We study theoretically the electronic properties of $c$-plane GaN/AlN quantum dots (QDs) with focus on their potential as sources of single polarized photons for future quantum communication systems. Within the framework of eight-band k.p theory we calculate the optical interband transitions of the QDs and their polarization properties. We show that an anisotropy of the QD confinement potential in the basal plane (e.g. QD elongation or strain anisotropy) leads to a pronounced linear polarization of the ground state and excited state transitions. An externally applied uniaxial stress can be used to either induce a linear polarization of the ground-state transition for emission of single polarized photons or even to compensate the polarization induced by the structural elongation.
The strain induced by lattice mismatch at the interface is responsible for the different value of the band discontinuities observed recently for the AlN/GaN (AlN on GaN) and the GaN/AlN (GaN on AlN) polar (0001) interface. We present a first-principles calculation of valence band offsets, interface dipoles, strain-induced piezoelectric fields, relaxed geometric structure, and formation energies. Our results confirm the existence of a large forward-backward asymmetry for this interface.
Grazing incidence anomalous x-ray scattering was used to monitor in situ the molecular beam epitaxy growth of GaN/AlN quantum dots (QDs). The strain state was studied by means of grazing incidence Multi-wavelength Anomalous Di raction (MAD) in both the QDs and the AlN during the progressive coverage of QDs by AlN monolayers. Vertical correlation in the position of the GaN QDs was also studied by both grazing incidence MAD and anomalous Grazing Incidence Small Angle Scattering (GISAXS) as a function of the number of GaN planes and of the AlN spacer thickness. In a regime where the GaN QDs and t…
First-principles investigations of the structural, electronic and magnetic properties of Cr-doped AlN/GaN (0001) heterostructures reveal that Cr segregates into the GaN region, that these interfaces retain their important half-metallic character and thus yield efficient (100 %) spin polarized injection from a ferromagnetic GaN:Cr electrode through an AlN tunnel barrier - whose height and width can be controlled by adjusting the Al concentration in the graded bandgap engineered Al(1-x)Ga(x)N (0001) layers.
We demonstrate the growth of GaN/AlN quantum well structures by plasma-assisted molecular-beam epitaxy by taking advantage of the surfactant effect of Ga. The GaN/AlN quantum wells show photoluminescence emission with photon energies in the range between 4.2 and 2.3 eV for well widths between 0.7 and 2.6 nm, respectively. An internal electric field strength of $9.2\pm 1.0$ MV/cm is deduced from the dependence of the emission energy on the well width.
In this work, we present an off-axis holography study of GaN/AlN heterostructured nanowires grown by plasma-assisted molecular-beam epitaxy. We discuss the sample preparation of nanowire samples for electron holography and combine potential profiles obtained using holography with theoretical calculations of the projected potential in order to gain understanding of the potential distribution in these nanostructures. The effects of surface states are discussed
We report on electrostatic screening of polarization-induced internal electric fields in AlN/GaN nanowire heterostructures with Germanium-doped GaN nanodiscs embedded between AlN barriers. The incorporation of Germanium at concentrations above $10^{20}\,\text{cm}^{-3}$ shifts the photoluminescence emission energy of GaN nanodiscs to higher energies accompanied by a decrease of the photoluminescence decay time. At the same time, the thickness-dependent shift in emission energy is significantly reduced. In spite of the high donor concentration a degradation of the photoluminescence properties is…
We report on the impact of growth conditions on surface hillock density of N-polar GaN grown on nominally on-axis (0001) sapphire substrate by metal organic chemical vapor deposition (MOCVD). Large reduction in hillock density was achieved by implementation of an optimized high temperature AlN nucleation layer and use of indium surfactant in GaN overgrowth. A reduction by more than a factor of five in hillock density from 1000 to 170 hillocks/cm$^{-2}$ was achieved as a result. Crystal quality and surface morphology of the resultant GaN films were characterized by high resolution x-ray diffrac…
Interface phonon (IF) modes of c-plane oriented [AlN/GaN]20 and Al0.35Ga0.65N/Al0.55Ga0.45N]20 multi quantum well (MQW) structures grown via plasma assisted molecular beam epitaxy are reported. The effect of variation in dielectric constant of barrier layers to the IF optical phonon modes of well layers periodically arranged in the MQWs investigated.
