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Showing papers on "Doping published in 2019"


Journal ArticleDOI
TL;DR: An overview on the doping of carbon materials for metal-free electrocatalysis, especially the development of doping strategies and doping-induced structure and property changes for potential catalytic applications is presented.
Abstract: Carbon atoms in the graphitic carbon skeleton can be replaced by heteroatoms with different electronegative from that of the carbon atom (i.e., heteroatom doping) to modulate the charge distribution over the carbon network. The charge modulation can be achieved via direct charge transfer with an electron acceptor/donor (i.e., charge transfer doping) or through introduction of defects (i.e., defective doping). Various doping strategies, including heteroatom doping, charge-transfer doping, and defective doping, have now been devised for modulating the charge distribution of numerous graphite carbon materials to impart new properties to carbon materials. Consequently, carbon nanomaterials with defined doping have recently become prominent members in the carbon family, promising for a variety of applications, including catalysis, energy conversion and storage, environmental remediation, and important chemical production and industrial processes. The purpose of this review is to present an overview on the doping of carbon materials for metal-free electrocatalysis, especially the development of doping strategies and doping-induced structure and property changes for potential catalytic applications. Current challenges and future perspectives in the doped carbon-based metal-free catalyst field are also discussed.

358 citations


Journal ArticleDOI
TL;DR: The correlation between N dopants and interlayer distance of resultant N-FLG-T highlights the effect of pyrrolic N on the enlargement of graphene interlayer spacing, due to its stronger electrostatic repulsion.
Abstract: Heteroatom-doped carbon materials with expanded interlayer distance have been widely studied as anodes for sodium-ion batteries (SIBs). However, it remains unexplored to further enlarge the interlayer spacing and reveal the influence of heteroatom doping on carbon nanostructures for developing more efficient SIB anode materials. Here, a series of N-rich few-layer graphene (N-FLG) with tuneable interlayer distance ranging from 0.45 to 0.51 nm is successfully synthesized by annealing graphitic carbon nitride (g-C3 N4 ) under zinc catalysis and selected temperature (T = 700, 800, and 900 °C). More significantly, the correlation between N dopants and interlayer distance of resultant N-FLG-T highlights the effect of pyrrolic N on the enlargement of graphene interlayer spacing, due to its stronger electrostatic repulsion. As a consequence, N-FLG-800 achieves the optimal properties in terms of interlayer spacing, nitrogen configuration and electronic conductivity. When used as an anode for SIBs, N-FLG-800 shows remarkable Na+ storage performance with ultrahigh rate capability (56.6 mAh g-1 at 40 A g-1 ) and excellent long-term stability (211.3 mAh g-1 at 0.5 A g-1 after 2000 cycles), demonstrating the effectiveness of material design.

330 citations


Journal ArticleDOI
TL;DR: In this paper, a fast screening methodology for doping LiNi0.8Co0.1O2 with cations Mg2+, Al3+, Si4+, Ti4+, Zr4+, and Ta5+ was proposed.
Abstract: Ni-rich materials of layered structure LiNixCoyMnzO2, x > 0.5, are promising candidates as cathodes in high-energy-density Li-ion batteries for electric vehicles. The structural and cycling stability of Ni-rich cathodes can be remarkably improved by doping with a small amount of extrinsic multivalent cations. In this study, we examine development of a fast screening methodology for doping LiNi0.8Co0.1Mn0.1O2 with cations Mg2+, Al3+, Si4+, Ti4+, Zr4+, and Ta5+ by a “top-down” approach. The cathode material is coated by a precursor layer that contains the dopant, which then is introduced into the particles by diffusion during heat treatment at elevated temperatures. The methodology described herein can be applied to Ni-rich cathode materials and allows relatively easy and prompt identification of the most promising dopants. Then further optimization work can lead to development of high-capacity stable cathode materials. The present study marks Ta5+ cations as very promising dopants for Ni-rich NCM cathodes.

