Wurtzite Quantum Research Articles

Efficiency droop in zincblende InGaN/GaN quantum wells.

The decrease in emission efficiency with increasing drive current density, known as 'droop', of c-plane wurtzite InGaN/GaN quantum wells presently limits the use of light-emitting diodes based on them for high brightness lighting applications. InGaN/GaN quantum wells grown in the alternative zincblende phase are free of the strong polarisation fields that exacerbate droop and so were investigated by excitation-dependent photoluminescence and photoreflectance studies. Polarisation-resolved measurements revealed that for all excitation densities studied the emission from such samples largely originates from similar microstructures or combinations of microstructures that form within the quantum well layers. Emission efficiency varies significantly with excitation at 10 K showing that non-radiative recombination processes are important even at low temperature. The onset of efficiency droop, as determined by photomodulated reflection measurements, occurred at a carrier density of around 1.2 × 1020 cm-3 - an order of magnitude greater than the value reported for a reference wurtzite quantum well sample using the same method. The high carrier density droop onset combined with the much shorter carrier lifetime within zincblende InGaN/GaN quantum wells indicate they have the potential to effectively delay efficiency droop when used in GaN based light-emitting diodes. However, the material quality of the quantum well layers need to be improved by preventing the formation of microstructures within these layers, and the importance of the role played by non-radiative centres in the QW layer needs to be elucidated, to fully realise the material's potential.

State of the Art of Continuous and Atomistic Modeling of Electromechanical Properties of Semiconductor Quantum Dots.

The main intent of this paper is to present an exhaustive description of the most relevant mathematical models for the electromechanical properties of heterostructure quantum dots. Models are applied both to wurtzite and zincblende quantum dot due to the relevance they have shown for optoelectronic applications. In addition to a complete overview of the continuous and atomistic models for the electromechanical fields, analytical results will be presented for some relevant approximations, some of which are unpublished, such as models in cylindrical approximation or a cubic approximation for the transformation of a zincblende parametrization to a wurtzite one and vice versa. All analytical models will be supported by a wide range of numerical results, most of which are also compared with experimental measurements.

Shell effects on the dielectric properties of core-shell quantum dots.

The dielectric properties in semiconductor quantum dots are crucial for exciton formation, migration, and recombination. Different from 3D bulk materials, the dielectric response is, however, ambiguous for the small-sized 0D dots in which the effect of outer atoms on the inner atoms is usually described qualitatively. Based on the first-principles calculated electron density, the polarizability of the core-shell CdSe@ZnS wurtzite quantum dots is decomposed into the distributional contributions among which the dipole polarizability of the core is proposed to measure the shell effect on the dielectric properties of core-shell quantum dots. The shell thickness dependence on the shell effect is then studied, which is significant for the outermost shell but decays rapidly in the additional shells. Moreover, this model gives explicit physical origins of the core dipole polarizability in the core-shell QDs, which is determined by the intra-shell polarization and inter-core-shell charge transfer. Our study proposes a new approach for studying the dielectric properties of core-shell quantum dots, which is effective and extendable for other low-dimensional structures.

Spin polarization in quantum point contact based on wurtzite topological quantum well.

Manipulating spin polarization in wide-gap wurtzite semiconductors is crucial for the development of high-temperature spintronics applications. A topological insulator revealed recently in wurtzite quantum wells (QWs) provides a platform to mediate spin-polarized transport through the polarization field-driven topological edges and large Rashba spin-orbit coupling (SOC). Here, we propose a spin-polarized device in a quantum point contact (QPC) structure based on ZnO/CdO wurtzite topological QWs. The results show that the QPC width can sufficiently control the lateral spin-orbit coupling (SOC) as well as the band gap of the edge states through the quantum size effect. As a result, the spin-polarized conductance exhibits oscillation due to the spin precession, which can be controlled by adjusting the voltage imposed on the split gate. The QPC-induced large spin splitting is highly nonlinear and becomes strong close to the gap. The spin splitting of the edge states will be suppressed for QPC widths greater than 50 nm, and thus lead to an extremely long spin precession length. This QPC width-dependent lateral SOC effect provides an emerging electrical approach to manipulate spin-polarized electron transport in topological wurtzite systems.

Purifying single photon emission from giant shell CdSe/CdS quantum dots at room temperature.

