Showing papers by "King Abdullah University of Science and Technology published in 2015"
TL;DR: An antisolvent vapor-assisted crystallization approach is reported that enables us to create sizable crack-free MAPbX3 single crystals with volumes exceeding 100 cubic millimeters, which enabled a detailed characterization of their optical and charge transport characteristics.
Abstract: The fundamental properties and ultimate performance limits of organolead trihalide MAPbX3 (MA = CH3NH3(+); X = Br(-) or I(-)) perovskites remain obscured by extensive disorder in polycrystalline MAPbX3 films. We report an antisolvent vapor-assisted crystallization approach that enables us to create sizable crack-free MAPbX3 single crystals with volumes exceeding 100 cubic millimeters. These large single crystals enabled a detailed characterization of their optical and charge transport characteristics. We observed exceptionally low trap-state densities on the order of 10(9) to 10(10) per cubic centimeter in MAPbX3 single crystals (comparable to the best photovoltaic-quality silicon) and charge carrier diffusion lengths exceeding 10 micrometers. These results were validated with density functional theory calculations.
3,939 citations
07 Jun 2015
TL;DR: This paper introduces ActivityNet, a new large-scale video benchmark for human activity understanding that aims at covering a wide range of complex human activities that are of interest to people in their daily living.
Abstract: In spite of many dataset efforts for human action recognition, current computer vision algorithms are still severely limited in terms of the variability and complexity of the actions that they can recognize. This is in part due to the simplicity of current benchmarks, which mostly focus on simple actions and movements occurring on manually trimmed videos. In this paper we introduce ActivityNet, a new large-scale video benchmark for human activity understanding. Our benchmark aims at covering a wide range of complex human activities that are of interest to people in their daily living. In its current version, ActivityNet provides samples from 203 activity classes with an average of 137 untrimmed videos per class and 1.41 activity instances per video, for a total of 849 video hours. We illustrate three scenarios in which ActivityNet can be used to compare algorithms for human activity understanding: untrimmed video classification, trimmed activity classification and activity detection.
2,158 citations
TL;DR: Detailed kinetic analyses of aqueous electrochemistry involving gaseous H2 or O2 involving hydrogen evolution reaction, hydrogen oxidation reaction, oxygen reduction reaction, and oxygen evolution reaction are revisited and the limitation of Butler-Volmer expression in electrocatalysis is discussed.
Abstract: Microkinetic analyses of aqueous electrochemistry involving gaseous H2 or O2, i.e., hydrogen evolution reaction (HER), hydrogen oxidation reaction (HOR), oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), are revisited. The Tafel slopes used to evaluate the rate determining steps generally assume extreme coverage of the adsorbed species (θ ≈ 0 or ≈1), although, in practice, the slopes are coverage-dependent. We conducted detailed kinetic analyses describing the coverage-dependent Tafel slopes for the aforementioned reactions. Our careful analyses provide a general benchmark for experimentally observed Tafel slopes that can be assigned to specific rate determining steps. The Tafel analysis is a powerful tool for discussing the rate determining steps involved in electrocatalysis, but our study also demonstrated that overly simplified assumptions led to an inaccurate description of the surface electrocatalysis. Additionally, in many studies, Tafel analyses have been performed in conjunction with the Butler-Volmer equation, where its applicability regarding only electron transfer kinetics is often overlooked. Based on the derived kinetic description of the HER/HOR as an example, the limitation of Butler-Volmer expression in electrocatalysis is also discussed in this report.
1,830 citations
TL;DR: Bychkov and Rashba as discussed by the authors introduced a simple form of spin-orbit coupling to explain the peculiarities of electron spin resonance in two-dimensional semiconductors, which has inspired a vast number of predictions, discoveries and innovative concepts far beyond semiconductor devices.
