Atomic steps at growth surfaces are important heterogeneous sources for nucleation of epitaxial nano-objects. In the presence of misfit strain, we show that the nucleation process takes place preferentially at the upper terrace of the step as a result of the local stress relaxation. Evidence for strain-induced nucleation comes from the direct observation by postgrowth, atomic resolution, Z-contrast imaging of an InAs-rich region in a nanowire located on the upper terrace surface of an interfacial diatomic step. © 2007 American Institute of Physics. ͓DOI: 10.1063/1.2790483͔Atomic steps located at the surfaces of substrates play a central role in controlling the growth mechanism of a wide range of materials. The effect of such steps on the growth process, the morphology, the stress and strain distributions, and the functionality of the materials has been extensively investigated. [1][2][3][4][5][6][7][8][9][10][11] In particular, these steps are thought to constitute a heterogeneous source of nucleation for the formation of nano-objects and structural defects at the initial stages of the growth of many semiconductor nanostructures. 12,13 It is critically important to identify the nucleation sources for individual nano-objects such as quantum dots and wires because they constitute the fundamental blocks of future nanoelectronics and nanophotonics devices. 14 The ability to control the nucleation of these nano-objects will contribute significantly to the development of reliable single-photon sources for applications in quantum information technology. [15][16][17] Nanowires constitute a special case of self-assembled nano-objects. 18 Self-assembled nano-objects can be formed spontaneously via the Stranski-Krastanov growth mode for certain semiconductor materials when a few monolayers are epitaxially deposited on a lattice-mismatched substrate. 19,20 Strain is widely accepted to be the driving force for the nucleation of these nano-objects, but as yet there has been no direct experimental evidence for the role of steps, and their associated stress enhancement, in the self-organized growth of nanowire arrays. 21,22 In this letter we show the direct imaging, by aberrationcorrected Z-contrast scanning transmission electron microscopy ͑STEM͒ and atomic force microscopy, that, in the presence of misfit strain, nanowires preferentially nucleate on the upper terrace of a diatomic step. With finite element elasticity calculations, we demonstrate that the driving force is the stress relaxation at the upper terrace of a diatomic step, which explains the observed nucleation site of semiconductor nanowires.The nanowires investigated consist of InAs͑P͒ selfassembled quantum wires grown by solid source molecular beam epitaxy ͑MBE͒ on InP ͑001͒ substrates. The lattice mismatch between InAs and InP is 3.2%. The control of the relaxation process of these nanostructures has recently been followed with high precision by in situ accumulated stress measurements from the initial phases of the self-assembly process. 23 The process of format...