Giant shell CdSe/CdS quantum dots are bright and flexible emitters, with near-unity quantum yield and suppressed blinking, but their single photon purity is reduced by efficient multiexcitonic emission. We report the observation, at the single dot level, of a large blueshift of the photoluminescence biexciton spectrum (24 ± 5 nm over a sample of 32 dots) for pure-phase wurtzite quantum dots. By spectral filtering, we demonstrate a 2.3 times reduction of the biexciton quantum yield relative to the exciton emission, while preserving as much as 60% of the exciton single photon emission, thus improving the purity from g2(0) = 0.07 ± 0.01 to g2(0) = 0.03 ± 0.01. At a larger pump fluency, spectral purification is even more effective with up to a 6.6 times reduction in g2(0), which is due to the suppression of higher order excitons and shell states experiencing even larger blueshifts. Our results indicate the potential for the synthesis of engineered giant shell quantum dots, with further increased biexciton blueshifts, for quantum optical applications requiring both high purity and brightness.

Wurtzite Quantum Wires with Strong Spatial Confinement: Polarization Anisotropies in Single-Wire Spectroscopy

We report GaAs/AlGaAs nanowires in the one-dimensional (1D) quantum limit. The ultrathin wurtzite GaAs cores between 20-40\,nm induce large confinement energies of several tens of meV, allowing us to experimentally resolve up to four well separated subband excitations in microphotoluminescence spectroscopy. Our detailed experimental and theoretical polarization-resolved study reveals a strong diameter-dependent anisotropy of these transitions: We demonstrate that the polarization of the detected photoluminescence is governed by the symmetry of the wurtzite 1D quantum wire subbands on the one hand, but also by the dielectric mismatch of the wires with the surrounding material on the other hand. The latter effect leads to a strong attenuation of perpendicularly polarized light in thin dielectric wires, making the thickness of the AlGaAs shell an important factor in the observed polarization behavior. Including the dielectric mismatch to our k.p-based simulated polarization-resolved spectra of purely wurtzite GaAs quantum wires, we find an excellent agreement between experiment and theory.

Effect of uniaxial compressive stress with different orientations on the hole mobility of wurtzite GaN heterojunction quantum well

The influence of uniaxial compressive stress with different orientations to the current channel on the physical and transport properties of the wurtzite GaN heterojunction quantum well is investigated in this work. By using the six-band stress-dependent k × p Hamiltonian, accurate two-dimensional physical pictures are given for the quantized valence subband under the uniaxial compressive stress on the (0001) transport plane. The low-field hole mobility is obtained by the Kubo–Greenwood formula, taking the scattering rates for acoustic phonon, polar optical phonon, and surface roughness into account. Using these methods, the microscopic relationship between the orientation of uniaxial compressive stress and low-field hole mobility is obtained according to the variations of valence subband dispersion and hole effective mass. Results show that for temperatures around and above room temperature, the acoustic phonon scattering is predominant. We find that the mobility gain is mostly contributed from effective mass, and there is an increasing trend under uniaxial compressive stress with all orientations due to the effective mass reduction. For the same stress value, the mobility decreases monotonically as the stress orientation changes from 0° to 90° with respect to the current channel. At room temperature, the calculated low-field hole mobility is 182 cm2/V s under 8 GPa uniaxial compressive stress parallel to the current channel, with the hole density of 5.5 × 1013 cm−2 and the effective electric field of 0.93 MV/cm.

Piezo-phototronic spin laser based on wurtzite quantum wells

Piezo-phototronic spin lasers are studied based on wurtzite quantum wells. The strain-induced polarization changes the gain spectrum and gain asymmetry at room temperature. In this work, the gain properties of piezo-phototronic spin lasers based on InGaN/GaN quantum wells can be modulated by strain-induced polarization. This work not only paves a new way for the room-temperature applications of quantum piezotronic and piezo-phototronic devices, but also provides new method of regulation for wurtzite spin lasers by strain-induced polarization.

Efficient Fourier space quantum dot k ⋅ p for wurtzite systems including smooth alloy profile and spatially varying elastic and dielectric constants

We present methods to calculate the electronic structure of wurtzite quantum dot systems with continuous alloy profiles within Fourier-space-based k⋅p theory. We incorporate spatially varying elastic and dielectric constants in strain and piezoelectric potential calculations. A method to incorporate smooth alloy profiles in all aspects of the calculations is presented. We demonstrate our methodology for the case of a 1-dimensional InGaN quantum dot array and show the importance of including these spatially varying parameters in the modeling of devices. We demonstrate that the convergence of the lowest bound state energies is for good approximation determined by the largest wave vector used in constructing the states. We also present a novel approach of coupling strain into the k⋅p Hamiltonian, greatly reducing the computational cost of generating the Hamiltonian.

