Nanocrystal Layer Research Articles

Air-Stable Thin Films of Tin Halide Perovskite Nanocrystals by Polymers and Al2O3 Encapsulation.

Tin halide perovskites are promising for optoelectronics, although their sensitivity to ambient conditions due to Sn(II) oxidation presents a challenge. Encapsulation techniques can mitigate degradation and facilitate advanced studies of the intrinsic properties. To study and improve the ambient stability of CsSnBr3 and CsSnI3 nanocrystal (NC) thin films, we explored various encapsulation methods: organic, inorganic, and hybrid. We employed three methods for organic encapsulation: co-deposition with NCs, co-deposition with an additional top layer, and in situ polymerization with NCs. We synthesized thin layers of alumina by using atomic layer deposition for inorganic encapsulation. While individual methods offered marginal improvements, the hybrid approach provided the best results. By employing a hybrid heterostructured thin-film strategy, with the NC layer covered by a thin layer of poly(methyl methacrylate) followed by a 40 nm alumina layer, the stability in air was improved from a few seconds to a record period of 15 days, a crucial advancement for the further exploration of tin halide perovskites.

Electrically Controlled Smart Window for Seasonally Adaptive Thermal Management in Buildings.

Smart windows offer a sustainable solution for energy-efficient buildings by adapting to various weather conditions. However, the challenge lies in achieving precise control over specific sunlight bands to effectively respond to complex weather changes and individual needs. Herein, a novel electrochromic smart window fabricated by integrating a self-assembled cellulose nanocrystals (CNCs) layer with an electrochromic poly(3,4-ethylenedioxythiophene):poly(styrene sulfonic acid) (PEDOT:PSS) layer is reported, which exhibits high near-infrared transmittance, low solar reflectivity (26%), and infrared emissivity (20%) in winter, and low near-infrared transmittance, high solar reflectivity (91%), and infrared emissivity (≈94%) in summer. Interestingly, the material offers dynamic temperature control based on its photothermal properties, maintaining the internal temperature of buildings within a comfortable range of 20-25 °C from morning to night, particularly in winter with significant daily temperature fluctuations. Simulations show that the CNC-PED device demonstrates excellent energy-saving and CO2 emission reduction capacities across various global climate zones. This study presents a feasible pathway for constructing season-adaptive smart windows, making them suitable for energy-efficient buildings.

Osmotic energy conversion in serpentinite-hosted deep-sea hydrothermal vents

Cells harvest energy from ionic gradients by selective ion transport across membranes, and the same principle is recently being used for osmotic power generation from salinity gradients at ocean-river interfaces. Common to these ionic gradient conversions is that they require intricate nanoscale structures. Here, we show that natural submarine serpentinite-hosted hydrothermal vent (HV) precipitates are capable of converting ionic gradients into electrochemical energy by selective transport of Na+, K+, H+, and Cl-. Layered hydroxide nanocrystals are aligned radially outwards from the HV fluid channels, constituting confined nanopores that span millimeters in the HV wall. The nanopores change the surface charge depending on adsorbed ions, allowing the mineral to function as a cation- and anion-selective ion transport membrane. Our findings indicate that chemical disequilibria originating from flow and concentration gradients in geologic environments generate confined nanospaces which enable the spontaneous establishment of osmotic energy conversion.

Application of AgInSe2 nanoparticles to boost the power conversion efficiency of CdS QDs-sensitized solar cells

In this study, bandgap engineering was utilized to assess the efficiency of photoanodes incorporating CdS nanocrystals and AgInSe2 (AISe) quantum dots (QDs) in quantum dot-sensitized solar cells (QDSSCs). Initially, the deposition of CdS(Xc) nanocrystal layers on a TiO2 substrate was tested using the SILAR method with varying cycles (X = 1–6). Optical transmission analysis revealed a redshift in the absorption edge and reduced transmission with an increasing number of cycles. J-V analysis of TiO2 NCs/CdS(Xc) photoanodes identified cycle X = 5 as optimal. The short-circuit current density (Jsc), open-circuit voltage (Voc), fill factor (FF) and maximum power conversion efficiency (PCE) were 15.5 mA/cm2, 614 mV, 40 %, and 3.76 %, respectively. Subsequently, pre-synthesized AISe QDs were deposited on TiO2 nanocrystals/CdS(Xc) photoanodes, exhibiting a single absorption edge with a bandgap energy of 2.19 eV for all photoanodes. The TiO2 NCs/CdS(5c)/AISe/ZnS photoanode showed an increase in Jsc and efficiency, reaching 17.25 mA/cm2 and 4.27 %, respectively. Utilizing sub-micron-sized TiO2 hollow spheres (HSs) as a light-scattering layer further enhanced light absorption and performance. It was demonstrated that this approach increased the photovoltaic parameters to a Jsc of 19.12 mA/cm2, FF of 43 %, and an overall efficiency of 4.75 %.

