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We present a novel concept for optical spectroscopy called nonlinear correlation spectroscopy (NLCS). NLCS analyses coherent field fluctuations of the second and third harmonic light generated by diffusing nanoparticles. Particles based on noncentrosymmetric nonlinear materials such as KNbO3 show a strong second as well as third harmonic response. The method and the theory are introduced and experimental NLCS results in fetal calf serum are presented showing the promising selectivity of this technique for measurement in complex biological environments.
Olivier Martin, Fabien Sorin, Jérémy Butet, Wei Yan, Dang Tùng Nguyen, Kuang-Yu Yang, Andreas Leber, Louis Marie Philippe Martin-Monier, Chaoqun Dong