High-performance perovskite/Cu(In,Ga)Se2 monolithic tandem solar cells.

The combination of hybrid perovskite and Cu(In,Ga)Se2 (CIGS) has the potential for realizing high-efficiency thin-film tandem solar cells because of the complementary tunable bandgaps and excellent photovoltaic properties of these materials. In tandem solar device architectures, the interconnecting layer plays a critical role in determining the overall cell performance, requiring both an effective electrical connection and high optical transparency. We used nanoscale interface engineering of the CIGS surface and a heavily doped poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) hole transport layer between the subcells that preserves open-circuit voltage and enhances both the fill factor and short-circuit current. A monolithic perovskite/CIGS tandem solar cell achieved a 22.43% efficiency, and unencapsulated devices under ambient conditions maintained 88% of their initial efficiency after 500 hours of aging under continuous 1-sun illumination.

High Mobility Indium Oxide Electron Transport Layer for an Efficient Charge Extraction and Optimized Nanomorphology in Organic Photovoltaics.

The electron transport layer (ETL) plays an important role in determining the device efficiency of organic solar cells (OSCs). A rational design of an ETL for OSCs targets high charge extraction and induction of an optimized active layer morphology. In this Letter, a high mobility In2O3 synthesized via a solution-processed combustion reaction is successfully used as a universal ETL in an organic photovoltaic device. With the modification of a thin layer of polyethylenimine ethoxylated (PEIE), a device based on crystalline In2O3 outperforms its counterpart, ZnO, in both PBDTTT-EFT-based fullerene and nonfullerene systems. As ZnO is replaced by In2O3, the average efficiency increases from 9.5% to 10.5% for PBDTTT-EFT-PC71BM fullerene-based organic solar cells and also increases from 10.8% to 11.5% for PBDTTT-EFT-IEICO-4F nonfullerene-based organic solar cells, respectively. Morphological studies have unraveled the fact that the crystalline In2O3 ETL with highly aligned nanocrystallites has induced the crystallization of polymer into a preferential molecular packing that favors the charge transport across an active layer. From the photophysical study, it is found that charge extraction in the crystalline In2O3 device is significantly faster than in the ZnO device due to the higher mobility of In2O3 and optimized nanomorphology of the active layer.

Halide Perovskites for Tandem Solar Cells.

Perovskite solar cells have become one of the strongest candidates for next-generation solar energy technologies. A myriad of beneficial optoelectronic properties of the perovskite materials have enabled superb power conversion efficiencies (PCE) exceeding 22% for a single-junction device. The high PCE achievable via low processing costs and relatively high variability in optical properties have opened new possibilities for perovskites in tandem solar cells. In this Perspective, we will discuss current research trends in fabricating tandem perovskite-based solar cells in combination with a variety of mature photovoltaic devices such as organic, silicon, and Cu(In,Ga)(S,Se)2 (CIGS) solar cells. Characteristic features and present limitations of each tandem cell will be discussed and elaborated upon. Finally, key issues for further improvement and the future outlook will be discussed.

Tailoring the Interfacial Chemical Interaction for High-Efficiency Perovskite Solar Cells.

The ionic nature of perovskite photovoltaic materials makes it easy to form various chemical interactions with different functional groups. Here, we demonstrate that interfacial chemical interactions are a critical factor in determining the optoelectronic properties of perovskite solar cells. By depositing different self-assembled monolayers (SAMs), we introduce different functional groups onto the SnO2 surface to form various chemical interactions with the perovskite layer. It is observed that the perovskite solar cell device performance shows an opposite trend to that of the energy level alignment theory, which shows that chemical interactions are the predominant factor governing the interfacial optoelectronic properties. Further analysis verifies that proper interfacial interactions can significantly reduce trap state density and facilitate the interfacial charge transfer. Through use of the 4-pyridinecarboxylic acid SAM, the resulting perovskite solar cell exhibits striking improvements to the reach the highest efficiency of 18.8%, which constitutes an ∼10% enhancement compared to those without SAMs. Our work highlights the importance of chemical interactions at perovskite/electrode interfaces and paves the way for further optimizing performances of perovskite solar cells.