297 citations


Journal ArticleDOI
TL;DR: In this article, the authors demonstrate that metal-free graphitic carbon nitride (g-C3N4) can be simultaneously co-doped with S, P and O nonmetal-atoms and exfoliated into ultrathin 2D nanosheets with a thickness of ∼3nm by a simple, sequential thermal synthesis.
Abstract: Recently, metal-free graphitic carbon nitride (g-C3N4) has been recognized as a potential candidate for high-performance photocatalytic hydrogen production while challenges still remain due to poor electronic properties and limited surface active sites. We demonstrate that g-C3N4 can be simultaneously co-doped with S, P and O nonmetal-atoms and exfoliated into ultrathin 2D nanosheets with a thickness of ∼3 nm by a simple, sequential thermal synthesis. The multi-atoms doping and nanostructure modulation remarkably enhanced the photocatalytic hydrogen production under illumination, with the optimal H2 evolution rate reaching 2480 μmol g−1 h−1. First-principle calculations and experimental evidences suggest that, upon elemental doping within the g-C3N4 framework, S atoms occupied the interstitial sites and P and O atoms replaced the C and N atoms, respectively. Consequently, photo-induced charge transfer and separation significantly improved owing to the construction of a more favorable charge transfer pathway. Furthermore, introducing heteroatoms into the structure of g-C3N4 narrowed the bandgap and negatively shifted the conduction band edge, leading to extended visible-light absorption and stronger electron reducibility for subsequent H2 production. Importantly, the in-situ generated 2D g-C3N4 nanosheets exhibited more catalytic surface sites, which was highly beneficial to the photocatalytic water splitting.

286 citations


PatentDOI
TL;DR: Hole-transport-layer-free PSCs with improved photovoltaic performance are fabricated via a scalable doctor-blading process by molecularly doping the perovskite layer without using hole-transporting layers, thus simplify the device architecture and processing steps.
Abstract: A method of forming a photoactive device includes steps of: forming a photoactive layer, the photoactive layer comprising a perovskite material and a dopant; wherein the photoactive device comprises a positive electrode and a negative electrode; wherein said photoactive layer is directly or indirectly in electronic communication with the positive electrode and directly or indirectly in electronic communication with the negative electrode; and wherein the photoactive device is free of a hole transport layer between the photoactive layer and the positive electrode.

282 citations


Journal ArticleDOI
TL;DR: In this paper, a simple co-pyrolysis of dicyandiamide and ammonium persulphate ((NH4)2S2O8) was proposed to improve the photocatalytic activity of graphitic carbon nitride (g-C3N4) by changing the electron transition through a rational band structure engineering.
Abstract: Porous structure, nitrogen defects and oxygen dopants are simultaneously introduced into the framework of graphitic carbon nitride (g-C3N4) by a simple co-pyrolysis of dicyandiamide and ammonium persulphate ((NH4)2S2O8). The (NH4)2S2O8 plays multi-function roles in the co-pyrolysis process. It not only restrains polycondensation to generate nitrogen defects but also introduces porous structure and oxygen dopants due to its strong oxidative ability. The synergetic effect of the nitrogen defects and oxygen dopants leads to the change of π band state and LP state (lone pair electrons), causing the change of electron transition in the modified g-C3N4. The transitions from impurity levels play a predominant role in excitation process while the transition from intrinsic HOMO to LUMO becomes subordinate, which improve the charge separation significantly. The modified g-C3N4 exhibits excellent photocatalytic hydrogen evolution activity under visible light illumination, which is almost 6 times higher than pristine g-C3N4 because of the improved efficiency of charge separation and increased specific surface area. These findings provide a simple and efficient method to improve the photocatalytic activity of g-C3N4 by changing the electron transition through a rational band structure engineering.

254 citations


Journal ArticleDOI
TL;DR: The onset potential and charge separation of bismuth vanadate photoanode water splitting performances are improved by work function tuning and heterojunction engineering.
Abstract: We herein demonstrate the unusual effectiveness of two strategies in combination to enhance photoelectrochemical water splitting. First, the work function adjustment via molybdenum (Mo) doping significantly reduces the interfacial energy loss and increases the open-circuit photovoltage of bismuth vanadate (BiVO4) photoelectrochemical cells. Second, the creation and optimization of the heterojunction of boron (B) doping carbon nitride (C3N4) and Mo doping BiVO4 to enforce directional charge transfer, accomplished by work function adjustment via B doping for C3N4, substantially boost the charge separation of photo-generated electron-hole pairs at the B-C3N4 and Mo-BiVO4 interface. The synergy between the above efforts have significantly reduced the onset potential, and enhanced charge separation and optical properties of the BiVO4-based photoanode, culminating in achieving a record applied bias photon-to-current efficiency of 2.67% at 0.54 V vs. the reversible hydrogen electrode. This work sheds light on designing and fabricating the semiconductor structures for the next-generation photoelectrodes. While photoelectrodes represent a promising solar-to-fuel conversion technology, material challenges limit performances. Here, authors improve the onset potential and charge separation of bismuth vanadate photoanode water splitting performances by work function tuning and heterojunction engineering.