High-Performance Piezo-Phototronic Devices Based on Intersubband Transition of Wurtzite Quantum Well.

III-nitride semiconductors play much more important roles in the areas of modern photoelectric applications, whereas strong polarization in their heterostructures is always a challenge to restrict the efficiency and performance of photoelectric devices. In this study, piezo-phototronic effect on near-infrared intersubband absorption is explored based on polar GaN/AlN quantum wells. The results show that externally applied pressure leads to the redshift of absorption wavelength by reducing polarization field of the quantum well. The sensitivity to estimate pressure-dependent intersubband absorption wavelength is almost two orders of magnitude higher than interband photoelectric devices. Additionally, such sensitivity is further enhanced by 2.6 times at 20GPa as a result of piezo-phototronic effect. This study paves avenue for designing high-performance near-infrared piezo-phototronic devices based on intersubband transition.

Wurtzite quantum well structures under high pressure

Quantum well systems based on semiconductors with the wurtzite crystalline structure have found widespread applications in photonics and optoelectronic devices, such as light-emitting diodes, laser diodes, or single-photon emitters. In these structures, the radiative recombination processes can be affected by (i) the presence of strain and polarization-induced electric fields, (ii) quantum well thickness fluctuations and blurring of a well–barrier interface, and (iii) the presence of dislocations and native point defects (intentional and unintentional impurities). A separate investigation of these phenomena is not straightforward since they give rise to similar effects, such as a decrease of luminescence efficiency and decay rate, enhancement of the Stokes shift, and strong blueshift of the emission with increasing pump intensity. In this Perspective article, we review the usefulness of measurements of the quantum well luminescence as a function of the hydrostatic pressure for both scientific research and the development of light-emitting technologies. The results presented here show that high-pressure investigations combined with ab initio calculations can identify the nature of optical transitions and the main physical factors affecting the radiative efficiency in quantum well systems. Finally, we will discuss an outlook to the further possibilities to gain new knowledge about the nature of recombination processes in quantum wells using high-pressure spectroscopy.

Persistent spin textures and currents in wurtzite nanowire-based quantum structures

We explore the spin and charge properties of electrons in wurtzite semiconductor nanowires where radial and axial confinement leads to tubular or ring-shaped quantum structures. Accounting for spin-orbit interaction induced by the wurtzite lattice as well as a radial potential gradient, we analytically derive the corresponding low-dimensional Hamiltonians. It is demonstrated that the resulting tubular spin-orbit Hamiltonian allows to construct spin states that are persistent in time and robust against disorder. We find that these special scenarios are characterized by distinctive features in the optical conductivity spectrum, which enable an unambiguous experimental verification. In both types of quantum structures, we discuss the dependence of the occurring persistent charge and spin currents on an axial magnetic field and Fermi energy which show clear fingerprints of the electronic subband structure. Here, the spin-preserving symmetries become manifest in the vanishing of certain spin current tensor components. Our analytic description relates the distinctive features of the optical conductivity and persistent currents to bandstructure characteristics which allows to deduce spin-orbit coefficients and other band parameters from measurements.

Spin-orbit coupling in wurtzite heterostructures

Effective spin-orbit (SO) Hamiltonians for conduction electrons in wurtzite heterostructures are lacking in the literature, in contrast to zincblende structures. Here we address this issue by deriving such an effective Hamiltonian valid for quantum wells, wires, and dots with arbitrary confining potentials and external magnetic fields. We start from an 8$\times$8 Kane model accounting for the $s$--$p_z$ orbital mixing important to wurtzite structures, but absent in zincblende, and apply both quasi-degenerate perturbation theory (L\"owdin partitioning) and the folding down approach to derive an effective 2$\times$2 electron Hamiltonian. We obtain the usual $k$-linear Rashba term arising from the structural inversion asymmetry of the wells and, differently from zincblende structures, a bulk Rashba-type term induced by the inversion asymmetry of the wurtzite lattice. We also find linear- and cubic-in-momentum Dresselhaus contributions. Both the bulk Rashba-type term and the Dresselhaus terms originate exclusively from the admixture of $s$- and $p_z$-like states in wurtzites structures. Interestingly, in these systems the linear Rashba and the Dresselhaus terms have the same symmetry and can in principle cancel each other out completely, thus making the spin a conserved quantity. We determine the intrasubband (intersubband) Rashba $\alpha_\nu$ ($\eta$) and linear Dresselhaus $\beta_\nu$ ($\Gamma$) SO strengths of GaN/AlGaN single and double wells with one and two occupied subbands ($\nu=1,2$). We believe our general effective Hamiltonian for electrons in wurtzite heterostructures put forward here, should stimulate additional theoretical works on wurtzite quantum wells, wires, and dots with variously defined geometries and external magnetic fields.

