interactions plays a vital role in the development of new joining techniques (nanosolder) that bond at lower processing temperatures but remain viable at higher temperatures. The primary objective of this project is t o develop a fundamental understanding of the actual reaction processes, associated atomic mechanisms, and the resulting microstructure that occur during thermally - driven bond formation concerning metal - metal nano - scale (50nm) interfaces. In this LDRD project, we have studied metallic NPs interaction at the elevated temperatures by combining in - situ transmission electron microscopy (TEM ) using an aberration - corrected scanning transmission electron microscope (AC - STEM) and atomic - scale modeling such as molecular dynamic (MD) simulations. Various metallic NPs such as Ag, Cu and Au are synthesized by chemical routines. Numerous in - situ experiments were carried out with focus of the research on study of Ag - Cu system. For the first time, using in - situ STEM heating experiments , we directly observed the formation of a 3 - dimensional (3 - D) epitaxial Cu - Ag core - shell nanoparticle during the thermal interaction of Cu and Ag NPs at elevated temperatures (150 - 300 o C). The reaction takes place at temperatures as low as 150 o C and was only observed when care was taken to circumvent the effects of electron beam irradiation during STEM imaging. Atomic - scale modeling verified that the Cu - Ag core - shell structure is energetically favored, and indicated that this phenomenon is a nano - scale effect related to the large surface - to - volume ratio of the NPs. The observation potentially can be used for developing new nanosolder technology that uses Ag shell as the %22glue%22 that sticks the particles of Cu together. The LDRD has led to several journal publications and numerous conference presentations, and a TA. In addition, we have developed new TEM characterization techniques and phase - field modeling tools that can be used for future materials research at Sandia. Acknowledgeme nts This work was supported by the Laboratory Directed Research and Development (LDRD) program of Sandia National Laboratories. Sandia National Laboratories is a multi - program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the US Department of Energy's National Nuclear Security Administration under contract DE - AC04 - 94AL85000.