Semi-transparent perovskite solar cells for tandems with silicon and CIGS

A promising approach for upgrading the performance of an established low-bandgap solar technology without adding much cost is to deposit a high bandgap polycrystalline semiconductor on top to make a tandem solar cell. We use a transparent silver nanowire electrode on perovskite solar cells to achieve a semi-transparent device. We place the semi-transparent cell in a mechanically-stacked tandem configuration onto copper indium gallium diselenide (CIGS) and low-quality multicrystalline silicon (Si) to achieve solid-state polycrystalline tandem solar cells with a net improvement in efficiency over the bottom cell alone. This work paves the way for integrating perovskites into a low-cost and high-efficiency (>25%) tandem cell.

Doped but Stable: Spirobisacridine Hole Transporting Materials for Hysteresis-Free and Stable Perovskite Solar Cells

Nikita Drigo, Marius Franckevicius, Hobeom Kim, Kun-Han Lin, Mohammad Khaja Nazeeruddin, Sanghyun Paek, Cristina Roldán Carmona, Pascal Alexander Schouwink, Muhammad Sohail, Albertus Adrian Sutanto

Four spirobisacridine (SBA) hole-transporting materials were synthesized and employed in perovskite solar cells (PSCs). The molecules bear electronically inert alkyl chains of different length and bulkiness, attached to in-plane N atoms of nearly orthogonal spiro-connected acridines. Di-p-methoxyphenylamine (DMPA) substituents tailored to the central SBA-platform define electronic properties of the materials mimicking the structure of the benchmark 2,2',7,7'-tetrakis(N,N-di-4-methoxyphenylamino)-9,9'-spirobifluorene (spiro-MeOTAD), while the alkyl pending groups affect molecular packing in thin films and affect the long-term performance of PSCs. Devices with SBA-based hole transporting layers (HTL) attain efficiencies on par with spiro-MeOTAD. More importantly, solar cells with the new HTMs are hysteresis-free and demonstrate good operational stability, despite being doped as spiro-MeOTAD. The best performing MeSBA-DMPA retained 88% of the initial efficiency after a 1000 h aging test under constant illumination. The results clearly demonstrate that SBA-based compounds are potent candidates for a design of new HTMs for PSCs with improved longevity.

AMER CHEMICAL SOC2020

Investigation in Crystal Growth/Morphology and Interface Engineering of Perovskite Solar Cells by Different Deposition Methods

Nadja Isabelle Desiree Klipfel

A new and promising technology has emerged to compete with traditional silicon photovoltaic semiconductors. The low material and processing costs and high-power conversion efficiencies of organic-inorganic metal halide perovskites make these a promising technology for the future. Despite record efficiencies for small-area devices, stability remains challenging. Due to rapid progress in the field, avenues for large-area commercial production are being explored. One approach is via thermal evaporation, which is presented in this work. The focus is on the vacuum-deposition method itself, the interface engineering of perovskite layers, and the study of a family of low-cost hole-transporting materials (HTM). To improve reproducibility among research groups in vacuum-deposition processes, a better understanding and control of the crystal formation is essential. Of the experimental parameters, two were investigated that were not yet considered in-depth or combined: deposition speed and underlayer material. It was shown that perovskite growth rate changes affect preferred crystal orientation. In addition, it was found that the final perovskite composition is influenced by its underlayer chemistry. Multi-source vacuum deposition of perovskite layers is complex due to the laborious calibration process necessary for proper stoichiometry. Single-source evaporation of pre-synthesized perovskite powders can reduce effort and time. The feasibility of obtaining pure phase films was demonstrated and confirmed by multiple analysis methods.Interfaces in contact with the perovskite can be a source of defects with a deteriorating effect on stability and efficiency. The charge transport processes at the interface of electron transport material (ETM) and perovskite were investigated. The results showed a synergetic effect between cTiO2 and C60 and the importance of C60 as a charge extraction layer. The perovskite hole transporting material (HTM) interface was also systematically studied. Monitoring of dopants showed, for the first time in literature, TFSI anion migration through grain boundaries to the perovskite surface. It was further shown that non-radiative recombination pathways are reduced, indi-cating self-passivating of crystal defects during migration processes.The state-of-the-art HTM 2,2',7,7'-tetrakis (N,N-di-p-methoxyphenylamine)-9,9'spirofluorene (spiro-OMeTAD) is widely employed in spin-coated PSCs. Devel-oping a less costly manufacturing alternative to this material that retains similar properties is a key challenge. A new class of Zn (II) and Cu (II)-based phthalocyanine HTMs functionalized with butyl- and ethylhexyl- groups in the periphery was investigated. Devices fabricated with the Zn (II)-based HTM (n-butyl functionalization) demonstrated the best performance. The device architecture with the highest stability maintained 80% of its initial power conversion efficiency (PCE) over 20h of illumination. At 20.2%, the perovskite architecture with the highest PCE also was the least stable, indicating a trade-off between these two characteristics for this HTM class.

