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The carrier extraction and transport mechanisms as well as the relative contributions of radiative and non-radiative recombination processes are investigated in high-quality strain-balanced GaInAs/GaAsP multi-quantum well solar cells recently implemented in record efficiency multijunction solar cells. A comprehensive suite of complementary characterization techniques including temperature- and suns-dependent photoluminescence and photovoltaic measurements are employed to analyze thermal escape and tunneling rates, which demonstrate the need to move beyond simple drift-diffusion models of p–n junctions. This study examines the processes that best characterize the operation of these devices across varying temperatures using a simple two-diode model, incorporating multiple transport protocols, and provides insights into the performance-limiting processes and pathways for their optimization.more » « less
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Abstract Quasi‐2D perovskite made with organic spacers co‐crystallized with inorganic cesium lead bromide inorganics is demonstrated for near unity photoluminescence quantum yield at room temperature. However, light emitting diodes made with quasi‐2D perovskites rapidly degrade which remains a major bottleneck in this field. In this work, It is shown that the bright emission originates from finely tuned multi‐component 2D nano‐crystalline phases that are thermodynamically unstable. The bright emission is extremely sensitive to external stimuli and the emission quickly dims away upon heating. After a detailed analysis of their optical and morphological properties, the degradation is attributed to 2D phase redistribution associated with the dissociation of the organic spacers departing from the inorganic lattice. To circumvent the instability problem, a diamine is investigated spacer that has both sides attached to the inorganic lattice. The diamine spacer incorporated perovskite film shows significantly improved thermal tolerance over maintaining a high photoluminescence quantum yield of over 50%, which will be a more robust material for lighting applications. This study guides designing quasi‐2D perovskites to stabilize the emission properties.more » « less
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Abstract Perovskite optoelectronics are regarded as a disruptive technology, but their susceptibility to environmental degradation and reliance on toxic solvents in traditional processing methods pose significant challenges to their practical implementation. Herein, methylammonium lead iodide (MAPbI3) perovskite films processed via a solvent‐free laser printing technique, that exhibit exceptional stability, are reported. These films withstand extreme conditions, including high doses of X‐ray radiation exceeding 200 Gy, blue laser illumination, 90% relative humidity, and thermal stress up to 80 °C for over 300 min in air. We demonstrate that laser‐printed films maintain their structural integrity and optoelectronic properties even after prolonged exposure to these stressors, significantly surpassing the stability of conventionally processed films. The enhanced stability is attributed to the unique film formation mechanism and resulting defect‐tolerant microstructure. These results underscore the potential of laser printing as a scalable, safe, and sustainable manufacturing route for producing stable perovskite‐based devices with potential applications in diverse fields, ranging from renewable energy to large‐area electronics and space exploration.more » « less
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