Oriented wide-bandgap perovskites for monolithic silicon-based tandems with over 1000 hours operational stability.

The instability of hybrid wide-bandgap (WBG) perovskite materials (with bandgap larger than 1.68 eV) still stands out as a major constraint for the commercialization of perovskite/silicon tandem photovoltaics, yet its correlation with the facet properties of WBG perovskites has not been revealed. Herein, we combine experiments and theoretical calculations to comprehensively understand the facet-dependent instability of WBG perovskites.

Identification and Suppression of Point Defects in Bromide Perovskite Single Crystals Enabling Gamma-Ray Spectroscopy.

Methylammonium lead tribromide (MAPbBr) stands out as the most easily grown wide-band-gap metal halide perovskite. It is a promising semiconductor for room-temperature gamma-ray (γ-ray) spectroscopic detectors, but no operational devices are realized. This can be largely attributed to a lack of understanding of point defects and their influence on detector performance.

Eliminating Resistance-Capacitance Coupling Shielding for Depicting the Defect Landscape in Perovskite Solar Cells by Capacitance Spectroscopy.

Capacitance spectroscopy techniques have been widely utilized to evaluate the defect properties in perovskites, which contribute to the efficiency and operation stability development for perovskite solar cells (PSCs). Yet the interplay between the charge transporting layer (CTL) and the perovskite on the capacitance spectroscopy results is still unclear. Here, they show that a pseudo-trap-state capacitance signal is generated in thermal admittance spectroscopy (TAS) due to the enhanced resistance capacitance (RC) coupling caused by the carrier freeze-out of the CTL in PSCs, which could be discerned from the actual defect-induced trap state capacitance signal by tuning the series resistance of PSCs.

Monolithic integration of perovskite heterojunction on TFT backplanes through vapor deposition for sensitive and stable x-ray imaging.

Metal halide perovskites exhibit substantial potential for advancing next-generation x-ray detection. However, fabricating high-performance pixelated imaging arrays remains challenging due to the substantial dark current density and stability issues associated with common organic-inorganic hybrid perovskites. Here, we develop a vapor deposition method to create the first all-inorganic perovskite heterojunction film.

All-silicon multidimensionally-encoded optical physical unclonable functions for integrated circuit anti-counterfeiting.

Integrated circuit anti-counterfeiting based on optical physical unclonable functions (PUFs) plays a crucial role in guaranteeing secure identification and authentication for Internet of Things (IoT) devices. While considerable efforts have been devoted to exploring optical PUFs, two critical challenges remain: incompatibility with the complementary metal-oxide-semiconductor (CMOS) technology and limited information entropy. Here, we demonstrate all-silicon multidimensionally-encoded optical PUFs fabricated by integrating silicon (Si) metasurface and erbium-doped Si quantum dots (Er-Si QDs) with a CMOS-compatible procedure.

Iodide manipulation using zinc additives for efficient perovskite solar minimodules.

Interstitial iodides are the most critical type of defects in perovskite solar cells that limits efficiency and stability. They can be generated during solution, film, and device processing, further accelerating degradation. Herein, we find that introducing a small amount of a zinc salt- zinc trifluoromethane sulfonate (Zn(OOSCF)) in the perovskite solution can control the iodide defects in resultant perovskites ink and films.

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.

Lead-chelating hole-transport layers for efficient and stable perovskite minimodules.

The defective bottom interfaces of perovskites and hole-transport layers (HTLs) limit the performance of p-i-n structure perovskite solar cells. We report that the addition of lead chelation molecules into HTLs can strongly interact with lead(II) ion (Pb), resulting in a reduced amorphous region in perovskites near HTLs and a passivated perovskite bottom surface. The minimodule with an aperture area of 26.

Self-powered perovskite photon-counting detectors.

Metal-halide perovskites (MHPs) have been successfully exploited for converting photons to charges or vice versa in applications of solar cells, light-emitting diodes and solar fuels, for which all these applications involve strong light. Here we show that self-powered polycrystalline perovskite photodetectors can rival the commercial silicon photomultipliers (SiPMs) for photon counting. The photon-counting capability of perovskite photon-counting detectors (PCDs) is mainly determined by shallow traps, despite that deep traps also limit charge-collection efficiency.

