Dale Barkey 9306837 This is a study of the spontaneous growth of electrodeposited metal dendrites. Both experimental and theoretical investigations of the initiation and propagation of dendrites are included, with emphasis on interfacial dynamics. Experimental studies of the metal/solution interface focus on nucleation and growth under pristine conditions with high spatial resolution. The theoretical component relates these interfacial processes to the appearance of macroscopic structure and to growth velocity. Experimental techniques include voltammetry, electrochemical impedance spectroscopy, atomic force and scanning tunnelling microscopies, and optical methods including shadowgraph imaging and holographic interferometry. Single-crystal electrodes and needle electrodes are used to examine the effects of crystalline anisotropy and curvature on the deposition dynamics. Spontaneous growth of dendrites is often the limiting factor for space-time yields in technologies using electrodeposition, including electrochemical processing, energy storage, and metal finishing. (For example, it is the principal cause of failure in automotive batteries.) This study is an attempt to relate microscopic interfacial processes with the appearance and growth of macroscopic dendrites. The emphasis is on metals of commercial significance in plating, energy storage (batteries), and structural materials.