Microscopy Visualization of Carrier Transport in CdSeTe/CdTe Solar Cells.

Solar cells are essentially minority carrier devices, and it is therefore of central importance to understand the pertinent carrier transport processes. Here, we advanced a transport imaging technique to directly visualize the charge motion and collection in the direction of relevant carrier transport and to understand the cell operation and degradation in state-of-the-art cadmium telluride solar cells. We revealed complex carrier transport profiles in the inhomogeneous polycrystalline thin-film solar cell, with the influence of electric junction, interface, recombination, and material composition. The pristine cell showed a unique dual peak in the carrier transport light intensity decay profile, and the dual peak feature disappeared on a degraded cell after light and heat stressing in the lab. The experiments, together with device modeling, suggested that selenium diffusion plays an important role in carrier transport. The work opens a new forum by which to understand the carrier transport and bridge the gap between atomic/nanometer-scale chemical/structural and submicrometer optoelectronic knowledge.

Consideration of the Intricacies Inherent in Molecular Beam Epitaxy of the NaCl/GaAs System.

The high cost of substrates for III-V growth can be cost limiting for technologies that require large semiconductor areas. Thus, being able to separate device layers and reuse the original substrate is highly desirable, but existing techniques to lift a film from a substrate have substantial drawbacks. This work discusses some of the complexities with the growth of a water-soluble, alkali halide salt thin film between a III-V substrate and overlayer. Much of the difficulty stems from the growth of GaAs on an actively decomposing NaCl surface at elevated temperatures. Interestingly, the presence of an in situ electron beam incident on the NaCl surface, prior to and during GaAs deposition, affects the crystallinity and morphology of the III-V overlayer. Here, we investigate a wide range of growth temperatures and the timing of the impinging flux of both elemental sources and high energy electrons at different points during the growth. We show that an assortment of morphologies (discrete islands, porous material, and fully dense layers with sharp interfaces) and crystallinity (amorphous, crystalline, and highly textured) occur depending on the specific growth conditions, driven largely by changes in GaAs nucleation which is greatly affected by the presence of the reflection high energy electron diffraction beam.

Scalable ultrafast epitaxy of large-grain and single-crystal II-VI semiconductors.

A general problem for semiconductor applications is that very slow deposition on expensive single-crystal substrates yields high crystalline quality with excellent electro-optical properties, but at prohibitive costs and throughput for many applications. In contrast, rapid deposition on inexpensive substrates or nanocrystalline films yields low costs, but comparatively inferior crystallinity, carrier transport, and recombination. Here, we present methods to deposit single-crystal material at rates 2-3 orders of magnitude faster than state-of-the-art epitaxy with low-cost methods without compromising crystalline or electro-optical quality. For example, single-crystal CdTe and CdZnTe films that would take several days to grow by molecular-beam epitaxy are deposited in 8 minutes by close-spaced sublimation, yet retain the same crystalline quality measured by X-ray diffraction rocking curves. The fast deposition is coupled with effective n- and p-type in-situ doping by In, P, and As. The epitaxy can be extended to nanocrystalline substrates. For example, we recrystallize thin CdTe films on glass to deposit large grains with low defect density. The results provide new research paths for photovoltaics, detectors, infrared imaging, flexible electronics, and other applications.

Carrier-Transport Study of Gallium Arsenide Hillock Defects.

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.

Overcoming Carrier Concentration Limits in Polycrystalline CdTe Thin Films with In Situ Doping.

Thin film materials for photovoltaics such as cadmium telluride (CdTe), copper-indium diselenide-based chalcopyrites (CIGS), and lead iodide-based perovskites offer the potential of lower solar module capital costs and improved performance to microcrystalline silicon. However, for decades understanding and controlling hole and electron concentration in these polycrystalline films has been extremely challenging and limiting. Ionic bonding between constituent atoms often leads to tenacious intrinsic compensating defect chemistries that are difficult to control. Device modeling indicates that increasing CdTe hole density while retaining carrier lifetimes of several nanoseconds can increase solar cell efficiency to 25%. This paper describes in-situ Sb, As, and P doping and post-growth annealing that increases hole density from historic 1014 limits to 1016-1017 cm-3 levels without compromising lifetime in thin polycrystalline CdTe films, which opens paths to advance solar performance and achieve costs below conventional electricity sources.

3D Lifetime Tomography Reveals How CdCl2 Improves Recombination Throughout CdTe Solar Cells.

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.

Angle-resolved XPS analysis and characterization of monolayer and multilayer silane films for DNA coupling to silica.

We measure silane density and Sulfo-EMCS cross-linker coupling efficiency on aminosilane films by high-resolution X-ray photoelectron spectroscopy (XPS) and atomic force microscopy (AFM) measurements. We then characterize DNA immobilization and hybridization on these films by (32)P-radiometry. We find that the silane film structure controls the efficiency of the subsequent steps toward DNA hybridization. A self-limited silane monolayer produced from 3-aminopropyldimethylethoxysilane (APDMES) provides a silane surface density of ~3 nm(-2). Thin (1 h deposition) and thick (19 h deposition) multilayer films are generated from 3-aminopropyltriethoxysilane (APTES), resulting in surfaces with increased roughness compared to the APDMES monolayer. Increased silane surface density is estimated for the 19 h APTES film, due to a ∼32% increase in surface area compared to the APDMES monolayer. High cross-linker coupling efficiencies are measured for all three silane films. DNA immobilization densities are similar for the APDMES monolayer and 1 h APTES. However, the DNA immobilization density is double for the 19 h APTES, suggesting that increased surface area allows for a higher probe attachment. The APDMES monolayer has the lowest DNA target density and hybridization efficiency. This is attributed to the steric hindrance as the random packing limit is approached for DNA double helices (dsDNA, diameter ≥ 2 nm) on a plane. The heterogeneity and roughness of the APTES films reduce this steric hindrance and allow for tighter packing of DNA double helices, resulting in higher hybridization densities and efficiencies. The low steric hindrance of the thin, one to two layer APTES film provides the highest hybridization efficiency of nearly 88%, with 0.21 dsDNA/nm(2). The XPS data also reveal water on the cross-linker-treated surface that is implicated in device aging.