Enhanced Photodetection Performance of an In Situ Core/Shell Perovskite-MoS2 Phototransistor.

While two-dimensional transition metal dichalcogenides (TMDCs)-based photodetectors offer prospects for high integration density and flexibility, their thinness poses a challenge regarding low light absorption, impacting photodetection sensitivity. Although the integration of TMDCs with metal halide perovskite nanocrystals (PNCs) has been known to be promising for photodetection with a high absorption coefficient of PNCs, the low charge mobility of PNCs delays efficient photocarrier injection into TMDCs. In this study, we integrated MoS2 with in situ formed core/shell PNCs with short ligands that minimize surface defects and enhance photocarrier injection. The PNCs/MoS2 heterostructure efficiently separates electrons and holes by establishing type II band alignment and consequently inducing a photogating effect. The synergistic interplay between photoconductive and photogating effects yields a high responsivity of 2.2 × 106 A/W and a specific detectivity of 9.0 × 1011 Jones. Our findings offer a promising pathway for developing low-cost, high-performance phototransistors leveraging the advantages of two-dimensional (2D) materials.

Spectrally Stable Deep-Blue Light-Emitting Diodes Based on Layer-Transferred Single-Crystalline Ruddlesden-Popper Halide Perovskites.

A novel approach to producing high-color-purity blue-light-emitting diodes based on single-crystalline Ruddlesden-Popper perovskites (RPPs) is reported. The utilization of a pure bromide composition eliminates any possibility of halide segregation, which can otherwise lead to undesired shifts in the emission wavelength or irreversible degradation of the spectral line width. Phase-pure PEA2MAPb2Br7 single crystals with a lateral size exceeding 1 cm2 can be synthesized using the inverse temperature crystallization method. To prepare RPP layers with a thickness of less than 50 nm, we employ a thinning process of the initially thick bulk crystals, followed by a dry-transfer process to place them onto a hole transport layer and an indium-tin-oxide-coated glass substrate. By utilizing polydimethylsiloxane as a handling layer, deformations of the bulk RPP crystal and exfoliated RPP layer, as well as the formation of defects such as pinholes, can be effectively suppressed. Subsequent depositions of an electron transport layer and a metal contact complete the fabrication of electroluminescence (EL) devices. The EL devices utilizing the single-crystalline RPP demonstrate excellent spectral stability across a broad range of the applied bias voltage spanning from 4.5 to 10 V, exhibiting a significantly narrow line width of 14 nm at an emission wavelength of 440 nm that can potentially cover 99.3% of the Rec. 2020 color gamut. The sharp EL emission spectrum can be effectively preserved, avoiding any broadening of the line width, by suppressing Joule heating throughout the device operation, in addition to the intrinsic stability of single-crystalline RPPs.

Pulsed-Mode Metalorganic Vapor-Phase Epitaxy of GaN on Graphene-Coated c-Sapphire for Freestanding GaN Thin Films.

We report the growth of high-quality GaN epitaxial thin films on graphene-coated c-sapphire substrates using pulsed-mode metalorganic vapor-phase epitaxy, together with the fabrication of freestanding GaN films by simple mechanical exfoliation for transferable light-emitting diodes (LEDs). High-quality GaN films grown on the graphene-coated sapphire substrates were easily lifted off by using thermal release tape and transferred onto foreign substrates. Furthermore, we revealed that the pulsed operation of ammonia flow during GaN growth was a critical factor for the fabrication of high-quality freestanding GaN films. These films, exhibiting excellent single crystallinity, were utilized to fabricate transferable GaN LEDs by heteroepitaxially growing InxGa1-xN/GaN multiple quantum wells and a p-GaN layer on the GaN films, showing their potential application in advanced optoelectronic devices.

Remote epitaxial interaction through graphene.

The concept of remote epitaxy involves a two-dimensional van der Waals layer covering the substrate surface, which still enable adatoms to follow the atomic motif of the underlying substrate. The mode of growth must be carefully defined as defects, e.g., pinholes, in two-dimensional materials can allow direct epitaxy from the substrate, which, in combination with lateral epitaxial overgrowth, could also form an epilayer. Here, we show several unique cases that can only be observed for remote epitaxy, distinguishable from other two-dimensional material-based epitaxy mechanisms. We first grow BaTiO3 on patterned graphene to establish a condition for minimizing epitaxial lateral overgrowth. By observing entire nanometer-scale nuclei grown aligned to the substrate on pinhole-free graphene confirmed by high-resolution scanning transmission electron microscopy, we visually confirm that remote epitaxy is operative at the atomic scale. Macroscopically, we also show variations in the density of GaN microcrystal arrays that depend on the ionicity of substrates and the number of graphene layers.

