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The over-dependence on fossil fuels is one of the critical issues to be addressed for combating greenhouse gas emissions. Hydrogen, one of the promising alternatives to fossil fuels, is renewable, carbon-free, and non-polluting gas. The complete utilization of hydrogen in every sector ranging from small to large scale could hugely benefit in mitigating climate change. One of the key aspects of the hydrogen sector is its production via cost-effective and safe ways. Electrolysis and photocatalysis are well-known processes for hydrogen production and their efficiency relies on electrocatalysts, which are generally noble metals. The usage of noble metals as catalysts makes these processes costly and their scarcity is also a limiting factor. Metal nitrides and their porous counterparts have drawn considerable attention from researchers due to their good promise for hydrogen production. Their properties such as active metal centres, nitrogen functionalities, and porous features such as surface area, pore-volume, and tunable pore size could play an important role in electrochemical and photocatalytic hydrogen production. This review focuses on the recent developments in metal nitrides from their synthesis methods point of view. Much attention is given to the emergence of new synthesis techniques, methods, and processes of synthesizing the metal nitride nanostructures. The applications of electrochemical and photocatalytic hydrogen production are summarized. Overall, this review will provide useful information to researchers working in the field of metal nitrides and their application for hydrogen production.

Novel structured thiadiazole-attached carbon nitrides are first synthesized via sintering 5-amino-1,3,4-thiadiazole-2-thiol, demonstrating excellent performances towards photocatalytic H2 evolution under visible light irradiation.

Fully solution-processed, large-area, electrical double-layer transistors (EDLTs) are presented by employing lead sulfide (PbS) colloidal quantum dots (CQDs) as active channels and Ti3C2Tx MXene as...

Structural defects are ubiquitous for polycrystalline perovskite films, compromising device performance and stability. Herein, a universal method is developed to overcome this issue by incorporating halide perovskite quantum dots (QDs) into perovskite polycrystalline films. CsPbBr3 QDs are deposited on four types of halide perovskite films (CsPbBr3, CsPbIBr2, CsPbBrI2, and MAPbI3) and the interactions are triggered by annealing. The ions in the CsPbBr3 QDs are released into the thin films to passivate defects, and concurrently the hydrophobic ligands of QDs self‐assemble on the film surfaces and grain boundaries to reduce the defect density and enhance the film stability. For all QD‐treated films, PL emission intensity and carrier lifetime are significantly improved, and surface morphology and composition uniformity are also optimized. Furthermore, after the QD treatment, light‐induced phase segregation and degradation in mixed‐halide perovskite films are suppressed, and the efficiency of mixed‐halide CsPbIBr2 solar cells is remarkably improved to over 11% from 8.7%. Overall, this work provides a general approach to achieving high‐quality halide perovskite films with suppressed phase segregation, reduced defects, and enhanced stability for optoelectronic applications., A universal approach is reported to fabricate perovskite films by incorporating inorganic CsPbBr3 quantum dots (QDs) into halide perovskite bulk films. Upon post‐annealing, the released elements from QDs compensate vacancies, and hydrophobic ligands on QDs passivate under‐charged Pb atoms and self‐assemble on surface. Therefore, the resulting films with reduced trap density, suppressed phase segregation, improved surface uniformity and enhanced stability are enabled.

This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Materials Letters, copyright © 2021 American Chemical Societ, after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsmaterialslett.1c00592. A cost-effective and environmentally friendly Pb source is a prerequisite for achieving large-scale, low-cost perovskite photovoltaic devices. Currently, the commonly used method to prepare the lead source is based on a fire smelting process, requiring a high temperature of more than 1000 °C, which results in environmental pollution. Spent car lead acid batteries are an environmentally hazardous waste; however, they can alternatively serve as an abundant and inexpensive Pb source. Due to “self-purification”, quantum dots feature a high tolerance of impurities in the precursor since the impurities tend to be expelled from the small crystalline cores during colloidal nucleation. Herein, PbI2 recycled from spent lead acid batteries via a facile low-temperature solution process is used to synthesize CsPbI3 quantum dots, which simultaneously brings multiple benefits including (1) avoiding pollution originating from the fire smelting process; (2) recycling the Pb waste from batteries; and (3) synthesizing high-quality quantum dots. The resulting CsPbI3 quantum dots have photophysical properties such as PLQY and carrier lifetimes on par with those synthesized from the commercial PbI2 due to expelling of the impurity Na atoms. The resulting solar cells deliver comparable power conversion efficiencies: 14.0% for the cells fabricated using recycled PbI2 and 14.7% for the cells constructed using commercial PbI2. This work paves a new and feasible path to applying recycled Pb sources in perovskite photovoltaics.

