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  1. Continuous flash sublimation of inorganic halide perovskites: overcoming rate and continuity limitations of vapor deposition

    Despite the outstanding progress in performance of halide perovskite solar cell absorbers fabricated via vapor-based approaches, increasing deposition rates as well as enabling continuous deposition has been woefully neglected. In fact, recent reports show deposition times for the fabrication of high performing absorbers typically in the range of hours, being orders of magnitude away from industrially reasonable process times. In this work, continuous flash sublimation (CFS) of halide perovskite absorbers is introduced as a concept to overcome the fundamental rate and continuity limitations of current approaches, while at the same time maintaining the performance of previously reported vapor deposition approaches.more » Using CFS, we reduce the time required to deposit a fully absorbing layer to less than 5 minutes, demonstrating the applicability of vapor deposited halide perovskites for commercialization. Additionally, the approach enables continuous deposition, thus circumventing another major bottleneck of established vapor deposition approaches.« less
  2. Monolithic Bifacial Halide Perovskite-Cadmium Selenide Telluride (CST) Tandem Thin-Film Solar Cells (Final Technical Report)

    In this project, we develop a bifacial tandem design for monolithic metal halide perovskite-cadmium selenide telluride (CST) tandem solar cells. The bifacial tandem design not only enables the monolithic integration of perovskite-CST tandems but also delivers high efficiency by harvesting the albedo light. It also allows better current match and thus enables higher power output of the tandem devices than conventional tandem cells. We worked on understanding the critical factors limiting bifacial CST cells and developing strategies to improve their bifaciality. We also developed efficient wide-bandgap perovskite subcells and interconnecting layers that enable the monolithic perovskite-CST tandem solar cells. Wemore » successfully demonstrated prototype monolithic bifacial perovskite-CST tandem solar cells with bifacial equivalent efficiencies of more than 25% under an albedo of 0.4. Additionally, we optimized the wide-bandgap perovskite to realize four-terminal perovskite-CST tandem devices with efficiencies of 25.5% under monofacial illumination. The team disseminated these results to stakeholders in the PV academic and industry and discussed the challenges and major technical barriers for their market entry. The technologies developed in the project are promising but are not yet ready for immediate commercialization. Future fundamental study and R&D work are needed to advance these promising technologies.« less
  3. Investigation of Defect Physics for Efficient, Durable and Ubiquitous Perovskite Solar Modules (Final Technical Report)

    Organometal halide perovskite solar cells have experienced eye-catching improvements in its recent few years. It serves as one of the most promising candidates to replace the currently widely used silicon-based solar modules. To implement its final step to the real application, functional longevity becomes the dernier continent to conquer. As a polycrystalline material, defect plays critical role in the efficiency and stability of the perovskite solar cells. Thus, the investigation of the defect physics of the perovskite layer is indispensable in this research field. However, hard evidence and a consensus are still lacking in terms of the specific nature ofmore » the defects and their effects on performance and hysteresis, and perhaps even more importantly, there is absence of fundamental understanding of the correlations between the defects and long-term operational stability of the device. A more fundamental understanding of the nature of defects in perovskite materials is of paramount importance to progress their efficiency and durability. In this work we propose in-depth studies of correlations of defects with performance and stability of perovskite solar cells. Our project aimed 1) to investigate the defects physics in perovskite solar cells, and 2) to develop a comprehensive understanding and physical model of defects and its influence on performance and stability of perovskite solar cells. With the support from program manager, Peter Lobaccaro, and the Solar Energy Technologies Office of U.S. Department of Energy, the project ends with impact achievements. Our research results have systematically provided strategies to analyze the influences of constructive molecular configurations to the charged defects in the perovskite lattices and developed in-depth understanding of chemical additive approach to improve the perovskite solar cell performance and stability. As history has shown us, control over defect properties of semiconductor materials is the key to achieving high performance and low cost devices. Therefore, the potential impact of unlocking the understanding and manipulation of defects in perovskites is great, enabling this technology to realize SETO goals. The research project is highly productive with 18 published papers in three years in top-level journals such as Science, Nature, Nature Materials, Nature Communications, Journal of American Chemistry Society, Joule, Advanced Materials, and Nano Letters. These works have drawn great attention nationwide with notable total citations over 700 times from 2020 to 2022.« less
  4. Scalable and Quench-Free Processing of Metal Halide Perovskites in Ambient Conditions