Prominent cycling reversibility and kinetics enabled by CaTiO3 protective layer on Zn metal for aqueous Zn-ion batteries

Aqueous Zn-ion batteries (AZIBs) have received considerable attention owing to their various advantages such as safety, low cost, simple battery assembly conditions, and high ionic conductivity. However, they still suffer from serious problems, including uncontrollable dendrite growth, corrosion, hydrogen evolution reaction (HER) from water decomposition, electrode passivation, and unexpected by-products. The creation of a uniform artificial nanocrystal layer on the Zn anode surface is a promising strategy for resolving these issues. Herein, we propose the use of a perovskite CaTiO3 (CTO) protective layer on Zn (CTO@Zn) as a promising approach for improving the performance of AZIBs. The CTO artificial layer provides an efficient pathway for Zn ion diffusion towards the Zn metal because of the high dielectric constant (εr = 180) and ferroelectric characteristics that enable the alignment of dipole moments and redistribute the Zn2+ ions in the CTO layer. By avoiding the direct contact of the Zn anode with the electrolyte solution, the uneven dendrite growth, corrosion, parasitic side reactions, and HER are mitigated, while CTO retains its mechanical and chemical robustness during cycling. Consequently, CTO@Zn demonstrates an improved lifespan in a symmetric cell configuration compared with bare Zn. CTO@Zn shows steady overpotential (∼68 mV) for 1500 h at 1 mA cm−2/0.5 mA h cm−2, excelling bare Zn. Moreover, when paired with the V2O5-C cathode, the CTO@Zn//V2O5-C full battery delivers 148.4 mA h g−1 (based on the mass of the cathode) after 300 cycles. This study provides new insights into Zn metal anodes and the development of high-performance AZIBs.

Investigations on structural, morphological and UV light detection characteristics in p- ZrO2/ n-Si Heterostructure based devices

The development of hetero-structured based UV photodiode is a rapidly growing interest in the area of optoelectronic applications. In recent years, one of the next generation semiconductor material zirconium dioxide (ZrO2), has attracted much attention for UV photodiode applications. The curent research work focuses on the fabrication of ultraviolet (UV) photodetectors using ZrO2 nanocrystals with different molar concentrations. Using the co-precipitation method, ZrO2 nanocrystals were formed onto n-Si substrate. The prepared ZrO2 nanocrystals were characterized by XRD, UV–visible spectroscopy, FeSEM, HRTEM, PL spectroscopic analysis. The structural analysis of ZrO2 nanoparticles shows the cubic space groups with ((Fm-3m, Z = 4) and (Im-3m, Z = 1) respectively. The morphological analysis reveals the irregular shape and highly agglomerated. The TEM and HR-TEM images, and SAED pattern of ZrO2 NPs were obtained at higher mole concentration. The optical energy band gap of ZrO2 nanocrystals were determined in between 3.12 and 2.86 eV. The PL emission spectrum of ZrO2 nanoparticles shows highly intensive emission bands between 360 nm and 520 nm. The optimum ZrO2 (0.3 M) nanocrystal layers were formed onto n-Si substrate which was stacked between top and bottom Ag electrodes. The current-voltage measurements (I–V) plots and ln J-V plots characteristics of the fabricated Ag/p-ZrO2/n-Si/Ag devices were investigated under dark and UV illumination. The p-ZrO2/n-Si junction diodes exhibit the ideal rectifying function at higher molar concentration of ZrO2 diode, and the reverse saturation with maximum photo sensitivity was investigated.