High magnetization materials are in great demand for the fabrication of advanced multifunctional magnetic devices. Notwithstanding this demand, the development of new materials with these attribute...

To investigate the quantum confinement effect on excitons in hybrid perovskites, single-crystal platelets of CH3NH3PbBr3 are grown on mica substrates using one-step chemical vapor deposition. Photoluminescence measurements reveal a monotonous blue shift with a decreasing platelet thickness, which is accompanied by a significant increase in exciton binding energy from approximately 70 to 150 meV. Those phenomena can be attributed to the one-dimensional (1D) quantum confinement effect in the two-dimensional platelets. Furthermore, we develop an analytical model to quantitatively elucidate the 1D confinement effect in such quantum wells with asymmetric barriers. Our analysis indicates that the exciton Bohr radius of single-crystal CH3NH3PbBr3 is compressed from 4.0 nm for the thick (26.2 nm) platelets to 2.2 nm for the thin (5.9 nm) ones. The critical understanding of the 1D quantum confinement effect and the development of a general model to elucidate the exciton properties of asymmetric semiconductor quantum wells pave the way toward developing high-performance optoelectronic heterostructures.

The surface chemistry of colloidal quantum dots (CQD) play a crucial role in fabricating highly efficient and stable solar cells. However, as‐synthesized PbS CQDs are significantly off‐stoichiometric and contain inhomogeneously distributed S and Pb atoms at the surface, which results in undercharged Pb atoms, dangling bonds of S atoms and uncapped sites, thus causing surface trap states. Moreover, conventional ligand exchange processes cannot efficiently eliminate these undesired atom configurations and defect sites. Here, potassium triiodide (KI3) additives are combined with conventional PbX2 matrix ligands to simultaneously eliminate the undercharged Pb species and dangling S sites via reacting with molecular I2 generated from the reversible reaction KI3 ⇌ I2 + KI. Meanwhile, high surface coverage shells on PbS CQDs are built via PbX2 and KI ligands. The implementation of KI3 additives remarkably suppresses the surface trap states and enhances the device stability due to the surface chemistry optimization. The resultant solar cells achieve the best power convention efficiency of 12.1% and retain 94% of its initial efficiency under 20 h continuous operation in air, while the control devices with KI additive deliver an efficiency of 11.0% and retains 87% of their initial efficiency under the same conditions., Ligand exchange is performed on PbS colloidal quantum dots using conventional PbX2 ligands and KI3 additives via a facile one‐step process, which simultaneously eliminate the undesirable sites and efficiently passivate the surface. The resulting solar cells achieve a power conversion efficiency of 12.1%.

Significant progress in PbS quantum dot solar cells has been achieved through designing device architecture, engineering band alignment, and optimizing the surface chemistry of colloidal quantum dots (CQDs). However, developing a highly stable device while maintaining the desirable efficiency is still a challenging issue for these emerging solar cells. In this study, by introducing an ultrathin NiO nanocrystalline interlayer between Au electrodes and the hole-transport layer of the PbS-EDT, the resulting PbS CQD solar cell efficiency is improved from 9.3 to 10.4% because of the improved hole-extraction efficiency. More excitingly, the device stability is significantly enhanced owing to the passivation effect of the robust NiO nanocrystalline interlayer. The solar cells with the NiO nanocrystalline interlayer retain 95 and 97% of the initial efficiency when heated at 80 °C for 120 min and treated with oxygen plasma irradiation for 60 min, respectively. In contrast, the control devices without the NiO nanocrystalline interlayer retain only 75 and 63% of the initial efficiency under the same testing conditions.

Halide perovskite quantum dots (PQDs) are promising materials for diverse applications including displays, light‐emitting diodes, and solar cells due to their intriguing properties such as tunable bandgap, high photoluminescence quantum yield, high absorbance, and narrow emission peaks. Despite the prosperous achievements over the past several years, PQDs face severe challenges in terms of stability under different circumstances. Currently, researchers have overcome part of the stability problem, making PQDs sustainable in water, oxygen, and polar solvents for long‐term use. However, halide PQDs are easily degraded under continuous irradiation, which significantly limits their potential for conventional applications. In this study, an oleic acid/oleylamine (traditional surface ligands)‐free method to fabricate perovskite quantum dot papers (PQDP) is developed by adding cellulose nanocrystals as long‐chain binding ligands that stabilize the PQD structure. As a result, the relative photoluminescence intensity of PQDP remains over ≈90% under continuous ultraviolet (UV, 16 W) irradiation for 2 months, showing negligible photodegradation. This proposed method paves the way for the fabrication of ultrastable PQDs and the future development of related applications., Solid‐state perovskite quantum dot papers are fabricated using a unique vacuum filtration growth method without a purification process. The bonding between cellulose nanocrystals and perovskite quantum dots makes the hybrid structure stable, and record high UV stability and thermal stability are achieved for perovskite quantum dot papers.

