Mapping Capillary Infiltration-Induced Potential in Water-Triggered Electric Generator Using an Electrical Probe Integrated Microscope.

Power generation from water-triggered capillary action in porous structures has recently geared extensive attention, offering the potential for generating electricity from ubiquitous water evaporation. However, conclusively establishing the nature of electrical generation and charge transfer is extremely challenging arising from the complicated aqueous solid-liquid interfacial phenomenon. Here, an electric probe-integrated microscope is developed to on-line monitor the correlation between water capillary action and potential values at any desired position of an active layer. With a probe spatial resolution reaching up to fifty micrometers, the internal factors prevailing over the potential distribution across the whole wet and dry regions are comprehensively identified. Further, the self-powered sensing capabilities of this integrated system are also demonstrated, including real-time monitoring of wind speed, environmental humidity, ionic strength, and inclination angle of generators. The combination of electric potential and chemical color indicator suggests that charge generation is likely correlated with ion-selective transport in the nanoporous channel during the water infiltration process. And unipolar ions (for instance protons) should be the dominant charge-transfer species. The work reveals the fundamental principles regulating charge generation/transfer during the water-triggered electric generation process.

Fine-Tuning Crystal Structures of Lead Bromide Perovskite Nanocrystals through Trace Cadmium(II) Doping for Efficient Color-Saturated Green LEDs.

Decreasing perovskite nanocrystal size increases radiative recombination due to the quantum confinement effect, but also increases the Auger recombination rate which leads to carrier imbalance in the emitting layers of electroluminescent devices. Here, we overcome this trade-off by increasing the exciton effective mass without affecting the size, which is realized through the trace Cd2+ doping of formamidinium lead bromide perovskite nanocrystals. We observe an ~2.7 times increase in the exciton binding energy benefiting from a slight distortion of the [BX6]4- octahedra caused by doping in the case of that the Auger recombination rate is almost unchanged. As a result, bright color-saturated green emitting perovskite nanocrystals with a photoluminescence quantum yield of 96 % are obtained. Cd2+ doping also shifts up the energy levels of the nanocrystals, relative to the Fermi level so that heavily n-doped emitters convert into only slightly n-doped ones; this boosts the charge injection efficiency of the corresponding light-emitting diodes. The light-emitting devices based on those nanocrystals reached a high external quantum efficiency of 29.4 % corresponding to a current efficiency of 123 cd A-1, and showed dramatically improved device lifetime, with a narrow bandwidth of 22 nm and Commission Internationale de I'Eclairage coordinates of (0.20, 0.76) for color-saturated green emission for the electroluminescence peak centered at 534 nm, thus being fully compliant with the latest standard for wide color gamut displays.

Fluorine Passivation Inhibits "Particle Talking" Behaviors under Thermal and Electrical Conditions of Pure Blue Mixed Halide Perovskite Nanocrystals.

Owing to outstanding optoelectronic properties, lead halide perovskite nanocrystals (PNCs) are considered promising emitters for next-generation displays. However, the development of pure blue (460-470 nm) perovskite nanocrystal light-emitting diodes (PNC-LEDs), which correspond to the requirements of Rec. 2020 standard, lag far behind that of their green and red counterparts. Here, pure blue CsPb(Br/Cl)3 nanocrystals with remarkable optical performance are demonstrated by a facile fluorine passivation strategy. Prominently, the fluorine passivation on halide vacancies and strong bonding of Pb-F intensely enhance crystal structure stability and inhibit "particle talking" behaviors under both thermal and electrical conditions. Fluorine-based PNCs with high resistance of luminescence thermal quenching retain 70% of photoluminescent intensity when heated to 343 K, which can be attributed to the elevated activation energy for carrier trapping and unchanged grain size. Fluorine-based PNC-LEDs also exhibit stable pure blue electroluminescence (EL) emission with sevenfold promoted luminance and external quantum efficiencies (EQEs), where the suppression of ion migration is further evidenced by a lateral structure device with applied polarizing potential.

Synergistic Solar-Driven Freshwater Generation and Electricity Output Empowered by Wafer-Scale Nanostructured Silicon.