Preparation and optical properties of ZnO/ZnS heterostructured nanomaterials

Firstly, Nano-ZnO materials are obtained by hydrothermal method, and Zinc acetate (Zn(CH3COO)2·2H2O) is selected as the Zn source, and potassium hydroxide (KOH) is used as the analytical reagent. Secondly, ZnO/ZnS composites are prepared by hydrothermal method using monomer nano-ZnO as a template, thioacetamide (CH3CSNH2) as a sulfur source, hexadecyl trimethyl Ammonium bromide (CTAB) as a surface modifier, and adjusting the molar mass ratio of Zn/S. The structure, morphology, and optical properties of the composite are characterized respectively by XRD, SEM, and PL, and the growth mechanism and fluorescence characteristics of the composite are explored. The results indicate that the crystal structure of the ZnO/ZnS complex is initially a hexagonal wurtzite structure. With the gradual increase of S element concentration, only the crystal plane diffraction peak of sphalerite structure ZnS is shown in the XRD spectrum. Besides, the morphology of the composite also grows from microsphere like to flocculent layered nano-crystals. There are strong characteristic absorption and green light absorption capabilities at 523 nm, and there is a relatively weak ultraviolet emission peak appeared at 380 nm in the PL spectrum. The optical properties and visible light absorption capabilities of the nano-ZnO/ZnS composite are superior to those of the monomer ZnO. Finally, the growth mechanism and luminescence mechanism of ZnO/ZnS are explored at the micro-level.

Impedance dynamics in tandem solar cells based on c-Si with upper layers of CsPbBr3 (CsPbI3) perovskite nanocrystals

The application of an additional nanoparticle layer is a common practice for enhancing the optical and electrical properties of third-generation solar cells. In this study, we present the results of impedance spectroscopy (IS) for modified solar cells using Nyquist and Bode diagrams. The structure investigated consists of a conventional double junction based on crystalline silicon (c-Si) coated with thin films of inorganic perovskite nanocrystals (NC) of lead halides CsPbI3 and CsPbBr3. The latter are characterized by a significant phonon disorder, which leads to unique electron-phonon interactions and dielectric responses. The IS results indicate that, under the same conditions, the measured Nyquist plots align well with the simulated ones. An equivalent circuit model is proposed, featuring ohmic resistance, recombination resistance, and geometric capacitance. These elements arise due to charge accumulation, charge transfer resistance, and/or additional interfacial electronic states. The study finds that the introduction of a CsPbI3 layer enhances the photoresponse under bias conditions, but this photoresponse leads to a decrease in DC conductivity. In contrast, the addition of a CsPbBr3 layer obstructs the photoresponse under bias while slightly improving the photoresponse in the absence of an applied voltage. The results obtained contribute to the improvement of tandem solar cell characteristics featuring top layers of perovskite nanocrystals.

Thermal management towards ultra-bright and stable perovskite nanocrystal-based pure red light-emitting diodes

Despite the promising candidacy of perovskite nanocrystals for light-emitting diodes, their pure red electroluminescence is hindered by low saturated luminance, severe external quantum efficiency roll-off, and inferior operational stability. Here, we report ultra-bright and stable pure red light-emitting diodes by manipulating Joule heat generation in the nanocrystal emissive layer and thermal management within the device. Diphenylphosphoryl azide-mediated regulation of the nanocrystal surface synergistically enhances the optical properties and carrier transport of the emissive layer, enabling reduced Joule heat generation and thus lowering the working temperature. These merits inhibit ion migration of the CsPb(Br/I)3 nanocrystal film, promising excellent spectra stability. Combined with the highly thermal-conductive sapphire substrates and implementation of pulse-driving mode, the pure red light-emitting diodes exhibit an ultra-bright luminance of 390,000 cd m−2, a peak external quantum efficiency of 25%, suppressed efficiency roll-off, an operational half-life of 20 hours, and superior spectral stability within 15 A cm−2.

Langmuir-Blodgett Transfer of Nanocrystal Monolayers: Layer Compaction, Layer Compression, and Lattice Stretching of the Transferred Layer.

