Strong intrinsic nonlinear optical (NLO) signals not only make nanostructures promising agents for bio-imaging, but also advance NLO microscopy for the study of interactions between nanomaterials and live cells. Single beam modalities such as multiphoton luminescence, second harmonic generation, and third harmonic generation provide a simple way to probe many types of nanostructures. As for more advanced modalities, photothermal heterodyne imaging provides improved detection sensitivity for smaller objects, and transient absorption microscopy provides structural information to distinguish metal from semiconducting carbon nanotubes, and eumelanin from pheomelanin. The four-wave mixing signal achieves chemical selectivity in the presence of either vibrational or electronic resonance, as used in coherent Raman scattering imaging of molecules and in electronically resonance enhanced four-wave mixing imaging of nanostructures.

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DOI: 10.1016/S1369-7021(11)70141-9