Hairen Tan

Efficient and stable solution-processed planar perovskite solar cells via contact passivation

Passivating traps in perovskites Low-temperature processing of planar organic-inorganic perovskite solar cells made through solution processing would allow for simpler manufacturing and the use of flexible substrates. However, materials currently in use form interfaces with charge carrier trap states that limit performance. Tan et al. used chlorine-capped TiO2 colloidal nanocrystal films as an electron-selective layer, which limited interface recombination in solution-processed solar cells. Such cells achieved certified efficiencies of 19.5% for active areas of 1.1 cm2. Science, this issue p. 722 Chlorine-capped TiO2 nanocrystal films processed below 150°C effectively passivate detrimental carrier trap states. Planar perovskite solar cells (PSCs) made entirely via solution processing at low temperatures (<150°C) offer promise for simple manufacturing, compatibility with flexible substrates, and perovskite-based tandem devices. However, these PSCs require an electron-selective layer that performs well with similar processing. We report a contact-passivation strategy using chlorine-capped TiO2 colloidal nanocrystal film that mitigates interfacial recombination and improves interface binding in low-temperature planar solar cells. We fabricated solar cells with certified efficiencies of 20.1 and 19.5% for active areas of 0.049 and 1.1 square centimeters, respectively, achieved via low-temperature solution processing. Solar cells with efficiency greater than 20% retained 90% (97% after dark recovery) of their initial performance after 500 hours of continuous room-temperature operation at their maximum power point under 1-sun illumination (where 1 sun is defined as the standard illumination at AM1.5, or 1 kilowatt/square meter).

10.6% Certified Colloidal Quantum Dot Solar Cells via Solvent-Polarity-Engineered Halide Passivation

Colloidal quantum dot (CQD) solar cells are solution-processed photovoltaics with broad spectral absorption tunability. Major advances in their efficiency have been made via improved CQD surface passivation and device architectures with enhanced charge carrier collection. Herein, we demonstrate a new strategy to improve further the passivation of CQDs starting from the solution phase. A cosolvent system is employed to tune the solvent polarity in order to achieve the solvation of methylammonium iodide (MAI) and the dispersion of hydrophobic PbS CQDs simultaneously in a homogeneous phase, otherwise not achieved in a single solvent. This process enables MAI to access the CQDs to confer improved passivation. This, in turn, allows for efficient charge extraction from a thicker photoactive layer device, leading to a certified solar cell power conversion efficiency of 10.6%, a new certified record in CQD photovoltaics.

Ultra-bright and highly efficient inorganic based perovskite light-emitting diodes

Inorganic perovskites such as CsPbX3 (X=Cl, Br, I) have attracted attention due to their excellent thermal stability and high photoluminescence quantum efficiency. However, the electroluminescence quantum efficiency of their light-emitting diodes was <1%. We posited that this low efficiency was a result of high leakage current caused by poor perovskite morphology, high non-radiative recombination at interfaces and perovskite grain boundaries, and also charge injection imbalance. Here, we incorporated a small amount of methylammonium organic cation into the CsPbBr3 lattice and by depositing a hydrophilic and insulating polyvinyl pyrrolidine polymer atop the ZnO electron-injection layer to overcome these issues. As a result, we obtained light-emitting diodes exhibiting a high brightness of 91,000 cd m−2 and a high external quantum efficiency of 10.4% using a mixed-cation perovskite Cs0.87MA0.13PbBr3 as the emitting layer. To the best of our knowledge, this is the brightest and most-efficient green perovskite light-emitting diodes reported to date.

Tailoring the Energy Landscape in Quasi-2D Halide Perovskites Enables Efficient Green-Light Emission

Organo-metal halide perovskites are a promising platform for optoelectronic applications in view of their excellent charge-transport and bandgap tunability. However, their low photoluminescence quantum efficiencies, especially in low-excitation regimes, limit their efficiency for light emission. Consequently, perovskite light-emitting devices are operated under high injection, a regime under which the materials have so far been unstable. Here we show that, by concentrating photoexcited states into a small subpopulation of radiative domains, one can achieve a high quantum yield, even at low excitation intensities. We tailor the composition of quasi-2D perovskites to direct the energy transfer into the lowest-bandgap minority phase and to do so faster than it is lost to nonradiative centers. The new material exhibits 60% photoluminescence quantum yield at excitation intensities as low as 1.8 mW/cm2, yielding a ratio of quantum yield to excitation intensity of 0.3 cm2/mW; this represents a decrease of 2 orders of magnitude in the excitation power required to reach high efficiency compared with the best prior reports. Using this strategy, we report light-emitting diodes with external quantum efficiencies of 7.4% and a high luminescence of 8400 cd/m2.

Pseudohalide-Exchanged Quantum Dot Solids Achieve Record Quantum Efficiency in Infrared Photovoltaics

Application of pseudohalogens in colloidal quantum dot (CQD) solar-cell active layers increases the solar-cell performance by reducing the trap densities and implementing thick CQD films. Pseudohalogens are polyatomic analogs of halogens, whose chemistry allows them to substitute halogen atoms by strong chemical interactions with the CQD surfaces. The pseudohalide thiocyanate anion is used to achieve a hybrid surface passivation. A fourfold reduced trap state density than in a control is observed by using a suite of field-effect transistor studies. This translates directly into the thickest CQD active layer ever reported, enabled by enhanced transport lengths in this new class of materials, and leads to the highest external quantum efficiency, 80% at the excitonic peak, compared with previous reports of CQD solar cells.