Grazing incidence small angle X-ray scattering (GISAXS) was used to study the structure and interparticle spacing of monolayers of organic ligand-stabilized iron oxide nanocrystals floating at the air-water interface on a Langmuir trough, and after transfer to a solid support via the Langmuir-Blodgett technique. GISAXS measurements of the nanocrystal arrangement at the air-water interface showed that lateral compression decreased the interparticle spacing of continuous films. GISAXS also revealed that Langmuir-Blodgett transfer of the nanocrystal layers to a silicon substrate led to a stretching of the film, with a significant increase in interparticle spacing.

Design strategy of TiO2/AgInSe/CdS/CdSe/ZnS photoanode and optimization of CdSe nanoparticles layer for increasing the efficiency of quantum dot-sensitized solar cells

In this study, ternary AgInSe (AISe) quantum dots compound were synthesized using a novel chemical precipitation method followed by a controlled hydrothermal treatment. The as-prepared particles were deposited onto a mesoporous TiO2 substrate to be applied as the photoelectrode of quantum dot sensitized solar cells (QDSSCs). Two configurations of multilayer photoanodes i.e. the TiO2 NCs/AgInSe/CdS/ZnS and TiO2 NCs/AgInSe/CdS/CdSe/ZnS were fabricated and employed for higher photovoltaic performance. The co-sensitizing CdS and CdSe nanocrystals layers were synthesized and deposited through successive ionic layer adsorption and reaction (SILAR) and chemical bath deposition (CBD) techniques, respectively. The results revealed that the QDSSCs with TiO2 NCs/AgInSe/ZnS photoanode initially showed an efficiency of 0.45 %. Incorporating CdS NCs as a quasi-shell film increased the efficiency to 3.9 % in the optimized TiO2/AgInSe/CdS(3 cycle)/ZnS configuration. Adding CdSe nanocrystals over-layer did not improve the efficiency of corresponding cells due to the increased thickness and resistance. Instead, the TiO2/AgInSe/CdS(2 cycle)/CdSe(12 min)/ZnS photoanode resulted in the efficiency of 4.10 % with 34 % improvement. Using the sub-micron size TiO2 hollow spheres (HSs) as the light scattering layer created further light absorption and enhanced performance. It was shown that the photovoltaic parameters were increased to short circuit current density (Jsc) of 23.25 mA/cm2, open-circuit voltage (Voc) of 512 mV and overall efficiency equal to 4.55 %

Capacitive and Efficient Near-Infrared Stimulation of Neurons via an Ultrathin AgBiS2 Nanocrystal Layer.

Colloidal nanocrystals (NCs) exhibit significant potential for photovoltaic bioelectronic interfaces because of their solution processability, tunable energy levels, and inorganic nature, lending them chemical stability. Silver bismuth sulfide (AgBiS2) NCs, free from toxic heavy-metal elements (e.g., Cd, Hg, and Pb), particularly offer an exceptional absorption coefficient exceeding 105 cm-1 in the near-infrared (NIR), surpassing many of their inorganic counterparts. Here, we integrated an ultrathin (24 nm) AgBiS2 NC layer into a water-stable photovoltaic bioelectronic device architecture that showed a high capacitive photocurrent of 2.3 mA·cm-2 in artificial cerebrospinal fluid (aCSF) and ionic charges over 10 μC·cm-2 at a low NIR intensity of 0.5 mW·mm-2. The device without encapsulation showed a halftime of 12.5 years under passive accelerated aging test and did not show any toxicity on neurons. Furthermore, patch-clamp electrophysiology on primary hippocampal neurons under whole-cell configuration revealed that the device elicited neuron firing at intensity levels more than an order of magnitude below the established ocular safety limits. These findings point to the potential of AgBiS2 NCs for photovoltaic retinal prostheses.

