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The development of methodologies for synthesizing carrier-transporting materials is critical for optoelectronic device fabrication. Amorphous metal oxides have emerged as potential carrier transport materials for perovskite tandem solar cells and flexible electronics due to their ease of fabrication and excellent electronic properties. However, perovskite solar cells employing amorphous metal oxides as the electron-transporting layers (ETLs) remain inefficient. This research describes a moderate dehydration reaction for the low-temperature synthesis of amorphous SnOx. We investigated this amorphous SnOx as the ETL for perovskite solar cells and demonstrated a maximum power conversion efficiency (PCE) of 20.4%, the greatest efficiency ever attained with an amorphous metal oxide ETL produced below 100 °C. Remarkably, the device maintained 85% of its initial efficiency for more than 4800 h. Furthermore, flexible perovskite solar cells based on this amorphous SnOx have a maximum PCE of 11.7%. Finally, this amorphous SnOx was used to fabricate LEDs and exhibited a maximum external quantum efficiency of over 3%.

Summary With rapid progress in perovskite light-emitting diodes (PeLEDs), the electroluminescence performance of large-area is of increasing interest. We investigated why large-area performance lags behind that achieved in laboratory-scale devices and found that defects in perovskite films—emerging from thermal convection during solvent evaporation, as well as electronic traps formed during perovskite crystallization—are chief causes. Here, we report a molecular modification strategy that simultaneously eliminates pinholes in perovskite layers by controlling the dynamics of film formation and that passivates defects in perovskites by incorporating Br species, thereby preventing shorts and non-radiative recombination. The molecular modifier 1,3,5-tris (bromomethyl) benzene (TBB) also modulates the electronic structure of injection or transport materials to achieve improved charge injection and balanced charge transport. As a result, we demonstrate 20 mm × 20 mm green perovskite nanocrystal LEDs that achieve an external quantum efficiency (EQE) of over 16%, a record for large-area PeLEDs.

Upconversion photodetectors convert photons from the infrared to the visible light spectrum and are of use in applications such as infrared detection and imaging. High-performance upconversion devices are, however, typically based on vacuum-deposited materials, which are expensive and require high operating voltages, which limits their implementation in flexible systems. Here we report solution-processed optical upconversion photodetectors with a high photon-to-photon conversion efficiency of 6.5% and a low turn-on voltage of 2.5 V. Our devices consist of a colloidal lead sulfide quantum dot layer for harvesting infrared light that is monolithically coupled to a cadmium selenide/zinc selenide quantum dot layer for visible-light emission. We optimized the charge-extraction layers in these devices by incorporating silver nanoparticles into the electron transport layers to enable carrier tunnelling. Our photodetectors exhibit a low dark current, high detectivity (6.4 × 1012 Jones) and millisecond response time, and are compatible with flexible substrates. We also show that the devices can be used for in vitro bioimaging. By embedding silver nanoparticles in the electron transport layer, solution-processed quantum-dot-based photodetectors with a high photon-to-electron conversion efficiency of 6.5% and a low turn-on voltage of 2.5 V can be created for use in infrared imaging applications.

Tin perovskite is rising as a promising candidate to address the toxicity and theoretical efficiency limitation of lead perovskite. However, the voltage and efficiency of tin perovskite solar cells are much lower than lead counterparts. Herein, indene-C60 bisadduct with higher energy level is utilized as an electron transporting material for tin perovskite solar cells. It suppresses carrier concentration increase caused by remote doping, which significantly reduces interface carriers recombination. Moreover, indene-C60 bisadduct increases the maximum attainable photovoltage of the device. As a result, the use of indene-C60 bisadduct brings unprecedentedly high voltage of 0.94 V, which is over 50% higher than that of 0.6 V for device based on [6,6]-phenyl-C61-butyric acid methyl ester. The device shows a record power conversion efficiency of 12.4% reproduced in an accredited independent photovoltaic testing lab., Despite the lower device efficiency, tin perovskite based solar cells are preferred choices compared to lead-based counterparts due to much lower toxicity. Here Jiang et al. use a fullerene derivative to greatly suppress carrier interface recombination and obtain record high cell efficiency of 12%.

