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Herein, the lasing threshold and gain characteristics of ultraviolet‐C optically pumped edge‐emitting lasers with thick single‐quantum‐well (SQW) active regions are investigated by the variable‐stripe length method. Positive net modal gain is observed in lasers with AlGaN‐based SQWs with thicknesses up to 12 nm. The lasers show a reduction of the threshold power density with increasing SQW thickness, with the lowest threshold of 1.3 MW cm−2 achieved for a 9 nm SQW laser. The high gain and low threshold in lasers with thick quantum wells are attributed to lasing from excited states, where the polarization fields are screened by the carriers in the fundamental state and the barriers, thus recovering larger electron and hole wavefunctions overlap. These findings are supported by k · p simulations, and for a 9 nm SQW, the calculation predicts a contribution of the fundamental transition to the gain of 75% for non‐resonant optical excitation and below 1% for resonant optical or electrical excitation. [ABSTRACT FROM AUTHOR]

Quantum well nanolasers usually show single‐mode lasing, as gain saturation suppresses emissions in other modes. In contrast, for whispering gallery mode microdisk lasers with GaN quantum wells as active material, above threshold multimode laser emission is observed. This intriguing emission feature is manifested in the fact that several modes simultaneously show the characteristic kink in the input–output curve at the onset of lasing. A quantum theory for nanolasers is used to support the experimental finding and to analyze this behavior in the presence of gain saturation. Coupling effects between neighboring modes are identified as the origin of multimode lasing, which initiate photon exchange between modes via population pulsations similar to classical wave‐mixing effects. A reduction of this type of mode coupling with increasing mode spacing is demonstrated. The results can pave the way for multimode application of nanolasers in integrated photonic circuits. [ABSTRACT FROM AUTHOR]

The monoclinic beta-phase of gallium oxide possesses an ultra-wide bandgap that surpasses other wide bandgap materials such as SiC and GaN, making it a promising candidate for power electronic device technologies. We investigate the first fundamental optical transitions in this material, which exhibit a strong directional dependence. To determine the energies and orientations of these transitions, temperature-dependent and angular resolved photoluminescence excitation spectroscopy is applied. We observe a distinct excitation channel located energetically between those of the first two optical transitions Γ 1 − 1 and Γ 1 − 2 . While previous absorption edge and reflectance spectroscopy studies have assigned a transition in this spectral range to either the Γ 1 − 1 or the Γ 1 − 2 transition, our findings demonstrate no pronounced polarization dependence of this excitation channel within the (010) plane, an observation not reflected in calculations of the band-to-band transitions in β - Ga 2 O 3 . [ABSTRACT FROM AUTHOR]

We report on the epitaxial growth, theoretical modeling, and structural as well as optical investigation of multi-layer, site-controlled quantum dots fabricated using the buried stressor method. This deterministic growth technique utilizes the strain from a partially oxidized AlAs layer to induce site-selective nucleation of InGaAs quantum dots. By implementing strain-induced spectral nano-engineering, we achieve spectral control of emission and a local increase in the emitter density. Furthermore, we achieve a threefold increase in the optical intensity and reduce the inhomogeneous broadening of the ensemble emission by 20% via stacking three layers of site-controlled emitters, which is valuable for using the SCQDs as a gain medium in microlaser applications. Our optimization of site-controlled growth of quantum dots enables the development of high-β microlasers with increased confinement factor. [ABSTRACT FROM AUTHOR]

Rutile GeO2 has been predicted to be an ultra-wide bandgap semiconductor suitable for future power electronic devices, while quartz-like GeO2 shows piezoelectric properties. To explore these crystalline phases for application and fundamental materials investigations, molecular beam epitaxy (MBE) is a well-suited thin film growth technique. In this study, we investigate the reaction kinetics of GeO2 during plasma-assisted MBE using elemental Ge and plasma-activated oxygen fluxes. The growth rate as a function of oxygen flux is measured in situ by laser reflectometry at different growth temperatures. A flux of the suboxide GeO desorbing off the growth surface is identified and quantified in situ by the line-of-sight quadrupole mass spectrometry. Our measurements reveal that the suboxide formation and desorption limits the growth rate under Ge-rich or high temperature growth conditions and leads to etching of the grown GeO2 layer under a Ge flux in the absence of oxygen. The quantitative results fit the sub-compound mediated reaction model, indicating the intermediate formation of the suboxide at the growth front. This model is further utilized to delineate the GeO2-growth window in terms of oxygen-flux and substrate temperature. Our study can serve as a guidance for the thin film synthesis of GeO2 and defect-free mesa etching in future GeO2-device processing. [ABSTRACT FROM AUTHOR]