Perovskite grain wrapping by converting interfaces and grain boundaries into robust and water-insoluble low-dimensional perovskites.

Stabilizing perovskite solar cells requires consideration of all defective sites in the devices. Substantial efforts have been devoted to interfaces, while stabilization of grain boundaries received less attention. Here, we report on a molecule tributyl(methyl)phosphonium iodide (TPI), which can convert perovskite into a wide bandgap one-dimensional (1D) perovskite that is mechanically robust and water insoluble.

Solution-Processed Ternary Tin (II) Alloy as Hole-Transport Layer of Sn-Pb Perovskite Solar Cells for Enhanced Efficiency and Stability.

Tin-lead (Sn-Pb) narrow-bandgap (NBG) perovskites show great potential in both single-junction and all-perovskite tandem solar cells. Sn-Pb perovskite solar cells (PSCs) are still limited by low charge collection efficiency and poor stability. Here, a ternary Sn (II) alloy of SnOCl is reported as the hole-transport material (HTM) with a work function of 4.

High grain boundary recombination velocity in polycrystalline metal halide perovskites.

Understanding carrier recombination processes in metal halide perovskites is fundamentally important to further improving the efficiency of perovskite solar cells, yet the accurate recombination velocity at grain boundaries (GBs) has not been determined. Here, we report the determination of carrier recombination velocities at GBs () of polycrystalline perovskites by mapping the transient photoluminescence pattern change induced by the nonradiative recombination of carriers at GBs. Charge recombination at GBs is revealed to be even stronger than at surfaces of unpassivated films, with average reaching 2200 to 3300 cm/s.

Blading of Conformal Electron-Transport Layers in p-i-n Perovskite Solar Cells.

Perovskite solar cells (PSCs) are promising to reduce the cost of photovoltaic system due to their low-cost raw materials and high-throughput solution process; however, fabrication of all the active layers in perovskite modules using a scalable solution process has not yet been demonstrated. Herein, the fabrication of highly efficient PSCs and modules in ambient conditions is reported, with all layers bladed except the metal electrode, by blading a 36 ± 9 nm-thick electron-transport layer (ETL) on perovskite films with a roughness of ≈80 nm. A combination of additives in phenyl-C -butyric acid methyl ester (PCBM) allows the PCBM to conformally cover the perovskites and still have a good electrical conductivity.

Heterojunction structures for reduced noise in large-area and sensitive perovskite x-ray detectors.

Polycrystalline perovskites can be readily fabricated into large areas using solution depositions; however, they suffer from large dark currents that are tens to hundreds times higher than industrially relevant values, limiting their application in low-dose x-ray detection. Here, we show that the application of a heterojunction structure into polycrystalline films significantly reduces the dark current density by more than 200 times to subnanoampere per square centimeter without reducing the sensitivity of the detectors. The heterojunction perovskite films are formed by laminating several membrane films filled with perovskites of different bandgaps.

Highly Efficient Pure-Blue Light-Emitting Diodes Based on Rubidium and Chlorine Alloyed Metal Halide Perovskite.

Perovskite light-emitting diodes (PeLEDs) are promising candidates for display and solid-state lighting, due to their tunable colors, high conversion efficiencies, and low cost. However, the performance of blue PeLEDs is far inferior to that of the near-infrared, red, and green counterparts. Here, the fabrication of pure-blue PeLEDs with an emission peak at 475 nm, a peak external quantum efficiency of 10.

Ligand assisted growth of perovskite single crystals with low defect density.

A low defect density in metal halide perovskite single crystals is critical to achieve high performance optoelectronic devices. Here we show the reduction of defect density in perovskite single crystals grown by a ligand-assisted solution process with 3-(decyldimethylammonio)-propane-sulfonate inner salt (DPSI) as an additive. DPSI ligands anchoring with lead ions on perovskite crystal surfaces not only suppress nucleation in solution, but also regulate the addition of proper ions to the growing surface, which greatly enhances the crystal quality.

Response to Comment on "Resolving spatial and energetic distributions of trap states in metal halide perovskite solar cells".