Mixing halides in perovskites has emerged as an effective strategy for tuning the band gap for optoelectronic applications and tackling the stability bottleneck. However, notable photoluminescence evolution has been observed in mixed-halide perovskites under external stimuli such as light illumination, which is attributed to phase segregation with halide inhomogeneity. In this work, we investigate the light illumination effect on the optical properties of all-inorganic mixed-halide perovskite CsPb(Br1-xIx)3 in the Br-rich regime. It is found that the critical iodine concentration, defined as the solubility limit against phase segregation, is significantly suppressed by light illumination to an extremely low level (x < 0.025), although the formation energy calculation suggests a wide range of halide mixing. Furthermore, at high I concentrations (x ≥ 0.2), the phase segregation can be rectified via dark storage within 1 h, but much slower and incomplete reversibility is observed at lower I concentrations. In the all-inorganic mixed-halide perovskite films, the light-induced phase segregation above the solubility limit is also accompanied by a monotonous increase in fluorescence lifetime. Last, we propose that light-induced phase segregation enables the potential application of encrypting erasable information in perovskite films with the aid of tailored light exposure and photoluminescence mapping.

Facile patterning technologies of silver nanowires (AgNWs) with low-cost, high-resolution, designable, scalable, substrate-independent, and transferable characteristics are highly desired. However, it remains a grand challenge for any material processing method to fulfil all desirable features. Herein, a new patterning method is introduced by combining inkjet printing with adhesion manipulation of substrate interfaces. Both positive and negative patterns (i.e., AgNW grid and rectangular patterns) have been simultaneously achieved, and the pattern polarity can be reversed through adhesion modification with judiciously selected supporting layers. The electrical performance of the AgNW grids depends on the AgNW interlocking structure, manifesting a strong structure-property correlation. High-resolution and complex AgNW patterns with line width and spacing as small as 10 μm have been demonstrated through selective deposition of poly(methyl methacrylate) layers. In addition, customized AgNW patterns, such as logos and words, can be fabricated onto A4-size samples and subsequently transferred to targeted substrates, including Si wafers, a curved glass vial, and a beaker. This reported inkjet-assisted process therefore offers a new effective route to manipulate AgNWs for advanced device applications.

Hybrid halide perovskites have emerged as highly promising photovoltaic materials because of their exceptional optoelectronic properties, which are often optimized via compositional engineering like mixing halides. It is well established that hybrid perovskites undergo a series of structural phase transitions as temperature varies. In this work, the authors find that phase transitions are substantially suppressed in mixed-halide hybrid perovskite single crystals of MAPbI3-xBrx (MA = CH3NH3+ and x = 1 or 2) using a complementary suite of diffraction and spectroscopic techniques. Furthermore, as a general behavior, multiple crystallographic phases coexist in mixed-halide perovskites over a wide temperature range, and a slightly distorted monoclinic phase, hitherto unreported for hybrid perovskites, is dominant at temperatures above 100 K. The anomalous structural evolution is correlated with the glassy behavior of organic cations and optical phonons in mixed-halide perovskites. This work demonstrates the complex interplay between composition engineering and lattice dynamics in hybrid perovskites, shedding new light on their unique properties.

Contact engineering is a prerequisite for achieving desirable functionality and performance of semiconductor electronics, which is particularly critical for organic-inorganic hybrid halide perovskites due to their ionic nature and highly reactive interfaces. Although the interfaces between perovskites and charge-transporting layers have attracted lots of attention due to the photovoltaic and light-emitting diode applications, achieving reliable perovskite/electrode contacts for electronic devices, such as transistors and memories, remains as a bottleneck. Herein, a critical review on the elusive nature of perovskite/electrode interfaces with a focus on the interfacial electrochemistry effects is presented. The basic guidelines of electrode selection are given for establishing non-polarized interfaces and optimal energy level alignment for perovskite materials. Furthermore, state-of-the-art strategies on interface-related electrode engineering are reviewed and discussed, which aim at achieving ohmic transport and eliminating hysteresis in perovskite devices. The role and multiple functionalities of self-assembled monolayers that offer a unique approach toward improving perovskite/electrode contacts are also discussed. The insights on electrode engineering pave the way to advancing stable and reliable perovskite devices in diverse electronic applications.