Electricity generation triggered by the ubiquitous water evaporation process provides an intriguing way to harvest energy from water. Meanwhile, natural water evaporation is also a fundamental way to obtain fresh water for human beings. Here, a wafer-scale nanostructured silicon-based device that takes advantage of its well-aligned configuration that simultaneously realizes solar steam generation (SSG) for freshwater collection and hydrovoltaic effect generation for electricity output is developed. An ingenious porous, black carbon nanotube fabric (CNF) electrode endows the device with sustainable water self-pumping capability, excellent durable conductivity, and intense solar spectrum harvesting. A combined device based on the CNF electrode integrated with nanostructured silicon nanowire arrays (SiNWs) provided an aligned numerous surface-to-volume water evaporation interface that enables a recorded continuous short-circuit current 8.65 mA and a water evaporation rate of 1.31 kg m-2 h-1 under one sun illumination. Such wafer-scale SiNWs-based SSG and hydrovoltaic integration devices would unchain the bottleneck of the weak and discontinuous electrical output of hydrovoltaic devices, which inspires other sorts of semiconductor-based hydrovoltaic device designs to target superior performance.

Donor-Acceptor Pair Quantum Emitters in Hexagonal Boron Nitride.

Quantum emitters are needed for a myriad of applications ranging from quantum sensing to quantum computing. Hexagonal boron nitride (hBN) quantum emitters are one of the most promising solid-state platforms to date due to their high brightness and stability and the possibility of a spin-photon interface. However, the understanding of the physical origins of the single-photon emitters (SPEs) is still limited. Here we report dense SPEs in hBN across the entire visible spectrum and present evidence that most of these SPEs can be well explained by donor-acceptor pairs (DAPs). On the basis of the DAP transition generation mechanism, we calculated their wavelength fingerprint, matching well with the experimentally observed photoluminescence spectrum. Our work serves as a step forward for the physical understanding of SPEs in hBN and their applications in quantum technologies.

Microcavity coupled quantum dot emission with detuning control.

Solution processed colloidal semiconductor quantum dots (QDs) have size-tunable optical transitions and high quantum efficiencies, enabling various applications in opto-electronic devices. To enrich the functionality of QD-based opto-electronic devices, colloidal semiconductor QDs have been frequently coupled with optical cavities to enable emission modulation. However, it remains a challenge to fully understand the interaction between the optical cavity resonance and the QD emission, especially for the planar optical microcavities. Here, we have investigated the light emission of colloidal semiconductor QDs in the planar Fabry-Perot microcavity consisted of two Ag mirrors. With the matched QD and cavity resonance, the microcavity coupled QD samples show a prominently narrower emission linewidth and emission angle range because of the efficient QD-cavity coupling, while with a slightly positive or negative energy detuning, the linewidth and angular distribution of the microcavity coupled QD emission both become broadened. Furthermore, with the standard lithography technique, the microcavity coupled QD sample can be patterned into arbitrary geometries, showing extra features of in-plane mode confinement. Our work highlights the important role of detuning in determining the coupling between colloidal semiconductor QDs and microcavities and paves the way for the future design of microcavity coupled QD devices.

Unveiling Crystal Orientation in Quasi-2D Perovskite Films by In Situ GIWAXS for High-Performance Photovoltaics.

Quasi-2D perovskites are enchanting alternative materials for solar cells due to their intrinsic stability. The manipulation of crystal orientation of quasi-2D perovskites is indispensable to target efficient devices, however, the origin of orientation during the film fabrication process still lacks in-depth understanding and convincing evidence yet, which hinders further boosting the performance of photovoltaic devices. Herein, the crystallizing processes during spin-coating and annealing are probed by in situ grazing-incidence wide-angle X-ray scattering (GIWAXS), and the incident-angle-dependent GIWAXS is conducted to unveil the phase distribution in the films. It is found that undesirable lead iodide sol-gel formed intermediate phase would disturb oriented crystalline growth, resulting in random crystal orientation in poor quasi-2D films. A general strategy is developed via simple additive agent incorporation to suppress the formation of the intermediate phase. Accordingly, highly oriented perovskite films with reduced trap density and higher carrier mobility are obtained, which enables the demonstration of optimized quasi-2D perovskite solar cells with a power conversion efficiency of 15.2% as well as improved stability. This work paves a promising way to manipulate the quasi-2D perovskites nucleation and crystallization processes via tuning nucleation stage.

