The effects of the CdCl 2 passivation treatment on thin-film CdTe photovoltaic films and devices have been extensively studied. Recently, with an addition of CdSeTe layer at the front of the absorber layer, device conversion efficiencies in excess of 19% have been demonstrated. The effects of the CdCl 2 passivation treatment for devices using CdSeTe has not been studied previously. This is the first reported study of the effect of the treatment on the microstructure of the CdSeTe /CdTe absorber. The device efficiency is <1% for the as-deposited device but this is dramatically increased by the CdCl 2 treatment. Using Scanning Transmission Electron Microscopy (STEM), we show that the CdCl 2 passivation of CdSeTe/CdTe films results in the removal of high densities of stacking faults and increase and reorientation of grains. The CdCl 2 treatment leads to grading of the absorber CdSeTe/CdTe films by diffusion of Se between the CdSeTe and CdTe regions. Chlorine decorates the CdSeTe and CdTe grain boundaries leading to their passivation. Direct evidence for these effects is presented using STEM and Energy Dispersive X-ray Analysis (EDX) on device cross-sections prepared using focused ion beam etching. The grading of the Se in the device is quantified using EDX line scans. The comparison of CdSeTe/CdTe device microstructure and composition before and after the CdCl 2 treatment provides insights into the important effects of the process and points the way to further improvements that can be made.

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Thin‐film photovoltaic device efficiencies are limited by carrier recombination, thus understanding recombination mechanisms is critical for performance improvements. Bulk minority carrier lifetime (τ bulk) is a critical parameter for solar cells but is difficult to determine in P–N junction devices, especially for high doping. As doping ≥1016 cm−3 is required for efficient drift‐charge‐carrier‐collection devices, a method for τ bulk determination in doped P–N junction devices is necessary. This work utilizes time‐resolved photoluminescence (TRPL) simulations to quantify bulk and interface recombination properties in highly doped, graded absorber CdSeTe structures. The two methods developed here for τ bulk determination include utilization of an instantaneous lifetime representation to guide TRPL fitting and direct comparison between measured and simulated decays. Simulations verified that both methods are valid for state‐of‐the‐art device architectures which include graded bandgap absorbers, graded doping, and graded lifetimes. Shifts in the dominant recombination mechanism are identified for sufficiently long τ bulk, where front and back interface quality plays a more prominent role. Evaluation of surface recombination velocities and conduction band offset illustrate electro‐optical advantages of a positive conduction band offset and highlight the necessity of improved interfaces as bulk quality in photovoltaic devices improves.

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