Overcoming Charge Confinement in Perovskite Nanocrystal Solar Cells.

The small nanoparticle size and long-chain ligands in colloidal metal halide perovskite quantum dots (PeQDs) cause charge confinement, which impedes exciton dissociation and carrier extraction in PeQD solar cells, so they have low short-circuit current density Jsc , which impedes further increases in their power conversion efficiency (PCE). Here, a re-assembling process (RP) is developed for perovskite nanocrystalline (PeNC) films made of colloidal perovskite nanocrystals to increase Jsc in PeNC solar cells. The RP of PeNC films increases their crystallite size and eliminates long-chain ligands, and thereby overcomes the charge confinement in PeNC films. These changes facilitate exciton dissociation and increase carrier extraction in PeNC solar cells. By use of this method, the gradient-bandgap PeNC solar cells achieve a Jsc = 19.30 mA cm-2 without compromising the photovoltage, and yield a high PCE of 16.46% with negligible hysteresis and good stability. This work provides a new strategy to process PeNC films and pave the way for high performance PeNC optoelectronic devices.

Structural Isomer of Fluorinated Ruddlesden-Popper Perovskites Toward Efficient and Stable 2D/3D Perovskite Solar Cells.

Defect passivation using two-dimensional (2D)-layered perovskites with organic spacers on 3D bulk perovskites has been proposed as an effective strategy to improve perovskite solar cell stability and efficiency. Specifically, fluorination of the organic spacers has been employed due to the resulting hydrophobic nature and the defect passivation characteristics. In addition to the type of functional groups attached to the spacer molecules, conformational changes of fluorine isomers on layered perovskites can provide an extended strategy to control a variety of opto-electrical properties related to the interlayer spacing. As a model system for the structural isomer of fluorinated spacers, meta-CF3 and para-CF3 groups anchored to phenethylammonium iodide (PEAI) spacer molecules are employed to synthesize 2D perovskites and to investigate their full potential as an interfacial modifier for perovskite solar cells. The fluorination position change leads to altered opto-electrical characteristics in layered perovskites. Although they possess identical functional groups, the different orientations of the functional groups used in the perovskite layer deposited on the 3D perovskite absorber result in distinct electrical properties of 2D/3D heterostructures due to dissimilar intermolecular interactions. The 2D perovskite with meta-CF3-PEAI spacers exhibits an enhancement of the charge transport in the out-of-plane orientation and an improved suppression of the trap states of 3D perovskites while also providing a more favorable energy alignment for efficient charge transfers. Theoretical simulations are consistent with the experimental results. The structural isomers of fluorination anchoring to spacer cations alter the structural configuration of the spacer as well as the interlayer spacing that can improve the performance and the stability of 2D/3D perovskite solar cells.

Chip-less wireless electronic skins by remote epitaxial freestanding compound semiconductors.

Recent advances in flexible and stretchable electronics have led to a surge of electronic skin (e-skin)-based health monitoring platforms. Conventional wireless e-skins rely on rigid integrated circuit chips that compromise the overall flexibility and consume considerable power. Chip-less wireless e-skins based on inductor-capacitor resonators are limited to mechanical sensors with low sensitivities. We report a chip-less wireless e-skin based on surface acoustic wave sensors made of freestanding ultrathin single-crystalline piezoelectric gallium nitride membranes. Surface acoustic wave-based e-skin offers highly sensitive, low-power, and long-term sensing of strain, ultraviolet light, and ion concentrations in sweat. We demonstrate weeklong monitoring of pulse. These results present routes to inexpensive and versatile low-power, high-sensitivity platforms for wireless health monitoring devices.

Semitransparent Perovskite Solar Cells with Enhanced Light Utilization Efficiencies by Transferable Ag Nanogrid Electrodes.

Solar cells that are semitransparent and highly efficient can find diverse applications in automobile windows, building walls, and wearable devices. Here, we present a semitransparent perovskite thin-film solar cell with an Ag nanogrid transparent electrode, where electrospun poly(ethylene oxide) (PEO) nanofibers are used as an etching mask. Directional electrospinning has allowed us to obtain a grid-shaped electrode of well-aligned Ag nanogrids. The performance of transparent electrodes can be controlled by the electrospinning conditions and the choice of substrate materials. We theoretically analyze the transmittance and sheet resistance of the electrode. Furthermore, transferable Ag nanogrid transparent electrodes are fabricated on poly(dimethylsiloxane) (PDMS) substrates for application in semitransparent perovskite solar cells. Using an electrode that shows a high transmittance (92.7%) with a low sheet resistance (18.0 Ω·sq-1), a semitransparent perovskite thin-film solar cell demonstrates average visible wavelength transmittance, power conversion efficiency, and light utilization efficiency rates as high as 25.2, 12.7, and 3.21%, respectively.

