We report on the systematical study of the second-harmonic generation (SHG) in single zinc sulfide nanowires (ZnS NWs). The high quality ZnS NWs with round cross-section were fabricated by chemical vapor deposition method. The transmission electron microscopy images show that the actual growth-axis has a deviation angle of 0o~20o with the preferential growth direction [120], which leads to the various polarization-dependent SHG response patterns in different individual ZnS NWs. The SHG response is quite sensitive to the orientations of c-axis as well as the (100) and (010) crystal-axis of ZnS NWs, thus all the three crystal-axis orientations of ZnS NWs are precisely determined by the SHG method. A high SHG conversion efficiency of 7*10^(-6) is obtained in single ZnS NWs, which shows potential applications in nanoscale ultraviolet light source, nonlinear optical microscopy and nanophotonic devices.
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