We report nanometer-scale hole-density imaging in As-doped CdTe films by scanning capacitance microscopy (SCM). The hole-density profiling is validated by contrasting a CdTe cross-section sample made ...by molecular-beam epitaxy with systematically increased As doping in a staircase pattern over the range of 1015-1018/cm3 within a single film. In polycrystalline films, the carrier distribution is significantly nonuniform, with inhomogeneity ranging from several hundred nm to several um and hole density varying by one order of magnitude (low 10^16 to low 1017/cm3). This nonuniformity is distributed randomly, independent of the grain structure and grain boundaries (GBs). Kelvin probe force microscopy (KPFM) maps the surface potential and is correlated to cathodoluminescence (CL) and SCM by imaging over identical areas. Higher potential and lower CL intensity are found on GBs but not by SCM contrast; this indicates positive GB charging and recombination, but not GB-specific hole-density changes. The overall KPFM potential image is in rough agreement with the SCM carrier distribution and indicates band-edge potential fluctuations. Nonuniform carrier concentration, potential fluctuations, and defect recombination can all cause voltage and performance loss in As-doped CdTe solar technology.
For decades, Cu has been the primary dopant in CdTe photovoltaic absorbers. Typically, Cu acceptor concentrations in these devices are on the order of 1 1014 cm-3, which has made it notoriously ...difficult to directly correlate nanoscale Cu distributions to the local charge transport properties of these devices. To measure and correlate these properties, measurement techniques require high sensitivity to elemental concentration, large penetration depth, and operando compatibility. Techniques such as secondary-ion mass spectroscopy and X-ray energy dispersive spectroscopy are widely adopted to measure Cu concentrations, but they are limited by penetration depth, sensitivity, or spatial resolution. Additionally, they lack the operando capabilities required to correlate one-to-one Cu concentrations to electrical performance. In this work, correlative X-ray microscopy is used to investigate the spatial distribution of Cu and its impact on charge collection through the depth and breadth of CdTe photovoltaic devices. Plan-view, nanoscale X-ray fluorescence maps clearly demonstrate the spatial segregation of copper around regions thought to be CdTe grain boundaries. Complementary cross-section imaging unveils the transition of the maximum charge-collection efficiency from the ZnTe-CdTe interface to the CdS-CdTe interface as a function of Cu incorporation. The copper concentration through the depth of the CdTe layer is characterized by slow and fast diffusion components, and cross-section charge-transport modeling shows that the experimentally obtained charge collection can be explained by the modeled acceptor distribution through the depth of the CdTe layer.
Using two‐photon tomography, carrier lifetimes are mapped in polycrystalline CdTe photovoltaic devices. These 3D maps probe subsurface carrier dynamics that are inaccessible with traditional optical ...techniques. They reveal that CdCl2 treatment of CdTe solar cells suppresses nonradiative recombination and enhances carrier lifetimes throughout the film with substantial improvements particularly near subsurface grain boundaries and the critical buried p–n junction.
Efficient, safe and cost-effective synthesis of CdTe from elements is rather challenging in silica sealed ampoules due to the high vapor pressure of Cd. In this article, we report on the integrated ...synthesis and crystal growth of high-purity CdTe using the high pressure Bridgman (HPB) technique that is scalable to large volumes. The process lends itself for cost competitive industrial production of polycrystalline feedstock material for photovoltaics, sensors and electro-optic applications. Cadmium telluride (CdTe) crystals exceeding 1 kg in size were synthesized from elemental Cd and Te sources with purity comparable to state-of-the-art gamma ray detector crystals. In addition, synthesis of highly-doped CdTe feedstock for thin film photovoltaics applications demonstrating effective incorporation of group V (As, Sb) dopants was achieved at growth speeds of ~500 mm/hr. The technique may be applicable to produce other II-VI compounds with volatile components.
Grain structure influences both transport and recombination in CdTe solar cells. Larger grains generally are obtained with higher deposition temperatures, but commercially it is important to avoid ...softening soda-lime glass. Furthermore, depositing at lower temperatures can enable different substrates and reduced cost in the future. We examine how initial deposition temperatures and morphology influence grain size and lifetime after CdCl 2 recrystallization. Techniques are developed to estimate grain distribution quickly with low-cost optical microscopy, which compares well with electron backscatter diffraction data providing corroborative assessments of exposed CdTe grain structures. Average grain size increases as a function of CdCl 2 temperature. For lower temperature close-spaced sublimation CdTe depositions, there can be more stress and grain segregation during recrystallization. However, the resulting lifetimes and grain sizes are similar to high-temperature CdTe depositions. The grain structures and lifetimes are largely independent of the presence and/or interdiffusion of Se at the interface, before and after the CdCl 2 treatment.
Grain structure influences both transport and recombination in CdTe solar cells. Larger grains generally are obtained with higher deposition temperatures, but commercially it is important to avoid ...softening soda-lime glass. Furthermore, depositing at lower temperatures can enable different substrates and reduced cost in the future. We examine how initial deposition temperatures and morphology influence grain size and lifetime after CdCl2 recrystallization. Techniques are developed to estimate grain distribution quickly with low-cost optical microscopy, which compares well with electron backscatter diffraction data providing corroborative assessments of exposed CdTe grain structures. Average grain size increases as a function of CdCl2 temperature. For lower temperature close-spaced sublimation CdTe depositions, there can be more stress and grain segregation during recrystallization. However, the resulting lifetimes and grain sizes are similar to high-temperature CdTe depositions. The grain structures and lifetimes are largely independent of the presence and/or interdiffusion of Se at the interface, before and after the CdCl2 treatment.
Strain within grains and at grain boundaries (GBs) in polycrystalline thin-film absorber layers limits the overall performance because of higher defect concentrations and band fluctuations. However, ...the nanoscale strain distribution in operational devices is not easily accessible using standard methods. X-ray nanodiffraction offers the unique possibility to evaluate the strain or lattice spacing at nanoscale resolution. Furthermore, the combination of nanodiffraction with additional techniques in the framework of multimodal scanning X-ray microscopy enables the direct correlation of the strain with material and device parameters such as the elemental distribution or local performance. This approach is applied for the investigation of the strain distribution in CdTe grains in fully operational photovoltaic solar cells. It is found that the lattice spacing in the (111) direction remains fairly constant in the grain cores but systematically decreases at the GBs. The lower strain at GBs is accompanied by an increase of the total tilt. These observations are both compatible with the inhomogeneous incorporation of smaller atoms into the lattice, and local stress induced by neighboring grains.
Using two-photon tomography, carrier lifetimes are mapped in polycrystalline CdTe photovoltaic devices. These 3D maps probe subsurface carrier dynamics that are inaccessible with traditional optical ...techniques. They reveal that CdCl sub(2) treatment of CdTe solar cells suppresses nonradiative recombination and enhances carrier lifetimes throughout the film with substantial improvements particularly near subsurface grain boundaries and the critical buried p-n junction.
Spatially resolved 3D carrier-lifetime maps were measured using 2P tomography to uncover carrier dynamics at buried structures in CdTe thin-films photovoltaics. When thin-film CdTe solar cells are ...initially deposited, we observe increased nonradiative carrier recombination at GBs throughout the 3D volume of the film, which is most pronounced in the critical junction region where small nucleation grains form at the buried CdTe/CdS interface. The data on CdTe films treated by exposure to CdCl2 vapor reveal that a critical function of the treatment is to reduce surface, interface and GB recombination throughout the entirety of these polycrystalline films. The CdCl2 treatment may also compensate CdTe films, making it difficult to exceed a hole density of 1015m-3 and achieve higher current density and efficiency.
PDF