Scalable High-Efficiency Bi-Facial Solar Evaporator with a Dendritic Copper Oxide Wick.

Solar thermal distillation is a promising way to harvest clean water due to its sustainability. However, the energy density of solar irradiation inevitably demands scalability of the systems. To realize practical applications, it is highly desirable to fabricate meter-scale solar evaporator panels with high capillary performance as well as optical absorptance using scalable and high-throughput fabrication methods. Here, we demonstrate a truly scalable fabrication process for a bi-facial solar evaporator with copper oxide dendrites via the hydrogen bubble templated electrochemical deposition technique. Furthermore, we construct a theoretical model combining capillarity and evaporative mass transfer, which leads to optimal operation conditions and wick characteristics, including superhydrophilicity, extreme capillary performance, and omni-angular high optical absorptance. The fabricated porous surfaces with excellent capillary performance and productivity provide a pathway toward a highly efficient bi-facial solar evaporator panel with meter-level scalability.

Carrier-resolved photo-Hall effect.

The fundamental parameters of majority and minority charge carriers-including their type, density and mobility-govern the performance of semiconductor devices yet can be difficult to measure. Although the Hall measurement technique is currently the standard for extracting the properties of majority carriers, those of minority carriers have typically only been accessible through the application of separate techniques. Here we demonstrate an extension to the classic Hall measurement-a carrier-resolved photo-Hall technique-that enables us to simultaneously obtain the mobility and concentration of both majority and minority carriers, as well as the recombination lifetime, diffusion length and recombination coefficient. This is enabled by advances in a.c.-field Hall measurement using a rotating parallel dipole line system and an equation, ΔµH = d(σ2H)/dσ, which relates the hole-electron Hall mobility difference (ΔµH), the conductivity (σ) and the Hall coefficient (H). We apply this technique to various solar absorbers-including high-performance lead-iodide-based perovskites-and demonstrate simultaneous access to majority and minority carrier parameters and map the results against varying light intensities. This information, which is buried within the photo-Hall measurement1,2, had remained inaccessible since the original discovery of the Hall effect in 18793. The simultaneous measurement of majority and minority carriers should have broad applications, including in photovoltaics and other optoelectronic devices.

Ultrathin high band gap solar cells with improved efficiencies from the world's oldest photovoltaic material.

Selenium was used in the first solid state solar cell in 1883 and gave early insights into the photoelectric effect that inspired Einstein's Nobel Prize work; however, the latest efficiency milestone of 5.0% was more than 30 years ago. The recent surge of interest towards high-band gap absorbers for tandem applications led us to reconsider this attractive 1.95 eV material. Here, we show completely redesigned selenium devices with improved back and front interfaces optimized through combinatorial studies and demonstrate record open-circuit voltage (V OC) of 970 mV and efficiency of 6.5% under 1 Sun. In addition, Se devices are air-stable, non-toxic, and extremely simple to fabricate. The absorber layer is only 100 nm thick, and can be processed at 200 ˚C, allowing temperature compatibility with most bottom substrates or sub-cells. We analyze device limitations and find significant potential for further improvement making selenium an attractive high-band-gap absorber for multi-junction device applications.Wide band gap semiconductors are important for the development of tandem photovoltaics. By introducing buffer layers at the front and rear side of solar cells based on selenium; Todorov et al., reduce interface recombination losses to achieve photoconversion efficiencies of 6.5%.

Unveiling the carrier transport mechanism in epitaxial graphene for forming wafer-scale, single-domain graphene.

Graphene epitaxy on the Si face of a SiC wafer offers monolayer graphene with unique crystal orientation at the wafer-scale. However, due to carrier scattering near vicinal steps and excess bilayer stripes, the size of electrically uniform domains is limited to the width of the terraces extending up to a few microns. Nevertheless, the origin of carrier scattering at the SiC vicinal steps has not been clarified so far. A layer-resolved graphene transfer (LRGT) technique enables exfoliation of the epitaxial graphene formed on SiC wafers and transfer to flat Si wafers, which prepares crystallographically single-crystalline monolayer graphene. Because the LRGT flattens the deformed graphene at the terrace edges and permits an access to the graphene formed at the side wall of vicinal steps, components that affect the mobility of graphene formed near the vicinal steps of SiC could be individually investigated. Here, we reveal that the graphene formed at the side walls of step edges is pristine, and scattering near the steps is mainly attributed by the deformation of graphene at step edges of vicinalized SiC while partially from stripes of bilayer graphene. This study suggests that the two-step LRGT can prepare electrically single-domain graphene at the wafer-scale by removing the major possible sources of electrical degradation.