In the current information age, the realization of memory devices with energy efficient design, high storage density, nonvolatility, fast access, and low cost is still a great challenge. As a promising technology to meet these stringent requirements, nonvolatile multistates memory (NMSM) has attracted lots of attention over the past years. Owing to the capability to store data in more than a single bit (0 or 1), the storage density is dramatically enhanced without scaling down the memory cell, making memory devices more efficient and less expensive. Multistates in a single cell also provide an unconventional in-memory computing platform beyond the Von Neumann architecture and enable neuromorphic computing with low power consumption. In this review, an in-depth perspective is presented on the recent progress and challenges on the device architectures, material innovation, working mechanisms of various types of NMSMs, including flash, magnetic random-access memory (MRAM), resistive random-access memory (RRAM), ferroelectric random-access memory (FeRAM), and phase-change memory (PCM). The intriguing properties and performance of these NMSMs, which are the key to realizing highly integrated memory hierarchy, are discussed and compared. Ministry of Education (MOE) Accepted version

Organolead trihalide perovskites have attracted substantial interest with regard to applications in charge-based photovoltaic and optoelectronic devices because of their low processing costs and remarkable light absorption and charge transport properties. Although spin is an intrinsic quantum descriptor of a particle and spintronics has been a central research theme in condensed matter physics, few studies have explored the spin degree of freedom in the emerging hybrid perovskites. Here, we report the characterization of a spin valve that uses hybrid perovskite films as the spin-transporting medium between two ferromagnetic electrodes. Because of the light-responsive nature of the hybrid perovskite, a high magnetoresistance of 97% and a large spin-diffusion length of 81 nm were achieved at 10 K under light illumination in polycrystalline films. Furthermore, by using thin perovskite single crystals, we discovered that the spin-diffusion length was able to reach 1 μm at low temperatures. Our results indicate that the spin relaxation is not significant as previously expected in such lead-containing materials and demonstrate the potential of low-temperature-processed hybrid perovskites as new active materials in spintronic devices.

Tandem cells are one of the most effective ways of breaking the single junction Shockley-Queisser limit. Solution-processable phosphate-buffered saline (PbS) quantum dots are good candidates for producing multiple junction solar cells because of their size-tunable band gap. The intermediate recombination layer (RL) connecting the subcells in a tandem solar cell is crucial for device performance because it determines the charge recombination efficiency and electrical resistance. In this work, a solution-processed ultrathin NiO and Ag nanoparticle film serves as an intermediate layer to enhance the charge recombination efficiency in PbS QD dual-junction tandem solar cells. The champion devices with device architecture of indium tin oxide/S-ZnO/1.45 eV PbS-PbI2/PbS-EDT/NiO/Ag NP/ZnO NP/1.22 eV PbS-PbI2/PbS-EDT/Au deliver a 7.1% power conversion efficiency, which outperforms the optimized reference subcells. This result underscores the critical role of an appropriate nanocrystalline RL in producing high-performance solution-processed PbS QD tandem cells.

Organic-inorganic mixed halide perovskites have emerged as an excellent class of materials with a unique combination of optoelectronic properties, suitable for a plethora of applications ranging from solar cells to light-emitting diodes and photoelectrochemical devices. Recent works have showcased hybrid perovskites for electronic applications through improvements in materials design, processing, and device stability. Herein, a comprehensive up-to-date review is presented on hybrid perovskite electronics with a focus on transistors and memories. These applications are supported by the fundamental material properties of hybrid perovskite semiconductors such as tunable bandgap, ambipolar charge transport, reasonable mobility, defect characteristics, and solution processability, which are highlighted first. Then, recent progresses on perovskite-based transistors are reviewed, covering aspects of fabrication process, patterning techniques, contact engineering, 2D versus 3D material selection, and device performance. Furthermore, applications of perovskites in nonvolatile memories and artificial synaptic devices are presented. The ambient instability of hybrid perovskites and the strategies to tackle this bottleneck are also discussed. Finally, an outlook and opportunities to develop perovskite-based electronics as a competitive and feasible technology are highlighted.

