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.
With the ever-growing interest in quantum computing, understanding the behaviour of excitons in monolayer quantum dots has become a topic of great relevance. In this paper, we consider a Wannier exciton confined in a triangular quantum dot of hexagonal Boron Nitride. We begin by outlining the adequate basis functions to describe a particle in a triangular enclosure, analyzing their degeneracy and symmetries. Afterwards, we discuss the excitonic hamiltonian inside the quantum dot and study the influence of the quantum dot dimensions on the excitonic states.
Electron states in a quantum dot (QD) located near a 2D system of dipolar excitons are perturbed by fluctuations of the exciton density caused by the electron-exciton interaction. This results in the frequency changes of electron transitions in a QD. The frequency depends on the exciton density, as well as on the exciton gas phase state. In the present work, the shifts of the two lowest QD energy levels are found both in the normal state of the exciton system and for the Bose-Einstein condensation (BEC) regime.
Excitons in alloyed nanowire quantum dots have unique spectra as shown here using atomistic calculations. The bright exciton splitting is triggered solely by alloying and despite cylindrical quantum dot shape reaches over $15~μ$eV, contrary to previous theoretical predictions, however, in line with experimental data. This splitting can however be tuned by electric field to go below $1$~$μ$eV threshold. The dark exciton optical activity is also strongly affected by alloying reaching notable $1/3500$ fraction of the bright exciton and having large out-of-plane polarized component.
Several important proposals to use semiconductor quantum dots in quantum information technology rely on the control of the dark exciton ground states, such as dark exciton based qubits with a $μ$s life time. In this paper, we present an efficient way to occupy the dark exciton ground state by a single short laser pulse. The scheme is based on an optical excitation with a longitudinal field component featured by, e.g., radially polarized beams or certain Laguerre-Gauss or Bessel beams. Utilizing this component, we show within a configuration interaction approach that high-energy exciton states …
The dephasing mechanisms of p-shell and s-shell excitons in an InAs self-assembled quantum dot ensemble are examined using two-dimensional coherent spectroscopy (2DCS). 2DCS provides a comprehensive picture of how the energy level structure of dots affects the exciton dephasing rates and recombination lifetimes. We find that at low temperatures, dephasing of s-shell excitons is lifetime limited, whereas p-shell excitons exhibit significant pure dephasing due to scattering between degenerate spin states. At elevated temperatures, quadratic exciton-phonon coupling plays an important role in both…
So far in the literature the terms "charged exciton" and "trion" are often confused with each other and mostly considered as the same. In this work we show this is not the case in 2D quantum dots with a parabolic confinement. By using the unrestricted Hartree-Fock method the energy and binding energy of both charged excitons and trions in 2D parabolic quantum dots are calculated in dependence on the confinements of charge carriers in quantum dot. It is shown that the binding energies of the charged exciton and the trion behave differently in regard to the ratios of the confinements between the…
We study the effect of Coulomb correlation on the emission properties of the ground state exciton in zincblende CdSe/ZnS core-shell and in wurtzite ZnO quantum dots. We validate our theory model by comparing results of computed exciton energies of CdSe/ZnS quantum dots to photoluminescence and scanning near-field optical microscopy measurements. We use that to estimate the diameter of the quantum dots using a simple model based on infinitely deep quantum well and compare the results with the statistics of the atomic force microscopy scans of CdSe/ZnS dots, obtaining excellent agreement. Therea…
Quantum dots are arguably one of the best platforms for optically accessible spin based qubits. The paramount demand of extended qubit storage time can be met by using quantum-dot-confined dark exciton: a longlived electron-hole pair with parallel spins. Despite its name the dark exciton reveals weak luminescence that can be directly measured. The origins of this optical activity remain largely unexplored. In this work, using the atomistic tight-binding method combined with configuration-interaction approach, we demonstrate that atomic-scale randomness strongly affects oscillator strength of d…
By pumping nonresonantly a MoS$_2$ monolayer at $13$ K under a circularly polarized cw laser, we observe exciton energy redshifts that break the degeneracy between B excitons with opposite spin. The energy splitting increases monotonically with the laser power reaching as much as $18$ meV, while it diminishes with the temperature. The phenomenon can be explained theoretically by considering simultaneously the bandgap renormalization which gives rise to the redshift and exciton-exciton Coulomb exchange interaction which is responsible for the spin-dependent splitting. Our results offer a simple…
We have closely examined the emission spectrum at the heavy-hole exciton resonance in a high-quality GaAs multi-quantum well (MQW) sample using picosecond excitation-correlation photoluminescence (ECPL) spectroscopy. Dynamics of the ECPL signal at low and high energy sides of the excitonic photoluminescence (PL) peak shows complementary behavior. The ECPL signal is positive (negative) below (above) the PL peak and it changes sign within a narrow band of energy lying between excitonic absorption and emission peaks. The energy at which this sign change takes place is interpreted as the excitonic…
The time evolution of a quantum dot exciton in Coulomb interaction with wetting layer carriers is treated using an approach similar to the independent boson model. The role of the polaronic unitary transform is played by the scattering matrix, for which a diagrammatic, linked cluster expansion is available. Similarities and differences to the independent boson model are discussed. A numerical example is presented.
Within the Floquet theory of periodically driven quantum systems, we demonstrate that a high-frequency electromagnetic field can be used as an effective tool to control excitonic properties of semiconductor quantum dots (QDs). It is shown, particularly, that the field both decreases the exciton binding energy and dynamically stabilizes the exciton, increasing its radiative lifetime. The developed theory can serve as a basis for the ultrafast method to tune spectral characteristics of the QD-based photon emitters by a high-frequency field.
