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Register a new userUniversal recovery of the bright-exciton level-degeneracy in quantum dots without structural symmetry
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The lack of structural symmetry which usually characterizes semiconductor quantum dots lifts the energetic degeneracy of the bright excitonic states and hampers severely their use as high fidelity sources of entangled photons. We demonstrate experimentally and theoretically that it is always possible to restore the excitonic degeneracy by the simultaneous application of large strain and electric fields, despite the fact that this possibility has fundamentally been doubted. This is achieved by using one external perturbation to align the polarization of the exciton emission along the axis of the second perturbation, which then erases completely the energy splitting of the states. This result, which holds for any QD structure, highlights the potential of combining complementary external fields to create artificial atoms meeting the stringent requirements posed by scalable semiconductor-based quantum-technology.
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We report on polarization-resolved resonant photoluminescence (PL) spectroscopy of bright (spin-1) and dark (spin-2) excitons in colloidal CdSe nanocrystal quantum dots. Using high magnetic fields to 33 T, we resonantly excite (and selectively analyze PL from) spin-up or spin-down excitons. At low temperatures (<4K) and above ~10 T, the spectra develop a narrow, circularly polarized peak due to spin-flipped bright excitons. Its evolution with magnetic field directly reveals a large (1-2 meV), intrinsic fine structure splitting of bright excitons, due to anisotropic exchange. These findings are supported by time-resolved PL studies and polarization-resolved PL from single nanocrystals.
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Sergio De Rinaldis (NNL-National Nanotechnology Laboratory of INFM
, n ISUFI-Istituto Superiore Universitario per la Formazione Interdisciplinare
, n University of Lecce
2002
We present a fully three-dimensional study of the multiexciton optical response of vertically coupled GaN-based quantum dots via a direct-diagonalization approach. The proposed analysis is crucial in understanding the fundamental properties of few-particle/exciton interactions and, more important, may play an essential role in the design/optimization of semiconductor-based quantum information processing schemes. In particular, we focus on the interdot exciton-exciton coupling, key ingredient in recently proposed all-optical quantum processors. Our analysis demonstrates that there is a large window of realistic parameters for which both biexcitonic shift and oscillator strength are compatible with such implementation schemes.
The demonstration of degeneracy of the exciton spin states is an important step towards the production of entangled photons pairs from the biexciton cascade. We measure the fine structure of exciton and biexciton states for a large number of single InAs quantum dots in a GaAs matrix; the energetic splitting of the horizontally and vertically polarised components of the exciton doublet is shown to decrease as the exciton confinement decreases, crucially passing through zero and changing sign. Thermal annealing is shown to reduce the exciton confinement, thereby increasing the number of dots with splitting close to zero.
Exciton spin dynamics in quasi-spherical CdS quantum dots is studied in detail experimentally and theoretically. Exciton states are calculated using the 6-band k.p Hamiltonian. It is shown that for various sets of Luttinger parameters, when the wurtzite lattice crystal field splitting and Coulomb interaction between the electron-hole pair are taken into account exactly, both the electron and hole wavefunction in the lowest exciton state are of S-type. This rules out the spatial-symmetry-induced origin of the dark exciton in CdS quantum dots. The exciton bleaching dynamics is studied using time- and polarization-resolved transient absorption technique of ultrafast laser spectroscopy. Several samples with a different mean size of CdS quantum dots in different glass matrices were investigated. This enabled the separation of effects that are typical for one particular sample from those that are general for this type of material. The experimentally determined dependence of the electron spin relaxation rate on the radius of quantum dots agrees well with that computed theoretically.
Micro-photoluminescence spectroscopy at variable temperature, excitation intensity and energy was performed on a single InAs/AlAs self-assembled quantum dot. The exciton emission line (zero-phonon line, ZPL) exhibits a broad sideband due to exciton-acoustic phonon coupling by the deformation potential mechanism. Additionally, narrow low-energy sidebands at about 0.25 meV of the ZPL are attributed to exciton-acoustic phonon piezoelectric coupling. In lowering the excitation energy or intensity these bands gradually dominate the emission spectrum of the quantum dot while the ZPL disappears. At high excitation intensity the sidebands due to piezoelectric coupling decrease strongly and the ZPL dominates the spectrum as a consequence of screening of the piezoelectric coupling by the photocreated free carriers.
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