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Abstract Halide perovskite solar cells (PSCs) are a state-of-the-art photovoltaic technology that exhibit high efficiencies and can be manufactured using roll-to-roll systems. However, PSCs are currently fabricated using sequential layer-by-layer deposition, which constrains the selection of suitable functional layers in the solar cell and limits the processing conditions and techniques that can be used. Lamination via diffusion bonding is a scalable parallel-processing technique that has the capability to overcome some of the challenges of sequential deposition by widening the thermal processing window and reducing the chemical compatibility requirements for PSC manufacturing. However, there remains a lack of detailed understanding of the process-structure-property relationships needed to accelerate the development of high-volume lamination-based manufacturing processes. In this work, we introduce a method to study the process-structure-property relationships of laminated perovskite semiconductors by using a custom photoluminescence (PL) spectroscopy system to quantify spatial heterogeneity in laminated halide perovskite (HP) materials. PL is an important figure-of-merit used to quantify the optoelectronic properties of semiconductor materials used in PV manufacturing. The spatial variation in PL of a laminated HP film is compared to that of an unlaminated HP film. The PL system uses servomotors and an Arduino microcontroller to automate a PL mapping procedure. The PL equipment is tunable to achieve a minimum possible spot size of ∼50 μm, enabling high-resolution measurements. The system is used to measure the PL of 19 separate locations on both a laminated and unlaminated HP material. The results of this study reveal that lamination at optimal conditions will improve the average PL peak intensity of the HP by 55%, indicating that lamination has the potential to improve the optoelectronic characteristics of PSCs. However, lamination also increases the standard deviation of PL peak intensity. Therefore, although lamination improves the PL of HPs, it also induces unwanted spatial heterogeneity. This warrants future studies on the governing physical mechanisms that determine quality control metrics in lamination-based PSC manufacturing. 

Abstract Understanding the optoelectronic properties of optically active materials at the nanoscale often proves challenging due to the diffraction-limited resolution of visible light probes and the dose sensitivity of many optically active materials to high-energy electron probes. In this study, we demonstrate correlative synchrotron-based scanning x-ray excited optical luminescence (XEOL) and x-ray fluorescence (XRF) to simultaneously probe local composition and optoelectronic properties of halide perovskite thin films of interest for photovoltaic and optoelectronic devices. We find that perovskite XEOL stability, emission redshifting, and peak broadening under hard x-ray irradiation correlates with trends seen in photoluminescence measurements under continuous visible light laser irradiation. The XEOL stability is sufficient under the intense x-ray probe irradiation to permit proof-of-concept correlative mapping. Typical synchrotron XRF and nano-diffraction measurements use acquisition times 10–100 x shorter than the 5-second acquisition employed for XEOL scans in this study, suggesting that improving luminescence detection should allow correlative XEOL measurements to be performed successfully with minimal material degradation. Analysis of the XEOL emission from the quartz substrate beneath the perovskite reveals its promise for use as a real-time in-situ x-ray dosimeter, which could provide quantitative metrics for future optimization of XEOL data collection for perovskites and other beam-sensitive materials. Overall, the data suggest that XEOL represents a promising route towards improved resolution in the characterization of nanoscale heterogeneities and defects in optically active materials that may be implemented into x-ray nanoprobes to complement existing x-ray modalities. 

There is great interest in developing inexpensive, molecular light-harvesting systems capable of efficiently converting photon energy to chemical potential energy. It is highly desirable to do so using self-assembly and in a manner that supports environmentally benign processing. A critical consideration in any such assembly is the ability to absorb a substantial fraction of the solar emission spectrum and to be able to efficiently move excited states through the space to a functional interface. We have previously shown that aqueous inter-conjugated polyelectrolyte (CPE) complexes can act as ultrafast and efficient energy-transfer antennae. Here we demonstrate formation of a hierarchically assembled, aqueous system based on an inter-CPE exciton donor/acceptor network and a lipid vesicle scaffold. Using a model small-molecule organic semiconductor embedded in the vesicle membrane, we form a ternary exciton funnel that is oriented towards the membrane interior. We show that, although energy transfer is efficient, the assembly morphology depends sensitively on preparation conditions and relative ionic stoichiometry. We propose several approaches towards stabilizing such aqueous assemblies. This work highlights a path to formation of an aqueous, panchromatic light-harvesting system, whose functional complexity can be systematically increased with modularity. 

Phase stability and the optoelectronic performance of the metastable CsPbI₃host can be improved with triple-halide alloying, without excessive Br addition which widens the gap beyond that ideal for tandem-photovoltaics.