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Materials with crystal structures containing tetrahedral motifs are preferable for optoelectronic applications because they often have direct band gaps and low electron effective masses. However, crystal structures of manganese chalcogenides typically contain octahedral motifs, such as in rock salt (RS) MnS and MnSe materials. Here, we experimentally show that MnS1−xSex alloys with tetrahedrally bonded wurtzite (WZ) structure can form between MnSe and MnS parent compounds with octahedral RS structures, at S-rich compositions (x < 0.4) and low synthesis temperatures (∼300 °C). The calculated mixing enthalpies of MnS1−xSex alloys in RS and WZ structures cannot explain this experimental observation, so we hypothesize that WZ stabilization may be related to smaller structure density and lower surface energy compared with RS. The resulting WZ MnS1−xSex alloys have 3.0–3.2 eV optical absorption onset and lower electrical conductivity (<0.0001 S/cm) than the parent RS compounds. These experimental measurement results are consistent with computationally predicted band gaps and effective masses.
Single-crystalline gallium arsenide (GaAs) grown by various techniques can exhibit hillock defects on the surface when sub-optimal growth conditions are employed. The defects act as nonradiative recombination centers and limit solar cell performance. In this paper, we applied near-field transport imaging to study hillock defects in a GaAs thin film. On the same defects, we also performed near-field cathodoluminescence, standard cathodoluminescence, electron-backscattered diffraction, transmission electron microscopy, and energy-dispersive X-ray spectrometry. We found that the luminescence intensity around the hillock area is two orders of magnitude lower than on the area without hillock defects in the millimeter region, and the excess carrier diffusion length is degraded by at least a factor of five with significant local variation. The optical and transport properties are affected over a significantly larger region than the observed topography and crystallographic and chemical compositions associated with the defect.
Here we report on the material chemistry following crystallization in the presence of water vapor of chlorinated formamidinium lead-triiodide (NH2CH = NH2PbI3−xClx) perovskite films. We found in-situ exposure to water vapor reduces, or possibly eliminates, the retention of chlorine (Cl) inside NH2CH = NH2PbI3−xClx crystals. There is a strong tendency toward Cl volatility, which indicates the sensitivity of these materials for their integration into solar cells. The requisite for additional efforts focused on the mitigation of water vapor is reported. Based on the in situ results, hot casting (<100 °C) in dry conditions demonstrates improved film coverage and Cl retention with efficiencies reaching 12.07%.
The highest efficiency CuIn1-xGaxSe2 (CIGS) based solar cells have been produced from films with x∼0.3 which gives a value of Eg around 1.1-1.2eV. Increasing the Ga content of the CIGS absorber provides an increase in Voc, allows tuning of the band gap that can enhance performance under actual operating conditions, and potentially makes it possible to use CIGS films in multi-junction devices. However, champion cells have not yet been produced for values of x significantly greater than 0.3. This work focuses on how increased Ga content in CIGS films affects the recombination behavior of grain boundaries. Cathodoluminescence spectral imaging (CLSI) measurements on fully processed devices allow us to compare device properties with recombination behavior and optical properties of grain boundaries in films with different Ga content. Our data suggests that grain boundaries in high efficiency films with x∼0.3 exhibit a significant red shift in the CL spectra whereas grain boundaries in films with higher Ga content typically show either a small shift or none at all. This shift indicates band bending near the boundaries which could enhance charge separation and subsequent collection of carriers generated near grain boundaries. This is investigated statistically to identify trends in different regions of the films.
CdTe is well known as an excellent photovoltaic material for high efficiency solar cell applications because it has a direct band-gap, low fabrication cost and high optical absorption coefficient. However, the nonradiative recombination and low average minority carrier lifetime caused by the defects in CdTe solar cells limit its efficiency. So far, grain boundaries (GB) have been considered to be the major origin of the nonradiative recombination. However, we show that CdTe grains contain many dislocations that could limit device efficiency. Scanning transmission electron microscopy (STEM) was used to determine the atomic structure of intrinsic and extrinsic stacking faults and their terminating partial dislocation cores. Z-contrast images are sensitive to atomic number and are able to distinguish Cd and Te atomic columns. Unpaired Cd and Te atomic columns were found to form the partial dislocation cores, suggesting the presence of dangling bonds. These defects are likely to be electrically active, and may be the origin of the low minority carrier lifetime.