Abstract: In 1984, Bychkov and Rashba introduced a simple form of spin-orbit coupling to explain the peculiarities of electron spin resonance in two-dimensional semiconductors. Over the past 30 years, Rashba spin-orbit coupling has inspired a vast number of predictions, discoveries and innovative concepts far beyond semiconductors. The past decade has been particularly creative, with the realizations of manipulating spin orientation by moving electrons in space, controlling electron trajectories using spin as a steering wheel, and the discovery of new topological classes of materials. This progress has reinvigorated the interest of physicists and materials scientists in the development of inversion asymmetric structures, ranging from layered graphene-like materials to cold atoms. This Review discusses relevant recent and ongoing realizations of Rashba physics in condensed matter.
1,533 citations
TL;DR: A rapid crystal growth process to obtain MAPbX3 single crystals, an order of magnitude faster than previous reports, and the grown crystals exhibit transport properties and trap densities comparable to the highest quality MAPb X3 reported to date.
Abstract: Single crystals of methylammonium lead trihalide perovskites (MAPbX3; MA=CH3NH3+, X=Br− or I−) have shown remarkably low trap density and charge transport properties; however, growth of such high-quality semiconductors is a time-consuming process. Here we present a rapid crystal growth process to obtain MAPbX3 single crystals, an order of magnitude faster than previous reports. The process is based on our observation of the substantial decrease of MAPbX3 solubility, in certain solvents, at elevated temperatures. The crystals can be both size- and shape-controlled by manipulating the different crystallization parameters. Despite the rapidity of the method, the grown crystals exhibit transport properties and trap densities comparable to the highest quality MAPbX3 reported to date. The phenomenon of inverse or retrograde solubility and its correlated inverse temperature crystallization strategy present a major step forward for advancing the field on perovskite crystallization. Hybrid perovskites are a promising class of materials for photovoltaic applications. Here, addressing the need for high-quality hybrid perovskite materials, the authors achieve the rapid growth of hybrid perovskite single crystals of high quality by inverse temperature crystallization.
1,448 citations
TL;DR: A comprehensive joint experiment–theory investigation of point defects in monolayer molybdenum disulphide prepared by mechanical exfoliation, physical and chemical vapour deposition and influence of defects on electronic structure and charge-carrier mobility is predicted by calculation and observed by electric transport measurement.
Abstract: Defects usually play an important role in tailoring various properties of two-dimensional materials. Defects in two-dimensional monolayer molybdenum disulphide may be responsible for large variation of electric and optical properties. Here we present a comprehensive joint experiment–theory investigation of point defects in monolayer molybdenum disulphide prepared by mechanical exfoliation, physical and chemical vapour deposition. Defect species are systematically identified and their concentrations determined by aberration-corrected scanning transmission electron microscopy, and also studied by ab-initio calculation. Defect density up to 3.5 × 1013 cm−2 is found and the dominant category of defects changes from sulphur vacancy in mechanical exfoliation and chemical vapour deposition samples to molybdenum antisite in physical vapour deposition samples. Influence of defects on electronic structure and charge-carrier mobility are predicted by calculation and observed by electric transport measurement. In light of these results, the growth of ultra-high-quality monolayer molybdenum disulphide appears a primary task for the community pursuing high-performance electronic devices. Imperfections can greatly alter a material’s properties. Here, the authors investigate the influence of point defects on the electronic structure, charge-carrier mobility and optical absorption of molybdenum disulphide prepared by mechanical exfoliation, physical and chemical vapour deposition.
1,109 citations
TL;DR: A combined theoretical and experimental study is presented to establish ternary pyrite-type cobalt phosphosulphide (CoPS) as a high-performance Earth-abundant catalyst for electrochemical and photoelectrochemical hydrogen production.
