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Superlattices and Microstructures

Pump–probe absorption/gain spectroscopy of strongly confined semiconductor nanocrystals

Pranay K. Sen, J. T. Andrews

Published Apr 1, 2001• 5 citations
Publisher
DOI
10.1006/spmi.2001.0975

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Journal of the Optical Society of America B•May 1, 1996•19 citations
Density matrix approach has been employed to analyze the pump-probe spectroscopic absorption spectra of small semiconductor quantum dots (QDs) under strong confinement regime with sizes smaller than the bulk exciton Bohr radius such that the Coulombic interaction energy becomes negligible in comparison to the confinement energy. The average time rate of absorption has been obtained by incorporating the radiative and nonradiative decay processes as well as the inhomogeneous broadening arising due to nonuniform QD sizes. The analytical results are obtained for QDs duly irradiated by a strong near resonant pump and broadband weak probe. Numerical estimations have been made for (1) isolated QDs and (2) QD-arrays of GaAs and CdS. The results agree very well with the available experimental observations in CdS QDs. The results in case of GaAs QDs can lead one to experimentally estimate absorption/gain spectra in the important III-V semiconducting mesoscopic structures.
Density matrix approach has been employed to analyze the pump-probe spectroscopic absorption spectra of small semiconductor quantum dots (QDs) under strong confinement regime (SCR) with sizes smaller than the bulk exciton Bohr radius such that the Columbic interaction energy becomes negligible in comparison to the confinement energy. The average time rate of absorption has been obtained by incorporating the radiative and nonradiative decay processes as well as the inhomogeneous broadening arising due to nonuniform QD sizes. The analytical results are obtained for QDs duly irradiated by a strong near resonant pump and broadband weak probe. Numerical estimations have been made for (i) isolated QDs and (ii) QD-arrays of GaAs and CdS. The results agree very well with the available experimental observations in CdS QDs. The results in case of GaAs QDs can lead one to experimentally estimate absorption/gain spectra in the important III-V semiconducting mesoscopic structures.
We investigate the dephasing times in highly excited CdSe and CdS0.3Se0.7 nanocrystals by spectral hole burning throughout the gain region. The energy dependence of the dephasing time T2 is compared between quantum dots in the strong-confinement regime and bulklike microcrystals. T2 in strongly confined quantum dots remains rather constant, whereas the bulklike sample shows a continuous increase of T2 toward the transparency point. This observation is attributed to the different gain mechanisms in the strong and the weak quantum-confinement regimes.