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Physics of the Solid State

Absorption saturation and self-action processes under resonant excitation of the basic exciton transition in CdSe/ZnS colloidal quantum dots

В. С. Днепровский, Evgeny A. Zhukov, M. V. Kozlova, Tuerdi Wumaier, Dau Sy Hieu, М. В. Артемьев

Published Sep 1, 2010• 14 citations
Publisher

Abstract

The revealed absorption saturation and Fresnel diffraction of ultrashort laser pulses under resonant excitation of the basic exciton transition in CdSe/ZnS quantum dots (a strongly absorbing colloidal solution) have been explained by the processes of filling of states of a two-level system with the excited-state lifetime dependent on the light intensity and self-diffraction of the laser beam due to the formation of the transparency channel and the induced diaphragm.

DOI
10.1134/s106378341009026x

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The revealed absorption saturation and Fresnel diffraction of ultrashort laser pulses under resonant excitation of the basic exciton transition in CdSe/ZnS quantum dots (a strongly absorbing colloidal solution) have been explained by the processes of filling of states of a two-level system with the excited-state lifetime dependent on the light intensity and self-diffraction of the laser beam due to the formation of the transparency channel and the induced diaphragm.
Self-diffraction at a one-dimensional dynamic photonic crystal formed in the colloidal solution of CdSe/ZnS quantum dots has been discovered. This self-diffraction appears simultaneously with self-diffraction at induced transparency channels at the resonant excitation of the main electron–hole (excitonic) transition of quantum dots by two laser beams with a Gaussian intensity distribution over the cross section. It is shown that a nonlinear change in the absorption of colloidal quantum dots results in the formation of a transparency channel and an induced amplitude diffraction grating, and a significant nonlinear change in the refractive index (Δ n ≈ 10 −3 ) in the absorbing medium is responsible for the formation of the dynamic photonic crystal. Self-diffracted laser beams are revealed propagating not only in directions corresponding to self-diffraction at the induced diffraction grating but also in directions satisfying the Laue condition.
The observation of quantum mechanical interference in the exciton photoluminescence excitation (PLE) process in a semiconductor quantum dot is reported. A simple PLE spectroscopy revealed in a single InGaAs quantum dot a dynamic and continuous evolution of a resonance profile from a peak into a dip and to near transparency caused by an increase of excitation power density of only a few 100 W/cm2. A one-photon process via exciton states and a two-photon process via biexciton states, both of which return to the radiative exciton state, interfere quantum mechanically, resulting in a progressive decrease in exciton absorption under increasing excitation.
Using two-photon excitation, stimulated emission from the biexciton state in a single CdSe/ZnSe quantum dot is observed in a two-pulse configuration. We directly time resolve the emission-absorption characteristics and verify the potential for laser action. By setting the polarization of the stimulation pulse, the recombination path of the biexciton and, by this, the state of the photons emitted in the decay cascade is controlled. We elaborate also the coherent response and address entanglement and disentanglement of the exciton-biexciton system.
The nonlinear optical transmission of CdSe single crystals and saturation thresholds at different polarizations of the pumping wave are studied in a range of the exponential absorption tail. Theoretical calculations performed in the framework of a two-level model with the twofold degenerate ground state corresponding to the optical transitions in E ⟂ C and E‖ C polarizations are also presented. Results obtained for the absorption saturation regime clearly witnesses in favour of the polarization self-action effect and relaxation processes between transitions polarized orthogonally.
Femtosecond-pulse propagation in resonantly excited semiconductors is investigated by numerically solving the semiconductor Maxwell-Bloch equations for plane waves. For excitation at the exciton resonance, it is shown that the pulse absorption exhibits a strongly nonlinear dependence on the input pulse area. Very long propagation distances for strong pulses are observed, but even when all dephasing processes have been neglected, no lossless propagation (self-induced transparency) was found. The influence of the electron-hole many-body effects, nonequilibrium carrier relaxation, and optical dephasing on the pulse-propagation dynamics is studied. The exchange interaction in the electron-hole plasma is shown to support large propagation distances. For excitation of the continuum states, the dependence of the absorption on the intensity of the input pulse is reduced due to the rapid carrier relaxation into quasiequilibrium distributions.