Abstract: The scalable and sustainable production of hydrogen fuel through water splitting demands efficient and robust Earth-abundant catalysts for the hydrogen evolution reaction (HER). Building on promising metal compounds with high HER catalytic activity, such as pyrite structure cobalt disulphide (CoS2), and substituting non-metal elements to tune the hydrogen adsorption free energy could lead to further improvements in catalytic activity. Here we present a combined theoretical and experimental study to establish ternary pyrite-type cobalt phosphosulphide (CoPS) as a high-performance Earth-abundant catalyst for electrochemical and photoelectrochemical hydrogen production. Nanostructured CoPS electrodes achieved a geometrical catalytic current density of 10 mA cm(-2) at overpotentials as low as 48 mV, with outstanding long-term operational stability. Integrated photocathodes of CoPS on n(+)-p-p(+) silicon micropyramids achieved photocurrents up to 35 mA cm(-2) at 0 V versus the reversible hydrogen electrode (RHE), onset photovoltages as high as 450 mV versus RHE, and the most efficient solar-driven hydrogen generation from Earth-abundant systems.
1,094 citations
TL;DR: This paper presents a meta-modelling system that automates the very labor-intensive and therefore time-heavy and expensive and therefore expensive and expensive process of designing and installing solar panels.
Abstract: Graham H. Carey,† Ahmed L. Abdelhady,‡ Zhijun Ning, Susanna M. Thon, Osman M. Bakr,‡ and Edward H. Sargent*,† †Department of Electrical and Computer Engineering, University of Toronto, 10 King’s College Road, Toronto, Ontario M5S 3G4, Canada ‡Division of Physical Sciences and Engineering, Solar & Photovoltaics Engineering Center, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia School of Physical Science and Technology, ShanghaiTech University, 100 Haike Road, Shanghai 201210, China Department of Electrical and Computer Engineering, Johns Hopkins University, 3400 North Charles Street, Baltimore, Maryland 21218, United States
1,036 citations
TL;DR: The motivation to replace fullerene acceptors stems from their synthetic inflexibility, leading to constraints in manipulating frontier energy levels, as well as poor absorption in the solar spectrum range, and an inherent tendency to undergo postfabrication crystallization, resulting in device instability.
Abstract: ConspectusThe active layer in a solution processed organic photovoltaic device comprises a light absorbing electron donor semiconductor, typically a polymer, and an electron accepting fullerene acceptor. Although there has been huge effort targeted to optimize the absorbing, energetic, and transport properties of the donor material, fullerenes remain as the exclusive electron acceptor in all high performance devices. Very recently, some new non-fullerene acceptors have been demonstrated to outperform fullerenes in comparative devices. This Account describes this progress, discussing molecular design considerations and the structure–property relationships that are emerging.The motivation to replace fullerene acceptors stems from their synthetic inflexibility, leading to constraints in manipulating frontier energy levels, as well as poor absorption in the solar spectrum range, and an inherent tendency to undergo postfabrication crystallization, resulting in device instability. New acceptors have to address ...
1,026 citations
TL;DR: The epitaxial growth process offers a controllable method to obtain lateral heterojunction with an atomically sharp interface, and direct growth favors the thermodynamically preferred TMDC alloys.
Abstract: Two-dimensional transition metal dichalcogenides (TMDCs) such as molybdenum sulfide MoS2 and tungsten sulfide WSe2 have potential applications in electronics because they exhibit high on-off current ratios and distinctive electro-optical properties. Spatially connected TMDC lateral heterojunctions are key components for constructing monolayer p-n rectifying diodes, light-emitting diodes, photovoltaic devices, and bipolar junction transistors. However, such structures are not readily prepared via the layer-stacking techniques, and direct growth favors the thermodynamically preferred TMDC alloys. We report the two-step epitaxial growth of lateral WSe2-MoS2 heterojunction, where the edge of WSe2 induces the epitaxial MoS2 growth despite a large lattice mismatch. The epitaxial growth process offers a controllable method to obtain lateral heterojunction with an atomically sharp interface.
1,011 citations
TL;DR: This article aims at providing an integration of brain energy metabolism across resolution scales with decisive insights into the understanding of the cellular and molecular bases of the coupling between neuronal activity and energy metabolism.