Seeking a better understanding of the electron transport in n-doped zinc blende GaN and wurtzite AlN, it was performed here a theoretical study resorting to Non Equilibrium Statistical Operator Method, which provides a set of coupled nonlinear differential evolution equations that provides a description of the dissipative phenomena developed in the system. The ultrafast time evolution (and the steady-state) of the electron drift velocity is obtained assuming different values for the electron effective mass.
We report the observation of ferromagnetism at over 900K in Cr-GaN and Cr-AlN thin films. The saturation magnetization moments in our best films of Cr-GaN and Cr-AlN at low temperatures are 0.42 and 0.6 u_B/Cr atom, respectively, indicating that 14% and 20%, of the Cr atoms, respectively, are magnetically active. While Cr-AlN is highly resistive, Cr-GaN exhibits thermally activated conduction that follows the exponential law expected for variable range hopping between localized states. Hall measurements on a Cr-GaN sample indicate a mobility of 0.06 cm^2/V.s, which falls in the range character…
Starting with empirical tight-binding band structures, the branch-point (BP) energies and resulting valence band offsets (VBOs) for the zincblende phase of InN, GaN and AlN are calculated from their k-averaged midgap energy. Furthermore, the directional dependence of the BPs of GaN and AlN is discussed using the Green's function method of Tersoff. We then show how to obtain the BPs for binary semiconductor alloys within a band-diagonal representation of the coherent potential approximation (CPA) and apply this method to cubic AlGaN alloys. The resulting band offsets show good agreement to avai…
An in situ study of the epitaxial growth of SmN thin films on Ga-polar GaN (0001)templates by molecular beam epitaxy is reported. Using X-ray photoelectron spectroscopy we found that Ga segregates at the surface during the first stages of growth. We showed that the problem related to Ga surface segregation can be simply suppressed by growing a few monolayers of AlN before starting the SmN growth. This results in a significant improvement of the crystallinity of SmN thin films assessed by X-ray diffraction.
We study the nucleation of GaN islands grown by plasma-assisted molecular-beam epitaxy on AlN(0001) in a Stranski-Krastanov mode. In particular, we assess the variation of their height and density as a function of GaN coverage. We show that the GaN growth passes four stages: initially, the growth is layer-by-layer; subsequently, two-dimensional precursor islands form, which transform into genuine three-dimensional islands. During the latter stage, island height and density increase with GaN coverage until the density saturates. During further GaN growth, the density remains constant and a bimo…
AlN layers with thicknesses between 2 and 14 nm were grown on Si(111) substrates by molecular beam epitaxy. The effect of the AlN layer thickness on the morphology and nucleation time of spontaneously formed GaN nanowires (NWs) was investigated by scanning electron microscopy and line-of-sight quadrupole mass spectrometry, respectively. We observed that the alignment of the NWs grown on these layers improves with increasing layer thickness while their nucleation time decreases. Our results show that 4 nm is the smallest thickness of the AlN layer that allows the growth of well-aligned NWs with…
Compositionally graded interfaces in power electronic devices eliminate dislocations, but they can also decrease thermal conduction, leading to overheating. We quantify the thermal resistances of GaN/AlN graded interfaces of varying thickness using ab initio Green's functions, and compare them with the abrupt interface case. A non-trivial power dependence of the thermal resistance versus interface thickness emerges from the interplay of alloy and mismatch scattering mechanisms. We show that the overall behavior of such graded interfaces is very similar to that of a thin-film of an effective al…
This work shows that the combination of ultrathin highly strained GaN quantum wells embedded in an AlN matrix, with controlled isotopic concentrations of Nitrogen enables a dual marker method for Raman spectroscopy. By combining these techniques, we demonstrate the effectiveness in studying strain in the vertical direction. This technique will enable the precise probing of properties of buried active layers in heterostructures, and can be extended in the future to vertical devices such as those used for optical emitters, and for power electronics.