EPFL2022

Compositional and interfacial optimization for enhancement of perovskite solar cells performance

Essa Awadh R Alharbi

Non-renewable sources are responsible for most of the overall greenhouse gas emissions, the development of sustainable energy sources is of prime importance to mitigate the negative effects of climate change. Among renewable sources, solar energy is one of the most abundant forms of energy available. Perovskite photovoltaics has emerged as one of the promising candidates for harvesting solar energy. However, these perovskite solar cells suffer from instability which is primarily due to the bulk and interface defects. In this thesis, we focus on the passivation of the bulk and interface defects to enable high-performance and stable devices. At the beginning of the thesis, we engineered the composition of mixed-cation and mixed-halide perovskite films by judicious incorporation of guanidinium iodide to suppress the parasitic charge carrier recombination, which enabled the fabrication of >20% efficient and operationally stable PSCs yielding reproducible photovoltage as high as 1.20 V. Thereafter, in our next project, we develop a facile strategy to reduce the level of electronic defects present at the interface between the perovskite film and the hole transport layer by treating the perovskite surface with different types of ammonium salts, namely ethylammonium, imidazolium, and guanidinium iodide. We find that this treatment boosts the power conversion efficiency from 20.5% for the control to 22.3%, 22.1%, and 21.0% for the devices treated with ethylammonium, imidazolium, and guanidinium iodide, respectively. Best performing devices showed a loss in efficiency of only 5% under full sunlight intensity with maximum power tracking for 550 h. We employed 2D-solid-state NMR (1H-1H correlation) spectroscopy to unravel the atomic-level mechanism of this passivation effect. Following that, we applied a facile and very effective method that employs methylammonium triiodide (MAI3) for bulk passivation together with interface passivation developed in the second project for holistic defect mitigation in perovskite solar cells. As a result, the champion device shows a power conversion efficiency (PCE) of 23.46% with a high fill factor (FF) of over 80%. Furthermore, these devices exhibit enhanced operational stability, with the best device retaining ~ 90% of its initial PCE under 1 Sun illumination with maximum power point tracking for 350 h. Finally, in our last project, we reconfigured the design of the alkylammonium halide salts to create a holistic bulk and interface engineering. We show that dimethylammonium head along with octyl chain and iodide counter anion works best in the bulk whereas dimethylammonium head along with octyl chain and fluoride counter anion works best at the interface. With a synergistic combination of both bulk and surface passivation, we achieved a high PCE of 24.91% along with exceptional long-term operational stability. In summary, in this thesis we employed different strategies based on organic ammonium salts to engineer the bulk and interface of the PSCs. We did an in-depth investigation of the optoelectronic properties, local structure, and molecular interactions with a combination of characterization at different length and time scales. Our results show that it is imperative to passivate both bulk and interface defects for obtaining high efficiency and stable solar cells. From our work, one can take inspiration from the design and analysis of new materials for the passivation of the PSCs.

EPFL2022

Compositional and interfacial optimization for enhancement of perovskite solar cells performance

Essa Awadh R Alharbi

EPFL2022

Investigation in Crystal Growth/Morphology and Interface Engineering of Perovskite Solar Cells by Different Deposition Methods

Nadja Isabelle Desiree Klipfel

EPFL2022