General condition for realizing a collinear spin-orbit effective magnetic field in two-dimensional electron systems and its application to zinc-blende and wurtzite quantum wells

In this paper, we have studied two-dimensional (2D) electron systems described by the effective Hamiltonians containing spin-orbit coupling (SOC) terms up to an arbitrary odd order in wave vector k. The general condition for realizing a SOC-induced effective magnetic field (SOF) in such systems, formulated only in terms of the SOC parameters, is derived. When this condition is satisfied, the projection of the electron spin on the direction of the collinear SOF is a conserved quantity. The complete set of the k-linear and k-cubic Dresselhaus SOC contributions to the effective 2D Hamiltonian of an arbitrarily oriented zinc-blende quantum well is computed by a proper averaging of the corresponding tight-binding bulk SOC Hamiltonian. We investigate possibilities for realization of the collinear SOF in zinc-blende quantum wells of different orientation and obtain some interesting findings, which supplement the results of earlier works. Application of the developed formalism to wurtzite semiconductor 2D systems shows that the collinear SOF can be also realized in a wide class of such quantum wells.

Realization of linearly polarized exciton emission in wurtzite zinc oxide quantum dots

Linearly polarized exciton emission from a quantum dot is very appealing for polarized light emitting diodes and quantum information science and technologies. However, it has been very difficult to access it, because conventional wurtzite quantum dots (QDs) usually favor circularly polarized exciton emission originating from a single electron bound to a hole with dominant heavy hole ($A$ band) character. Here we explore the exciton fine structure of wurtzite ZnO QDs by means of plane-wave million-atom atomistic pseudopotential calculations and a configuration interaction approach. We demonstrate that linearly polarized emission could be realized in these QDs by (i) enhancing the quantum confinement effects and (ii) applying hydrostatic pressure. Such an exciton has a polarization exclusively along the $c$-axis direction of the QDs, which derives from a single electron bounded to a hole state with a split-off hole ($C$-band) character. This work paves the way for the exploration of the fundamental properties of wurtzite ZnO QDs and their potential applications in optoelectronic devices and quantum technologies.

Wurtzite spin lasers

Semiconductor lasers are strongly altered by adding spin-polarized carriers. Such spin lasers could overcome many limitations of their conventional (spin-unpolarized) counterparts. While the vast majority of experiments in spin lasers employed zinc-blende semiconductors, the room temperature electrical manipulation was first demonstrated in wurtzite GaN-based lasers. However, the underlying theoretical description of wurtzite spin lasers is still missing. To address this situation, focusing on (In,Ga)N-based wurtzite quantum wells, we develop a theoretical framework in which the calculated microscopic spin-dependent gain is combined with a simple rate equation model. A small spin-orbit coupling in these wurtzites supports simultaneous spin polarizations of electrons and holes, providing unexplored opportunities to control spin lasers. For example, the gain asymmetry, as one of the key figures of merit related to spin amplification, can change the sign by simply increasing the carrier density. The lasing threshold reduction has a nonmonotonic depenedence on electron spin polarization, even for a nonvanishing hole spin polarization.