    With the rise of global warming and the growing energy crisis, scientists have pivoted from typical resources to look for new materials and technologies. Perovskite materials hold the potential for making high-efficiency, low-cost solar cells through solution processing of Earth-abundant materials; however, scalability, stability, and durability remain key challenges. In order to transition from small-scale processing in inert environments to higher throughput processing in ambient conditions, the fundamentals of perovskite crystallization must be understood. Classical nucleation theory, the LaMer relation, and nonclassical crystallization considerations are discussed to provide a mechanism by which a gellan gum (GG) additive—a nontoxic polymeric saccharide—hasmore » enabled researchers to produce quality halide perovskite thin-film blade coated in ambient conditions without a quench step. Furthermore, we report on the improved stability and durability properties inherent to these films, which feature improved morphologies and optoelectronic properties compared to films spin-coated in a glovebox with antisolvent. We tune the amount of GG in the perovskite precursor and study the interplay between GG concentration and processability, morphological control, and increased stability under humidity, heat, and mechanical testing. The simplicity of this approach and insensitivity to environmental conditions enable a wide process window for the production of low-defect, mechanically robust, and operationally stable perovskites with fracture energies among the highest obtained for perovskites.« less
  5. Managing potential environmental and human health risks of lead halide perovskite photovoltaic modules

    Perovskite solar cells (PSCs) are emerging photovoltaic (PV) technologies capable of matching power conversion efficiencies (PCEs) of current PV technologies in the market at lower manufacturing costs, making perovskite solar modules (PSMs) cost competitive if manufactured at scale and perform with minimal degradation. PSCs with the highest PCEs, to date, are lead halide perovskites. Lead presents potential environmental and human health risks if PSMs are to be commercialized, as the lead in PSMs are more soluble in water compared to other PV technologies. Therefore, prior to commercialization of PSMs, it is important to highlight, identify, and establish the potential environmentalmore » and human health risks of PSMs as well as develop methods for assessing the potential risks. Here, we identify and discuss a variety of international standards, U.S. regulations, and permits applicable to PSM deployment that relate to the potential environmental and human health risks associated with PSMs. The potential risks for lead and other hazardous material exposures to humans and the environment are outlined which include water quality, air quality, human health, wildlife, land use, and soil contamination, followed by examples of how developers of other PV technologies have navigated human health and environmental risks previously. Potential experimentation, methodology, and research efforts are proposed to elucidate and characterize potential lead leaching risks and concerns pertaining to fires, in-field module damage, and sampling and leach testing of PSMs at end of life. Lastly, lower technology readiness level solutions to mitigate lead leaching, currently being explored for PSMs, are discussed. PSMs have the potential to become a cost competitive PV technology for the solar industry and taking steps toward understanding, identifying, and creating solutions to mitigate potential environmental and human health risks will aid in improving their commercial viability.« less
  6. Inkjet-printed SnOx as an effective electron transport layer for planar perovskite solar cells and the effect of Cu doping

    Inkjet printing is a more sustainable and scalable fabrication method than spin coating for producing perovskite solar cells (PSCs). Although spin-coated SnO2 has been intensively studied as an effective electron transport layer (ETL) for PSCs, inkjet-printed SnO2 ETLs have not been widely reported. Here, we fabricated inkjet-printed, solution-processed SnOx ETLs for planar PSCs. A champion efficiency of 17.55% was achieved for the cell using a low-temperature processed SnOx ETL. The low-temperature SnOx exhibited an amorphous structure and outperformed high-temperature crystalline SnO2. The improved performance was attributed to enhanced charge extraction and transport and suppressed charge recombination at ETL/perovskite interfaces, whichmore » originated from enhanced electrical and optical properties of SnOx, improved perovskite film quality, and well-matched energy level alignment between the SnOx ETL and the perovskite layer. Furthermore, SnOx was doped with Cu. Cu doping increased surface oxygen defects and upshifted energy levels of SnOx, leading to reduced device performance. A tunable hysteresis was observed for PSCs with Cu-doped SnOx ETLs, decreasing at first and turning into inverted hysteresis afterwards with increasing Cu doping level. This tunable hysteresis was related to the interplay between charge/ion accumulation and recombination at ETL/perovskite interfaces in the case of electron extraction barriers.« less
  7. Minimizing Interfacial Recombination in 1.8 eV Triple‐Halide Perovskites for 27.5% Efficient All‐Perovskite Tandems