Hybrid halide perovskites are proposed for next-generation photovoltaics and lighting technologies due to their remarkable optoelectronic properties. In this study, we demonstrate printed perovskite nanowires (NWs) for lasing and wide-gamut phosphor using a combination of inkjet printing and nanoporous anodic aluminum oxide (AAO). The random lasing behaviors of the resulting perovskite NWs are analyzed and discussed. Moreover, by varying the composition of Cl−, Br−, and I− anions, we demonstrate tunable emission wavelengths of the perovskite NWs from 439 to 760 nm, with a large red-green-blue color space that extends to 117% of the color standard defined by the National Television Systems Committee (NTSC). Furthermore, we demonstrate passivation of the perovskite NWs against moisture due to their compact spatial confinement within the AAO template combined with a poly(methyl methacrylate) sealing process, resulting in highly stable emission intensity that degrades only 19% after continuous 250 h of 30 mW/cm2 UV excitation and degrades 30% after three months when stored in air at 50% humidity. This inkjet printing fabrication strategy involving AAO-confined perovskite NWs enables highly stable, large-area direct patterning and mass production of perovskite NWs, which is promising for modern lighting applications.

The direction of ferroelectric polarization is prescribed by the symmetry of the crystal structure. Therefore, rotation of the polarization direction is largely limited, despite the opportunity it offers in understanding important dielectric phenomena such as piezoelectric response near the morphotropic phase boundaries and practical applications such as ferroelectric memory. In this study, we report the observation of continuous rotation of ferroelectric polarization in order-disorder type LiNbO3 thin films. The spontaneous polarization could be tilted from an out-of-plane to an in-plane direction in the thin film by controlling the Li vacancy concentration within the hexagonal lattice framework. Partial inclusion of monoclinic-like phase is attributed to the breaking of macroscopic inversion symmetry along different directions and the emergence of ferroelectric polarization along the in-plane direction., 38 pages, 12 figures

Colloidal ZnO nanoparticle (NP) films are recognized as efficient electron transport layers (ETLs) for quantum dot light-emitting diodes (QD-LEDs) with good stability and high efficiency. However, because of the inherently high work function of such films, spontaneous charge transfer occurs at the QD/ZnO interface in such a QD-LED, thus leading to reduced performance. Here, to improve the QD-LED performance, we prepared Ga-doped ZnO NPs with low work functions and tailored band structures via a room-temperature (RT) solution process without the use of bulky organic ligands. We found that the charge transfer at the interface between the CdSe/ZnS QDs and the doped ZnO NPs was significantly weakened because of the incorporated Ga dopants. Remarkably, the as-assembled QD-LEDs, with Ga-doped ZnO NPs as the ETLs, exhibited superior luminances of up to 44 000 cd/m2 and efficiencies of up to 15 cd/A, placing them among the most efficient red-light QD-LEDs ever reported. This discovery provides a new strategy for ...

PbSe colloidal quantum dots (CQDs) possess the advantages of efficient multiple exciton generation (MEG) and a larger Bohr exciton radius compared with PbS CQDs, suggesting that PbSe CQDs can enable superior charge carrier generation and transport in optoelectronic devices. However, the efficiency of PbSe CQD solar cell is generally much lower than that of the PbS counterpart. This is due to the much more research effort dedicated to PbS CQDs solar cells, where effective strategies of ligand exchange, device configuration and charge transport layer engineering have been developed. Here, we combined ligand exchange and charge transport layer engineering to optimize PbSe CQD solar cell performance. The PbSe CQD absorber layer was deposited via one-step ink method on SnO2 with an ultra-thin PCBM serving as a modification interlayer. The champion device with the structure of ITO/SnO2/PCBM/PbSe-PbI2/PbS-EDT/Au achieved a 10.4% efficiency, which to the best of our knowledge the highest efficiency reported to date for PbSe CQD solar cell. This work demonstrates that PbSe CQDs are very promising for next-generation solution-processed photovoltaic technology with low cost and high performance.

Over the past few years, hybrid halide perovskites have emerged as a highly promising class of materials for photovoltaic technology, and the power conversion efficiency of perovskite solar cells (PSCs) has accelerated at an unprecedented pace, reaching a record value of over 22%. In the context of PSC research, wide-bandgap semiconducting metal oxides have been extensively studied because of their exceptional performance for injection and extraction of photo-generated carriers. In this comprehensive review, we focus on the synthesis and applications of metal oxides as electron and hole transporters in efficient PSCs with both mesoporous and planar architectures. Metal oxides and their doped variants with proper energy band alignment with halide perovskites, in the form of nanostructured layers and compact thin films, can not only assist with charge transport but also improve the stability of PSCs under ambient conditions. Strategies for the implementation of metal oxides with tailored compositions and structures, and for the engineering of their interfaces with perovskites will be critical for the future development and commercialization of PSCs.