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The thin-film vapor-liquid-solid (TF-VLS) growth technique presents a promising route for high quality, scalable, and cost-effective InP thin films for optoelectronic devices. Toward this goal, careful optimization of material properties and device performance is of utmost interest. Here, we show that exposure of polycrystalline Zn-doped TF-VLS InP to a hydrogen plasma (in the following referred to as hydrogenation) results in improved optoelectronic quality as well as lateral optoelectronic uniformity. A combination of low temperature photoluminescence and transient photocurrent spectroscopy was used to analyze the energy position and relative density of defect states before and after hydrogenation. Notably, hydrogenation reduces the relative intragap defect density by 1 order of magnitude. As a metric to monitor lateral optoelectronic uniformity of polycrystalline TF-VLS InP, photoluminescence and electron beam induced current mapping reveal homogenization of the grain versus grain boundary upon hydrogenation. At the device level, we measured more than 260 TF-VLS InP solar cells before and after hydrogenation to verify the improved optoelectronic properties. Hydrogenation increased the average open-circuit voltage (VOC) of individual TF-VLS InP solar cells by up to 130 mV and reduced the variance in VOC for the analyzed devices.

Inverted metamorphic Ga0.3In0.7As photovoltaic converters with sub‐0.60 eV bandgaps grown on InP and GaAs are presented. Threading dislocation densities are 1.3 ± 0.6 × 106 and 8.9 ± 1.7 × 106 cm−2 on InP and GaAs, respectively. The devices generate open‐circuit voltages of 0.386 and 0.383 V, respectively, under irradiance producing a short‐circuit current density of ≈10 A cm−2, yielding bandgap‐voltage offsets of 0.20 and 0.21 V. Power and broadband reflectance measurements are used to estimate thermophotovoltaic (TPV) efficiency. The InP‐based cell is estimated to yield 1.09 W cm−2 at 1100 °C versus 0.92 W cm−2 for the GaAs‐based cell, with efficiencies of 16.8 versus 9.2%. The efficiencies of both devices are limited by sub‐bandgap absorption, with power weighted sub‐bandgap reflectances of 81% and 58%, respectively, the majority of which is assumed to occur in the graded buffers. The 1100 °C TPV efficiencies are estimated to increase to 24.0% and 20.7% in structures with the graded buffer removed, if previously demonstrated reflectance is achieved. These devices also have application to laser power conversion in the 2.0–2.3 µm atmospheric window. Peak laser power converter efficiencies of 36.8% and 32.5% are estimated under 2.0 µm irradiances of 1.86 and 2.81 W cm−2, respectively. [ABSTRACT FROM AUTHOR]

Fluctuations refer to inhomogeneity in the distribution of donors and acceptors at the nanometer scale and occur in many compound solar cell materials such as Cu(In,Ga)Se2, Cu2ZnSn(S,Se)4, and CdSexTe1−x. In this work, numerical simulations show that these fluctuations produce not only electrostatic potential variation, but also, local changes in the carrier density and effective bandgap. For a CdSexTe1−x absorber doped with arsenic, simulations and cathodoluminescence data within single grains demonstrate how donor and acceptor densities—consistent with capacitance-voltage and secondary-ion mass-spectrometry data—produce tails in photoluminescence, quantum efficiency, and absorption measurements. Using multiple theoretical approaches, we demonstrate that the fluctuations can hinder expected performance gains from increased carrier density, and we describe the significant open-circuit voltage deficit observed in the CdSexTe1−x:As solar technology. Our results demonstrate that it is critical to characterize and reduce carrier compensation to realize a higher efficiency. [ABSTRACT FROM AUTHOR]

We conducted T = 6K cathodoluminescence (CL) spectrum imaging with a nanoscale electron beam on beveled surfaces of CdTe thin films at the critical stages of standard CdTe solar cell fabrication. We find that the through-thickness CL total intensity profiles are consistent with a reduction in grain-boundary recombination due to the CdCl2 treatment. The color-coded CL maps of the near-band-edge transitions indicate significant variations in the defect recombination activity at the micron and sub-micron scales within grains, from grain to grain, throughout the film depth, and between films with different processing histories. We estimated the grain-interior sulfur-alloying fraction in the interdiffused CdTe/CdS region of the CdCl2-treated films from a sample of 35 grains and found that it is not strongly correlated with CL intensity. A kinetic rate-equation model was used to simulate grain-boundary (GB) and grain-interior CL spectra. Simulations indicate that the large reduction in the exciton band intensity and relatively small decrease in the lower-energy band intensity at CdTe GBs or dislocations can be explained by an enhanced electron-hole non-radiative recombination rate at the deep GB or dislocation defects. Simulations also show that higher GB concentrations of donors and/or acceptors can increase the lower-energy band intensity, while slightly decreasing the exciton band intensity. [ABSTRACT FROM AUTHOR]

Direct bandgap AlxIn1−xP alloys offer an advantage for red and amber light-emitting diode (LED) operation over conventional (AlxGa1−x)0.5In0.5P alloys due to their higher direct bandgap energies. However, the coupled variation of its bandgap energy and lattice constant present challenges for fabricating quantum well (QW)-based LED devices on GaAs substrates. Here, we present the design and demonstration of AlxIn1−xP red and amber LEDs incorporating multiple QW structures. Strain balancing the QW layers and manipulating the AlxIn1−xP conduction band energy through control of spontaneous atomic ordering produce structures with higher energetic barriers to electron leakage compared to (AlxGa1−x)0.5In0.5P LEDs. We also discuss future improvements that must be made to realize high efficiency red and amber LEDs. [ABSTRACT FROM AUTHOR]

We conducted cathodoluminescence (CL) spectrum imaging and electron backscatter diffraction on the same microscopic areas of CdTe thin films to correlate grain-boundary (GB) recombination by GB "type." We examined misorientation-based GB types, including coincident site lattice (CSL) ∑=3, other-CSL (∑=5-49), and general GBs (∑>49), which make up ≥47%-48%, ≥6%-8%, and ≥44%-47%, respectively, of the GB length at the film back surfaces. Statistically averaged CL total intensities were calculated for each GB type from sample sizes of ∼97 GBs per type and were compared to the average grain-interior CL intensity. We find that only ≥16%-18% of ∑=3 GBs are active non-radiative recombination centers. In contrast, all other-CSL and general GBs are observed to be strong non-radiative centers and, interestingly, these GB types have about the same CL intensity. Both as-deposited and CdCl2-treated films were studied. The CdCl2 treatment reduces non-radiative recombination at both other-CSL and general GBs, but GBs are still recombination centers after the CdCl2 treatment. [ABSTRACT FROM AUTHOR]

Small voids in the absorber layer of thin-film solar cells are generally suspected to impair photovoltaic performance. They have been studied on Cu(In,Ga)Se 2 cells with conventional laboratory techniques, albeit limited to surface characterization and often affected by sample-preparation artifacts. Here, synchrotron imaging is performed on a fully operational as-deposited solar cell containing a few tens of voids. By measuring operando current and X-ray excited optical luminescence, the local electrical and optical performance in the proximity of the voids are estimated, and via ptychographic tomography, the depth in the absorber of the voids is quantified. Besides, the complex network of material-deficit structures between the absorber and the top electrode is highlighted. Despite certain local impairments, the massive presence of voids in the absorber suggests they only have a limited detrimental impact on performance., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)