Ravishankar claimed that drive-level capacitance profiling (DLCP) cannot resolve trap density in perovskites of given thickness. We point out that the trap densities derived by DLCP are from the differential capacitance at different frequencies; thus, the background charges caused by diffusion and geometry capacitance have been subtracted. Even for the nondifferential doping analysis, the contribution from diffusion capacitance is negligible and that from geometry capacitance is excluded.

Ultrafast Exciton Transport with a Long Diffusion Length in Layered Perovskites with Organic Cation Functionalization.

Layered perovskites have been employed for various optoelectronic devices including solar cells and light-emitting diodes for improved stability, which need exciton transport along both the in-plane and the out-of-plane directions. However, it is not clear yet what determines the exciton transport along the in-plane direction, which is important to understand its impact toward electronic devices. Here, by employing both steady-state and transient photoluminescence mapping, it is found that in-plane exciton diffusivities in layered perovskites are sensitive to both the number of layers and organic cations.

Interfacial Molecular Doping of Metal Halide Perovskites for Highly Efficient Solar Cells.

Tailoring the doping of semiconductors in heterojunction solar cells shows tremendous success in enhancing the performance of many types of inorganic solar cells, while it is found challenging in perovskite solar cells because of the difficulty in doping perovskites in a controllable way. Here, a small molecule of 4,4',4″,4″'-(pyrazine-2,3,5,6-tetrayl) tetrakis (N,N-bis(4-methoxyphenyl) aniline) (PT-TPA) which can effectively p-dope the surface of FA MA PbI (FA: HC(NH ) ; MA: CH NH ) perovskite films is reported. The intermolecular charge transfer property of PT-TPA forms a stabilized resonance structure to accept electrons from perovskites.

Resolving spatial and energetic distributions of trap states in metal halide perovskite solar cells.

We report the profiling of spatial and energetic distributions of trap states in metal halide perovskite single-crystalline and polycrystalline solar cells. The trap densities in single crystals varied by five orders of magnitude, with a lowest value of 2 × 10 per cubic centimeter and most of the deep traps located at crystal surfaces. The charge trap densities of all depths of the interfaces of the polycrystalline films were one to two orders of magnitude greater than that of the film interior, and the trap density at the film interior was still two to three orders of magnitude greater than that in high-quality single crystals.

Reducing Surface Halide Deficiency for Efficient and Stable Iodide-Based Perovskite Solar Cells.

State-of-the-art, high-performance perovskite solar cells (PSCs) contain a large amount of iodine to realize smaller bandgaps. However, the presence of numerous iodine vacancies at the surface of the film formed by their evaporation during the thermal annealing process has been broadly shown to induce deep-level defects, incur nonradiative charge recombination, and induce photocurrent hysteresis, all of which limit the efficiency and stability of PSCs. In this work, modifying the defective surface of perovskite films with cadmium iodide (CdI) effectively reduces the degree of surface iodine deficiency and stabilizes iodine ions via the formation of strong Cd-I ionic bonds.

Perovskite/Organic Bulk-Heterojunction Integrated Ultrasensitive Broadband Photodetectors with High Near-Infrared External Quantum Efficiency over 70.

Ultraviolet-visible-near infrared (UV-Vis-NIR) broadband detection is important for image sensing, communication, and environmental monitoring, yet remains as a challenge in achieving high external quantum efficiency (EQE) in the broad spectrum range. Herein, sensitive broadband integrated photodetectors (PDs) with high EQE levels are reported. The organic bulk-heterojunction (OBHJ) layer, based on a NIR sensitive organic acceptor, is employed to extend the response spectrum of the perovskite PDs.

Light-Emitting Diodes Based on Colloidal Silicon Quantum Dots with Octyl and Phenylpropyl Ligands.

Colloidal silicon quantum dots (Si QDs) hold ever-growing promise for the development of novel optoelectronic devices such as light-emitting diodes (LEDs). Although it has been proposed that ligands at the surface of colloidal Si QDs may significantly impact the performance of LEDs based on colloidal Si QDs, little systematic work has been carried out to compare the performance of LEDs that are fabricated using colloidal Si QDs with different ligands. Here, colloidal Si QDs with rather short octyl ligands (Octyl-Si QDs) and phenylpropyl ligands (PhPr-Si QDs) are employed for the fabrication of LEDs.