We employ effective mass theory for degenerate hole-bands to calculate the acceptor binding energies for Be, Mg, Zn, Ca, C and Si substitutional acceptors in GaN and AlN. The calculations are performed through the 6$\times $6 Rashba-Sheka-Pikus and the Luttinger-Kohn matrix Hamiltonians for wurtzite (WZ) and zincblende (ZB) crystal phases, respectively. An analytic representation for the acceptor pseudopotential is used to introduce the specific nature of the impurity atoms. The energy shift due to polaron effects is also considered in this approach. The ionization energy estimates are in very…
In this work we present a comparison of multiband k.p-models, the effective bond-orbital approach, and an empirical tight-binding model to calculate the electronic structure for the example of a truncated pyramidal GaN/AlN self-assembled quantum dot with a zincblende structure. For the system under consideration, we find a very good agreement between the results of the microscopic models and the 8-band k.p-formalism, in contrast to a 6+2-band k.p-model, where conduction band and valence band are assumed to be decoupled. This indicates a surprisingly strong coupling between conduction and valen…
We studied the persistent photoconductivity (PPC) effect in AlGaN/AlN/GaN heterostructures with two different Al-compositions (x=0.15 and x=0.25). The two-dimensional electron gas formed at the AlN/GaN heterointerface was characterized by Shubnikov-de Haas and Hall measurements. Using optical illumination, we were able to increase the carrier density of the Al0.15Ga0.85N/AlN/GaN sample from 1.6x10^{12} cm^{-2} to 5.9x1012 cm^{-2}, while the electron mobility was enhanced from 9540 cm2/Vs to 21400 cm2/Vs at T = 1.6 K. The persistent photocurrent in both samples exhibited a strong dependence on …
Resonant tunneling diodes are formed using AlN/GaN core-shell nanowire heterostructures grown by plasma assisted molecular beam epitaxy on n-Si(111) substrates. By using a coaxial geometry these devices take advantage of non-polar (m-plane) nanowire sidewalls. Device modeling predicts non-polar orientation should enhance resonant tunneling compared to a polar structure and that AlN double barriers will lead to higher peak-to-valley current ratios compared to AlGaN barriers. Electrical measurements of ensembles of nanowires show negative differential resistance appearing only at cryogenic tempe…
Heterostructures consisting of alternating GaN/AlN epitaxial layers represent the building-blocks of state-of-the-art devices employed for active cooling and energy-saving lightning. Insights into the heat conduction of these structures are essential in the perspective of improving the heat management for prospective applications. Here, the cross-plane (perpendicular to the sample's surface) thermal conductivity of GaN/AlN superlattices as a function of the layers' thickness is established by employing the $3ω$-method. Moreover, the role of interdiffusion at the interfaces on the phonon scatte…
High spin states of cation vacancies in GaP, GaN, AlN, BN, ZnO and BeO were analyzed by first principles calculations. The spin-polarized vacancy-induced level is located in the band gap in GaP, ZnO and BeO. In the nitrides, the stronger exchange coupling forces the vacancy states to be resonant with valence bands, forbids formation of positively charged vacancies in GaN and BN, and allows Al vacancy in p-AlN to assume the highest possible S=2 spin state. The shape of the spin density, isotropic in the zinc blende structure, has a pronounced directional character in the wurtzite structure. Sta…
Due to the wide range of possible applications, atomically thin two-dimensional heterostructures have attracted much attention. In this work, using first-principles calculations, we investigated the structural and electronic properties of planar AlN/GaN hybrid heterojunctions with the presence of vacancies at their interfaces. Our results reveal that a single vacant site, produced by the removal of Aluminum or Gallium atom, produces similar electronic band structures with localized states within the bandgap. We have also observed a robust magnetic behavior. A nitrogen-vacancy, on the other han…