In this work, we study CdTe thin films used in CdTe/CdS solar cells with a substrate configuration, which allows for better control in forming the junction, and the possibility for using flexible non-transparent substrates. We studied the properties of CdTe films grown at 450° and 550°C, with and without a CuxTe layer, and before and after CdCl2 treatment. We analyzed the structural and electro-optical properties using electron backscatter diffraction (EBSD), cathodoluminescence (CL) and X-ray diffraction (XRD), and investigated how the film structure, stress, and defect structure changes with the different growth conditions.
We report on the incorporation of molybdenum into tungsten oxide by co-sputtering and its effect on solar-powered photoelectrochemical (PEC) water splitting. Our study shows that Mo incorporation in the bulk of the film (WO3:Mo) results in poor PEC performance when compared with pure WO3, most likely due to defects that trap photo-generated charge carriers. However, when a WO3:Mo/WO3 bilayer electrode is used, a 20% increase of the photocurrent density at 1.6 V versus saturated calomel reference electrode is observed compared with pure WO3. Morphological and microstructural analysis of the WO3:Mo/WO3 bilayer structure reveals that it is formed by coherent growth of the WO3:Mo top layer on the WO3 bottom layer. This effect allows an optimization of the electronic surface structure of the electrode while maintaining good crystallographic properties in the bulk.
Scanning capacitance microscopy (SCM) often shows a change in contrast at grain boundaries [1-3]. The origins of this contrast and the efficacy of SCM as a tool to identify band bending at grain boundaries in pc-Si and mc-Si are discussed. Contrast at these grain boundaries could be influenced by different oxide growth rates or by defect states at the oxide interface. In order to determine the influence of such mechanisms on the SCM signal, such effects must be modeled; we show that a simple one-dimensional model agrees well with more detailed models of SCM signal strength and indicates, for example, that very small changes in oxide thickness measurably affect the SCM signal. In our experimental data, the uniformity and quality of the oxide layer are confirmed, and increased contrast consistent with depletion regions is still observed at higher order grain boundaries as identified by electron backscattering diffraction, including 9 and 27a. Scans of the SCM signal as a function of dc probe voltage allow such regions to be more quantitatively investigated.
ZnO thin films with significantly reduced band gaps were synthesized by doping N and codoping Al and N at 100 °C. All the films were synthesized by radiofrequency magnetron sputtering on F-doped tin-oxide-coated glass. We found that codoped ZnO:(Al,N) thin films exhibited significantly enhanced crystallinity compared with ZnO doped solely with N, ZnO:N, at the same growth conditions. Furthermore, annealed ZnO:(Al,N) thin films exhibited enhanced N incorporation over ZnO:N films. As a result, ZnO:(Al,N) films exhibited better photocurrents than ZnO:N films grown with pure N doping, suggesting that charge-compensated donor–acceptor codoping could be a potential method for band gap reduction of wide-band gap oxide materials to improve their photoelectrochemical performance.
We have investigated different methods for preparing CdTe/CdS cross sections for electrical measurements, including the following: cleaving; using GaAs substrates; and sandwiching the structure between the substrate and a glass slide, and polishing with diamond discs and alumina suspension. The latter method proved to be the most reliable, with a success rate of over 90%.
We investigated cross sections of CdTe/CdS samples with scanning Kelvin probe microscopy (SKPM) using two different methods: applying the alternate bias with a frequency equal to 18.5 kHz, or equal to the frequency of the second cantilever resonance peak. The results showed that using the second resonance frequency produced a smoother signal, allowing the calculation of the electric field inside the device using just the raw SKPM data.