Chemically Addressable Perovskite Nanocrystals for Light‐Emitting Applications

Whereas organic-inorganic hybrid perovskite nanocrystals (PNCs) have remarkable potential in the development of optoelectronic materials, their relatively poor chemical and colloidal stability undermines their performance in optoelectronic devices. Herein, this issue is addressed by passivating PNCs with a class of chemically addressable ligands. The robust ligands effectively protect the PNC surfaces, enhance PNC solution processability, and can be chemically addressed by thermally induced crosslinking or radical-induced polymerization. This thin polymer shield further enhances the photoluminescence quantum yields by removing surface trap states. Crosslinked methylammonium lead bromide (MAPbBr3 ) PNCs are applied as active materials to build light-emitting diodes that have low turn-on voltages and achieve a record luminance of over 7000 cd m-2 , around threefold better than previous reported MA-based PNC devices. These results indicate the great potential of this ligand passivation approach for long lifespan, highly efficient PNC light emitters.

Nanoimprint-Transfer-Patterned Solids Enhance Light Absorption in Colloidal Quantum Dot Solar Cells

Colloidal quantum dot (CQD) materials are of interest in thin-film solar cells due to their size-tunable bandgap and low-cost solution-processing. However, CQD solar cells suffer from inefficient charge extraction over the film thicknesses required for complete absorption of solar light. Here we show a new strategy to enhance light absorption in CQD solar cells by nanostructuring the CQD film itself at the back interface. We use two-dimensional finite-difference time-domain (FDTD) simulations to study quantitatively the light absorption enhancement in nanostructured back interfaces in CQD solar cells. We implement this experimentally by demonstrating a nanoimprint-transfer-patterning (NTP) process for the fabrication of nanostructured CQD solids with highly ordered patterns. We show that this approach enables a boost in the power conversion efficiency in CQD solar cells primarily due to an increase in short-circuit current density as a result of enhanced absorption through light-trapping.

Perovskite seeding growth of formamidinium-lead-iodide-based perovskites for efficient and stable solar cells

Formamidinium-lead-iodide (FAPbI3)-based perovskites with bandgap below 1.55 eV are of interest for photovoltaics in view of their close-to-ideal bandgap. Record-performance FAPbI3-based solar cells have relied on fabrication via the sequential-deposition method; however, these devices exhibit unstable output under illumination due to the difficulty of incorporating cesium cations (stabilizer) in sequentially deposited films. Here we devise a perovskite seeding method that efficiently incorporates cesium and beneficially modulates perovskite crystallization. First, perovskite seed crystals are embedded in the PbI2 film. The perovskite seeds serve as cesium sources and act as nuclei to facilitate crystallization during the formation of perovskite. Perovskite films with perovskite seeding growth exhibit a lowered trap density, and the resulting planar solar cells achieve stabilized efficiency of 21.5% with a high open-circuit voltage of 1.13 V and a fill factor that exceeds 80%. The Cs-containing FAPbI3-based devices show a striking improvement in operational stability and retain 60% of their initial efficiency after 140 h operation under one sun illumination.Formamidinium-lead-iodide-based perovskites have a preferred bandgap below 1.55 eV for solar cell applications but suffer from operational instability. Here, Zhao et al. improve the film quality using cesium-containing seeded growth to show high stabilized efficiency and more than 100 h lifetime under simulated sunlight.

A thin-film silicon based photocathode with a hydrogen doped TiO2 protection layer for solar hydrogen evolution

Photoelectrochemical (PEC) devices for solar water splitting require not only high solar to hydrogen conversion efficiency but also high chemical stability in strong acidic or alkaline electrolytes for long-term operation. Titanium dioxide (TiO2) has been considered as a highly promising protection layer to achieve high chemical stability for solar water splitting devices, especially for silicon based monolithic photovoltaic electrochemical (PV–EC) systems, while there is a trade-off relationship between activity and stability in these devices: the high charge transport barrier at the PV (silicon based thin film solar cells)/TiO2 interface and the high ohmic loss in TiO2 films hinder the device performance, especially when a thick TiO2 protection layer (preferred to enhance the chemical stability in the electrolyte) is used. Herein, we show that a hydrogen doped TiO2 protection layer can break this traditional trend to increase the activity without deteriorating the stability, when thick protection layers are employed to ensure stability. We demonstrated significant performance enhancement in hydrogenated amorphous silicon/silicon germanium (a-Si:H/a-SiGe:H) photocathodes through this approach. On one hand, the H-doping can shift up the Fermi level and reduce the electron transport barrier at the interface of the PV/TiO2 protection layer. On the other hand, the higher carrier density via H-doping leads to the enhancement of electron transport in TiO2 films and a shorter depletion layer barrier. Thus, the H-doping results in a higher photocurrent output at 0 V vs. reversible hydrogen electrode (RHE), indicating the high potential of the H-doped TiO2 protection layer for achieving stable and efficient monolithic solar water splitting devices.

Compound Homojunction:Heterojunction Reduces Bulk and Interface Recombination in ZnO Photoanodes for Water Splitting

Photoelectrochemical water splitting is far more efficient thanks to the novel ZnOSe/ZnO/BZO thin-film photoanodes fabricated in this work. A novel structure is developed for simultaneously suppressing the charge recombination in the ZnO bulk and at the semiconductor-electrolyte interface. This structure achieves a five-fold enhancement in water-splitting performance, compared to that of pristine ZnO photoanodes, when illuminated using visible light.