Direct observation of dopant atom diffusion in a bulk semiconductor crystal enhanced by a large size-mismatch.
R. Ishikawa, R. Mishra, A. R. Lupini, S. D. Findlay, T. Taniguchi, S. T. Pantelides, S. J. Pennycook, Phys. Rev. Lett. 113, 155501 (2014).
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Diffusion is one of the fundamental processes that govern the structure, processing, and properties of materials and it plays a crucial role in determining device lifetimes. However, direct observations of diffusion processes have been elusive and limited only to the surfaces of materials. Here we use an aberration-corrected electron microscope to locally excite and directly image the diffusion of single Ce and Mn dopants inside bulk wurtzite-type AlN single crystals, identifying correlated vacancy-dopant and interstitial-dopant kick-out mechanisms. Using a 200 kV electron beam to supply energy, we observe a higher frequency of dopant jumps for the larger and heavier Ce atoms than the smaller Mn atoms. These observations confirm density-functional-theory-based predictions of a decrease in diffusion barrier for large substitutional atoms. The results show that combining depth sensitive microscopy with theoretical calculations represents a new methodology to investigate diffusion mechanisms, not restricted to surface phenomena, but within bulk materials.