Lead halide perovskites with mixed cations/anions often suffer from phase segregation, which is detrimental to device efficiency and their long-term stability. During perovskite film growth, the gel stage (in between liquid and crystalline) correlates to phase segregation, which has been rarely explored. Herein, cation diffusion kinetics are systematically investigated at the gel stage to develop a diffusion model obeying Fick's second law. Taking 2D layered perovskite as an example, theoretical and experimental results reveal the impact of diffusion coefficient, temperature, and gel duration on the film growth and phase formation. A homogenous 2D perovskite thin film was then fabricated without significant phase segregation. This in-depth understanding of gel stage and relevant cation diffusion kinetics would further guide the design and processing of halide perovskites with mixed composition to meet requirements for optoelectronic applications.

Manganese-based organic-inorganic metal halide composites have been considered as promising candidates for lead-free emitters. However, in spite of their excellent luminescence properties in green and red regions, blue emission-a critical component for white light generation-from pristine manganese-based composites is currently missing. In this work, we successfully achieve blue luminescence center in manganese-based composites through selecting specific organic component methylbenzylamine (MBA). Our approach is fundamentally different from green and red emission in manganese-based composites, which result from manganese-halide frameworks. The coexistence of different luminescence centers in our manganese-based composites is confirmed by photoluminescence (PL) and photoluminescence excitation (PLE) results. As a result of different photoluminescence excitation responses of different emission centers, the resulting emission color can be tuned with selecting different excitation wavelengths. Specifically, a white light emission can be obtained with Commission Internationale de leclairage coordinates of (0.33, 0.35) upon the 330 nm excitation. We further demonstrate the promise of our manganese-based composites in the anti-counterfeiting technology and multicolor lighting. Our results provide a novel strategy for full-spectral emission in manganese-based organic-inorganic metal halide composites and lay a solid foundation for a range of new applications. (C) 2022 Author(s). Funding Agencies|Knut and Alice Wallenberg Foundation [Dnr KAW 2019.0082]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoeping University [2009-00971]; China Scholarship Council (CSC)

The development of methodologies for synthesizing carrier-transporting materials is critical for optoelectronic device fabrication. Amorphous metal oxides have emerged as potential carrier transport materials for perovskite tandem solar cells and flexible electronics due to their ease of fabrication and excellent electronic properties. However, perovskite solar cells employing amorphous metal oxides as the electron-transporting layers (ETLs) remain inefficient. This research describes a moderate dehydration reaction for the low-temperature synthesis of amorphous SnO

The optical responses of molecules and materials provide a basis for chemical measurement and imaging. The optical diffraction limit in conventional light microscopy is exceeded by mechanically probing optical absorption through the photothermal effect with atomic force microscopy (AFM). However, the spatial resolution of AFM-based photothermal optical microscopy is still limited, and the sample surface is prone to damage from scratching due to tip contact, particularly for measurements on soft matter. In this article, we develop peak force visible (PF-vis) microscopy for the measurement of visible optical absorption of soft matter. The spatial resolution of PF-vis microscopy is demonstrated to be 3 nm on green fluorescent protein-labeled virus-like particles, and the imaging sensitivity may approach a single protein molecule. On organic photovoltaic polymers, the spatial distribution of the optical absorption probed by PF-vis microscopy is found to be dependent on the diffusion ranges of excitons in the donor domain. Through finite element modeling and data analysis, the exciton diffusion range of organic photovoltaics can be directly extracted from PF-vis images, saving the need for complex and delicate sample preparations. PF-vis microscopy will enable high-resolution nano-imaging based on light absorption of fluorophores and chromophores, as well as deciphering the correlation between the spatial distribution of photothermal signals and underlying photophysical parameters at the tens of nanometer scale.

The power conversion efficiency (PCE) of tin perovskite solar cells is impeded by the extremely poor resistance to oxidation and high density of intrinsic Sn vacancies. Herein, we grow a 2D-quasi-2D-3D Sn perovskite film using removable pseudohalogen NH4SCN as a structure regulator. This hierarchy structure remarkably enhances air stability resulting from the parallel growth of 2D PEA(2)SnI(4) as the surface layer. We then explore the hierarchy structure perovskite films in planar structural solar cells, which generate a PCE up to 9.41%. The device retains 90% of its initial performance for almost 600 hr. Our results suggest that adding removable NH4SCN in a perovskite precursor can significantly improve the stability and photovoltaic performance of Sn perovskite. This finding provides a powerful strategy to manipulate the structure of low-dimensional perovskite in order to enhance the performance of perovskite solar cells.

