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Register a new userAnalysis of Emission Dynamics of a Long Lifetime in Single InAs/GaAs Quantum Dots
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A very long lifetime emission with non-single exponential decay characteristic has been reported for single InAs/GaAs quantum dot (QD) samples, in which there exists a long-lived metastable state in the wetting layer (WL) [ACS Photonics 2020,7,3228-3235]. In this article we have proposed a new three-level model to simulate the emission decay curve. In this model, assuming that the excitons in metastable state will diffuse and be trapped by QDs, and then emit fluorescence in QDs, a stretched-like exponential decay formula is derived as I(t)=At^({beta}-1)e^(-(rt)^{beta}), which can well describe the long lifetime decay curve with an analytical expression of average lifetime <{tau}>=1/r{Gamma}(1/{beta}+1), where {Gamma} is the Gamma function. Furthermore, based on the proposed three-level model, an expression of the second-order auto-correlation function g^2 (t) which can well fit the measured g^2 (t) curve is also obtained.
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Systematic time-resolved measurements on neutral and charged excitonic complexes (X, XX, X+, and XX+) of 26 different single InAs/GaAs quantum dots are reported. The ratios of the decay times are discussed in terms of the number of transition channels determined by the excitonic fine structure and a specific transition time for each channel. The measured ratio for the neutral complexes is 1.7 deviating from the theoretically predicted value of 2. A ratio of 1.5 for the positively charged exciton and biexciton decay time is predicted and exactly matched by the measured ratio indicating identical specific transition times for the transition channels involved.
The exciton lifetimes $T_1$ in arrays of InAs/GaAs vertically coupled quantum dot pairs have been measured by time-resolved photoluminescence. A considerable reduction of $T_1$ by up to a factor of $sim$ 2 has been observed as compared to a quantum dots reference, reflecting the inter-dot coherence. Increase of the molecular coupling strength leads to a systematic decrease of $T_1$ with decreasing barrier width, as for wide barriers a fraction of structures shows reduced coupling while for narrow barriers all molecules appear to be well coupled. The coherent excitons in the molecules gain the oscillator strength of the excitons in the two separate quantum dots halving the exciton lifetime. This superradiance effect contributes to the previously observed increase of the homogeneous exciton linewidth, but is weaker than the reduction of $T_2$. This shows that as compared to the quantum dots reference pure dephasing becomes increasingly important for the molecules.
We investigate the electronic structure of the InAs/InP quantum dots using an atomistic pseudopotential method and compare them to those of the InAs/GaAs QDs. We show that even though the InAs/InP and InAs/GaAs dots have the same dot material, their electronic structure differ significantly in certain aspects, especially for holes: (i) The hole levels have a much larger energy spacing in the InAs/InP dots than in the InAs/GaAs dots of corresponding size. (ii) Furthermore, in contrast with the InAs/GaAs dots, where the sizeable hole $p$, $d$ intra-shell level splitting smashes the energy level shell structure, the InAs/InP QDs have a well defined energy level shell structure with small $p$, $d$ level splitting, for holes. (iii) The fundamental exciton energies of the InAs/InP dots are calculated to be around 0.8 eV ($sim$ 1.55 $mu$m), about 200 meV lower than those of typical InAs/GaAs QDs, mainly due to the smaller lattice mismatch in the InAs/InP dots. (iii) The widths of the exciton $P$ shell and $D$ shell are much narrower in the InAs/InP dots than in the InAs/GaAs dots. (iv) The InAs/GaAs and InAs/InP dots have a reversed light polarization anisotropy along the [100] and [1$bar{1}$0] directions.
Excitonic polaron is directly demonstrated for the first time in InAs/GaAs quantum dots with photoluminescence method. A new peak ($s$) below the ground state of exciton ($s$) comes out as the temperature varies from 4.2 K to 285 K, and a huge anticrossing energy of 31 meV between $s$ and $s$ is observed at 225 K, which can only be explained by the formation of excitonic polaron. The results also provide a strong evidence for the invalidity of Huang-Rhys formulism in dealing with carrier-longitudinal optical phonon interaction in quantum dot. Instead, we propose a simple two-band model, and it fits the experimental data quite well. The reason for the finding of the anticrossing is also discussed.
The light emission of self-assembled (In,Ga)As/GaAs quantum dots embedded in single GaAs-based micropillars has been studied by time-resolved photoluminescence spectroscopy. The altered spontaneous emission is found to be accompanied by a non-exponential decay of the photoluminescence where the decay rate strongly depends on the excitation intensity. A microscopic theory of the quantum dot photon emission is used to explain both, the non-exponential decay and its intensity dependence. Also the transition from spontaneous to stimulated emission is studied.
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