Ag2ZnSn(S,Se)4: A highly promising absorber for thin film photovoltaics.

The growth in efficiency of earth-abundant kesterite Cu2ZnSn(S,Se)4 (CZTSSe) solar cells has slowed, due in part to the intrinsic limitations imposed by the band tailing attributed primarily to I-II antisite exchange. In this study, density functional theory simulations show that when Ag is substituted for Cu to form kesterite Ag2ZnSnSe4 (AZTSe), the I-II isolated antisite formation energy becomes 3.7 times greater than in CZTSSe, resulting in at least an order of magnitude reduction in I-II antisite density. Experimental evidence of an optoelectronically improved material is also provided. Comparison of the low-temperature photoluminescence (PL) structure of Cu(In,Ga)Se2 (CIGSe), CZTSSe, and AZTSe shows that AZTSe has a shallow defect structure with emission significantly closer to the band edge than CZTSe. Existence of suppressed band tailing is found in the proximity of the room-temperature PL peak of AZTSe to its measured band gap. The results are consistent with AZTSe being a promising alternative to CZTSSe and CIGSe for thin film photovoltaics.

Phase transition-induced band edge engineering of BiVO4 to split pure water under visible light.

Through phase transition-induced band edge engineering by dual doping with In and Mo, a new greenish BiVO4 (Bi1-XInXV1-XMoXO4) is developed that has a larger band gap energy than the usual yellow scheelite monoclinic BiVO4 as well as a higher (more negative) conduction band than H(+)/H2 potential [0 VRHE (reversible hydrogen electrode) at pH 7]. Hence, it can extract H2 from pure water by visible light-driven overall water splitting without using any sacrificial reagents. The density functional theory calculation indicates that In(3+)/Mo(6+) dual doping triggers partial phase transformation from pure monoclinic BiVO4 to a mixture of monoclinic BiVO4 and tetragonal BiVO4, which sequentially leads to unit cell volume growth, compressive lattice strain increase, conduction band edge uplift, and band gap widening.

10.5% efficient polymer and amorphous silicon hybrid tandem photovoltaic cell.

Thin-film solar cells made with amorphous silicon (a-Si:H) or organic semiconductors are considered as promising renewable energy sources due to their low manufacturing cost and light weight. However, the efficiency of single-junction a-Si:H or organic solar cells is typically <10%, insufficient for achieving grid parity. Here we demonstrate an efficient double-junction photovoltaic cell by employing an a-Si:H film as a front sub-cell and a low band gap polymer:fullerene blend film as a back cell on planar glass substrates. Monolithic integration of 6.0% efficienct a-Si:H and 7.5% efficient polymer:fullerene blend solar cells results in a power conversion efficiency of 10.5%. Such high-efficiency thin-film tandem cells can be achieved by optical management and interface engineering of fully optimized high-performance front and back cells without sacrificing photovoltaic performance in both cells.

High efficiency Cu2ZnSn(S,Se)4 solar cells by applying a double In2S3/CdS emitter.

High-efficiency Cu2ZnSn(S,Se)4 solar cells are reported by applying In2S3/CdS double emitters. This new structure offers a high doping concentration within the Cu2ZnSn(S,Se)4 solar cells, resulting in a substantial enhancement in open-circuit voltage. The 12.4% device is obtained with a record open-circuit voltage deficit of 593 mV.

3.88% efficient tin sulfide solar cells using congruent thermal evaporation.

Tin sulfide (SnS), as a promising absorber material in thin-film photovoltaic devices, is described. Here, it is confirmed that SnS evaporates congruently, which provides facile composition control akin to cadmium telluride. A SnS heterojunction solar cell is demons trated, which has a power conversion efficiency of 3.88% (certified), and an empirical loss analysis is presented to guide further performance improvements.

Atomic layer deposited gallium oxide buffer layer enables 1.2 V open-circuit voltage in cuprous oxide solar cells.

The power conversion efficiency of solar cells based on copper (I) oxide (Cu2 O) is enhanced by atomic layer deposition of a thin gallium oxide (Ga2 O3 ) layer. By improving band-alignment and passivating interface defects, the device exhibits an open-circuit voltage of 1.20 V and an efficiency of 3.97%, showing potential of over 7% efficiency.

High photocurrent in silicon photoanodes catalyzed by iron oxide thin films for water oxidation.

Silicon splits: The application of silicon to water oxidation is limited due to unfavorable interface properties. However, these can be circumvented by using a high-performance silicon photoanode with a catalytically active iron oxide thin film (see picture). This approach results in photocurrents as high as 17 mA cm(-2) under 1 sun and zero overpotential conditions.