TL;DR: Self-healing hydrophobic light- to-heat conversion membranes for interfacial solar heating are fabricated by deposition of light-to- Heat conversion material of polypyrrole onto a porous stainless-steel mesh, followed by hydrophilic fluoroalkylsilane modification.
Abstract: Self-healing hydrophobic light-to-heat conversion membranes for interfacial solar heating are fabricated by deposition of light-to-heat conversion material of polypyrrole onto a porous stainless-steel mesh, followed by hydrophobic fluoroalkylsilane modification. The mesh-based membranes spontaneously stay at the water-air interface, collect and convert solar light into heat, and locally heat only the water surface for enhanced evaporation.
TL;DR: In this paper, the effect of post-etch annealing ambient (Ar, N2, N 2/H2, and air) on the structure and electrochemical properties of two-dimensional Ti2CTx MXene nanosheets was investigated in detail.
Abstract: Two-dimensional Ti2CTx MXene nanosheets were prepared by the selective etching of Al layer from Ti2AlC MAX phase using HF treatment. The MXene sheets retained the hexagonal symmetry of the parent Ti2AlC MAX phase. Effect of the postetch annealing ambient (Ar, N2, N2/H2, and air) on the structure and electrochemical properties of the MXene nanosheets was investigated in detail. After annealing in air, the MXene sheets exhibited variations in structure, morphology, and electrochemical properties as compared to HF treated MAX phase. In contrast, samples annealed in Ar, N2, and N2/H2 ambient retained their original morphology. However, a significant improvement in the supercapacitor performance is observed upon heat treatment in Ar, N2, and N2/H2 ambients. When used in symmetric two-electrode configuration, the MXene sample annealed in N2/H2 atmosphere exhibited the best capacitive performance with specific capacitance value (51 F/g at 1A/g) and high rate performance (86%). This improvement in the electrochem...
TL;DR: This tutorial review will introduce the latest development of the synthesis of monolayer TMDs by CVD approaches, and shows great promise to generate high-quality TMD layers with a scalable size, controllable thickness and excellent electronic properties.
Abstract: In recent years there have been many breakthroughs in two-dimensional (2D) nanomaterials, among which the transition metal dichalcogenides (TMDs) attract significant attention owing to their unusual properties associated with their strictly defined dimensionalities. TMD materials with a generalized formula of MX2, where M is a transition metal and X is a chalcogen, represent a diverse and largely untapped source of 2D systems. Semiconducting TMD monolayers such as MoS2, MoSe2, WSe2 and WS2 have been demonstrated to be feasible for future electronics and optoelectronics. The exotic electronic properties and high specific surface areas of 2D TMDs offer unlimited potential in various fields including sensing, catalysis, and energy storage applications. Very recently, the chemical vapour deposition technique (CVD) has shown great promise to generate high-quality TMD layers with a scalable size, controllable thickness and excellent electronic properties. Wafer-scale deposition of mono to few layer TMD films has been obtained. Despite the initial success in the CVD synthesis of TMDs, substantial research studies on extending the methodology open up a new way for substitution doping, formation of monolayer alloys and producing TMD stacking structures or superlattices. In this tutorial review, we will introduce the latest development of the synthesis of monolayer TMDs by CVD approaches.
TL;DR: In this article, the authors discuss the complex network of signaling pathways occurring during PTI, focusing on the involvement of mitogen-activated protein kinases, and discuss the role of the kinases in the defense against pathogen attacks.
TL;DR: This review highlights various design and synthesis approaches toward the construction of ZMOFs, which are metal-organic frameworks (MOFs) with topologies and, in some cases, features akin to traditional inorganic zeolites.
Abstract: This review highlights various design and synthesis approaches toward the construction of ZMOFs, which are metal–organic frameworks (MOFs) with topologies and, in some cases, features akin to traditional inorganic zeolites. The interest in this unique subset of MOFs is correlated with their exceptional characteristics arising from the periodic pore systems and distinctive cage-like cavities, in conjunction with modular intra- and/or extra-framework components, which ultimately allow for tailoring of the pore size, pore shape, and/or properties towards specific applications.