Spray-dried ternary bioactive glass microspheres: Direct and indirect structural effects of copper-doping on acellular degradation behavior

Silicate-based bioactive glass nano/microspheres hold significant promise for bone substitution by facilitating osteointegration through the release of biologically active ions and the formation of a biomimetic apatite layer. Cu-doping enhances properties such as pro-angiogenic and antibacterial behavior. While sol-gel methods usually yield homogeneous spherical particles for pure silica or binary glasses, synthesizing poorly aggregated Cu-doped ternary glass nano/microparticles without a secondary CuO crystalline phase remains challenging. This article introduces an alternative method for fabricating Cu-doped ternary microparticles using sol-gel chemistry combined with spray-drying. The resulting microspheres exhibit well-defined, poorly aggregated particles with spherical shapes and diameters of a few microns. Copper primarily integrates into the microspheres as Cu0 nanoparticles and as Cu2+ within the amorphous network. This doping affects silica network connectivity, as calcium and phosphorus are preferentially distributed in the glass network (respectively as network modifiers and formers) or involved in amorphous calcium phosphate nano-domains depending on the doping rate. These differences affect the interaction with simulated body fluid. Network depolymerization, ion release (SiO44−, Ca2+, PO43−, Cu2+), and apatite nanocrystal layer formation are impacted, as well as copper release. The latter is mainly provided by the copper involved in the silica network and not from metal nanoparticles, most of which remain in the microspheres after interaction. This understanding holds promising implications for potential therapeutic applications, offering possibilities for both short-term and long-term delivery of a tunable copper dose. Statement of significanceA novel methodology, scalable to industrial levels, enables the synthesis of copper-doped ternary bioactive glass microparticles by combining spray-drying and sol-gel chemistry. It provides precise control over the copper percentage in microspheres. This study explores the influence of synthesis conditions on the copper environment, notably Cu0 and Cu2+ ratios, characterized by EPR spectroscopy, an aspect poorly described for copper-doped bioactive glass. Additionally, copper indirectly affects silica network connectivity and calcium/phosphorus distribution, as revealed by SSNMR. Multiscale characterization illustrates how these features impact acellular degradation in simulated body fluid, highlighting the therapeutic potential for customizable copper dosing to address short- and long-term needs.

Stable Inverted Perovskite Solar Cells with Efficiency over 23.0% via Dual-Layer SnO2 on Perovskite.

Perovskite solar cells (PSCs) have shown great potential for reducing costs and improving power conversion efficiency (PCE). One effective method to achieve the latter is to use an all-inorganic charge transport layer (ICTL). However, traditional methods for crystallizing inorganic layers often result in the formation of a powder instead of a continuous film. To address this issue, we designed a dual-layer inorganic electron transport layer (IETL). This dual-layer structure consists of a layer of SnO2 nanocrystals (SnO2 NCs) deposited via a solution process and a dense SnO2 layer deposited through atomic layer deposition (ALD SnO2) to fill the cracks and gaps between the SnO2 NCs. PSCs having these dual-layer SnO2 ETLs achieved a high efficiency of 23.0%. This efficiency surpasses the recorded performance of ICTLs deposited on the perovskite. Furthermore, the PCE is comparable to that achieved with a C60 ETL. Moreover, the high-density structure of the ALD SnO2 layer inhibits the vertical migration of ions, resulting in improved thermal stability. After continuous heating at 85 °C in 10% humidity for 1000 h, the PCE of the dual-layer SnO2 structure decreased by 18%, whereas that of the C60/BCP structure decreased by 36%. The integration of dual-layer SnO2 into PSCs represents a significant advancement in achieving high-performance, commercially viable inverted monolithic PSCs or tandem solar cells.

Self‐strengthened hydrogel actuator based on the distribution of size‐differentiated PVA crystallites

AbstractSoft tissues, such as muscle could autonomously grow through re‐alignment and/or ‐combination of collagen nanofibrils upon the mechanical training. This adaptive capability is highly expected in artificial materials, particularly in hydrogel actuator. In order to avoid the failure for devices by suffering from the accumulated mechanical loading, in this work, a double layered thermo‐responsive hydrogel actuator capable of self‐strengthening was successfully prepared. In the bilayer, PVA nanocrystals with different particle sizes were uniformly distributed in each monolayer matrix, giving rise to the asymmetric structure and the resultant differentiated de‐swelling behaviors. Thus, the obtained hydrogel actuator with the semi‐interpenetrating network of P(NIPAM‐co‐NMA) can display diverse programmable transformations by varying the temperatures. The existence of PVA nanocrystals in both layers not only can enhance the mechanical strength, dramatically minimizing the collapse of hydrogel actuator in service due to the imbalance of the mechanical properties for bilayer structure, but also was greatly involved in the self‐reinforcing behavior. After repetitive tensile training with 80% strain, the tensile strength and fracture strain increased from 29.6 to 45.8 kPa and 95% to 104%, respectively. The experimental results indicated that the anisotropic orientation and strain‐induced‐crystallization for PVA crystalline domains readily occurred along the tensile direction, finally leading to the synchronous enhancement in mechanical strength for both layers. This work provides a new strategy for designing smart and robust biomimetic hydrogel systems that can be further used as the intelligent soft robotics in various fields.

