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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.

Cadmium telluride (CdTe) solar cell technology is a promising candidate to help boost green energy production. However, impurities and structural defects are major barriers to improving the solar power conversion efficiency. Grain boundaries often act as aggregation sites for impurities, resulting in strain localization in areas of high diffusion. In this study, we demonstrate the use of scanning 3D X-ray diffraction microscopy to non-destructively make 3D maps of the grains – their phase, orientation, and local strain – within a CdTe solar cell absorber layer with a resolution of 100 nm. We quantify twin boundaries and suggest how they affect grain size and orientation distribution. Local strain analysis reveals that strain is primarily associated with high misorientation grain boundaries, whereas twin boundaries do not have high strain values. We also observe that high-strain grain boundaries form a continuous pathway connected to the CdS layer. Hence, this high-strain region is believed to be associated with the diffusion of sulfur from the CdS layer along grain boundaries. This hypothesis is supported by SEM-EDS and X-ray fluorescence experiments. The method and analysis demonstrated in this work can be applied to different polycrystalline materials where the characterization of grain boundary properties is essential to understand the microstructural phenomena. [ABSTRACT FROM AUTHOR]

We determine the grain-boundary (GB) recombination velocity, S G B , and grain-interior (GI) lifetime, τ G I , parameters in superstrate CdS/CdTe thin-film solar cell technology by combining cathodoluminescence (CL) spectrum imaging and time-resolved photoluminescence (TRPL) measurements. We consider critical device formation stages, including after CdTe deposition, CdCl2 treatment, and Cu diffusion. CL image analysis methods extract GB and GI intensities and grain size for hundreds of grains per sample. Concurrently, a three-dimensional CL model is developed to simulate the GI intensity as a function of τ G I , S G B , grain size, and the surface recombination velocity, S surf . TRPL measurements provide an estimate of S surf for the CL model. A fit of GI intensity vs. grain size data with the CL model gives a self-consistent and representative set of S G B and τ G I values for the samples: S G B (τ G I) = 2.6 × 106 cm/s (68–250 ps), S G B (τ G I) = 4.1 × 105 cm/s (1.5–3.3 ns), and S G B (τ G I) = 5.5 × 105 cm/s (1.0–3.8 ns) for as-deposited, CdCl2-treated, and CdCl2- and Cu-treated samples, respectively. Thus, we find that the CdCl2 treatment both helps to passivate GBs and significantly increase the GI lifetime. Subsequent Cu diffusion increases GB recombination slightly and has nuanced effects on the GI lifetime. Finally, as a partial check on the S G B and τ G I values, they are input to a Sentaurus device model, and the simulated performance is compared to the measured performance. The methodology developed here can be applied broadly to CdTe and CdSeTe thin-film technology and to other thin-film solar cell materials including Cu(In1-xGax)Se2, Cu2ZnSnS4, and perovskites. [ABSTRACT FROM AUTHOR]

We analyze charge-carrier dynamics using time-resolved spectroscopy and varying epitaxial CdTe thickness in undoped heteroepitaxial CdTe/ZnTe/Si. By employing one-photon and nonlinear two-photon excitation, we assess surface, interface, and bulk recombination. Two-photon excitation with a focused laser beam enables characterization of recombination velocity at the buried epilayer/substrate interface, 17.5 µm from the sample surface. Measurements with a focused two-photon excitation beam also indicate a fast diffusion component, from which we estimate an electron mobility of 650 cm² (Vs)-1 and diffusion coefficient D of 17 cm² s-1. We find limiting recombination at the epitaxial film surface (surface recombination velocity Ssurface = (2.8 ± 0.3) x 105 cm s-1) and at the heteroepitaxial interface (interface recombination velocity Sinterface = (4.8 ± 0.5) x 105 cm s-1). The results demonstrate that reducing surface and interface recombination velocity is critical for photovoltaic solar cells and electronic devices that employ epitaxial CdTe. [ABSTRACT FROM AUTHOR]

Manipulating CdSeTe bandgrading to enhance photocurrent and carrier lifetime is an essential part of high-performance CdTe photovoltaics (PVs). In this work, we examine Se diffusion kinetics in single-crystal and polycrystalline CdTe during deposition, thermal annealing, and CdCl2 treatments. Se distributions are determined by dynamic secondary-ion-mass spectroscopy and Auger electron spectroscopy depth profiling and coupled with electron backscatter diffraction images of the crystalline structure. Effective bulk and grain boundary diffusion coefficients are determined by analytical models and discussed in the context of processing and film morphology. Se is found to diffuse in CdTe at much higher rates during CdCl2 treatments than with thermal processing alone. GB diffusion also occurs at a significantly faster rate than bulk diffusion. As a result of these two effects, the near interface bulk and GB Se diffusion during CdCl2 treatments dominates the bandgrading profiles in CdTe PVs. [ABSTRACT FROM AUTHOR]