TL;DR: This work shows, for the first time, the energy band structure, charge recombination, and transport properties of CH3NH3PbCl3 single crystals, and builds an efficient visible-blind UV-photodetector, demonstrating its potential in optoelectronic applications.
Abstract: Single crystals of hybrid perovskites have shown remarkably improved physical properties compared to their polycrystalline film counterparts, underscoring their importance in the further development of advanced semiconductor devices. Here we present a new method of growing sizable CH3NH3PbCl3 single crystals based on the retrograde solubility behavior of hybrid perovskites. We show, for the first time, the energy band structure, charge recombination, and transport properties of CH3NH3PbCl3 single crystals. These crystals exhibit trap-state density, charge carrier concentration, mobility, and diffusion length comparable with the best quality crystals of methylammonium lead iodide or bromide perovskites reported so far. The high quality of the crystal along with its suitable optical band gap enabled us to build an efficient visible-blind UV-photodetector, demonstrating its potential in optoelectronic applications.
TL;DR: Large-area planar-integrated films made up of large perovskite single crystals are produced, showing mobility and diffusion length comparable with those of single crystals, and a high-performance light detector is produced.
Abstract: Hybrid perovskites are promising semiconductors for optoelectronic applications. However, they suffer from morphological disorder that limits their optoelectronic properties and, ultimately, device performance. Recently, perovskite single crystals have been shown to overcome this problem and exhibit impressive improvements: low trap density, low intrinsic carrier concentration, high mobility, and long diffusion length that outperform perovskite-based thin films. These characteristics make the material ideal for realizing photodetection that is simultaneously fast and sensitive; unfortunately, these macroscopic single crystals cannot be grown on a planar substrate, curtailing their potential for optoelectronic integration. Here we produce large-area planar-integrated films made up of large perovskite single crystals. These crystalline films exhibit mobility and diffusion length comparable with those of single crystals. Using this technique, we produced a high-performance light detector showing high gain (above 10(4) electrons per photon) and high gain-bandwidth product (above 10(8) Hz) relative to other perovskite-based optical sensors.
TL;DR: It was found that shortening the parent Al-soc-MOF-1 linker resulted in a noticeable enhancement in the working volumetric capacity at specific temperatures and pressures with amply conserved gravimetric uptake/working capacity.
Abstract: The molecular building block approach was employed effectively to construct a series of novel isoreticular, highly porous and stable, aluminum-based metal–organic frameworks with soc topology. From this platform, three compounds were experimentally isolated and fully characterized: namely, the parent Al-soc-MOF-1 and its naphthalene and anthracene analogues. Al-soc-MOF-1 exhibits outstanding gravimetric methane uptake (total and working capacity). It is shown experimentally, for the first time, that the Al-soc-MOF platform can address the challenging Department of Energy dual target of 0.5 g/g (gravimetric) and 264 cm3 (STP)/cm3 (volumetric) methane storage. Furthermore, Al-soc-MOF exhibited the highest total gravimetric and volumetric uptake for carbon dioxide and the utmost total and deliverable uptake for oxygen at relatively high pressures among all microporous MOFs. In order to correlate the MOF pore structure and functionality to the gas storage properties, to better understand the structure–propert...
TL;DR: This review focuses on SL biosynthesis, describes the hormonal and environmental factors that determine this process, and discusses SL transport and downstream signaling as well as the role of SLs in regulating plant development.
Abstract: Strigolactones (SLs) are carotenoid-derived plant hormones and signaling molecules. When released into the soil, SLs indicate the presence of a host to symbiotic fungi and root parasitic plants. In planta, they regulate several developmental processes that adapt plant architecture to nutrient availability. Highly branched/tillered mutants in Arabidopsis, pea, and rice have enabled the identification of four SL biosynthetic enzymes: a cis/trans-carotene isomerase, two carotenoid cleavage dioxygenases, and a cytochrome P450 (MAX1). In vitro and in vivo enzyme assays and analysis of mutants have shown that the pathway involves a combination of new reactions leading to carlactone, which is converted by a rice MAX1 homolog into an SL parent molecule with a tricyclic lactone moiety. In this review, we focus on SL biosynthesis, describe the hormonal and environmental factors that determine this process, and discuss SL transport and downstream signaling as well as the role of SLs in regulating plant development.