249 citations


Journal ArticleDOI
TL;DR: Doping divalent Cu2+ ions into the perovskite lattice is addressed, resulting in the improvement of both the thermal stability and the optical performance of CsPb1- xCu x(Br/Cl)3 QDs, which exhibit bright blue photoluminescence at 450-460 nm, with a high quantum yield of over 80%.
Abstract: All-inorganic perovskite quantum dots (QDs) have emerged as potentially promising materials for lighting and displays, but their poor thermal stability restricts their practical application. In addition, optical characteristics of the blue-emitting CsPbX3 QDs lag behind their red- and green-emitting counterparts. Herein, we addressed these two issues by doping divalent Cu2+ ions into the perovskite lattice to form CsPb1–xCuxX3 QDs. Extended X-ray absorption fine structure (EXAFS) measurements reveal that doping smaller Cu2+ guest ions induces a lattice contraction and eliminates halide vacancies, which leads to an increased lattice formation energy and improved short-range order of the doped perovskite QDs. This results in the improvement of both the thermal stability and the optical performance of CsPb1–xCux(Br/Cl)3 QDs, which exhibit bright blue photoluminescence at 450–460 nm, with a high quantum yield of over 80%. The CsPb1–xCuxX3 QD films maintain stable luminescence performance even when annealed at...

236 citations


Journal ArticleDOI
TL;DR: In this paper, a density functional theory (DFT) method was carried out to simulate the adsorption of three dissolved gases on Pd-doped MOS2 (Pd-MoS2) monolayer.

222 citations


Journal ArticleDOI
TL;DR: Theoretical calculations prove that the new electron excitation from N to B is much easier than N to C 2pz, and improves the charge transfer and localization, and thus the reaction dynamics, and the optimal sample of 1%B/g‐C3N4 exhibits better selectivity for CH4 with ≈32 times higher yield than that of pure g‐C 3N4.
Abstract: The photoreduction of CO2 to hydrocarbon products has attracted much attention because it provides an avenue to directly synthesize value-added carbon-based fuels and feedstocks using solar energy. Among various photocatalysts, graphitic carbon nitride (g-C3N4) has emerged as an attractive metal-free visible-light photocatalyst due to its advantages of earth-abundance, nontoxicity, and stability. Unfortunately, its photocatalytic efficiency is seriously limited by charge carriers' ready recombination and their low reaction dynamics. Modifying the local electronic structure of g-C3N4 is predicted to be an efficient way to improve the charge transfer and reaction efficiency. Here, boron (B) is doped into the large cavity between adjacent tri-s-triazine units via coordination with two-coordinated N atoms. Theoretical calculations prove that the new electron excitation from N (2p x , 2p y ) to B (2p x , 2p y ) with the same orbital direction in B-doped g-C3N4 is much easier than N (2p x , 2p y ) to C 2p z in pure g-C3N4, and improves the charge transfer and localization, and thus the reaction dynamics. Moreover, B atoms doping changes the adsorption of CO (intermediate), and can act as active sites for CH4 production. As a result, the optimal sample of 1%B/g-C3N4 exhibits better selectivity for CH4 with ≈32 times higher yield than that of pure g-C3N4.

