With rapid progress in the deployment of metal halide perovskites in various device applications such as solar cells, light-emitting devices, field-effect transistors, photodetectors, etc., the next eminent focus is on the single crystals of these materials. With a lack of grain boundaries and low trap densities, remarkably long charge carrier diffusion lengths, and high ambient and operational stabilities, this class of materials seems greatly promising. Yet, the growing concern for lead toxicity in commercial semiconductor devices has entailed a thrust in the research of alternative lead-free perovskites, including their single crystalline forms. However, there is still no consolidated account of the state-of-the-art in this domain and accordingly, countless feasible systems still remain unexplored. To bridge this gap, we attempt to provide here, an up-to-date overview of lead-free perovskite single crystals with respect to their synthesis methods, structural diversity, stability, photophysical and electrical properties, and device applications. We discuss various approaches to designing, modeling, fabricating, and characterizing new single-crystal systems and conclude with some critical insights for further investigating this field of research.
Large datasets are now ubiquitous as technology enables higher-throughput experiments, but rarely can a research field truly benefit from the research data generated due to inconsistent formatting, undocumented storage or improper dissemination. Here we extract all the meaningful device data from peer-reviewed papers on metal-halide perovskite solar cells published so far and make them available in a database. We collect data from over 42,400 photovoltaic devices with up to 100 parameters per device. We then develop open-source and accessible procedures to analyse the data, providing examples of insights that can be gleaned from the analysis of a large dataset. The database, graphics and analysis tools are made available to the community and will continue to evolve as an open-source initiative. This approach of extensively capturing the progress of an entire field, including sorting, interactive exploration and graphical representation of the data, will be applicable to many fields in materials science, engineering and biosciences.
Perovskite semiconductors have experienced meteoric rise in a variety of optoelectronic applications. With a strong foothold on photovoltaics, much focus now lies on their light emission applications. Rapid progress in materials engineering have led to the demonstration of external quantum efficiencies that surpass the previously established theoretical limits. However, there remains much scope to further optimize the light propagation inside the device stack through careful tailoring of the optical processes that take place at the bulk and interface levels. Photon recycling in the emitter material followed by efficient outcoupling can result in boosting external efficiencies up to 100%. In addition, the poor ambient and operational stability of these materials and devices restrict further commercialization efforts. With best operational lifetimes of only a few hours reported, there is a long way to go before perovskite LEDs can be perceived as reliable alternatives to more established technologies like organic or quantum dot-based LED devices. This review article starts with the discussions of the mechanism of luminescence in these perovskite materials and factors impacting it. It then looks at the possible routes to achieve efficient outcoupling through nanostructuring of the emitter and the substrate. Next, we analyse the instability issues of perovskite-based LEDs from a photophysical standpoint, taking into consideration the underlying phenomena pertaining to defects, and summarize recent advances in mitigating the same. Finally, we provide an outlook on the possible routes forward for the field and propose new avenues to maximally exploit the excellent light-emitting capabilities of this family of semiconductors.
With halide perovskite gaining popularity for optoelectronics application, it is imperative to push for device stacks with minimum optical losses and maximum efficiency. However, the vast plethora of material systems and device architectures available through computerized combinatorial analysis made experimental trials for each proposed possibility impractical. Thus, high-throughput optical simulations in conjunction to comprehensive electronic modeling are necessary to predict outputs and minimize experimental efforts involved. Here, we aim to critically summarize some of the most intuitive and efficient approaches to optical modeling for perovskite-based devices and work toward a consensus on the best avenues to utilize these models. First, the nuances of ellipsometry measurements for ascertaining accurate optical constants of perovskite are discussed. Modeling techniques (such as ray tracing, transfer matrices, finite difference time domain, and finite element methods) to simulate the optical interaction within the device are then elaborated focusing on their advantages and limitations. Next, the primary challenges to attaining greater accuracy of optical constant data as well as insights on the future trends are identified. Finally, an interactive flowchart-based decision tree to ascertain the best simulation technique for a given optoelectronic device architecture is built, which will greatly help experimental scientists and beginners in optical modeling.
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