TL;DR: Plastic debris in the Mediterranean surface waters was dominated by millimeter-sized fragments, but showed a higher proportion of large plastic objects than that present in oceanic gyres, reflecting the closer connection with pollution sources.
Abstract: Concentrations of floating plastic were measured throughout the Mediterranean Sea to assess whether this basin can be regarded as a great accumulation region of plastic debris. We found that the average density of plastic (1 item per 4 m2), as well as its frequency of occurrence (100% of the sites sampled), are comparable to the accumulation zones described for the five subtropical ocean gyres. Plastic debris in the Mediterranean surface waters was dominated by millimeter-sized fragments, but showed a higher proportion of large plastic objects than that present in oceanic gyres, reflecting the closer connection with pollution sources. The accumulation of floating plastic in the Mediterranean Sea (between 1,000 and 3,000 tons) is likely related to the high human pressure together with the hydrodynamics of this semi-enclosed basin, with outflow mainly occurring through a deep water layer. Given the biological richness and concentration of economic activities in the Mediterranean Sea, the affects of plastic pollution on marine and human life are expected to be particularly frequent in this plastic accumulation region.
TL;DR: In this article, the authors discuss the current development of graphene-based metal and metal oxide nanocomposites, with a detailed account of their synthesis and properties, including their applications in various fields including electronics, electrochemical and electrical fields.
Abstract: Graphene, an atomically thin two-dimensional carbonaceous material, has attracted tremendous attention in the scientific community, due to its exceptional electronic, electrical, and mechanical properties. Indeed, with the recent explosion of methods for a large-scale synthesis of graphene, the number of publications related to graphene and other graphene based materials has increased exponentially. Particularly the development of easy preparation methods for graphene like materials, such as highly reduced graphene oxide (HRG) via reduction of graphite oxide (GO), offers a wide range of possibilities for the preparation of graphene based inorganic nanocomposites by the incorporation of various functional nanomaterials for a variety of applications. In this review, we discuss the current development of graphene based metal and metal oxide nanocomposites, with a detailed account of their synthesis and properties. Specifically, much attention has been given to their wide range of applications in various fields, including electronics, electrochemical and electrical fields. Overall, by the inclusion of various references, this review covers in detail the aspects of graphene-based inorganic nanocomposites.
TL;DR: The phototransistors based on hybrid perovskite films are investigated and provide direct evidence for their superior carrier transport property with ambipolar characteristics and exhibit an ultrafast photoresponse speed of less than 10 μs.
Abstract: Organolead halide perovskites have attracted substantial attention because of their excellent physical properties, which enable them to serve as the active material in emerging hybrid solid-state solar cells. Here we investigate the phototransistors based on hybrid perovskite films and provide direct evidence for their superior carrier transport property with ambipolar characteristics. The field-effect mobilities for triiodide perovskites at room temperature are measured as 0.18 (0.17) cm(2) V(-1) s(-1) for holes (electrons), which increase to 1.24 (1.01) cm(2) V(-1) s(-1) for mixed-halide perovskites. The photoresponsivity of our hybrid perovskite devices reaches 320 A W(-1), which is among the largest values reported for phototransistors. Importantly, the phototransistors exhibit an ultrafast photoresponse speed of less than 10 μs. The solution-based process and excellent device performance strongly underscore hybrid perovskites as promising material candidates for photoelectronic applications.
TL;DR: In this paper, the authors measured the conduction and valance band offsets at the interface between two two-dimensional materials: molybdenum disulphide and tungsten diselenide.
