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Register a new userStatistical Properties of Exciton Fine Structure Splittings and Polarization Angles in Quantum Dot Ensembles
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We propose an effective model to describe the statistical properties of exciton fine structure splitting (FSS) and polarization angle of quantum dot ensembles (QDEs). We derive the distributions of FSS and polarization angle for QDEs and show that their statistical features can be fully characterized using at most three independent measurable parameters. The effective model is confirmed using atomistic pseudopotential calculations as well as experimental measurements for several rather different QDEs. The model naturally addresses three fundamental questions that are frequently encountered in theories and experiments: (I) Why the probability of finding QDs with vanishing FSS is generally very small? (II) Why FSS and polarization angle differ dramatically from QD to QD? and (III) Is there any direct connection between FSS, optical polarization and the morphology of QDs? The answers to these fundamental questions yield a completely new physical picture for understanding optical properties of QDEs.
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Lead-halide perovskite nanocrystals (PNCs) exhibit unique optoelectronic properties, many of which originate from a purported bright-triplet exciton fine-structure. A major impediment to measuring this fine-structure is inhomogeneous spectral broadening, which has limited most experimental studies to single-nanocrystal spectroscopies. It is shown here that the linearly-polarized single-particle selection rules in PNCs are preserved in nonlinear spectroscopies of randomly-oriented ensembles. Simulations incorporating rotational-averaging demonstrate that techniques such as transient absorption and two-dimensional coherent spectroscopy are capable of resolving exciton fine-structure in PNCs, even in the presence of inhomogeneous broadening and orientation disorder.
We derive a general relation between the fine structure splitting (FSS) and the exciton polarization angle of self-assembled quantum dots (QDs) under uniaxial stress. We show that the FSS lower bound under external stress can be predicted by the exciton polarization angle and FSS under zero stress. The critical stress can also be determined by monitoring the change in exciton polarization angle. We confirm the theory by performing atomistic pseudopotential calculations for the InAs/GaAs QDs. The work provides a deep insight into the dots asymmetry and their optical properties, and a useful guide in selecting QDs with smallest FSS which are crucial in entangled photon sources applications.
Exciton levels and fine-structure splitting in laterally-coupled quantum dot molecules are studied. The electron and hole tunneling energies as well as the direct Coulomb interaction are essential for the exciton levels. It is found that fine-structure splitting of the two-lowest exciton levels is contributed from the intra- and inter-dot exchange interactions, both of which are largely influenced by the symmetry and tunnel-coupling between the two dots. As the inter-dot separation is reduced, fine-structure splitting of the exciton ground state is largely increased while those of the excited states are decreased. Moreover, the dependence of the fine-structure splitting in quantum dot molecules on the Coulomb correlation is clearly clarified.
The fine structure of the neutral exciton in a single self assembled InGaAs quantum dot is investigated under the effect of a lateral electric field. Stark shifts up to 1.5 meV, an increase in linewidth, and a decrease in photoluminescence intensity were observed due to the electric field. We show that the lateral electric field strongly affects the exciton fine structure splitting due to active manipulation of the single particle wave-functions. Remarkably, the splitting can be tuned over large values and through zero.
Emission spectra of quantum dot arrays in zero-dimensional microcavities are studied theoretically, and it is shown that they are determined by the competition between the formation of the collective superradiant mode and inhomogeneous broadening. The random sources method for the calculation of photoluminescence spectra under a non-resonant pumping is developed, and a microscopic justification of the random sources method within a framework of the standard diagram technique is given. The emission spectra of a microcavity are analyzed with allowance for the spread of exciton states energies caused by an inhomogeneous distribution of quantum dots and a tunneling between them. It is demonstrated that in the case of a strong tunneling coupling the luminescence spectra are sensitive to the geometric positions of the dots, and the collective mode can, under certain conditions, be stabilized by the random tunnel junctions.
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