Optical pressure and temperature sensing properties of Nd3+:YTaO4.

The pressure- and temperature-dependent luminescence properties of M'-phase Nd3+:YTaO4 synthesized by a molten salt method are presented. Ten near-infrared emission lines originating from the transitions between the two Stark levels R1,2 of the 3F3/2 state and the five Stark levels Z1,2,3,4,5 of the 4I9/2 state for the doped Nd3+ ions can be clearly identified. All these emission lines are found to shift linearly with pressure in a range up to ∼11 GPa. The R2,1 → Z5 emission lines have larger pressure sensitivities, which are 16.44 and 14.27 cm-1 GPa-1. The intensities of all the emission lines evolve with pressure non-monotonically, and peak at ∼1 GPa. The R1 → Z4,5 and R2 → Z1 emission lines can be obviously narrowed under the hydrostatic pressure, and broadened under the non-hydrostatic pressure, indicating their potential capability for reflecting the characteristic of a pressure environment. The intensity ratio of the R2,1 → Z5 emission lines exhibits a large temperature dependence, with a relative sensitivity between 0.129% and 0.108% K-1 in the physiological temperature range of 290-320 K. Thermal variations of the spectral positions and widths of the R2,1 → Z5 emission lines are also investigated. A high thermal stability for the position of the R2 → Z5 emission line is revealed. Based on the experimental results, the advantages and potential of Nd3+:YTaO4 as a multi-functional sensor for pressure and temperature are discussed.

Synergistic Effect of Dielectric Property and Energy Transfer on Charge Separation in Non-Fullerene-Based Solar Cells.

In non-fullerene-based photovoltaic devices, it is unclear how excitons efficiently dissociate into charge carriers under small driving force. Here, we developed a modified method to estimate dielectric constants of PM6 donor and non-fullerene acceptors. Surprisingly, most non-fullerene acceptors and blend films showed higher dielectric constants. Moreover, they exhibited larger dielectric constants differences at the optical frequency. These results are likely bound to reduced exciton binding energy and bimolecular recombination. Besides, the overlap between the emission spectrum of donor and absorption spectra of non-fullerene acceptors allowed the energy transfer from donor to acceptors. Hence, based on the synergistic effect of dielectric property and energy transfer resulting in efficient charge separation, our finding paves an alternative path to elucidate the physical working mechanism in non-fullerene-based photovoltaic devices.

Constant Electricity Generation in Nanostructured Silicon by Evaporation-Driven Water Flow.

Recently, hydrovoltaic technology emerged as a novel renewable energy harvesting method, which dramatically extends the capability to harvest water energy. However, the urgent issue restricting its device performance is poor carrier transport properties of the solid surface if large charged interface is considered simultaneously. Herein, a hydrovoltaic device based on silicon nanowire arrays (SiNWs), which provide large charged surface/volume ratio and excellent carrier transport properties, yields sustained electricity by a carrier concentration gradient induced by evaporation-induced water flow inside nanochannels. The device can yield direct current with a short-circuit current density of over 55 µA cm-2 , which is three orders larger than a previously reported analogous device (approximately 40 nA cm-2 ). Moreover, it exhibits a constant output power density of over 6 µW cm-2 and an open-circuit voltage of up to 400 mV. Our finding may pave a way for developing energy-harvesting devices from ubiquitous evaporation-driven internal water flow in nature with semiconductor material of silicon.

High-Performance Perovskite Light-Emitting Diode with Enhanced Operational Stability Using Lithium Halide Passivation.

Defect passivation has been demonstrated to be effective in improving the radiative recombination of charge carriers in perovskites, and consequently, the device performance of the resultant perovskite light-emitting diodes (LEDs). State-of-the-art useful passivation agents in perovskite LEDs are mostly organic chelating molecules that, however, simultaneously sacrifice the charge-transport properties and thermal stability of the resultant perovskite emissive layers, thereby deteriorating performance, and especially the operational stability of the devices. We demonstrate that lithium halides can efficiently passivate the defects generated by halide vacancies and reduce trap state density, thereby suppressing ion migration in perovskite films. Efficient green perovskite LEDs based on all-inorganic CsPbBr3 perovskite with a peak external quantum efficiency of 16.2 %, as well as a high maximum brightness of 50 270 cd m-2 , are achieved. Moreover, the device shows decent stability even under a brightness of 104  cd m-2 . We highlight the universal applicability of defect passivation using lithium halides, which enabled us to improve the efficiency of blue and red perovskite LEDs.

