Polar Second-Harmonic Imaging to Resolve Pure and Mixed Crystal Phases along GaAs Nanowires

In this work, we report an optical method for characterizing crystal phases along single-semiconductor III-V nanowires based on the measurement of polarization-dependent second-harmonic generation. This powerful imaging method is based on a per-pixel analysis of the second-harmonic-generated signal on the incoming excitation polarization. The dependence of the second-harmonic generation responses on the nonlinear second-order susceptibility tensor allows the distinguishing of areas of pure wurtzite, zinc blende, and mixed and rotational twins crystal structures in individual nanowires. With a far-field nonlinear optical microscope, we recorded the second-harmonic generation in GaAs nanowires and precisely determined their various crystal structures by analyzing the polar response for each pixel of the images. The predicted crystal phases in GaAs nanowire are confirmed with scanning transmission electron and high-resolution transmission electron measurements. The developed method of analyzing the nonlinear polar response of each pixel can be used for an investigation of nanowire crystal structure that is quick, sensitive to structural transitions, nondestructive, and on-the-spot. It can be applied for the crystal phase characterization of nanowires built into optoelectronic devices in which electron microscopy cannot be performed (for example, in lab-on-a-chip devices). Moreover, this method is not limited to GaAs nanowires but can be used for other nonlinear optical nanostructures.