Analysis of the exciton–LO-phonon coupling in single wurtzite GaN quantum dots

In this study, we analyze the interaction between excitons and longitudinal-optical phonons (LO phonons) in single, wurtzite GaN quantum dots (QDs) by means of micro-photoluminescence $(\ensuremath{\mu}\mathrm{PL})$ spectroscopy. We report on Stokes-shifted emission lines measured for hundreds of single QDs. A decrease of the Huang-Rhys factor $(\ensuremath{\sim}0.5\text{--}0.01)$ is observed with increasing QD emission energy that can be modeled in an adiabatic approximation applying two-particle eight-band $\mathbf{k}\ifmmode\cdot\else\textperiodcentered\fi{}\mathbf{p}$ wave functions. In order to obtain the QD dimensions and shape needed for these calculations, we conduct a scanning transmission electron microscope (STEM) analysis, not only focusing on the QD dimensions, but also on alloying effects. The QD height is identified as the most detrimental parameter for the exciton-LO-phonon interaction in strongly polar QD systems based on nitrides. Additionally, we extract the LO-phonon energy for a significant number of individual QDs from our $\ensuremath{\mu}\mathrm{PL}$ data set scaling in-between the bulk values for the QD (GaN) and the matrix material (AlN). Such a large variation of the LO-phonon energy cannot be explained by the alloying effects attested by our STEM analysis. Hence, the exciton-LO-phonon interaction resides in a volume that encloses the QD in the growth direction and a fraction of the matrix material depending on the QD height. We approximate this exciton-LO-phonon interaction volume by a sphere with a constant diameter of $2.6\phantom{\rule{0.16em}{0ex}}\ifmmode\pm\else\textpm\fi{}\phantom{\rule{0.16em}{0ex}}0.2$ nm.

Accelerating atomistic calculations of quantum energy eigenstates on graphic cards

Electronic properties of nanoscale materials require the calculation of eigenvalues and eigenvectors of large matrices. This bottleneck can be overcome by parallel computing techniques or the introduction of faster algorithms. In this paper we report a custom implementation of the Lanczos algorithm with simple restart, optimized for graphical processing units (GPUs). The whole algorithm has been developed using CUDA and runs entirely on the GPU, with a specialized implementation that spares memory and reduces at most machine-to-device data transfers. Furthermore parallel distribution over several GPUs has been attained using the standard message passing interface (MPI). Benchmark calculations performed on a GaN/AlGaN wurtzite quantum dot with up to 600,000 atoms are presented. The empirical tight-binding (ETB) model with an sp3d5s∗+spin–orbit parametrization has been used to build the system Hamiltonian (H).

Hartree-Fock Problem of Electron-Hole Pair in Quantum Well GаN

We present microscopic calculations of the absorption spectra for GaN=AlxGa1 xN quantum well systems. Whereas the quantum well structures with the parabolic law of dispersion exhibit the usual bleaching of an exciton resonance without shifting a spectral position, the significant red-shift of an exciton peak is found with increasing the electron-hole gas density for a wurtzite quantum well. The energy of the exciton resonance for a wurtzite quantum well is found. The obtained results can be explained by the influence of the valence band structure on quantum confinement effects. The optical gain spectrum in the Hartree–Fock approximation and the Sommerfeld enhancement are calculated. A red shift of the gain spectrum in the Hartree–Fock approximation with respect to the Hartree gain spectrum is found.

Coupled electromechanical effects in wurtzite quantum dots with wetting layers in gate controlled electric fields: The multiband case

We quantify the influence of coupled electromechanical effects on the band structure calculations of wurtzite AlN/GaN quantum dots with wetting layers (WLs). Based on a strain dependent fully coupled 8-band k·p method, we computed eigenvalues and wavefunctions of electrons in quantum dots with WLs of different aspect ratios. These computed eigenvalues are compared to those obtained from the method based on decoupled 2-conduction and 6-valence bands envelope functions. Previously, such comparisons, accounting for the wetting layer, were systematically done only for models based on not more than 4-bands. In addition, we apply gate potential along z-direction to bring the conduction and valence bands closer so that we numerically estimate the influence of gate controlled electric fields on the intra-subband energy in quantum dots. Due to the non-parabolicity term in the effective mass approximation, our study shows that the intra-sub band energy (i.e., the energy difference between ground and first excited states) is smaller for electrons and larger for holes in the 8-band k·p method than those eigenvalues obtained from the decoupled 2-conduction and 6-valence bands envelope functions method. In this paper, we show that the intra-sub band energy increases in presence of piezo-electromechanical effects and externally applied gate potentials along z-direction. We numerically estimate the distribution (i.e., the probability density) of electrons and holes wavefunctions in the dots that is obtained from both the 8-band k·p method and the decoupled 2- and 6-bands envelope functions method.