Unintentionally doped (001)‐oriented orthorhombic κ‐Ga2O3 epitaxial films on c‐plane sapphire substrates are characterized by the presence of ≈ 10 nm wide columnar rotational domains that can severely inhibit in‐plane electronic conduction. Comparing the in‐ and out‐of‐plane resistance on well‐defined sample geometries, it is experimentally proved that the in‐plane resistivity is at least ten times higher than the out‐of‐plane one. The introduction of silane during metal‐organic vapor phase epitaxial growth not only allows for n‐type Si extrinsic doping, but also results in the increase of more than one order of magnitude in the domain size (up to ≈ 300 nm) and mobility (highest µ ≈ 10 cm2V−1s−1, with corresponding lowest ρ ≈ 0.2 Ωcm). To qualitatively compare the mean domain dimension in κ‐Ga2O3 epitaxial films, non‐destructive experimental procedures are provided based on X‐ray diffraction and Raman spectroscopy. The results of this study pave the way to significantly improved in‐plane conduction in κ‐Ga2O3 and its possible breakthrough in new generation electronics. The set of cross‐linked experimental techniques and corresponding interpretation here proposed can apply to a wide range of material systems that suffer/benefit from domain‐related functional properties. [ABSTRACT FROM AUTHOR]

We developed a novel contactless frequency-domain thermoreflectance approach to study thermal transport, which is particularly convenient when thermally anisotropic materials are considered. The method is based on a line-shaped heater geometry, produced with a holographic diffractive optical element, instead of using a spot heater as in conventional thermoreflectance. The heater geometry is similar to the one used in the 3-omega method, however, keeping all the technical advantages offered by non-contact methodologies. The present method is especially suitable to determine all the elements of the thermal conductivity tensor, which is experimentally achieved by simply rotating the sample with respect to the line-shaped optical heater. We provide the mathematical solution of the heat equation for the cases of anisotropic substrates, thin films, and multilayer systems. This methodology allows an accurate determination of the thermal conductivity and does not require complex modeling or intensive computational efforts to process the experimental data, i.e., the thermal conductivity is obtained through a simple linear fit ("slope method"), in a similar fashion to the 3-omega method. We demonstrate the potential of this approach by studying isotropic and anisotropic materials in a wide range of thermal conductivities. In particular, we have studied the following inorganic and organic systems: (i) glass, Si, and Ge substrates (isotropic), (ii) β-Ga2O3 and a Kapton substrate (anisotropic), and (iii) a 285 nm thick SiO2 thin film deposited on a Si substrate. The accuracy in the determination of the thermal conductivity is estimated as ≈5%, whereas the temperature uncertainty is ΔT ≈ 3 mK. [ABSTRACT FROM AUTHOR]

Gallium oxide (Ga2O3) is an ultra-wide bandgap material, which has recently attracted widespread attention for holding promising applications in power electronics and solar blind UV photodetectors, outclassing GaN or SiC in terms of a larger bandgap and higher breakdown voltages. The orthorhombic κ phase (also referred to as ε) has sparked particular interest for offering higher symmetry than β, while featuring ferroelectric behavior paired with a large predicted spontaneous polarization, paving the way to fabricating high-quality two-dimensional electron gases for application in heterostructure field effect transistors. The presently available κ phase samples are characterized by a domain structure, in which orthorhombic domains are rotated 120° against each other within the c-plane forming a pseudo-hexagonal structure, which has previously often been ascribed to ε-Ga2O3 and incorrectly been viewed as this polymorph's true crystal structure. A detailed investigation into the phonon modes of orthorhombic κ-Ga2O3 provides insights into fundamental material properties such as crystal structure and orientation as well as the vibrational symmetries of Raman active modes. We investigate the Raman active phonon modes of an MBE-grown orthorhombic κ-Ga2O3 thin film featuring the domain structure deposited on (0001)-Al2O3 by experiment and theory: Polarized micro-Raman spectroscopy measurements in conjunction with density functional perturbation theory (DFPT) calculations enable the identification of both the frequencies and vibrational symmetries of the Raman active phonons. Presenting comprehensive Raman spectra of the orthorhombic κ phase, the experimental frequencies of more than 90 Raman modes are determined and correlated with the 117 modes predicted by the calculations. Angular-resolved Raman measurements are utilized to provide an experimental verification of phonon mode symmetries. We present an analytical tool to deal with the domain structure and its effect on the obtained Raman spectra. [ABSTRACT FROM AUTHOR]