Recently, layered perovskites attracted great attention for its excellent stability and light-emitting property. However, most of them rely on the toxic element lead and their emission quantum yields are generally low. Here, a unique hollow two-dimensional perovskite was developed in which the organic hexamethylene diamines (C6H18N22+) strongly coupled with distorted tin bromide anions (SnBr64-). This toxic-free low-dimensional tin perovskite exhibits a broadband emission in the visible region with a high luminescence quantum yield of 86%. First-principles calculation indicate the broadband emission is associated with the recombination of self-trapped excitons. And the emission is related to the geometry of tin bromide anions. An ultraviolet light-pumped white light emitting diode with excellent color-rendering index of 94 was fabricated using it together with a commercially available blue phosphor.

The stability of perovskite is a bottleneck for the application of perovskite solar cells. Herein, 4-ethylamine Phenylphosphate disodium salt (EAPP) was explored as a functional surface ligand to passivate perovskite surface. As the addition of 1 mol% of EAPP, the degradation of the film in high humidity condition was effectively reduced. Solar cells based on EAPP doped perovskite film show merely slight decrease of its initial efficiency in high humidity condition, whereas the control device show catastrophic decrease. Apart from as a passivating molecule to protect perovskite from contacting with water, EAPP show function as a reducing reagent to bond with hydrogen iodide formed in perovskite decomposition.

Although halide perovskite nanocrystals (NCs) are promising materials for optoelectronic devices, they suffer severely from chemical and phase instabilities. Moreover, the common capping ligands like oleic acid and oleylamine that encapsulate the NCs will form an insulating layer, precluding their utility in optoelectronic devices. To overcome these limitations, we develop a postsynthesis passivation process for CsPbI3 NCs by using a bidentate ligand, namely 2,2′-iminodibenzoic acid. Our passivated NCs exhibit narrow red photoluminescence with exceptional quantum yield (close to unity) and substantially improved stability. The passivated NCs enabled us to realize red light-emitting diodes (LEDs) with 5.02% external quantum efficiency and 748 cd/m2 luminance, surpassing by far LEDs made from the nonpassivated NCs.

Halide perovskites have emerged as superstar materials for optoelectronic devices. Besides the fever of research in solar cells, these materials show great promise on light emitting diodes (LEDs), photodetectors and lasers as well. Rapid advances in bulk perovskite materials aroused universal interest for the development of perovskite nanocrystals, inspired by the great progress of classic colloidal semiconductor quantum dots. Perovskite nanocrystals have been synthesized based on solution process and exhibited high luminescence quantum yield, sharp emission peak, and emission color tunability. Significant progresses have been made about the application of perovskite nanocrystals for LED and lasers in recent years. In this paper, we will comprehensively introduce the synthesis strategies, physical and chemical characteristics, as well as their applications in optoelectronic devices.

The Dion-Jacobson quasi-2D structure improves the stability of perovskite light-emitting diodes., Organic-inorganic hybrid halide perovskites are emerging as promising materials for next-generation light-emitting diodes (LEDs). However, the poor stability of these materials has been the main obstacle challenging their application. Here, we performed first-principles calculations, revealing that the molecule dissociation energy of Dion-Jacobson (DJ) structure using 1,4-bis(aminomethyl)benzene molecules as bridging ligands is two times higher than the typical Ruddlesden-Popper (RP) structure based on phenylethylammonium ligands. Accordingly, LEDs based on the DJ structure show a half-lifetime over 100 hours, which is almost two orders of magnitude longer compared with those based on RP structural quasi–two-dimensional perovskite. To the best of our knowledge, this is the longest lifetime reported for all organic-inorganic hybrid perovskites operating at the current density, giving the highest external quantum efficiency (EQE) value. In situ tracking of the film composition in operation indicates that the DJ structure was maintained well after continuous operation under an electric field.

The application of colloidal quantum dots for light-emitting devices has attracted considerable attention in recent years, due to their unique optical properties such as size-dependent emission wavelength, sharp emission peak and high luminescent quantum yield. Tremendous efforts have been made to explore quantum dots for light-emission applications such as light-emitting diodes (LEDs) and light converters. The performance of quantum-dots-based light-emitting diodes (QD-LEDs) has been increasing rapidly in recent decades as the development of quantum-dots synthesis, surface-ligand engineering and device-architecture optimization. Recently, the external quantum efficiencies of red quantum-dots LEDs have exceeded 20.5% with good stability and narrow emission peak. In this review, we summarize the recent advances in QD-LEDs, focusing on quantum-dot surface engineering and device-architecture optimization.

