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Register a new userManipulating exciton fine-structure in quantum dots with a lateral electric field
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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.
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Quantum dots (QDs) can act as convenient hosts of two-level quantum szstems, such as single electron spins, hole spins or excitons (bound electron-hole pairs). Due to quantum confinement, the ground state of a single hole confined in a QD usually has dominant heavy-hole (HH) character. For this reason light-hole (LH) states have been largely neglected, despite the fact that may enable the realilzation of coherent photon-to-spin converters or allow for faster spin manipulation compared to HH states. In this work, we use tensile strains larger than 0.3% to switch the ground state of excitons confined in high quality GaAs/AlGaAs QDs from the conventional HH- to LH-type. The LH-exciton fine structure is characterized by two in-plane-polarized lines and, ~400 micro-eV above them, by an additional line with pronounced out-of-plane oscillator strength, consistent with theoretical predictions based on atomistic empirical pseudopotential calculations and a simple mesoscopic model.
In a charge tunable device, we investigate the fine structure splitting of neutral excitons in single long-wavelength (1.1mu m < lambda < 1.3 mu m) InGaAs quantum dots as a function of external uniaxial strain. Nominal fine structure splittings between 16 and 136 mu eV are measured and manipulated. We observe varied response of the splitting to the external strain, including positive and negative tuning slopes, different tuning ranges, and linear and parabolic dependencies, indicating that these physical parameters depend strongly on the unique microscopic structure of the individual quantum dot. To better understand the experimental results, we apply a phenomenological model describing the exciton polarization and fine-structure splitting under uniaxial strain. The model predicts that, with an increased experimental strain tuning range, the fine-structure can be effectively canceled for select telecom wavelength dots using uniaxial strain. These results are promising for the generation of on-demand entangled photon pairs at telecom wavelengths.
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 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.
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.
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