General Mild Reaction Creates Highly Luminescent Organic-Ligand-Lacking Halide Perovskite Nanocrystals for Efficient Light-Emitting Diodes.

The presence of labile bulky insulating hydrocarbon ligands in halide perovskite nanocrystals (NCs) passivates surface traps but concurrently makes charge transport difficult in optoelectronic devices. Early efforts routinely rely on the replacement of long-chain ligands with short-chain cousins, leading to notable changes in NC's sizes and photophysical properties and thus making it hard to obtain devices with nearly designed emissions. Here we report a general solution-phase ligand-exchange strategy to produce organic-ligand-lacking halide perovskite NCs with high photoluminescence (PL) quantum yields and good stability in ambient air. We demonstrate that the ligand exchange can be achieved by a well-controlled mild reaction of thionyl halide with the carboxylic and amine groups on the NC's surface, resulting in nearly dry NCs with well-passivated surfaces and almost unaltered emission characteristics. Consequently, we achieve exceptionally high-performance blue perovskite NC light-emitting diodes (LEDs) with an external quantum efficiency of up to 1.35% and an extremely narrow full width at half-maximum of 14.6 nm. Our work provides a systematic framework for preparing high-quality organic-ligand-lacking perovskite NC inks that can be directly cast as films featuring effective charge transport, thereby providing the foundation for further development of a wide range of efficient perovskite optoelectronic devices.

Air-Processed, Stable Organic Solar Cells with High Power Conversion Efficiency of 7.41.

High efficiency, excellent stability, and air processability are all important factors to consider in endeavoring to push forward the real-world application of organic solar cells. Herein, an air-processed inverted photovoltaic device built upon a low-bandgap, air-stable, phenanthridinone-based ter-polymer (C150 H218 N6 O6 S4 )n (PDPPPTD) and [6,6]-phenyl-C61 -butyric acid methyl ester (PC61 BM) without involving any additive engineering processes yields a high efficiency of 6.34%. The PDPPPTD/PC61 BM devices also exhibit superior thermal stability and photo-stability as well as long-term stability in ambient atmosphere without any device encapsulation, which show less performance decay as compared to most of the reported organic solar cells. In view of their great potential, solvent additive engineering via adding p-anisaldehyde (AA) is attempted, leading to a further improved efficiency of 7.41%, one of the highest efficiencies for all air-processed and stable organic photovoltaic devices. Moreover, the device stability under different ambient conditions is also further improved with the AA additive engineering. Various characterizations are conducted to probe the structural, morphology, and chemical information in order to correlate the structure with photovoltaic performance. This work paves a way for developing a new generation of air-processable organic solar cells for possible commercial application.

Interfacial Synthesis of Highly Stable CsPbX3/Oxide Janus Nanoparticles.

The poor stability of CsPbX3 (X = Cl, Br, I) nanocrystals (NCs) has severely impeded their practical applications. Although there are some successful examples on encapsulating multiple CsPbX3 NCs into an oxide or polymer matrix, it has remained a serious challenge for the surface modification/encapsulation using oxides or polymers at a single particle level. In this work, monodisperse CsPbX3/SiO2 and CsPbBr3/Ta2O5 Janus nanoparticles were successfully prepared by combining a water-triggered transformation process and a sol-gel method. The CsPbBr3/SiO2 NCs exhibited a photoluminescence quantum yield of 80% and a lifetime of 19.8 ns. The product showed dramatically improved stability against destruction by air, water, and light irradiation. Upon continuous irradiation by intense UV light for 10 h, a film of the CsPbBr3/SiO2 Janus NCs showed only a slight drop (2%) in the PL intensity, while a control sample of unmodified CsPbBr3 NCs displayed a 35% drop. We further highlighted the advantageous features of the CsPbBr3/SiO2 NCs in practical applications by using them as the green light source for the fabrication of a prototype white light emitting diode, and demonstrated a wide color gamut covering up to 138% of the National Television System Committee standard. This work not only provides a novel approach for the surface modification of individual CsPbX3 NCs but also helps to address the challenging stability issue; therefore, it has an important implication toward their practical applications.

