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Tuning biexciton binding and anti-binding in core/shell quantum dots

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 Added by John Shumway Jr.
 Publication date 2012
  fields Physics
and research's language is English




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We use a path integral quantum Monte Carlo method to simulate excitons and biexcitons in core shell nanocrystals with Type-I, II and quasi-Type II band alignments. Quantum Monte Carlo techniques allow for all quantum correlations to be included when determining the thermal ground state, thus producing accurate predictions of biexciton binding. These subtle quantum correlations are found to cause the biexciton to be binding with Type-I carrier localization and strongly anti-binding with Type-II carrier localization, in agreement with experiment for both core shell nanocrystals and dot in rod nanocrystal structures. Simple treatments based on perturbative approaches are shown to miss this important transition in the biexciton binding. Understanding these correlations offers prospects to engineer strong biexciton anti-binding which is crucial to the design of nanocrystals for single exciton lasing applications.



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We characterized stacked double-pyramidal quantum dots which showed biexciton binding energies close to zero by means of photoluminescence and cross-correlation measurements. It was possible to obtain a sequence of two photons with (nearly) the same energy from the biexciton-exciton-ground state cascade, as corroborated by a basic rate-equation model. This type of two-photon emission is both of relevance for fundamental quantum information theory studies as well as for more exotic applicative fields such as quantum biology.
Previous single-particle spectroscopic studies of colloidal quantum dots have indicated a significant spread in biexciton lifetimes across an ensemble of nominally identical nanocrystals. It has been speculated that in addition to dot-to-dot variation in physical dimensions, this spread is contributed to by variations in the structure of the quantum dot interface, which controls the shape of the confinement potential. Here we directly evaluate the effect of the composition of the core-shell interface on single- and multi-exciton dynamics via side-by-side measurements of individual core-shell CdSe-CdS nanocrystals with a sharp vs. smooth (graded) interface. To realize the latter type of structures, we incorporate a CdSexS1-x alloy layer of controlled composition and thickness between the CdSe core and the CdS shell. We observe that while having essentially no effect on single-exciton decay, the interfacial alloy layer leads to a systematic increase in biexciton lifetimes. This observation provides direct experimental evidence that in addition to the size of the quantum dot, its interfacial properties also significantly affect the rate of Auger recombination, which governs biexciton decay. These findings help rationalize previous observations of a significant heterogeneity in the biexciton lifetimes across similarly sized quantum dots and should facilitate the development of Auger-recombination-free colloidal nanostructures for a range of applications from lasers and light-emitting diodes to photodetectors and solar cells.
The radiative recombination rates of interacting electron-hole pairs in a quantum dot are strongly affected by quantum correlations among electrons and holes in the dot. Recent measurements of the biexciton recombination rate in single self-assembled quantum dots have found values spanning from two times the single exciton recombination rate to values well below the exciton decay rate. In this paper, a Feynman path-integral formulation is developed to calculate recombination rates including thermal and many-body effects. Using real-space Monte Carlo integration, the path-integral expressions for realistic three-dimensional models of InGaAs/GaAs, CdSe/ZnSe, and InP/InGaP dots are evaluated, including anisotropic effective masses. Depending on size, radiative rates of typical dots lie in the regime between strong and intermediate confinement. The results compare favorably to recent experiments and calculations on related dot systems. Configuration interaction calculations using uncorrelated basis sets are found to be severely limited in calculating decay rates.
158 - Xuefei Wu , Hai Wei , Xiuming Dou 2013
We demonstrate that the exciton and biexciton emission energies as well as exciton fine structure splitting (FSS) in single (In,Ga)As/GaAs quantum dots (QDs) can be efficiently tuned using hydrostatic pressure in situ in an optical cryostat at up to 4.4 GPa. The maximum exciton emission energy shift was up to 380 meV, and the FSS was up to 180 $mu$eV. We successfully produced a biexciton antibinding-binding transition in QDs, which is the key experimental condition that generates color- and polarization-indistinguishable photon pairs from the cascade of biexciton emissions and that generates entangled photons via a time-reordering scheme. We perform atomistic pseudopotential calculations on realistic (In,Ga)As/GaAs QDs to understand the physical mechanism underlying the hydrostatic pressure-induced effects.
We study the dynamics of excitons in GaAs/(Al,Ga)As core-shell nanowires by continuous-wave and time-resolved photoluminescence and photoluminescence excitation spectroscopy. Strong Al segregation in the shell of the nanowires leads to the formation of Ga-rich inclusions acting as quantum dots. At 10 K, intense light emission associated with these shell quantum dots is observed. The average radiative lifetime of excitons confined in the shell quantum dots is 1.7 ns. We show that excitons may tunnel toward adjacent shell quantum dots and nonradiative point defects. We investigate the changes in the dynamics of charge carriers in the shell with increasing temperature, with particular emphasis on the transfer of carriers from the shell to the core of the nanowires. We finally discuss the implications of carrier localization in the (Al,Ga)As shell for fundamental studies and optoelectronic applications based on core-shell III-As nanowires.
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