Exceptional Stability against Water, UV Light, and Heat for CsPbBr3@Pb-MOF Composites.

All-inorganic lead halide perovskite nanocrystals (NCs) have been widely applied in optoelectronic devices owing to their excellent photoluminescence (PL) properties. However, poor stability upon exposure to water, UV light or heat strongly limits their practical application. Herein, CsPbBr3@Pb-MOF composites with exceptional stability against water, UV light, and heat are synthesized by ultrasonic processing the precursors of lead-based MOF (Pb-MOF), oleylammonium bromide (OAmBr) and cesium oleate (Cs-OA) solutions at room temperature. Pb-MOF can not only provide the lead source for the in situ growth of CsPbBr3 NCs, but also the protective layer of perovskites NCs. The formed CsPbBr3@Pb-MOF composites show a considerable PL quantum yield (PLQY) of 67.8%, and can maintain 90% of the initial PL intensity when immersed in water for 2 months. In addition, the outstanding PL stability against UV light and heat is demonstrated with CsPbBr3 NCs synthesized by the conventional method as a comparison. Finally, a green (light-emitting diode) LED is fabricated using green-emitting CsPbBr3@Pb-MOF composites and exhibits excellent stability without packaging when immersed in water for 30 days. This study provides a practical approach to improve the stability in aqueous phase, which may pave the way for future applications for various optoelectronic devices.

Nanocrystal residual strains and density layers enhance failure resistance in the cleithrum bone of evolutionary advanced pike fish

Failure-resistant designs are particularly crucial for bones subjected to rapid loading, as is the case for the ambush-hunting northern pike (Esox lucius). These fish have slim and low-density osteocyte-lacking bones. As part of the swallowing mechanism, the cleithrum bone opens and closes the jaw. The cleithrum needs sufficient strength and damage tolerance, to withstand years of repetitive rapid gape-and-suck cycles of feeding. The thin wing-shaped bone comprises anisotropic layers of mineralized collagen fibers that exhibit periodic variations in mineral density on the mm and micrometer length scales. Wavy collagen fibrils interconnect these layers yielding a highly anisotropic structure. Hydrated cleithra exhibit Young's moduli spanning 3-9 GPa where the yield stress of ∼40 MPa increases markedly to exceed ∼180 MPa upon drying. This 5x observation of increased strength corresponds to a change to brittle fracture patterns. It matches the emergence of compressive residual strains of ∼0.15% within the mineral crystals due to forces from shrinking collagen layers. Compressive stresses on the nanoscale, combined with the layered anisotropic microstructure on the mm length scale, jointly confer structural stability in the slender and lightweight bones. By employing a range of X-ray, electron and optical imaging and mechanical characterization techniques, we reveal the structure and properties that make the cleithra impressively damage resistant composites. Statement of significanceBy combining structural and mechanical characterization techniques spanning the mm to the sub-nanometer length scales, this work provides insights into the structural organization and properties of a resilient bone found in pike fish. Our observations show how the anosteocytic bone within the pectoral gridle of these fish, lacking any biological (remodeling) repair mechanisms, is adapted to sustain natural repeated loading cycles of abrupt jaw-gaping and swallowing. We find residual strains within the mineral apatite nanocrystals that contribute to forming a remarkably resilient composite material. Such information gleaned from bony structures that are different from the usual bones of mammals showcases how nature incorporates smart features that induce damage tolerance in bone material, an adaptation acquired through natural evolutionary processes.