We report the first realization of molecular beam epitaxy grown strained GaN quantum well field-effect transistors on single-crystal bulk AlN substrates. The fabricated double heterostructure FETs exhibit a two- dimensional electron gas (2DEG) density in excess of 2x10^13/cm2. Ohmic contacts to the 2DEG channel were formed by n+ GaN MBE regrowth process, with a contact resistance of 0.13 Ohm-mm. Raman spectroscopy using the quantum well as an optical marker reveals the strain in the quantum well, and strain relaxation in the regrown GaN contacts. A 65-nm-long rectangular-gate device showed a r…
In this paper, we present a collection of results focussing on the transport properties of doped direct-gap inverted-band highly polar III-nitride semiconductors (GaN, AlN, InN) and GaAs in the transient and steady state, calculated by using nonlinear quantum kinetic theory based on a non-equilibrium statistical ensemble formalism (NESEF). In the present paper, these results are compared with calculations usingMonteCarlo modelling simulations and experimental measurements. Both n-type and p-type materials, in the presence of intermediate to high electric fields, are considered for several temp…
Ultra-wide-band-gap group-III nitrides are of interest for applications in deep-ultraviolet optoelectronics and power electronics. Such devices must be able to efficiently dissipate heat generated from their operation, making the thermal conductivity of the constituent materials an important parameter for high-power applications. We have investigated the phonon-limited thermal conductivity of AlN, GaN, and Al$_x$Ga$_{1-x}$N using first-principles calculations, with a focus on the effects of compositional and isotopic disorder. Our Boltzmann-transport-equation calculations show that the maximum…
RF plasma assisted MBE growth of Scandium Nitride (ScN) thin films on GaN (0001)/SiC, AlN (0001)/Al2O3 and on 6H-SiC (0001) hexagonal substrates is found to lead to a face centered cubic (rock-salt) crystal structure with (111) out-of-plane orientation instead of hexagonal orientation. For the first time, cubic (111) twinned patterns in ScN are observed by in-situ electron diffraction during epitaxy, and the twin domains in ScN are detected by electron backscattered diffraction, and further corroborated with X-ray diffraction. The epitaxial ScN films display very smooth, sub nanometer surface …
The investigation of small size embedded nanostructures, by a combination of complementary anomalous diffraction techniques, is reported. GaN Quantum Dots (QDs), grown by molecular beam epitaxy in a modified Stranski-Krastanow mode, are studied in terms of strain and local environment, as a function of the AlN cap layer thickness, by means of grazing incidence anomalous diffraction. That is, the X-ray photons energy is tuned across the Ga absorption K-edge which makes diffraction chemically selective. Measurement of \textit{hkl}-scans, close to the AlN (30-30) Bragg reflection, at several ener…
The single crystal elastic constants, polycrystalline elastic moduli and related properties of orthorhombic MgSiN$_{2}$, MgGeN$_{2}$ and MgSnN$_{2}$ have been calculated using density functional theory and compared to the related wurtzite structured AlN, GaN and InN. Since there are no experimental studies of single crystal elastic properties of neither MgSiN$_{2}$, MgGeN$_{2}$ or MgSnN$_{2}$, we have established the accuracy of the calculations by comparison with experimental data for AlN, GaN and InN. The calculated polycrystalline elastic moduli of MgSiN$_{2}$ are found to be in good agreem…
We have demonstrated surface-plasmon induced change in spontaneous emission rate in the ultraviolet regime at ~ 375-380 nm, using AlN/GaN quantum dots (QD). Using time-resolved and continuous-wave photoluminescence measurements, the recombination rate in AlN/GaN QD is shown to be enhanced when spontaneous emission is resonantly coupled to a metal-surface plasmon mode. The exciton recombination process via Ag-surface plasmon modes is observed to be as much as 3-7 times faster than in normal QD spontaneous emission and depends strongly on the emission wavelength and silver thickness.
