Conventional approaches to the determination of the two-photon absorption cross-section (TPACS) of fluorescent semiconductor nanocrystals, including quantum dots (QDs) and nanoplatelets (NPLs), cannot be applied to samples with unknown concentrations and low optical densities and may be inaccurate in the case of multiexciton nanocrystal excitation. Here, we have studied the two-photon-excited photoluminescence saturation in QD and NPL samples and propose a novel technique for determining of their TPACS from the parameters of this process. The technique allows the measurement of the TPACSs of single exciton states in the samples of unknown concentration, as well as in thin films with ultralow optical densities. The calculated values agreed with the results obtained by conventional methods. The new technique paves new ways to studying small amounts of fluorescent nanocrystals of unknown quantity under two-photon excitation.
Efficient biexciton (BX) photoluminescence (PL) from quantum dots (QDs) paves the way to the generation of entangled photons and related applications. However, the quantum yield (QY) of BX PL is much lower than that for single excitons (EX) due to efficient Auger-like recombination. In the vicinity of plasmon nanoparticles, the recombination rates of EX and BX may be affected by the Purcell effect, fluorescence quenching, and the excitation rate enhancement. Here, the effect of the plasmon resonance spectral position on the EX and BX PL is experimentally studied in two cases: when the plasmon band overlaps with the excitation wavelength and when it coincides with the QDs PL band. In the first case, the EX and BX excitation efficiencies are significantly increased but the EX QY reduced. As a result, the BX-to-EX QY ratio is higher than 1 at plasmon-exciton systems separations shorter than 40 nm. In the second case, the radiative recombination rates are enhanced by several orders of magnitude, which led to an increase in BX QY over distances of up to 90 nm. Finally, these two effects are obtained in the same hybrid structure, with the resultant increase in both excitation efficiency and QY of BX PL.
Semiconductor quantum dots (QDs) are widely used as components of hybrid materials for development of efficient light emitters and convertors. Their unique nonlinear optical properties, such as two-photon absorption and two-photon photoluminescence from biexcitons, make them promising materials for photovoltaic and optoelectronic applications. In this study, thin-film hybrid materials based on the CdSe(core)/ZnS/CdS/ZnS(multishell) QDs have been fabricated, and the two-photon photoluminescence (PL) from the generated biexcitons have been studied. The results show that fabricated thin-film hybrid materials based on the QDs are efficient fluorophores in the one- and two-photon PL regimes for applications in optoelectronics and biosensing.
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