Cavity-enhanced photoluminescence of semiconductor quantum dot thin films under two-photon excitation

Semiconductor quantum dots (QDs) feature high values of the two-photon absorption (TPA) cross-sections, enabling their applications in biosensing and nonlinear optoelectronics. However, the efficient QD photoluminescence (PL) intensity caused by TPA requires high-intensity laser excitation which hinders these applications. Placing the QDs in the micro- or nanocavities leads to a change in their PL properties. Particularly, near plasmon nanoparticles (open nanocavities) the local field may be enhanced by the localized plasmons, which will lead to an increase of the TPA efficiency. Alternatively, placing QDs in a photonic crystal may boost an increase of their PL quantum yield due to the Purcell effect and also increase their PL intensity at the photonic mode wavelength due to the redistribution of the density of photonic states. In this study, we have fabricated thin-film hybrid materials based on QDs placed near plasmonic nanoparticles or in the photonic crystal. We have demonstrated a 4.3-fold increase of the radiative recombination rate of QDs in the photonic crystal cavity under the two-photon excitation, resulting in the increase of the PL quantum yield. In turn, the coating of the QDs films with the gold nanorods led to the 12-fold increase in TPA at the maximum of the plasmon spectrum. Our results pave the way to a strong increase of the PL efficiency of the QDs under two-photon excitation for their applications in biosensing and nonlinear optoelectronics.