N-polar GaN/AlN resonant tunneling diodes are realized on single-crystal N-polar GaN bulk substrate by plasma-assisted molecular beam epitaxy growth. The room-temperature current-voltage characteristics reveal a negative differential conductance (NDC) region with a peak tunneling current of 6.8$\pm$ 0.8 kA/cm$^2$ at a forward bias of ~8 V. Under reverse bias, the polarization-induced threshold voltage is measured at ~$-$4 V. These resonant and threshold voltages are well explained with the polarization field which is opposite to that of the metal-polar counterpart, confirming the N-polarity of…
A number of diverse bulk properties of the zincblende and wurtzite III-V nitrides AlN, GaN, and InN, are predicted from first principles within density functional theory using the plane-wave ultrasoft pseudopotential method, within both the LDA (local density) and GGA (generalized gradient) approximations to the exchange-correlation functional. Besides structure and cohesion, we study formation enthalpies (a key ingredient in predicting defect solubilities and surface stability), spontaneous polarizations and piezoelectric constants (central parameters for nanostructure modeling), and elastic …
The optical orientation of the exciton spin in an ensemble of self-organized cubic GaN/AlN quantum dots is studied by time-resolved photoluminescence. Under a polarized quasi-resonant excitation, the luminescence linear polarization exhibits no temporal decay, even at room temperature. This demonstrates the robustness of the exciton spin polarization in these cubic nitride nanostructures, with characteristic decay times longer than 10 ns.
We have derived consistent sets of band parameters (band gaps, crystal field-splittings, band gap deformation potentials, effective masses, Luttinger and EP parameters) for AlN, GaN, and InN in the zinc-blende and wurtzite phases employing many-body perturbation theory in the G0W0 approximation. The G0W0 method has been combined with density-functional theory (DFT) calculations in the exact-exchange optimized effective potential approach (OEPx) to overcome the limitations of local-density or gradient-corrected DFT functionals (LDA and GGA). The band structures in the vicinity of the Gamma-poin…
In this paper, we study band-to-band and intersubband characteristics of GaN/AlN heterostructures (planar and nanowires) structurally designed to absorb in the short-wavelength infrared region, particularly at 1.55 microns. We compare the effect of doping the GaN sections with Si and Ge, and we discuss the variation of free-carrier screening with the doping density and well/nanodisk size. We observe that nanowire heterostructures consistently present longer photoluminescence decay times than their planar counterparts, which supports the existence of an in-plane piezoelectric field associated t…
O2-plamsa-based digital etching of Al0.25Ga0.75N with a 0.8 nm AlN spacer on GaN was investigated. At 40 W RF bias power and 40 sccm oxygen flow, the etch depth of Al0.25Ga0.75N was 5.7 nm per cycle. The 0.8 nm AlN spacer layer acted as an etch-stop layer in 3 cycles. The surface roughness improved to 0.33 nm after 7 digital etch cycles. Compared to the dry etch only approach, this technique causes less damages. It was shown to be effective in precisely controlling the AlGaN etch depth required for recessed-AlGaN HEMTs.
Interplay between growth conditions and formation of localized light emitters in epitaxial AlN thin films
Paul-Drude-Institut für Festkörperelektronik, Leibniz-Institut im Forschungsverbund Berlin e.V.（柏林莱布尼茨固体电子学保罗·德鲁德研究所）；Helmholtz-Zentrum Dresden-Rossendorf, Institute of Ion Beam Physics and Materials Research（德累斯顿-罗斯多夫亥姆霍兹中心离子束物理与材料研究所）
We present ab initio density-functional calculations for acceptors, donors, and native defects in aluminum nitride, showing that acceptors are deeper (Be ~ 0.25 eV, Mg_ 0.45 eV) and less soluble than in GaN; at further variance with GaN, both the extrinsic donors Si_Al and C_Al, and the native donor V_N (the anion vacancy) are found to be deep (about 1 to 3 eV below the conduction). We thus predict that doped AlN will generally turn out to be semi-insulating in the normally achieved Al-rich conditions, in agreement with the known doping difficulties of high-x AlGaN alloys.