Formamidinium lead iodide (FAPbI3) can be used in its cubic, black form as a light absorber material in single-junction solar cells. It has a band-gap (1.5 eV) close to the maximum of the Shockley–Queisser limit, and reveals a high absorption coefficient. Its high thermal stability up to 320 °C has also a downside, which is the instability of the photo-active form at room temperature (RT). Thus, the black α-phase transforms at RT with time into a yellow non-photo-active δ-phase. The black phase can be recovered by annealing of the yellow state. In this work, a polymorphism of the α-phase at room temperature was found: as-synthesized (αi), degraded (αδ) and thermally recovered (αrec). They differ in the Raman spectra and PL signal, but not in the XRD patterns. Using temperature-dependent Raman spectroscopy, we identified a structural change in the αi-polymorph at ca. 110 °C. Above 110 °C, the FAPbI3 structure has undoubtedly cubic Pm3¯m symmetry (high-temperature phase: αHT). Below that temperature, the αi-phase was suggested to have a distorted perovskite structure with Im3¯ symmetry. Thermally recovered FAPbI3 (αrec) also demonstrated the structural transition to αHT at the same temperature (ca. 110 °C) during its heating. The understanding of hybrid perovskites may bring additional assets in the development of new and stable structures. [ABSTRACT FROM AUTHOR]

Holding promising applications in power electronics, the ultra-wide band gap material gallium oxide has emerged as a vital alternative to materials like GaN and SiC. The detailed study of phonon modes in β-Ga2O3 provides insights into fundamental material properties such as crystal structure and orientation and can contribute to the identification of dopants and point defects. We investigate the Raman active phonon modes of β-Ga2O3 in two different oxygen isotope compositions (16O,18O) by experiment and theory: By carrying out polarized micro-Raman spectroscopy measurements on the (010) and (2¯01) planes, we determine the frequencies of all 15 Raman active phonons for both isotopologues. The measured frequencies are compared with the results of density functional perturbation theory (DFPT) calculations. In both cases, we observe a shift of Raman frequencies towards lower energies upon substitution of 16O with 18O. By quantifying the relative frequency shifts of the individual Raman modes, we identify the atomistic origin of all modes (Ga–Ga, Ga–O or O–O) and present the first experimental confirmation of the theoretically calculated energy contributions of O lattice sites to Raman modes. The DFPT results enable the identification of Raman modes that are dominated by the different, inequivalent O- or Ga-atoms of the unit cell. We find that oxygen substitution on the OIII site leads to an elevated relative mode frequency shift compared to OI and OII sites. This study presents a blueprint for the future identification of different point defects in Ga2O3 by Raman spectroscopy. [ABSTRACT FROM AUTHOR]

Lead halide perovskite semiconductors providing record efficiencies of solar cells have usually mixed compositions doped in A- and X-sites to enhance the phase stability. The cubic form of formamidinium (FA) lead iodide reveals excellent opto-electronic properties but transforms at room temperature (RT) into a hexagonal structure which does not effectively absorb visible light. This metastable form and the mechanism of its stabilization by Cs+ and Br− incorporation are poorly characterized and insufficiently understood. We report here the vibrational properties of cubic FAPbI3 investigated by DFT calculations on phonon frequencies and intensities, and micro-Raman spectroscopy. The effects of Cs+ and Br− partial substitution are discussed. We support our results with the study of FAPbBr3 which expands the identification of vibrational modes to the previously unpublished low frequency region (<500 cm−1). Our results show that the incorporation of Cs+ and Br− leads to the coupling of the displacement of the A-site components and weakens the bonds between FA+ and the PbX6 octahedra. We suggest that the enhancement of α-FAPbI3 stability can be a product of the release of tensile stresses in the Pb–X bond, which is reflected in a red-shift of the low frequency region of the Raman spectrum (<200 cm−1). [ABSTRACT FROM AUTHOR]

We report on fundamental structural and optical properties of lateral polarity junctions in GaN. GaN with Ga- to N-polar junctions was grown on sapphire using an AlN buffer layer. Results from scanning electron microscopy and Raman spectroscopy measurements indicate a superior quality of the Ga-polar GaN. An extremely strong luminescence signal is observed at the inversion domain boundary (IDB). Temperature dependent micro photoluminescence measurements are used to reveal the recombination processes underlying this strong emission. At 5 K the emission mainly arises from a stripe along the inversion domain boundary with a thickness of 4-5 μm. An increase of the temperature initially leads to a narrowing to below 2 μm emission area width followed by a broadening at temperatures above 70 K. The relatively broad emission area at low temperatures is explained by a diagonal IDB. It is shown that all further changes in the emission area width are related to thermalization effects of carriers and defects attracted to the IDB. The results are successfully used to confirm a theoretical model for GaN based lateral polarity junctions. Due to the strong and pronounced emission of IDBs even at elevated temperatures, it is demonstrated that lateral polarity junctions exhibit a strong potential for future high efficiency devices. [ABSTRACT FROM AUTHOR]

