Nonlinear diffuse femtosecond-pulse reflectometry is introduced as a powerful experimental tool for the unambiguous characterization of polar and non-polar point symmetry groups of harmonic upconversion nanoparticles. Using intense ultrashort 40 femtosecond laser pulses and an appropriate figure of merit (FOM), second and third harmonic emission serve for the structural characterization of polar Yb-doped lithium niobate and non-polar titanium dioxide nanoparticles. The tool is capable of differentiating these two samples by FOM values that differ by up to 13 orders of magnitude. The general applicability to harmonic upconversion nanoparticles over a broad range of intensities and wavelength spectrum, is discussed.

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