Electrically injected deep ultra-violet (UV) emission is obtained using monolayer (ML) thin GaN/AlN quantum structures as active regions. The emission wavelength is tuned by controlling the thickness of ultrathin GaN layers with monolayer precision using plasma assisted molecular beam epitaxy (PAMBE). Single peaked emission spectra is achieved with narrow full width at half maximum (FWHM) for three different light emitting diodes (LEDs) operating at 232 nm, 246 nm and 270 nm. 232 nm (5.34 eV) is the shortest EL emission wavelength reported so far using GaN as the light emitting material and em…
The rapidly increasing interest in nanowires (NWs) of GaN and associated III-Nitrides for (opto-)electronic applications demands immediate addressal of the technological challenges associated with both NW-growth and device processing. Towards this end, we demonstrate in this work an approach to suppress thermal decomposition of GaN NWs, which also serves to remedy the effect of NW-coalescence during growth. While both these effects are well-known to be major hurdles in the development of GaN-NW-devices, reliable methods to tackle these issues have not been reported so far. We show that by prov…
The optical properties of a stack of GaN/AlN quantum discs (QDiscs) in a GaN nanowire have been studied by spatially resolved cathodoluminescence (CL) at the nanoscale (nanoCL) using a Scanning Transmission Electron Microscope (STEM) operating in spectrum imaging mode. For the electron beam excitation in the QDisc region, the luminescence signal is highly localized with spatial extension as low as 5 nm due to the high band gap difference between GaN and AlN. This allows for the discrimination between the emission of neighbouring QDiscs and for evidencing the presence of lateral inclusions, abo…
We propose a new method to calculate polarization induced interfacial charges in semiconductor heterostructures using classical electrostatics applied to real-space band diagrams from first principles calculations and apply it to GaN/AlN heterostructures with ultrathin AlN layers (4-6 monolayers). We show that the calculated electric fields and interfacial charges are independent of the exchange-correlation functionals used (local-density approximation and hybrid functionals). We also find the calculated interfacial charge of (6.8 +/- 0.4) x 10^13 cm-2 to be in excellent agreement with experim…
A new mechanism (DeltaC1-DeltaC3 coupling) is accounted for the spin splitting of wurtzite GaN, which is originated from the intrinsic wurtzite effects (band folding and structure inversion asymmetry). The band-folding effect generates two conduction bands (DeltaC1 and DeltaC3), in which p-wave probability has tremendous change when kz approaches anti-crossing zone. The spin-splitting energy induced by the DeltaC1-DeltaC3 coupling and wurtzite structure inversion asymmetry is much larger than that evaluated by traditional Rashba or Dresselhaus effects. When we apply the coupling to GaN/AlN qua…
Spin-orbit coupling is studied using the quantum interference corrections to conductance in AlGaN/AlN/GaN two-dimensional electron systems where the carrier density is controlled by the persistent photoconductivity effect. All the samples studied exhibit a weak antilocalization feature with a spin-orbit field of around 1.8 mT. The zero-field electron spin splitting energies extracted from the weak antilocalization measurements are found to scale linearly with the Fermi wavevector with an effective linear spin-orbit coupling parameter 5.5x10^{-13} eV m. The spin-orbit times extracted from our m…
We have characterized the photodetection capabilities of single GaN nanowires incorporating 20 periods of AlN/GaN:Ge axial heterostructures enveloped in an AlN shell. Transmission electron microscopy confirms the absence of an additional GaN shell around the heterostructures. In the absence of a surface conduction channel, the incorporation of the heterostructure leads to a decrease of the dark current and an increase of the photosensitivity. A significant dispersion in the magnitude of dark currents for different single nanowires is attributed to the coalescence of nanowires with displaced na…
Several ten $μ$m GaN have been deposited on a silicon substrate using a two-step hydride vapor phase epitaxy (HVPE) process. The substrates have been covered by AlN layers and GaN nanostructures grown by plasma-assisted molecular-beam epitaxy. During the first low-temperature (low-T) HVPE step, stacking faults (SF) form, which show distinct luminescence lines and stripe-like features in cathodoluminescence images of the cross-section of the layers. These cathodoluminescence features allow for an insight into the growth process. During a second high-temperature (high-T) step, the SFs disappear,…
