We analyze the morphological stability against azimuthal, axial, and general helical perturbations for epitaxial core-shell nanowires in the growth regimes limited by either surface diffusion or evaporation-condensation surface kinetics. For both regimes, we find that geometric parameters (i.e., core radius and shell thickness) play a central role in determining whether the nanowire remains cylindrical or its shell breaks up into epitaxial islands similar to those observed during Stranski-Krastanow growth in thin epilayers. The combination of small cores and rapid growth of the shell emerge as key ingredients for stable shell growth. Our results provide an explanation for the different core-shell morphologies reported in the Si-Ge system experimentally, and also identify a growth-induced intrinsic mechanism for the formation of helical nanowires.The combination of dimensionally confined transport and engineered interfaces inherent in heterostructured nanowires has led to their emergence as an important class of low dimensional, multifunctional nanostructures.1,2,3 In particular, radially heterostructured core-shell nanowires (CSNWs) have enjoyed considerable attention from the synthesis and design communities, mainly due to an unprecedented range of reported electronic properties such as high mobility carrier transport, tunable band gaps, non-linear optical gains, and giant magnetoresistance. 4,5,6,7,8,9,10 Modifications to usual nanowire synthesis routes, based on tailoring the rate and chemistry of radial growth during catalysis and/or vapor transport, have allowed the realization of several nanowire systems, including Si/Ge, 11,12,13 GaN/GaP,
14GaN/InGaN, 9 GaAs-Ga x In 1−x P, 15 and metal oxides such as SnO 2 /In 2 O 3 .
16The direct control over the size and composition of the core and shell during synthesis should translate to wires with tailored orientations, degree of interface mixing and overall surface structure. Surface morphology is crucial as it drastically modifies the eventual function, yet its control remains an open issue. Indeed, recent studies in epitaxial systems have shown that the wires do not always remain cylindrical but can develop nanoscale surface modulations that tend to self-organize in a manner akin to quantum dots on thin films. For example, consider the Si-Ge system. The experiments of Lauhon et al. revealed that for small core radii (r c ∼ 10 − 15 nm), the shell grows uniformly in both Si/Ge and Ge/Si nanowires (see Fig. 1a).11 For large core radii (r c ≥ 50nm), Pan et * Corresponding author, email: mupmanyu@mines.edu al. found that Ge shells grow non-uniformly on Si cores and eventually develop into well-defined Ge islands, 12 as shown in Fig. 1b: this observation strongly suggests that the growth occurs in the Stranski-Krastanow mode in which the shell first develops a wetting layer and subsequently forms islands that grow and coarsen. Similar islands morphologies have also been observed in PbSe/PbS 17 and SnO 2 /In 2 O 3 CSNWs.
16The reports of these intriguing morphologies le...