Morphology Evolution of High Efficiency Perovskite Solar Cells via Vapor Induced Intermediate Phases.

Morphology is critical component to achieve high device performance hybrid perovskite solar cells. Here, we develop a vapor induced intermediate phase (VIP) strategy to manipulate the morphology of perovskite films. By exposing the perovskite precursor films to different saturated solvent vapor atmospheres, e.g., dimethylformamide and dimethylsufoxide, dramatic film morphological evolution occurs, associated with the formation of different intermediate phases. We observe that the crystallization kinetics is significantly altered due to the formation of these intermediate phases, yielding highly crystalline perovskite films with less defect states and high carrier lifetimes. The perovskite solar cells with the reconstructed films exhibits the highest power conversion efficiency (PCE) up to 19.2% under 1 sun AM 1.5G irradiance, which is among the highest planar heterojunction perovskite solar cells. Also, the perovskite solar cells with VIP processing shows less hysteresis behavior and a stabilized power output over 18%. Our work opens up a new direction for morphology control through intermediate phase formation, and paves the way toward further enhancing the device performances of perovskite solar cells.

Single Crystal Formamidinium Lead Iodide (FAPbI3): Insight into the Structural, Optical, and Electrical Properties.

5 mm-scale large FAPbI 3 single crystals and corresponding photoconductive properties are shown. The phase transition of FAPbI3 between the α-phase and δ-phase is studied. The carrier mobility is 4.4 cm(2) V(-1) s(-1) with a lifetime of 484 ns in the bulk of the single crystal. Finally, photodetectors based on single-crystal FAPbI3 are demonstrated.

Multifunctional Fullerene Derivative for Interface Engineering in Perovskite Solar Cells.

In perovskite based planar heterojunction solar cells, the interface between the TiO2 compact layer and the perovskite film is critical for high photovoltaic performance. The deep trap states on the TiO2 surface induce several challenging issues, such as charge recombination loss and poor stability etc. To solve the problems, we synthesized a triblock fullerene derivative (PCBB-2CN-2C8) via rational molecular design for interface engineering in the perovskite solar cells. Modifying the TiO2 surface with the compound significantly improves charge extraction from the perovskite layer. Together with its uplifted surface work function, open circuit voltage and fill factor are dramatically increased from 0.99 to 1.06 V, and from 72.2% to 79.1%, respectively, resulting in 20.7% improvement in power conversion efficiency for the best performing devices. Scrutinizing the electrical properties of this modified interfacial layer strongly suggests that PCBB-2CN-2C8 passivates the TiO2 surface and thus reduces charge recombination loss caused by the deep trap states of TiO2. The passivation effect is further proven by stability testing of the perovskite solar cells with shelf lifetime under ambient conditions improved by a factor of more than 4, from ∼40 h to ∼200 h, using PCBB-2CN-2C8 as the TiO2 modification layer. This work offers not only a promising material for cathode interface engineering, but also provides a viable approach to address the challenges of deep trap states on TiO2 surface in planar perovskite solar cells.

Highly Robust Silver Nanowire Network for Transparent Electrode.

Solution-processed silver nanowire networks are one of the promising candidates to replace a traditional indium tin oxide as next-generation transparent and flexible electrodes due to their ease of processing, moderate flexibility, high transparency, and low sheet resistance. To date, however, high stability of the nanowire networks remains a major challenge because the long-term usages of these electrodes are limited by their poor thermal and chemical stabilities. Existing methods for addressing this challenge mainly focus on protecting the nanowire network with additional layers that require vacuum processes, which can lead to an increment in manufacturing cost. Here, we report a straightforward strategy of a sol-gel processing as a fast and robust way to improve the stabilities of silver nanowires. Compared with reported nanoparticles embedded in nanowire networks, better thermal and chemical stabilities are achieved via sol-gel coating of TiO2 over the silver nanowire networks. The conformal surface coverage suppressed surface diffusion of silver atoms and prevented chemical corrosion from the environment. These results highlight the important role of the functional layer in providing better thermal and chemical stabilities along with improved electrical properties and mechanical robustness. The silver nanowire/TiO2 composite electrodes were applied as the source and drain electrodes for In2O3 thin-film transistors (TFTs) and the devices exhibited improved electrical performance annealed at 300 °C without the degradation of the electrodes. These key findings not only demonstrated a general and effective method to improve the thermal and chemical stabilities of metal nanowire networks but also provided a basic guideline toward rational design of highly efficient and robust composite electrodes.

