The gallium gradient in Cu(In,Ga)Se2 (CIGS) layers, which forms during the two industrially relevant deposition routes, the sequential and co‐evaporation processes, plays a key role in the device performance of CIGS thin‐film modules. In this contribution, we present a comprehensive study on the formation, nature, and consequences of gallium gradients in CIGS solar cells. The formation of gallium gradients is analyzed in real time during a rapid selenization process by in situ X‐ray measurements. In addition, the gallium grading of a CIGS layer grown with an in‐line co‐evaporation process is analyzed by means of depth profiling with mass spectrometry. This gallium gradient of a real solar cell served as input data for device simulations. Depth‐dependent occurrence of lateral inhomogeneities on the µm scale in CIGS deposited by the co‐evaporation process was investigated by highly spatially resolved luminescence measurements on etched CIGS samples, which revealed a dependence of the optical bandgap, the quasi‐Fermi level splitting, transition levels, and the vertical gallium gradient. Transmission electron microscopy analyses of CIGS cross‐sections point to a difference in gallium content in the near surface region of neighboring grains. Migration barriers for a copper‐vacancy‐mediated indium and gallium diffusion in CuInSe2 and CuGaSe2 were calculated using density functional theory. The migration barrier for the InCu antisite in CuGaSe2 is significantly lower compared with the GaCu antisite in CuInSe2, which is in accordance with the experimentally observed Ga gradients in CIGS layers grown by co‐evaporation and selenization processes. Copyright © 2014 John Wiley & Sons, Ltd.
The authors present a detailed study of Al1−xInxN layers covering the whole composition range of 0.09<x<1. All layers were grown on GaN on Si(111) templates using metal-organic vapor phase epitaxy. For 0.13<x<0.32 samples grow fully strained and without phase separation. At higher In concentrations, the crystalline quality starts to deteriorate and a transition to three-dimensional growth is observed. A comparison of their experimental data with theoretically predicted phase diagrams reveals that biaxial strain increases the stability of the alloy.
GaN growth on Si is very attractive for low-cost optoelectronics and high-frequency, high-power electronics. It also opens a route towards an integration with Si electronics. Early attempts to grow GaN on Si suffered from large lattice and thermal mismatch and the strong chemical reactivity of Ga and Si at elevated temperatures. The latter problem can be easily solved using gallium-free seed layers as nitrided AlAs and AlN. The key problem for device structure growth on Si is the thermal mismatch leading to cracks for layer thicknesses above 1 µm. Meanwhile, several concepts for strain engineering exist as patterning, Al(Ga)N/GaN superlattices, and low-temperature (LT) AlN interlayers which enable the growth of device-relevant GaN thicknesses. The high dislocation density in the heteropitaxial films can be reduced by several methods which are based on lateral epitaxial overgrowth using ex-situ masking or patterning and by in-situ methods as masking with monolayer thick SiN. With the latter method in combination with strain engineering by LT-AlN interlayers dislocation densities around 109 cm -2 can be achieved for 2.5 µm thick device structures.
Al x Ga 1−x N layers with 0.05⩽x⩽0.25 were studied using spectrally and time resolved cathodoluminescence (CL). Continuous wave spectra were taken at temperatures ranging from 5 to 300 K. The near-band-edge peak emission energy exhibits an s-shaped temperature dependence characteristic of disordered systems. This effect is quantitatively explained within a model of potential fluctuations caused by alloy disorder. An s-shape temperature dependence has been observed in other alloy systems including InGaN, however, no systematic study exists for AlGaN. In this work, the s-shape temperature dependence is systematically analyzed as a function of aluminum content and quantitatively correlated with a model of alloy disorder. The shift in the luminescence peak position with respect to the usual temperature dependence of the band gap has been quantified by −σE2/kBT, where σE is the standard deviation of the potential fluctuations. Its dependence on aluminum concentration, x, was found to systematically increase from 7 meV at x=0.05 to 21 meV at x=0.25, following the theory for alloy disorder. The recombination and relaxation kinetics investigated using time-resolved CL are fully consistent with our potential fluctuation model. At 5 K, when the excitons are strongly localized, the exciton lifetime increases monotonically with aluminum content. At elevated temperatures, when the excitons are delocalized, the decay is significantly faster and preferentially nonradiative, regardless of the aluminum content.
Luminescence experiments provide a powerful and nondestructive approach to the ex situ investigation of semiconductor heterointerfaces which might be buried up to several μm below the surface in a given complex sample structure. Combined with the ability of taking images simply by scanning the exciting focused electron beam across the area under investigation, lateral fluctuations of electronic properties like the variation of the fundamental band gap Eg(x,y) can be directly visualized by scanning cathodoluminescence (CL). The novel experimental approach, cathodoluminescence wavelength imaging (CLWI), which involves recording of a complete CL spectrum at every scanning position (x,y), yields direct 3D images of the atomic-scale morphology of quantum wells (QWs) as sensed by the QW exciton: similar to the tip of a scanning tunneling microscope, the exciton samples the local fluctuations of QW thickness Lz and transforms this structural information Lz(x,y) into a spectral one, the lateral variation of band gap Eg(x,y) and thus the CL emission wavelength λ(x,y). Topological maps of QW interfaces can thus be recorded at various positions and at various magnifications. The interface roughness can be investigated statistically at lateral resolution starting with the diameter of the QW exciton up to the mm regime. The same experimental principle for recording λ(x,y) and Eg(x,y) maps is successfully applied for the analysis of patterned structures. In the nonlattice-matched system GaAs on Si, the lateral strain variation causes Eg(x,y) fluctuations and can thus be directly imaged by CLWI. Metalorganic chemical vapor deposition grown GaAs layers on micropatterned Si(001) substrates show strongly inhomogeneous doping with Si impurities. By means of CLWI the strong increase of this Si incorporation in the vicinity of free {111} surfaces is measured and Si concentration maps are recorded across the complete sample pattern.
Selective-area epitaxy is used to form three-dimensional (3D) GaN structures providing semipolar crystal facets. On full 2-in. sapphire wafers we demonstrate the realization of excellent semipolar material quality by introducing inverse GaN pyramids. When depositing InGaN quantum wells on such a surface, the specific geometry influences thickness and composition of the films and can be nicely modeled by gas phase diffusion processes. Various investigation methods are used to confirm the drastically reduced piezoelectric polarization on the semipolar planes. Complete electrically driven light-emitting diode test structures emitting in the blue and blue/green spectral regions show reasonable output powers in the milliwatt regime. Finally, first results of the integration of the 3D structures into a conventional laser design are presented
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