Colloidal metal oxide nanocrystals as charge transporting layers for solution-processed light-emitting diodes and solar cells.

Colloidal metal oxide nanocrystals offer a unique combination of excellent low-temperature solution processability, rich and tuneable optoelectronic properties and intrinsic stability, which makes them an ideal class of materials as charge transporting layers in solution-processed light-emitting diodes and solar cells. Developing new material chemistry and custom-tailoring processing and properties of charge transporting layers based on oxide nanocrystals hold the key to boosting the efficiency and lifetime of all-solution-processed light-emitting diodes and solar cells, and thereby realizing an unprecedented generation of high-performance, low-cost, large-area and flexible optoelectronic devices. This review aims to bridge two research fields, chemistry of colloidal oxide nanocrystals and interfacial engineering of optoelectronic devices, focusing on the relationship between chemistry of colloidal oxide nanocrystals, processing and properties of charge transporting layers and device performance. Synthetic chemistry of colloidal oxide nanocrystals, ligand chemistry that may be applied to colloidal oxide nanocrystals and chemistry associated with post-deposition treatments are discussed to highlight the ability of optimizing processing and optoelectronic properties of charge transporting layers. Selected examples of solution-processed solar cells and light-emitting diodes with oxide-nanocrystal charge transporting layers are examined. The emphasis is placed on the correlation between the properties of oxide-nanocrystal charge transporting layers and device performance. Finally, three major challenges that need to be addressed in the future are outlined. We anticipate that this review will spur new material design and simulate new chemistry for colloidal oxide nanocrystals, leading to charge transporting layers and solution-processed optoelectronic devices beyond the state-of-the-art.

A Uniform Linear Multi-Coil Array-Based Borehole Transient Electromagnetic System for Non-Destructive Evaluations of Downhole Casings.

Borehole transient electromagnetic (TEM) techniques have been proven to be efficient for nondestructive evaluations (NDEs) of metal casings using eddy-current properties. However, physical limitations and bad borehole conditions restrict the use of eddy-current sensors, which makes downhole casing inspections very different from those of conventional NDE systems. In this paper, we present a uniform linear multi-coil array-based borehole TEM system for NDEs of downhole casings. On the basis of the borehole TEM signal model, a numerical multi-coil array approach using the Gauss⁻Legendre quadrature is derived. The TEM response can be divided into two independent parts related to the transmitting-receiving distance (TRD) and the observation time and casing thickness. Using this property, the signal received by the multi-coil array is weighted to cancel the influence of the TRDs of the different array elements to obtain the optimal response according to the linearly constrained minimum variance criterion, which can be shown to be identical to that of achieving the maximum signal-to-noise ratio. The effectiveness of the proposed method was verified by applying the uniform linear multi-coil array to a borehole TEM system for NDEs of oil-well casings. Field experiments were conducted, and the results demonstrate the effectiveness of the proposed method.

From Nonluminescent Cs4PbX6 (X = Cl, Br, I) Nanocrystals to Highly Luminescent CsPbX3 Nanocrystals: Water-Triggered Transformation through a CsX-Stripping Mechanism.

We report a novel CsX-stripping mechanism that enables the efficient chemical transformation of nonluminescent Cs4PbX6 (X = Cl, Br, I) nanocrystals (NCs) to highly luminescent CsPbX3 NCs. During the transformation, Cs4PbX6 NCs dispersed in a nonpolar solvent are converted into CsPbX3 NCs by stripping CsX through an interfacial reaction with water in a different phase. This process takes advantage of the high solubility of CsX in water as well as the ionic nature and high ion diffusion property of Cs4PbX6 NCs, and produces monodisperse and air-stable CsPbX3 NCs with controllable halide composition, tunable emission wavelength covering the full visible range, narrow emission width, and high photoluminescent quantum yield (up to 75%). An additional advantage is that this is a clean synthesis as Cs4PbX6 NCs are converted into CsPbX3 NCs in the nonpolar phase while the byproduct of CsX is formed in water that could be easily separated from the organic phase. The as-prepared CsPbX3 NCs show enhanced stability against moisture because of the passivated surface. Our finding not only provides a new pathway for the preparation of highly luminescent CsPbX3 NCs but also adds insights into the chemical transformation behavior and stabilization mechanism of these emerging perovskite nanocrystals.