The polar nature of the wurtzite crystalline structure of GaN and ZnO results in the existence of a spontaneous electric polarization within these materials and their associated alloys (Ga,Al,In)N and (Zn,Mg,Cd)O. The polarity has also important consequences on the stability of the different crystallographic surfaces, and this becomes especially important when considering epitaxial growth. Furthermore, the internal polarization fields may adversely affect the properties of optoelectronic devices but is also used as a potential advantage for advanced electronic devices. In this article, polarity-related issues in GaN and ZnO are reviewed, going from theoretical considerations to electronic and optoelectronic devices, through thin film, and nanostructure growth. The necessary theoretical background is first introduced and the stability of the cation and anion polarity surfaces is discussed. For assessing the polarity, one has to make use of specific characterization methods, which are described in detail. Subsequently, the nucleation and growth mechanisms of thin films and nanostructures, including nanowires, are presented, reviewing the specific growth conditions that allow controlling the polarity of such objects. Eventually, the demonstrated and/or expected effects of polarity on the properties and performances of optoelectronic and electronic devices are reported. The present review is intended to yield an indepth view of some of the hot topics related to polarity in GaN and ZnO, a fast growing subject over the last decade. [ABSTRACT FROM AUTHOR]

We obtain temperature-dependent recombination coefficients by measuring the quantum efficiency and differential carrier lifetimes in the state-of-the-art InGaN light-emitting diodes. This allows us to gain insight into the physical processes limiting the quantum efficiency of such devices. In the green spectral range, the efficiency deteriorates, which we assign to a combination of diminishing electron-hole wave function overlap and enhanced Auger processes, while a significant reduction in material quality with increased In content can be precluded. Here, we analyze and quantify the entire balance of all loss mechanisms and highlight the particular role of hole localization. [ABSTRACT FROM AUTHOR]

The design and fabrication of phononic crystals (PnCs) hold the key to control the propagation of heat and sound at the nanoscale. However, there is a lack of experimental studies addressing the impact of order/disorder on the phononic properties of PnCs. Here, we present a comparative investigation of the influence of disorder on the hypersonic and thermal properties of two-dimensional PnCs. PnCs of ordered and disordered lattices are fabricated of circular holes with equal filling fractions in free-standing Si membranes. Ultrafast pump and probe spectroscopy (asynchronous optical sampling) and Raman thermometry based on a novel two-laser approach are used to study the phononic properties in the gigahertz (GHz) and terahertz (THz) regime, respectively. Finite element method simulations of the phonon dispersion relation and three-dimensional displacement fields furthermore enable the unique identification of the different hypersonic vibrations. The increase of surface roughness and the introduction of short-range disorder are shown to modify the phonon dispersion and phonon coherence in the hypersonic (GHz) range without affecting the room-temperature thermal conductivity. On the basis of these findings, we suggest a criteria for predicting phonon coherence as a function of roughness and disorder. [ABSTRACT FROM AUTHOR]

Atmospheric contamination with organic compounds is undesired in industry and in society because of odor nuisance or potential toxicity. Resistive gas sensors made of semiconducting metal oxides are effective in the detection of gases even at low concentration. Major drawbacks are low selectivity and missing sensitivity toward a targeted compound. Acetaldehyde is selected due to its high relevance in chemical industry and its toxic character. Considering the similarity between gas-sensing and heterogeneous catalysis (surface reactions, activity, selectivity), it is tempting to transfer concepts. A question of importance is how doping and the resulting change in electronic properties of a metal-oxide support with semiconducting properties alters reactivity of the surfaces and the functionality in gas-sensing and in heterogeneous catalysis. A gas-phase synthesis method is employed for aerogel-like zinc oxide materials with a defined content of aluminum (n-doping), which were then used for the assembly of gas sensors. It is shown that only Al-doped ZnO represents an effective sensor material that is sensitive down to very low concentrations (<350 ppb). The advance in properties relates to a catalytic effect for the doped semiconductor nanomaterial. [ABSTRACT FROM AUTHOR]