Quantum efficiencies of organic-inorganic hybrid lead halide perovskite light-emitting devices (LEDs) have increased significantly, but poor device operational stability still impedes their further development and application. All-inorganic perovskites show better stability than the hybrid counterparts, but the performance of their respective films used in LEDs is limited by the large perovskite grain sizes, which lowers the radiative recombination probability and results in grain boundary related trap states. We realize smooth and pinhole-free, small-grained inorganic perovskite films with improved photoluminescence quantum yield by introducing trifluoroacetate anions to effectively passivate surface defects and control the crystal growth. As a result, efficient green LEDs based on inorganic perovskite films achieve a high current efficiency of 32.0 cd A−1 corresponding to an external quantum efficiency of 10.5%. More importantly, our all-inorganic perovskite LEDs demonstrate a record operational lifetime, with a half-lifetime of over 250 h at an initial luminance of 100 cd m−2., All-inorganic cesium lead bromide perovskite based light-emitting diodes show improved operational stability but the film quality limits their performance. Here Wang et al. use trifluoroacetate anions to passivate defects and achieve excellent device performance and stability.

Colloidal quantum dots (CQDs) are fast-improving materials for next-generation solution-processed optoelectronic devices such as solar cells, photocatalysis, light emitting diodes, and photodetectors. Nanoscale CQDs exhibit a high surface to volume ratio, and a significant fraction of atoms making up the quantum dots are thus located on the surface. CQD surface states therefore play a critical role in determining these materials' properties, influencing luminescence, defect energy levels, and doping type and density. In the past five years, halide ligands were applied to CQD solar cells, and these not only improved charge carrier mobility, but also reduced defects on the surface. With the inclusion of halide ligands, CQD solar cell certified power conversion efficiencies have increased rapidly from an initial 5% in 2010 to the latest certified values over 10%. In this perspective article, we summarize recent advances in ligand engineering that improve the performance of CQD solar cells, focusing on the use of halide inorganic ligands to improve CQD surface passivation and film conductivity simultaneously.

A Cu‐doped, NiO‐based quantum dot light‐emitting diode (QLED) reported by Xuyong Yang and co‐workers in article number 1704278 exhibits a significant operating lifetime enhancement compared with organic PEDOT:PSS‐based QLEDs. Relying on an inorganic hole transport lay...

Highly efficient PbS colloidal quantum dot (QD) solar cells based on an inverted structure have been missing for a long time. The bottlenecks are the construction of an effective p-n heterojunction at the illumination side with smooth band alignment and the absence of serious interface carrier recombination. Here, solution-processed nickel oxide (NiO) as the p-type layer and lead sulfide (PbS) QDs with iodide ligand as the n-type layer are explored to build a p-n heterojunction at the illumination side. The large depletion region in the QD layer at the illumination side leads to high photocurrent. Interface carrier recombination at the interface is effectively prohibited by inserting a layer of slightly doped p-type QDs with 1,2-ethanedithiol as ligands, leading to improved voltage of the device. Based on this graded device structure design, the efficiency of inverted structural heterojunction PbS QD solar cells is improved to 9.7%, one time higher than the highest efficiency achieved before.

The low toxicity and a near-ideal choice of bandgap make tin perovskite an attractive alternative to lead perovskite in low cost solar cells. However, the development of Sn perovskite solar cells has been impeded by their extremely poor stability when exposed to oxygen. We report low-dimensional Sn perovskites that exhibit markedly enhanced air stability in comparison with their 3D counterparts. The reduced degradation under air exposure is attributed to the improved thermodynamic stability after dimensional reduction, the encapsulating organic ligands, and the compact perovskite film preventing oxygen ingress. We then explore these highly oriented low-dimensional Sn perovskite films in solar cells. The perpendicular growth of the perovskite domains between electrodes allows efficient charge carrier transport, leading to power conversion efficiencies of 5.94% without the requirement of further device structure engineering. We tracked the performance of unencapsulated devices over 100 h and found no appreciable decay in efficiency. These findings raise the prospects of pure Sn perovskites for solar cells application.