215 citations


Journal ArticleDOI
TL;DR: In this paper, high electron mobilities were achieved for silicon-doped (010) β-Ga2O3 homoepitaxial films grown via metalorganic chemical vapor deposition (MOCVD).
Abstract: Record-high electron mobilities were achieved for silicon-doped (010) β-Ga2O3 homoepitaxial films grown via metalorganic chemical vapor deposition (MOCVD). Key growth parameters were investigated to reduce the background doping and compensation concentration. Controllable n-type Si doping was achieved as low as low-1016 cm−3. Record carrier mobilities of 184 cm2/V s at room temperature and 4984 cm2/V s at low temperature (45 K) were measured for β-Ga2O3 thin films with room-temperature doping concentrations of 2.5 × 1016 and 2.75 × 1016 cm−3, respectively. Analysis of temperature-dependent Hall mobility and carrier concentration data revealed a low compensation concentration of 9.4 × 1014 cm−3. Using the two-donor model, Si on the tetrahedrally coordinated Ga(I) site represented the primary shallow donor state, and the secondary donor state was found to possess an activation energy of 120 meV. The demonstration of high-purity and high-quality β-Ga2O3 thin films with uniform and smooth surface morphology via MOCVD will harness its advantages as an ultrawide-bandgap semiconductor for power electronic and short-wavelength optoelectronic device applications.

Journal ArticleDOI
TL;DR: In this paper, a significant ZT enhancement from 1.0 to 2.0 by suppressing the formation of Ge vacancies and band convergence was achieved by simply optimizing the amount of excessive Ge, which greatly reduced the hole carrier concentration.
Abstract: GeTe is a promising thermoelectric material at medium temperature, but its carrier concentration tends to go beyond the optimal range for thermoelectrics. This work realized a significant ZT enhancement from 1.0 to 2.0 by suppressing the formation of Ge vacancies and band convergence. By simply optimizing the amount of excessive Ge, the hole carrier concentration is greatly reduced. It is demonstrated that the suppression of Ge vacancies can not only optimize the carrier concentration but also recover the mobility to a high value of 90 cm2 V−1 s−1, which well exceeds the previously reported data and guarantees superior electrical transport properties, leading to a ZT of 1.6. Further Bi doping facilitates band convergence as featured by the increased band effective mass and high mobility, which in turn yields large power factors and low electronic thermal conductivity. Bi doping induced mass and strain fluctuation also favors the reduction of the lattice thermal conductivity. Consequently, a maximum ZT of ∼ 2.0 at 650 K with an average ZT of over 1.2 is achieved in the nominal composition Bi0.05Ge0.99Te, which is one of the best thermoelectric materials for medium temperature applications.

Journal ArticleDOI
TL;DR: In this paper, a deep-ultraviolet semiconductor laser diode that operates under current injection at room temperature and at a very short wavelength was presented, achieving a low operation voltage of 13.8 V at a lasing threshold current of 0.4 A. The laser structure was grown on the (0001) face of a single-crystal aluminum nitride substrate.
Abstract: We present a deep-ultraviolet semiconductor laser diode that operates under current injection at room temperature and at a very short wavelength. The laser structure was grown on the (0001) face of a single-crystal aluminum nitride substrate. The measured lasing wavelength was 271.8 nm with a pulsed duration of 50 ns and a repetition frequency of 2 kHz. A polarization-induced doping cladding layer was employed to achieve hole conductivity and injection without intentional impurity doping. Even with this undoped layer, we were still able to achieve a low operation voltage of 13.8 V at a lasing threshold current of 0.4 A.

Journal ArticleDOI
TL;DR: It is established that common p-dopants can in fact accept two electrons per molecule from conjugated polymers with a low ionization energy and it is shown that the resulting integer charge-transfer complex can dissociate with an efficiency of up to 170%.
Abstract: Molecular doping is a crucial tool for controlling the charge-carrier concentration in organic semiconductors. Each dopant molecule is commonly thought to give rise to only one polaron, leading to a maximum of one donor:acceptor charge-transfer complex and hence an ionization efficiency of 100%. However, this theoretical limit is rarely achieved because of incomplete charge transfer and the presence of unreacted dopant. Here, we establish that common p-dopants can in fact accept two electrons per molecule from conjugated polymers with a low ionization energy. Each dopant molecule participates in two charge-transfer events, leading to the formation of dopant dianions and an ionization efficiency of up to 200%. Furthermore, we show that the resulting integer charge-transfer complex can dissociate with an efficiency of up to 170%. The concept of double doping introduced here may allow the dopant fraction required to optimize charge conduction to be halved.