The benefits and promise of nanoscale dimensions for the properties of (ceramic) semiconductors are widely known. 1-D nanostructures in particular have proven to be of extraordinary relevance due to their applicability in future electronic and optoelectronic devices. Key to successful technological implementation of semiconductor nanostructures is the control of their electronic properties via doping. Despite its tremendous importance, precise chemical doping of defined nano-objects has been addressed rarely so far. Frequent problems are the creation of secondary defects and related undesired property changes by incorporation of hetero-elements, and the difficulty in ensuring a uniform and precise positioning of the dopant in the nanocrystal lattice. Here, we present the synthesis of Li-doped zinc oxide nanorods, which possess excellent (single-crystal) quality. The method is based on a novel non-classical crystallization mechanism, comprising an unusually oriented disassembly step. Afterwards, the nanorods are incorporated into mesoporous layers using colloidal self-assembly. Proof-of-principle gas sensing measurements with these novel materials demonstrate the beneficial role of Li-doping, indicating not only better conductivity but also the occurrence of catalytic effects. [ABSTRACT FROM AUTHOR]

The uniaxial stress dependence of the band structure and the exciton-polariton transitions in wurtzite ZnO is thoroughly studied using modern first-principles calculations based on the HSE + G0W0 approach, kp modeling using the deformation potential framework, and polarized photoluminescence measurements. The ordering of the valence bands [A(Γ7), B(Γ9), C(Γ7)] is found to be robust even for high uniaxial and biaxial strains. Theoretical results for the uniaxial pressure coefficients and splitting rates of the A, B, and C valence bands and their optical transitions are obtained including the effects of the spin-orbit interaction. The excitonic deformation potentials are derived and the stress rates for hydrostatic pressure are determined based on the results for uniaxial and biaxial stress. In addition, the theory for the stress dependence of the exchange interaction and longitudinal-transversal splitting of the exciton polaritons is developed using the basic exciton functions of the quasicubic approximation and taking the interaction between all exciton states into account. It is shown that the consideration of these effects is crucial for an accurate description of the stress dependence of the optical spectra in ZnO. The theoretical results are compared to polarized photoluminescence measurements of different ZnO substrates as function of uniaxial pressure and experimental values reported in the literature demonstrating an excellent agreement with the computed pressure coefficients. [ABSTRACT FROM AUTHOR]

The effect of a trimethylgallium (TMGa) preflow on the structural and optical properties of MOCVD grown AlN layers on sapphire substrates is investigated. Secondary ion mass spectroscopy measurements were performed to investigate the incorporation of Ga in the layers. It is shown that for AlN layers grown with a TMGa preflow Ga atoms incorporate mainly near the substrate/epilayer interface. Photoluminescence spectra exhibit a free exciton and a donor bound exciton. By analyzing the full width at half maximum of the free exciton and the defect luminescence an increased optical quality for the sample grown with TMGa preflow is demonstrated. Additionally, Raman spectroscopy reveals a higher crystal quality for this sample. Comparing the results from Raman spectroscopy and luminescence measurements a shift rate of 60 meV GPa−1 is determined for the free A-exciton. Finally, cross-sectional Raman spectroscopy is used to compare the strain at the AlN/sapphire interface for a sample grown with and without TMGa preflow. [ABSTRACT FROM AUTHOR]

Compensation effects in metal organic chemical vapour deposition grown GaN doped with magnesium are investigated with Raman spectroscopy and photoluminescence measurements. Examining the strain sensitive E2(high) mode, an increasing compressive strain is revealed for samples with Mg-concentrations lower than 7 × 1018 cm-3. For higher Mg-concentrations, this strain is monotonically reduced. This relaxation is accompanied by a sudden decrease in crystal quality. Luminescence measurements reveal a well defined near band edge luminescence with free, donor bound, and acceptor bound excitons as well as a characteristic donor acceptor pair (DAP) luminescence. Following recent results, three acceptor bound excitons and donor acceptor pairs are identified. Along with the change of the strain, a strong modification in the luminescence of the dominating acceptor bound exciton and DAP luminescence is observed. The results from Raman spectroscopy and luminescence measurements are interpreted as fingerprints of compensation effects in GaN:Mg leading to the conclusion that compensation due to defect incorporation triggered by Mg-doping already affects the crystal properties at doping levels of around 7 × 1018 cm-3. Thereby, the generation of nitrogen vacancies is introduced as the driving force for the change of the strain state and the near band edge luminescence. [ABSTRACT FROM AUTHOR]