Observation of Distinct Two-Photon Transition Channels in CdTe Quantum Dots in a Regime of Very Strong Confinement.

We report here on the direct observation of distinct two-photon transition channels in glutathione-capped (GSH) CdTe quantum dots (QDs) in a very strong confinement regime. CdTe-GSH QDs with different average diameters (2.5, 3.0, and 3.3 nm) were synthesized through the one-pot method and their two-photon absorption (2PA) spectrum determined by a femtosecond wavelength-tunable Z-scan. Our results show that the two lower-energy one-photon-allowed excitonic transitions, 1S3/2(h) → 1S(e) and 2S3/2(h) → 1S(e), are also accessed via 2PA. These results were ascribed to the relaxation of the parity selection rules due to the noncentrosymmetric structure of the CdTe QDs (zinc-blended structure), whose magnitude are determined by surface defects and structural irregularities present in CdTe-GSH QDs, in the strong confinement regime.