Colloidal semiconductor quantum dots (QDs) constitute zero-dimension excitonic materials characterized by quantized states and able to emit fluorescence. QDs are promising materials for catalysis, molecular recognition and biosensing. In this context, our work consists in the design of a new class of biochemical sensors based on QD-grafted chips to benefit from their high opto-electronic activity in the visible range. In order to achieve this, we functionalize silica and CaF2 susbtrates with 4 nm-diameter CdTe QDs and organic molecules (e.g. phenylamine). The originality of our work then lies in two-colour sum-frequency generation nonlinear optical spectroscopy, mixing Raman and IR spectroscopies. This technique enables to probe and to quantify the coupling between the excitonic properties of the QDs and the vibrational response of their molecular environment: two tunable visible and IR laser beams are mixed on the QD-grafted chips to electronically excite the QDs while the vibrational spectroscopy of the surrounding organic species is performed. Through this approach, we clearly demonstrated a correlation between QDs and molecules. Especially, the vibrational response of the molecules is maximized when the first excitonic state of the CdTe QDs is pumped by the visible beam, which means it is possible to enhance the detection of given biomolecules thanks to QDs. Considering that confined excitons transfer their energy to molecules through dipolar interaction, the model we developed accounts indeed for such a behaviour.
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