Identifying multi‐excitons in quantum dots: the subtle connection between electric dipole moments and emission linewidths

The emission linewidths of excitonic complexes confined in quantum dots (QDs) mirror their interaction with a defect‐induced, fluctuating charge environment, a phenomenon known as spectral diffusion. Interestingly, extended excitonic complexes that comprise several interacting excitons exhibit significantly smaller emission linewidths if compared to the optical fingerprint of their building block, a sole exciton. Hence, it is not the absolute, but the relative electric dipole moment that governs the directly accessible emission linewidths. Exemplarily we investigate this matter based on differing exciton and biexciton emission linewidths of single GaN QDs with varying emission energies, i.e. QD dimensions. Our results establish the full width at half maximum (FWHM) or any other linewidths criterion for the identification of excitonic complexes, a technique that can directly be applied to polar but even non‐polar QD materials. Additionally, we find an emission energy dependent trend for the FWHM ratios of the biexciton and the exciton (XX_FWHM/X_FWHM) in perfect agreement with their relative dipole moment ratios as derived from our 8‐band‐ k · p based treatment of the Coulomb and exchange interaction within these multi‐particle complexes. (© 2015 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

Theoretical study of quantum confined Stark shift in InAs／GaAs quantum dots

The quantum confined Stark effect (QCSE) of the self-assembled InAs/GaAs quantum dots has been investigated theoretically. The ground-state transition energies for quantum dots in the shape of a cube, pyramid or “truncated pyramid” are calculated and analysed. We use a method based on the Green function technique for calculating thestrain in quantum dots and an efficient plane-wave envelope-function technique to determine the ground-state electronic structure of them with different shapes. The symmetry of quantum dots is broken by the effect of strain. So the properties of carriers show different behaviours from the traditional quantum device. Based on these results, we also calculate permanent built-in dipole moments and compare them with recent experimental data. Our results demonstrate that the measured Stark effect in self-assembled InAs/GaAs quantum dot structures can be explained by including linear grading.     

Structure and effects of annealing in colloidal matrix‐free Ge quantum dots

The structure of small (2–5 nm) Ge quantum dots prepared by the colloidal synthesis route is examined. Samples were synthesized using either GeO₂ or GeCl₄ as precursor. As‐prepared samples were further annealed under Ar or H₂/Ar atmosphere at different temperatures in order to understand the effect of annealing on their structure. It was found that as‐prepared samples possess distinctly different structures depending on their synthesis route as indicated by their long‐range ordering. An appreciable amount of oxygen was found to be bound to Ge in samples prepared with GeO₂ as a precursor; however, not for GeCl₄. Based on combined transmission electron microscope, Raman, X‐ray diffraction and X‐ray absorption measurements, it is suggested that as‐prepared samples are best described by the core‐shell model with a small nano‐crystalline core and an amorphous outer layer terminated either with oxygen or hydrogen depending on the synthesis route. Annealing in an H₂Ar atmosphere leads to sample crystallization and further nanoparticle growth, while at the same time reducing the Ge—O bonding. X‐ray diffraction measurements for as‐prepared and annealed samples indicate that diamond‐type and metastable phases are present.     

All‐optical modulation based on silicon quantum dot doped SiOx:Si‐QD waveguide

All‐optical modulation based on silicon quantum dot doped SiO_x:Si‐QD waveguide is demonstrated. By shrinking the Si‐QD size from 4.3 nm to 1.7 nm in SiO_x matrix (SiO_x:Si‐QD) waveguide, the free‐carrier absorption (FCA) cross section of the Si‐QD is decreased to 8 × 10⁻¹⁸ cm² by enlarging the electron/hole effective masses, which shortens the PL and Auger lifetime to 83 ns and 16.5 ps, respectively. The FCA loss is conversely increased from 0.03 cm⁻¹ to 1.5 cm⁻¹ with the Si‐QD size enlarged from 1.7 nm to 4.3 nm due to the enhanced FCA cross section and the increased free‐carrier density in large Si‐QDs. Both the FCA and free‐carrier relaxation processes of Si‐QDs are shortened as the radiative recombination rate is enlarged by electron–hole momentum overlapping under strong quantum confinement effect. The all‐optical return‐to‐zero on‐off keying (RZ‐OOK) modulation is performed by using the SiO_x:Si‐QD waveguides, providing the transmission bit rate of the inversed RZ‐OOK data stream conversion from 0.2 to 2 Mbit/s by shrinking the Si‐QD size from 4.3 to 1.7 nm.     

Electron energy state spin-splitting in 3D cylindrical semiconductor quantum dots

In this article we study the impact of the spin-orbit interaction on the electron quantum confinement for narrow gap semiconductor quantum dots. The model formulation includes: (1) the effective one-band Hamiltonian approximation; (2) the position- and energy-dependent quasi-particle effective mass approximation; (3) the finite hard wall confinement potential; and (4) the spin-dependent Ben Daniel-Duke boundary conditions. The Hartree-Fock approximation is also utilized for evaluating the characteristics of a two-electron quantum dot system. In our calculation, we describe the spin-orbit interaction which comes from both the spin-dependent boundary conditions and the Rashba term (for two-electron quantum dot system). It can significantly modify the electron energy spectrum for InAs semiconductor quantum dots built in the GaAs matrix. The energy state spin-splitting is strongly dependent on the dot size and reaches an experimentally measurable magnitude for relatively small dots. In addition, we have found the Coulomb interaction and the spin-splitting are suppressed in quantum dots with small height. Received 15 May 2001 / Received in final form 14 May 2002 Published online 13 August 2002     

Raman spectroscopy of very small Cd1−xCoxS quantum dots grown by a novel protocol: direct observation of acoustic‐optical phonon coupling

Glass‐embedded Cd_1−xCo_xS quantum dots (QDs) with mean radius of R ≈ 1.70 nm were successfully synthesized by a novel protocol on the basis of the melting‐nucleation synthesis route and herein investigated by several experimental techniques. Incorporation of Co²⁺ ions into the QD lattice was evidenced by X‐ray diffraction and magnetic force microscopy results. Optical absorption features with irregular spacing in the ligand field region confirmed that the majority of the incorporated Co²⁺ ions are under influence of a low‐symmetry crystal field located near to the Cd_1−xCo_xS QD surface. Electron paramagnetic resonance data confirmed the presence of Co²⁺ ions in a highly inhomogeneous crystal field environment identified at the interface between the hosting glass matrix (amorphous) and the crystalline QD. The acoustic‐optical phonon coupling in the Cd_1−xCo_xS QDs (x ≠ 0.000) was directly observed by Raman measurements, which have shown a high‐frequency shoulder of the longitudinal optical phonon peak. This effect is tuned by the size‐dependent sp‐d exchange interaction due to the magnetic doping, causing variations in the coupling between electrons and longitudinal optical phonon. Copyright © 2013 John Wiley & Sons, Ltd.