Controlling Solid-Gas Reactions at Nanoscale for Enhanced Thin Film Morphologies and Device Performances in Solution-Processed Cu2ZnSn(S,Se)4 Solar Cells.

Using Cu2ZnSn(S,Se)4 (CZTSSe) as a model system, we demonstrate the kinetic control of solid-gas reactions at nanoscale by manipulating the surface chemistry of both sol-gel nanoparticles (NPs) and colloidal nanocrystals (NCs). Specifically, we first identify that thiourea (commonly used as sulfur source in sol-gel processes for metal sulfides) can transform into melamine upon film formation, which serves as surface ligands for as-formed Cu2ZnSnS4 (CZTS) NPs. We further reveal that the presence of these surface ligands can significantly affect the outcome of the solid-gas reactions, which enables us to effectively control the selenization process during the fabrication of CZTSSe solar cells and achieve optimal film morphologies (continuous large grains) by fine-tuning the amount of surface ligands used. Such enhancement leads to better light absorption and allows us to achieve 6.5% efficiency from CZTSSe solar cells processed via a sol-gel process using nontoxic, low boiling point mixed solvents. We believe our discovery that the ligand of particulate precursors can significantly affect solid-gas reactions is universal to solid-state chemistry and will boost further research in both understanding the fundamentals of solid-state reactions at nanoscale and taking advantage of these reactions to fabricate crystalline thin film semiconductors with better morphologies and performances.

Multilayer Transparent Top Electrode for Solution Processed Perovskite/Cu(In,Ga)(Se,S)2 Four Terminal Tandem Solar Cells.

Halide perovskites (PVSK) have attracted much attention in recent years due to their high potential as a next generation solar cell material. To further improve perovskites progress toward a state-of-the-art technology, it is desirable to create a tandem structure in which perovskite may be stacked with a current prevailing solar cell such as silicon (Si) or Cu(In,Ga)(Se,S)2 (CIGS). The transparent top electrode is one of the key components as well as challenges to realize such tandem structure. Herein, we develop a multilayer transparent top electrode for perovskite photovoltaic devices delivering an 11.5% efficiency in top illumination mode. The transparent electrode is based on a dielectric/metal/dielectric structure, featuring an ultrathin gold seeded silver layer. A four terminal tandem solar cell employing solution processed CIGS and perovskite cells is also demonstrated with over 15% efficiency.

Spatial element distribution control in a fully solution-processed nanocrystals-based 8.6% Cu2ZnSn(S,Se)4 device.

A fully solution-processed high performance Cu2ZnSn(S,Se)4 (CZTSSe, kesterite) device has been demonstrated. It is based on the rational engineering of elemental spatial distributions in the bulk and particularly near the surface of the film from nanocrystal precursors. The nanocrystals are synthesized through a modified colloidal approach, with excellent solubility over a large compositional window, followed by a selenization process to form the absorber. The X-ray photoluminescence (XPS) depth profiling indicates an undesirable Sn-rich surface of the selenized film. An excessive Zn species was quantitatively introduced through nanocrystals precursor to correct the element distribution, and accordingly a positive correlation between the spatial composition in the bulk/surface film and the resulting device parameter is established. The enhanced device performance is associated with the reduced interfacial recombination. With a Zn content 1.6 times more than the stoichiometry; the optimized device, which is fabricated by employing a full solution process from the absorber to the transparent top electrode, demonstrates a performance of 8.6%. This composition-control approach through stoichiometric adjustments of nanocrystal precursors, and the developed correlation between the spatial composition and device performance may also benefit other multielement-based photovoltaics.