Organic-MPS3 nanocomposites with large second-order nonlinear optical response

Intercalated hybrid materials alternating highly nonlinear optical organic ionic dyes and inorganic MnPS3 layers have been elaborated. We show that a spontaneous poling of the organic molecules is induced at the macroscopic scale by an ionic exchange process. In some cases, UV–visible spectroscopy evidences strong intermolecular interactions between inserted chromophores, resulting in the formation of extended J–aggregates. High nonlinear optical efficiencies are obtained in powdered samples and in nanoparticles, then confirming the interest of these structures for potential applications in photonics.