    Abstract All‐perovskite tandem solar cells show great potential to enable the highest performance at reasonable costs for a viable market entry in the near future. In particular, wide‐bandgap (WBG) perovskites with higher open‐circuit voltage ( V OC ) are essential to further improve the tandem solar cells’ performance. Here, a new 1.8 eV bandgap triple‐halide perovskite composition in conjunction with a piperazinium iodide (PI) surface treatment is developed. With structural analysis, it is found that the PI modifies the surface through a reduction of excess lead iodide in the perovskite and additionally penetrates the bulk. Constant light‐induced magneto‐transport measurements are appliedmore » to separately resolve charge carrier properties of electrons and holes. These measurements reveal a reduced deep trap state density, and improved steady‐state carrier lifetime (factor 2.6) and diffusion lengths (factor 1.6). As a result, WBG PSCs achieve 1.36 V V OC , reaching 90% of the radiative limit. Combined with a 1.26 eV narrow bandgap (NBG) perovskite with a rubidium iodide additive, this enables a tandem cell with a certified scan efficiency of 27.5%.« less
  8. Measuring metal halide perovskite single cell degradation consistent with module-based conditions

    In past years, there has been progress towards increasing the efficiency of metal halide perovskite solar cells (PSCs) without sacrificing long-term stability. However, preventing or mitigating degradation remains one of the major challenges for the commercialization of PSCs. Researchers must ensure that information learned from cell-level studies is relevant to the ultimate target of module application. In this work, we demonstrate that the bias condition used during aging studies has a measurable impact on degradation. We compared the performance of a large number of devices (n = 486) which were aged either under open-circuit (OC) or quasi-maximum power point (qMPP)more » conditions. The performance losses between the two conditions are found to be correlated, but notably, aging at OC leads to a more rapid performance decrease. Furthermore, this faster degradation in the OC condition compared with the qMPP condition occurs regardless of device stack design, treatments, or additives as demonstrated across approximately 160 variants of the p-i-n device stack. The OC condition is an important factor for field stability because partial shading of a module can result in individual cells going into OC. The fact that the degradation dynamics between qMPP and OC conditions are highly correlated indicates that aging studies at OC are related to relevant degradation processes. Consequently, stability studies to generate relevant insights into the degradation processes of PSCs can be executed without requiring sophisticated electronic infrastructure. However, care must be taken with cell-level experimental configurations because unintended, artificial degradation mechanisms may arise that are either not relevant to the application (e.g., modules) or obfuscate the results of the study being undertaken.« less
  9. Work Function Tuning of a Weak Adhesion Homojunction for Stable Perovskite Solar Cells

    Perovskite solar cells (PSCs) have demonstrated a comparable efficiency to Si-based cells. However, the buried interface with weak adhesion remains a critical issue since the ion migration enhanced by the built-in electric field at this interface might lead to instability. We report here that adjusting the energy-level alignment at the weak adhesion homojunction interface can mitigate ion migration and thereby enhance the stability and photovoltaic performance of PSCs. Functional molecules with self-assembled monolayer characteristics were introduced to the surface of the SnO2 layer using silane derivatives, which tuned the work function of the homojunction depending on the functional groups inmore » the molecules and thereby significantly reduced the built-in electric field. The PSC exhibited a power conversion efficiency (PCE) of 25.3%. The maximum power point (MPP) tracking under continuous illumination confirmed that the device retained more than 97% of its initial PCE, even after 1,000 h.« less
  10. Unraveling radiation damage and healing mechanisms in halide perovskites using energy-tuned dual irradiation dosing

    Perovskite photovoltaics have been shown to recover, or heal, after radiation damage. Here, we deconvolve the effects of radiation based on different energy loss mechanisms from incident protons which induce defects or can promote efficiency recovery. We design a dual dose experiment first exposing devices to low-energy protons efficient in creating atomic displacements. Devices are then irradiated with high-energy protons that interact differently. Correlated with modeling, high-energy protons (with increased ionizing energy loss component) effectively anneal the initial radiation damage, and recover the device efficiency, thus directly detailing the different interactions of irradiation. We relate these differences to the energymore » loss (ionization or non-ionization) using simulation. Dual dose experiments provide insight into understanding the radiation response of perovskite solar cells and highlight that radiation-matter interactions in soft lattice materials are distinct from conventional semiconductors. These results present electronic ionization as a unique handle to remedying defects and trap states in perovskites.« less
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