Hydrogen generation via photocatalysis-driven water splitting provides a convenient approach to turn solar energy into chemical fuel. The development of photocatalysis system that can effectively harvest visible light for hydrogen generation is an essential task in order to utilize this technology. Herein, a kind of cadmium free Zn-Ag-In-S (ZAIS) colloidal quantum dots (CQDs) that shows remarkably photocatalytic efficiency in the visible region is developed. More importantly, a nanocomposite based on the combination of 0D ZAIS CQDs and 2D MoS2 nanosheet is developed. This can leverage the strong light harvesting capability of CQDs and catalytic performance of MoS2 simultaneously. As a result, an excellent external quantum efficiency of 40.8% at 400 nm is achieved for CQD-based hydrogen generation catalyst. This work presents a new platform for the development of high-efficiency photocatalyst based on 0D-2D nanocomposite.

Small bandgap Sn-Pb mixed perovskite is generally regarded as the most promising structure to further enhance the power conversion efficiency of perovskite solar cells. However, the open circuit voltages (V(OC)s) are usually lower than expected. In this work, by doping the generally used hole transporting layer (HTL) poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS) with a perfluorinated ionomer (PFI), we can tune the work function of it from -5.02 to -5.19eV. This reduces the energy level mismatch between the FA(0.6)MA(0.4) Sn0.6Pb0.4I3 (FAMA) absorber and HTL, giving rise to enhanced built-in voltage and better carrier extraction. The V-OC improves to over 50mV, up to 0.783V, resulting in an improved champion power conversion efficiency (PCE) of 15.85%. Moreover, the devices based on modified HTLs show improved stability at maximum power point. These results demonstrate that energy level tuning of the HTL is a promising strategy for the improvement of the PCEs of Sn-Pb mixed inverted PSCs, and the addition of PFI is an effective method to tune the work function of PEDOT:PSS.

Metal halide perovskites are rising as a competitive material for next-generation light-emitting diodes (LEDs). However, the development of perovskite LEDs is impeded by their fast carriers diffusion and poor stability in bias condition. Herein, quasi-2D CsPbBr3 quantum wells homogeneously surrounded by inorganic crystalline Cs4PbBr6 of large bandgap are grown. The centralization of carriers in nanoregion facilitates radiative recombination and brings much enhanced luminescence quantum yield. The external quantum efficiency and luminescence intensity of the LEDs based on this nanocomposite are one order of magnitude higher than the conventional low-dimensional perovskite. Meanwhile, the use of inorganic nanocomposite materials brings much improved device operation lifetime under constant electrical field.

Programming living cells to organize inorganic nano-objects (NOs) in a spatiotemporally precise fashion would advance new techniques for creating ordered ensembles of NOs and new bio-abiotic hybrid materials with emerging functionalities. Bacterial cells often grow in cellular communities called biofilms. Here, a strategy is reported for programming dynamic biofilm formation for the synchronized assembly of discrete NOs or hetero-nanostructures on diverse interfaces in a dynamic, scalable, and hierarchical fashion. By engineering Escherichia coli to sense blue light and respond by producing biofilm curli fibers, biofilm formation is spatially controlled and the patterned NOs' assembly is simultaneously achieved. Diverse and complex fluorescent quantum dot patterns with a minimum patterning resolution of 100 µm are demonstrated. By temporally controlling the sequential addition of NOs into the culture, multilayered heterostructured thin films are fabricated through autonomous layer-by-layer assembly. It is demonstrated that biologically dynamic self-assembly can be used to advance a new repertoire of nanotechnologies and materials with increasing complexity that would be otherwise challenging to produce.

Stabilization is one critical issue that needs to be improved for future application of colloidal quantum dot (QD)-based light-emitting diodes (QLEDs). This study reports highly efficient and stable QLEDs based on solution-processsed, metal-doped nickel oxide films as hole injection layer (HIL). Several kinds of metal dopants (Li, Mg, and Cu) are introduced to improve the hole injection capability of NiO films. The resulting device with Cu:NiO HIL exhibits superior performance compared to the state-of-the-art poly(3,4-ethylenedioxythiophene):poly(styrene-sulfonate) (PEDOT:PSS)-based QLEDs, with a maximum current efficiency and external quantum efficiency of 45.7 cd A(-1) and 10.5%, respectively. These are the highest values reported so far for QLEDs with PEDOT:PSS-free normal structure. Meanwhile, the resulting QLED shows a half-life time of 87 h at an initial luminance of 5000 cd m(-2), almost fourfold longer than that of the PEDOT:PSS-based device.