Abstract: The emergence of two-dimensional electronic materials has stimulated proposals of novel electronic and photonic devices based on the heterostructures of transition metal dichalcogenides. Here we report the determination of band offsets in the heterostructures of transition metal dichalcogenides by using microbeam X-ray photoelectron spectroscopy and scanning tunnelling microscopy/spectroscopy. We determine a type-II alignment between MoS2 and WSe2 with a valence band offset value of 0.83 eV and a conduction band offset of 0.76 eV. First-principles calculations show that in this heterostructure with dissimilar chalcogen atoms, the electronic structures of WSe2 and MoS2 are well retained in their respective layers due to a weak interlayer coupling. Moreover, a valence band offset of 0.94 eV is obtained from density functional theory, consistent with the experimental determination. The alignment of the bandgap of adjacent materials in a heterostructure largely determines the electronic properties of a device. Here, the authors measure the conduction and valance band offsets at the interface between two two-dimensional materials: molybdenum disulphide and tungsten diselenide.
TL;DR: The authors used passive microwave observations to provide global estimates for forest and non-forest biomass trends over the past two decades and found that vegetation change is a key component of the carbon cycle, but quantifying these changes is challenging.
Abstract: Vegetation change is a key component of the carbon cycle, but quantifying these changes is challenging. Research using passive microwave observations now provides global estimates for forest and non-forest biomass trends over the past two decades.
TL;DR: Passivated perovskite QD films showed remarkable photostability under continuous pulsed laser excitation in ambient conditions for at least 34 h, substantially exceeding the stability of other colloidal QD systems in which ASE has been observed.
Abstract: We demonstrate ultra-air- and photostable CsPbBr3 quantum dots (QDs) by using an inorganic–organic hybrid ion pair as the capping ligand. This passivation approach to perovskite QDs yields high photoluminescence quantum yield with unprecedented operational stability in ambient conditions (60 ± 5% lab humidity) and high pump fluences, thus overcoming one of the greatest challenges impeding the development of perovskite-based applications. Due to the robustness of passivated perovskite QDs, we were able to induce ultrastable amplified spontaneous emission (ASE) in solution processed QD films not only through one photon but also through two-photon absorption processes. The latter has not been observed before in the family of perovskite materials. More importantly, passivated perovskite QD films showed remarkable photostability under continuous pulsed laser excitation in ambient conditions for at least 34 h (corresponds to 1.2 × 108 laser shots), substantially exceeding the stability of other colloidal QD sys...
University of Copenhagen1, University of California, Berkeley2, University of Massachusetts Amherst3, Wellcome Trust Sanger Institute4, Technical University of Denmark5, Pennsylvania State University6, La Trobe University7, Stanford University8, University of Cambridge9, King Abdullah University of Science and Technology10, University of Tartu11, Estonian Biocentre12, University of California, San Francisco13, Washington State University14, University of Porto15, University of Illinois at Urbana–Champaign16, Carlos III Health Institute17, University of Utah18, Science for Life Laboratory19, Aarhus University20, University College London21, University of Reading22, University of Bristol23, University of Guadalajara24, University of Bologna25, Oregon State University26, University of Paris27, University of Zurich28, Max Planck Society29, St. John's University30, University of California, Irvine31, University of Tarapacá32, University of Toulouse33, Russian Academy of Sciences34, Novosibirsk State University35, Kemerovo State University36, Bashkir State University37, North-Eastern Federal University38, Western Washington University39, Northwest Community College40, University of Western Ontario41, Simon Fraser University42, Laboratory of Molecular Biology43, University of Kansas44, University of California, Davis45, Texas A&M University46, Santa Barbara Museum of Natural History47, Southern Methodist University48
TL;DR: The results suggest that there has been gene flow between some Native Americans from both North and South America and groups related to East Asians and Australo-Melanesians, the latter possibly through an East Asian route that might have included ancestors of modern Aleutian Islanders.
