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Register a new userPolarization Response in InAs Quantum Dots: Theoretical Correlation between Composition and Electronic Properties
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III-V growth and surface conditions strongly influence the physical structure and resulting optical properties of self-assembled quantum dots (QDs). Beyond the design of a desired active optical wavelength, the polarization response of QDs is of particular interest for optical communications and quantum information science. Previous theoretical studies based on a pure InAs QD model failed to reproduce experimentally observed polarization properties. In this work, multi-million atom simulations are performed to understand the correlation between chemical composition and polarization properties of QDs. A systematic analysis of QD structural parameters leads us to propose a two layer composition model, mimicking In segregation and In-Ga intermixing effects. This model, consistent with mostly accepted compositional findings, allows to accurately fit the experimental PL spectra. The detailed study of QD morphology parameters presented here serves as a tool for using growth dynamics to engineer the strain field inside and around the QD structures, allowing tuning of the polarization response.
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Built-in electrostatic fields in Zincblende quantum dots originate mainly from - (1) the fundamental crystal atomicity and the interfaces between two dissimilar materials, (2) the strain relaxation, and (3) the piezoelectric polarization. In this paper, using the atomistic NEMO 3-D simulator, we study the origin and nature of the internal fields in InAs/GaAs quantum dots with three different geometries, namely, box, dome, and pyramid. We then calculate and delineate the impact of the internal fields in the one-particle electronic states in terms of shift in the conduction band energy states, anisotropy and non-degeneracy in the P level, and formation of mixed excited bound states. Models and approaches used in this study are as follow: (1) Valence force field (VFF) with strain-dependent Keating potentials for atomistic strain relaxation; (2) 20-band nearest-neighbor sp3d5s* tight-binding model for the calculation of single-particle energy states; and (3) For piezoelectricity, for the first time within the framework of sp3d5s* tight-binding theory, four different recently-proposed polarization models (linear and non-linear) have been considered in conjunction with an atomistic 3-D Poisson solver that also takes into account the image charge effects. Specifically, in contrast to recent studies on similar quantum dots, our calculations yield a non-vanishing net piezoelectric contribution to the built-in electrostatic field. Demonstrated also is the importance of full three-dimensional (3-D) atomistic material representation and the need for using realistically-extended substrate and cap layers (systems containing ~2 million atoms) in the numerical modeling of these reduced-dimensional quantum dots.
Luminescent colloidal CdSe nanorings are a new type of semiconductor structure that have attracted interest due to the potential for unique physics arising from their non-trivial toroidal shape. However, the exciton properties and dynamics of these materials with complex topology are not yet well understood. Here, we use a combination of femtosecond vibrational spectroscopy, temperature-resolved photoluminescence (PL), and single particle measurements to study these materials. We find that on transformation of CdSe nanoplatelets to nanorings, by perforating the center of platelets, the emission lifetime decreases and the emission spectrum broadens due to ensemble variations in the ring size and thickness. The reduced PL quantum yield of nanorings (~10%) compared to platelets (~30%) is attributed to an enhanced coupling between: (i) excitons and CdSe LO-phonons at 200 cm-1 and (ii) negatively charged selenium-rich traps which give nanorings a high surface charge (~-50 mV). Population of these weakly emissive trap sites dominates the emission properties with an increased trap emission at low temperatures relative to excitonic emission. Our results provide a detailed picture of the nature of excitons in nanorings and the influence of phonons and surface charge in explaining the broad shape of the PL spectrum and the origin of PL quantum yield losses. Furthermore, they suggest that the excitonic properties of nanorings are not solely a consequence of the toroidal shape but are also a result of traps introduced by puncturing the platelet center.
The GaAs-based material system is well-known for the implementation of InAs quantum dots (QDs) with outstanding optical properties. However, these dots typically emit at a wavelength of around 900nm. The insertion of a metamorphic buffer (MMB) can shift the emission to the technologically attractive telecom C-band range centered at 1550nm. However, the thickness of common MMB designs limits their compatibility with most photonic resonator types. Here we report on the MOVPE growth of a novel InGaAs MMB with a non-linear indium content grading profile designed to maximize plastic relaxation within minimal layer thickness. Single-photon emission at 1550nm from InAs QDs deposited on top of this thin-film MMB is demonstrated. The strength of the new design is proven by integrating it into a bullseye cavity via nano-structuring techniques. The presented advances in the epitaxial growth of QD/MMB structures form the basis for the fabrication of high-quality telecom non-classical light sources as a key component of photonic quantum technologies.
Magnetic two-dimensional (2D) materials have received tremendous attention recently due to its potential application in spintronics and other magnetism related fields. To our knowledge, five kinds of 2D materials with intrinsic magnetism have been synthesized in experiment. They are CrI3, Cr2Ge2Te6, FePS3, Fe3GeTe2 and VSe2. Apart from the above intrinsic magnetic 2D materials, many strategies have also been proposed to induce magnetism in normal 2D materials such as atomic modification, spin valve and proximity effect. Various devices have also been designed to fulfill the basic functions of spintronics: inducing spin, manipulating spin and detecting spin.
Based on first-principles method we predict a new low-energy Stone-Wales graphene SW40, which has an orthorhombic lattice with Pbam symmetry and 40 carbon atoms in its crystalline cell forming well-arranged Stone-Wales patterns. The calculated total energy of SW40 is just about 133 meV higher than that of graphene, indicating its excellent stability exceeds all the previously proposed graphene allotropes. We find that SW40 processes intrinsic Type-III Dirac-cone (Phys. Rev. Lett., 120, 237403, 2018) formed by band-crossing of a local linear-band and a local flat-band, which can result in highly anisotropic Fermions in the system. Interestingly, such intrinsic type-III Dirac-cone can be effectively tuned by inner-layer strains and it will be transferred into Type-II and Type-I Dirac-cones under tensile and compressed strains, respectively. Finally, a general tight-binding model was constructed to understand the electronic properties nearby the Fermi-level in SW40. The results show that type-III Dirac-cone feature can be well understood by the $pi$-electron interactions between adjacent Stone-Wales defects.
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