Nondestructive Direct Optical Patterning of Perovskite Nanocrystals with Carbene-Based Ligand Cross-Linkers.

Microscale patterning of colloidal perovskite nanocrystals (NCs) is essential for their integration in advanced device platforms, such as high-definition displays. However, perovskite NCs usually show degraded optical and/or electrical properties after patterning with existing approaches, posing a critical challenge for their optoelectronic applications. Here we achieve nondestructive, direct optical patterning of perovskite NCs with rationally designed carbene-based cross-linkers and demonstrate their applications in high-performance light-emitting diodes. We reveal that both the photochemical properties and the electronic structures of cross-linkers need to be carefully tailored to the material properties of perovskite NCs. This method produces high-resolution (∼4000 ppi) NC patterns with preserved photoluminescent quantum efficiencies and charge transport properties. Prototype light-emitting diodes with patterned/cross-linked NC layers show a maximum luminance of over 60000 cd m-2 and a peak external quantum efficiency of 16%, among the highest for patterned perovskite electroluminescent devices. Such a material-adapted patterning method enabled by designs from a photochemistry perspective could foster the applications of perovskite NCs in system-level electronic and optoelectronic devices.

Dynamic Behavior of Platinum Atoms and Clusters in the Native Oxide Layer of Aluminum Nanocrystals.

Strong metal-support interactions (SMSIs) are well-known in the field of heterogeneous catalysis to induce the encapsulation of platinum (Pt) group metals by oxide supports through high temperature H2 reduction. However, demonstrations of SMSI overlayers have largely been limited to reducible oxides, such as TiO2 and Nb2O5. Here, we show that the amorphous native surface oxide of plasmonic aluminum nanocrystals (AlNCs) exhibits SMSI-induced encapsulation of Pt following reduction in H2 in a Pt structure dependent manner. Reductive treatment in H2 at 300 °C induces the formation of an AlOx SMSI overlayer on Pt clusters, leaving Pt single-atom sites (Ptiso) exposed available for catalysis. The remaining exposed Ptiso species possess a more uniform local coordination environment than has been observed on other forms of Al2O3, suggesting that the AlOx native oxide of AlNCs presents well-defined anchoring sites for individual Pt atoms. This observation extends our understanding of SMSIs by providing evidence that H2-induced encapsulation can occur for a wider variety of materials and should stimulate expanded studies of this effect to include nonreducible oxides with oxygen defects and the presence of disorder. It also suggests that the single-atom sites created in this manner, when combined with the plasmonic properties of the Al nanocrystal core, may allow for site-specific single-atom plasmonic photocatalysis, providing dynamic control over the light-driven reactivity in these systems.

Efficient All-Perovskite Tandem Solar Cells with Low-Optical-Loss Carbazolyl Interconnecting Layers.

Combining wide-band gap (WBG) and narrow-band gap (NBG) perovskites with interconnecting layers (ICLs) to construct monolithic all-perovskite tandem solar cell is an effective way to achieve high power conversion efficiency (PCE). However, optical losses from ICLs need to be further reduced to leverage the full potential of all-perovskite tandem solar cells. Here, metal oxide nanocrystal layers anchored with carbazolyl hole-selective-molecules (CHs), which exhibit much lower optical loss, is employed to replace poly(3,4-ethylenedioxythiophene) polystyrenesulfonate (PEDOT : PSS) as the hole transporting layers (HTLs) in lead-tin (Pb-Sn) perovskite sub-cells and ICLs in all-perovskite tandem solar cells. Optically transparent indium tin oxide nanocrystals (ITO NCs) layers are employed to enhance anchoring of CHs, while a mixture of two CHs is adopted to tune the surface energy-levels of ITO NCs. The optimized mixed Pb-Sn NBG perovskite solar cells demonstrate a high PCE of 23.2 %, with a high short-circuit current density (Jsc ) of 33.5 mA cm-2 . A high PCE of 28.1 % is further obtained in all-perovskite tandem solar cells, with the highest Jsc of 16.7 mA cm-2 to date. Encapsulated tandem solar cells maintain 90 % of their reference point after 500 h of operation at the maximum power point (MPP) under 1-Sun illumination.