Abstract: How and when the Americas were populated remains contentious. Using ancient and modern genome-wide data, we found that the ancestors of all present-day Native Americans, including Athabascans and Amerindians, entered the Americas as a single migration wave from Siberia no earlier than 23 thousand years ago (ka) and after no more than an 8000-year isolation period in Beringia. After their arrival to the Americas, ancestral Native Americans diversified into two basal genetic branches around 13 ka, one that is now dispersed across North and South America and the other restricted to North America. Subsequent gene flow resulted in some Native Americans sharing ancestry with present-day East Asians (including Siberians) and, more distantly, Australo-Melanesians. Putative "Paleoamerican" relict populations, including the historical Mexican Pericues and South American Fuego-Patagonians, are not directly related to modern Australo-Melanesians as suggested by the Paleoamerican Model.
TL;DR: The key insights reported here—strong many-body effects and intrinsically rapid radiative recombination—are expected to be ubiquitous in atomically thin semiconductors.
Abstract: The band-edge optical response of transition metal dichalcogenides, an emerging class of atomically thin semiconductors, is dominated by tightly bound excitons localized at the corners of the Brillouin zone (valley excitons). A fundamental yet unknown property of valley excitons in these materials is the intrinsic homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath (vacuum and other quasiparticles) interactions and determines the timescale during which excitons can be coherently manipulated. Here we use optical two-dimensional Fourier transform spectroscopy to measure the exciton homogeneous linewidth in monolayer tungsten diselenide (WSe2). The homogeneous linewidth is found to be nearly two orders of magnitude narrower than the inhomogeneous width at low temperatures. We evaluate quantitatively the role of exciton-exciton and exciton-phonon interactions and population relaxation as linewidth broadening mechanisms. The key insights reported here—strong many-body effects and intrinsically rapid radiative recombination—are expected to be ubiquitous in atomically thin semiconductors.
TL;DR: It was determined that the P3 HT:FBR blend is highly intermixed, leading to increased charge generation relative to comparative devices with P3HT:PC60BM, but also faster recombination due to a nonideal morphology, demonstrating that this acceptor shows great promise for further optimization.
Abstract: A novel small molecule, FBR, bearing 3-ethylrhodanine flanking groups was synthesized as a nonfullerene electron acceptor for solution-processed bulk heterojunction organic photovoltaics (OPV). A straightforward synthesis route was employed, offering the potential for large scale preparation of this material. Inverted OPV devices employing poly(3-hexylthiophene) (P3HT) as the donor polymer and FBR as the acceptor gave power conversion efficiencies (PCE) up to 4.1%. Transient and steady state optical spectroscopies indicated efficient, ultrafast charge generation and efficient photocurrent generation from both donor and acceptor. Ultrafast transient absorption spectroscopy was used to investigate polaron generation efficiency as well as recombination dynamics. It was determined that the P3HT:FBR blend is highly intermixed, leading to increased charge generation relative to comparative devices with P3HT:PC60BM, but also faster recombination due to a nonideal morphology in which, in contrast to P3HT:PC60BM d...
TL;DR: This synthesized nanocluster is the only silver nanoparticle that has a virtually identical analogue in gold, i.e., [Au25(SR)18](-), in terms of number of metal atoms, ligand count, superatom electronic configuration, and atomic arrangement.
Abstract: Silver nanoparticles with an atomically precise molecular formula [Ag25(SR)18]− (−SR: thiolate) are synthesized, and their single-crystal structure is determined. This synthesized nanocluster is the only silver nanoparticle that has a virtually identical analogue in gold, i.e., [Au25(SR)18]−, in terms of number of metal atoms, ligand count, superatom electronic configuration, and atomic arrangement. Furthermore, both [Ag25(SR)18]− and its gold analogue share a number of features in their optical absorption spectra. This unprecedented molecular analogue in silver to mimic gold offers the first model nanoparticle platform to investigate the centuries-old problem of understanding the fundamental differences between silver and gold in terms of nobility, catalytic activity, and optical property.