Near Full-Composition-Range High-Quality GaAs1-xSbx Nanowires Grown by Molecular-Beam Epitaxy.

Here we report on the Ga self-catalyzed growth of near full-composition-range energy-gap-tunable GaAs1-xSbx nanowires by molecular-beam epitaxy. GaAs1-xSbx nanowires with different Sb content are systematically grown by tuning the Sb and As fluxes, and the As background. We find that GaAs1-xSbx nanowires with low Sb content can be grown directly on Si(111) substrates (0 ≤ x ≤ 0.60) and GaAs nanowire stems (0 ≤ x ≤ 0.50) by tuning the Sb and As fluxes. To obtain GaAs1-xSbx nanowires with x ranging from 0.60 to 0.93, we grow the GaAs1-xSbx nanowires on GaAs nanowire stems by tuning the As background. Photoluminescence measurements confirm that the emission wavelength of the GaAs1-xSbx nanowires is tunable from 844 nm (GaAs) to 1760 nm (GaAs0.07Sb0.93). High-resolution transmission electron microscopy images show that the grown GaAs1-xSbx nanowires have pure zinc-blende crystal structure. Room-temperature Raman spectra reveal a redshift of the optical phonons in the GaAs1-xSbx nanowires with x increasing from 0 to 0.93. Field-effect transistors based on individual GaAs1-xSbx nanowires are fabricated, and rectifying behavior is observed in devices with low Sb content, which disappears in devices with high Sb content. The successful growth of high-quality GaAs1-xSbx nanowires with near full-range bandgap tuning may speed up the development of high-performance nanowire devices based on such ternaries.

Silicon Nanowire/Polymer Hybrid Solar Cell-Supercapacitor: A Self-Charging Power Unit with a Total Efficiency of 10.5.

An integrated self-charging power unit, combining a hybrid silicon nanowire/polymer heterojunction solar cell with a polypyrrole-based supercapacitor, has been demonstrated to simultaneously harvest solar energy and store it. By efficiency enhancement of the hybrid nanowire solar cells and a dual-functional titanium film serving as conjunct electrode of the solar cell and supercapacitor, the integrated system is able to yield a total photoelectric conversion to storage efficiency of 10.5%, which is the record value in all the integrated solar energy conversion and storage system. This system may not only serve as a buffer that diminishes the solar power fluctuations from light intensity, but also pave its way toward cost-effective high efficiency self-charging power unit. Finally, an integrated device based on ultrathin Si substrate is demonstrated to expand its feasibility and potential application in flexible energy conversion and storage devices.

Improving the Stability and Size Tunability of Cesium Lead Halide Perovskite Nanocrystals Using Trioctylphosphine Oxide as the Capping Ligand.

Recently, all-inorganic cesium lead halide (CsPbX3, X = Cl, Br, and I) nanocrystals (NCs) have drawn wide attention because of their excellent optoelectronic properties and potential applications. However, one of the most significant challenges of such NCs is their low stability against protonic solvents. In this work, we demonstrate that by incorporating a highly branched capping ligand, trioctylphosphine oxide (TOPO), into the traditional oleic acid/oleylamine system, monodisperse CsPbX3 NCs with excellent optoelectronic properties can be achieved at elevated temperatures (up to 260 °C). The size of such NCs can be varied in a relatively wide range. The capping of TOPO on NCs has been verified through Fourier transform infrared spectroscopy measurement. More importantly, the presence of TOPO can dramatically improve the stability of CsPbX3 NCs against ethanol treatment. After ethanol treatment for 100 min, the emission intensity of the TOPO-capped sample dropped only 5%, whereas that of non-TOPO-capped NCs dropped up to 86%. This work may shed some light on the preparation and application of CsPbX3 NCs with higher stability.