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Triplet–triplet annihilation-based photon upconversion (UC) using bulk perovskite sensitizers has been previously shown to facilitate efficient UC at low fluences. However, the fabrication of the UC devices has not been fully optimized; thus, there is room for improvement. Here, we apply techniques that have been successful in enhancing the performance of perovskite solar cells in order to also improve perovskite-sensitized UC devices. In particular, we investigate the use of a post-fabrication thermal annealing step, overstoichiometric vs stoichiometric addition of PbI2 to the perovskite precursors, methylammonium vs formamidinium cation-rich lead halide perovskite compositions, and the use of different solvents for the annihilator molecules on the perovskite/annihilator interface. We find that excess PbI2 does not significantly affect the UC process, while the perovskite composition is crucial for the yield of extracted carriers across the interface. Comparing toluene and chlorobenzene, we find that the solvent used to deposit the annihilator is also a key factor in the overall device performance. Moreover, we find that thermal annealing of the whole device architecture significantly improves the UC performance by a factor of three. [ABSTRACT FROM AUTHOR]

Photon upconversion via triplet–triplet annihilation could allow for the existing efficiency limit of single junction solar cells to be surpassed. Indeed, efficient upconversion at subsolar fluences has been realized in bulk perovskite-sensitized systems. Many questions have remained unanswered, in particular, regarding their behavior under photovoltaic operating conditions. Here, we investigate the impact of repeated and continuous illumination on bilayer perovskite/rubrene upconversion devices. We find that variations of the underlying perovskite carrier recombination dynamics greatly impact the upconversion process. Trap filling and triplet sensitization are in direct competition: more saturated trap states in the perovskite and, thus, longer underlying perovskite photoluminescence lifetimes allow for an increased number of carriers to diffuse to the perovskite/rubrene interface and undergo charge extraction to the triplet state of rubrene. As a result, the upconversion efficiency is greatly influenced by the underlying trap density: the upconverted photoluminescence intensity increases by two orders of magnitude under continuous illumination for 4 h. This shows that the upconversion efficiency is difficult to define for this system. Importantly, these results indicate that perovskite-sensitized upconversion devices exhibit peak performance under continuous illumination, which is a requirement for their successful integration into photovoltaics to help overcome the Shockley–Queisser limit in single junction solar cells. [ABSTRACT FROM AUTHOR]

Abstract High capital expenditures associated with manufacturing thin silicon wafers make it difficult for the industry to scale up and prevent novel technologies from entering the market. Thin wafers fail largely due to breakage during solar cell processing and handling. One of the root causes for breakage is sub-mm edge cracks in the silicon wafer, and these cracks cannot be reliably detected by most commercially-available crack detection tools. In this work, we first investigate the correlation between wafer thickness and critical crack length, and explain the importance of detecting sub-500-μm edge cracks as the wafer thickness is reduced. Secondly, we extend our previous work of micro-crack detection to demonstrate an edge illumination technique using a near-infrared laser to image edge cracks less than 500 μm in length in multicrystalline silicon. Thirdly, we investigate two fundamental edge illumination mechanisms based on dark-field imaging; namely, direct and vicinal illumination. We will then compare these methods to a state-of-the-art rear illumination method. The advantages and disadvantages of both illumination methods are presented and provide an in-depth analysis of light-crack interaction. In particular, we find that the robustness of vicinal illumination is due to diffuse reflectance. The diffuse reflectance has less dependence on crack configurations, while direct illumination has more dependence on the crack configurations because it utilizes specular reflectance. Our results show that our proposed prototype can detect sub-mm edge cracks in multicrystalline silicon wafers, which is an important step in enabling thin silicon wafer manufacturing. Highlights • Sub-mm cracks are not reliably detected by most of the commercially-available crack detection tools • Our prototype captures the images of edge cracks in multicrystalline silicon wafers based on the dark-field imaging technique with vicinal illumination • Edge-coupling images show a higher contrast than the rear side illumination technique • Physical mechanisms of NIR crack detection via 1D optical simulation indicate that the robustness of the vicinal illumination is due to the diffuse reflectance [ABSTRACT FROM AUTHOR]

The role of the alkali metal cations in halide perovskite solar cells is not well understood. Using synchrotron-based nano–x-ray fluorescence and complementary measurements, we found that the halide distribution becomes homogenized upon addition of cesium iodide, either alone or with rubidium iodide, for substoichiometric, stoichiometric, and overstoichiometric preparations, where the lead halide is varied with respect to organic halide precursors. Halide homogenization coincides with long-lived charge carrier decays, spatially homogeneous carrier dynamics (as visualized by ultrafast microscopy), and improved photovoltaic device performance. We found that rubidium and potassium phase-segregate in highly concentrated clusters. Alkali metals are beneficial at low concentrations, where they homogenize the halide distribution, but at higher concentrations, they form recombination-active second-phase clusters. [ABSTRACT FROM AUTHOR]

Inspired by the rapid rise in efficiencies of lead halide perovskite (LHP) solar cells, lead-free alternatives are attracting increasing attention. In this work, we study the photovoltaic potential of solution-processed antimony (Sb)-based compounds with the formula A3Sb2I9 (A = Cs, Rb, and K). We experimentally determine bandgap magnitude and type, structure, carrier lifetime, exciton binding energy, film morphology, and photovoltaic device performance. We use density functional theory to compute the equilibrium structures, band structures, carrier effective masses, and phase stability diagrams. We find the A-site cation governs the structural and optoelectronic properties of these compounds. Cs3Sb2I9 has a 0D structure, the largest exciton binding energy (175 ± 9 meV), an indirect bandgap, and, in a solar cell, low photocurrent (0.13 mA cm–2). Rb3Sb2I9 has a 2D structure, a direct bandgap, and, among the materials investigated, the lowest exciton binding energy (101 ± 6 meV) and highest photocurrent (1.67 mA cm–2). K3Sb2I9 has a 2D structure, intermediate exciton binding energies (129 ± 9 meV), and intermediate photocurrents (0.41 mA cm–2). Despite remarkably long lifetimes in all compounds (54, 9, and 30 ns for Cs-, Rb-, and K-based materials, respectively), low photocurrents limit performance of all devices. We conclude that carrier collection is limited by large exciton binding energies (experimentally observed) and large carrier effective masses (calculated from density functional theory). The highest photocurrent and efficiency (0.76%) were observed in the Rb-based compound with a direct bandgap, relatively lower exciton binding energy, and lower calculated electron effective mass. To reliably screen for candidate lead-free photovoltaic absorbers, we advise that faster and more accurate computational tools are needed to calculate exciton binding energies and effective masses. [ABSTRACT FROM AUTHOR]