We were able to measure the distribution of the electrical potential inside working devices. Then, by taking the first derivative of the potential, we calculated the electric field and determined the location of the p-n junction.
We report on recent advances in the development of a luminescence spectroscopy based on scanning tunneling microscopy (STM) and its application to fundamental aspects of Cu(In,Ga)Se2 (CIGS) thin films. Relevant to our discussion is the specifics of the surface electronics. The CIGS shows pronounced stoichiometric deviations at the surface and, consequently, distinct surface electronics that has been shown to be critical in achieving high efficiency. Cathodoluminescence (CL), a luminescence spectrum imaging mode in scanning electron microscopy (SEM), provides a direct correlation between the microstructure of the CIGS and its electronic properties. As such, cathodoluminescence can resolve the emission spectrum between grain boundaries and grain interiors or be used to investigate the influence of local orientation and stoichiometry on the electronic properties of the CIGS at the microscale. Cathodoluminescence is not a surface microscopy, however, and resolving the electronic structure of the CIGS surface remains elusive to all luminescence microscopies. With this motivation, we have developed a luminescence microscopy based on STM, in which tunneling electrons are responsible for the excitation of luminescence (scanning tunneling luminescence or STL). The hot-tunneling-electron excitation is confined to the surface and, consequently, the tunneling luminescence spectrum reveals the electronic states near the surface. The STM is integrated inside the SEM and, therefore, both CL and STL can be measured over the same location and compared. Using this setup, the transition from the grain interior to the surface can be investigated. We have improved the collection of our optics to a level in which tunneling luminescence spectrum imaging can be performed. Here we present a detailed account on our investigation of the surface electronics in CIGS deposited in the regime of selenium deficiency as defined by <Se>/(<Cu> + <In> + < Ga >) = 1.
Phosphorus and Boron doping effects on the microstructure of nanocrystallites in hydrogenated amorphous and nanocrystalline mixed-phase silicon films were investigated using Raman spectroscopy, secondary ion mass spectrometry, cross-sectional transmission electron microscopy, atomic force microscopy, and conductive atomic force microscopy. The characterizations revealed the following observations. First, the mixed-phase Si:H films can be heavily doped in ˜1021/cm3 by adding PH3 and BF3 in the precursor gases. Second, the intrinsic and doped films can be made in a similar crystalline volume fraction by adjusting hydrogen dilution ratio. The hydrogen dilution ratio is much higher for P-doped films than for the intrinsic film with the similar crystallinity. Third, the doping impacts the nanostructures in the films significantly. Nanograins aggregate to form cone-shaped clusters in the intrinsic and B-doped films but isolate and randomly distribute in amorphous tissues in the P-doped films. The cones in the intrinsic and B-doped films are also different. The cone-angle is smaller and the nanograin density is lower in the B-doped films than in the intrinsic films. These P- and B-doping effects on the nanocrystalline formation are interpreted in terms of diffusions of Si-related radicals during the film growth.
We have investigated the local electron transport in polycrystalline silicon (pc-Si) thin-films by atomic force microscopy (AFM)-based measurements of the electron-beam-induced current (EBIC). EVA solar cells are produced at UNSW by <i>EVAporation</i> of a-Si and subsequent <i>solid-phase crystallization</i>–a potentially cost-effective approach to the production of pc-Si photovoltaics. A fundamental understanding of the electron transport in these pc-Si thin films is of prime importance to address the factors limiting the efficiency of EVA solar cells. EBIC measurements performed in combination with an AFM integrated inside an electron microscope can resolve the electron transport across individual grain boundaries. AFM-EBIC reveals that most grain boundaries present a high energy barrier to the transport of electrons for both p-type and n-type EVA thin-films. Furthermore, for p-type EVA pc-Si, in contrast with n-type, charged grain boundaries are seen. Recombination at grain boundaries seems to be the dominant factor limiting the efficiency of these pc-Si solar cells.