Journal ArticleDOI
TL;DR: In this paper, the authors report record electron mobility values in unintentionally doped β-Ga2O3 films grown by metal-organic chemical vapor deposition, using degenerately Sn-doped regrown n+β-Ga 2O3 contact layers.
Abstract: In this work, we report record electron mobility values in unintentionally doped β-Ga2O3 films grown by metal-organic chemical vapor deposition. Using degenerately Sn-doped regrown n+ β-Ga2O3 contact layers, we were able to maintain Ohmic contact to the β-Ga2O3 films down to 40 K, allowing for reliable temperature-dependent Hall measurement. An electron mobility of 176 cm2/V s and 3481 cm2/V s were measured at room temperature and 54 K, respectively. The room and low temperature mobilities are both among the highest reported values in a bulk β-Ga2O3 film. A low net background charge concentration of 7.4 × 1015 cm−3 was confirmed by both temperature dependent Hall measurement and capacitance-voltage measurement. The feasibility of achieving low background impurity concentration and high electron mobility paves the road for the demonstration of high performance power electronics with high breakdown voltages and low on-resistances.

Journal ArticleDOI
TL;DR: This work illustrates an effective and facile route toward modifying and optimizing optical properties of double perovskite Cs2AgBiX6 (X = Cl-, Br-) NCs with an indirect bandgap nature, which can broaden a range of their potential applications in optoelectronic devices.
Abstract: Lead-free double perovskite nanocrystals (NCs) have emerged as a new category of materials that hold the potential for overcoming the instability and toxicity issues of lead-based counterparts. Doping chemistry represents a unique avenue toward tuning and optimizing the intrinsic optical and electronic properties of semiconductor materials. In this study, we report the first example of doping Yb3+ ions into lead-free double perovskite Cs2AgBiX6 (X = Cl-, Br-) NCs via a hot injection method. The doping of Yb3+ endows the double perovskite NCs with a newly emerged near-infrared emission band (sensitized from the NC hosts) in addition to their intrinsic trap-related visible photoluminescence. By controlling the Yb-doping concentration, the dual emission profiles and photon relaxation dynamics of the double perovskite NCs can be systematically tuned. Furthermore, we have successfully inserted divalent Mn2+ ions in Cs2AgBiCl6 NCs and observed emergence of dopant emission. Our work illustrates an effective and facile route toward modifying and optimizing optical properties of double perovskite Cs2AgBiX6 (X = Cl-, Br-) NCs with an indirect bandgap nature, which can broaden a range of their potential applications in optoelectronic devices.

Journal ArticleDOI
TL;DR: In this article, the effect of Al dopant on the crystal structure, surface morphology, optical and electrical properties of films were studied using powder X-ray diffractometer (XRD), scanning electron microscopy (SEM), UV-vis spectrophotometer, and four point probe technique respectively.

Journal ArticleDOI
TL;DR: In this paper, the effect of fluorine dopant and oxygen vacancy on electrochemical performance of a fluorine-doped oxygen-deficient Co2MnO4 nanowires grown on carbon fiber (CF) as advanced electrode materials for supercapacitor was investigated.

Journal ArticleDOI
01 Oct 2019-Small
TL;DR: A facile method is developed to synthesize a series of trimetallic (W/Co/Fe) metal-organic frameworks (MOFs)-derived carbon nanoflakes (CNF) with various Fe content, and an Fe-dependent volcano-type plot can be drawn out for WCoFex -CNF.
Abstract: The construction of efficient, durable, and non-noble metal electrocatalysts for oxygen evolution reaction (OER) is of great value but challenging. Herein, a facile method is developed to synthesize a series of trimetallic (W/Co/Fe) metal-organic frameworks (MOFs)-derived carbon nanoflakes (CNF) with various Fe content, and an Fe-dependent volcano-type plot can be drawn out for WCoFex -CNF. The optimized WCoFe0.3 -CNF (when the feed ratio of Fe/Co is 0.3) demonstrates superior electrocatalytic performance with a low overpotential of only 254 mV@10 mA cm-2 and excellent durability of 100 h. Further researches show that appropriate amount of iron doping can regulate the electronic structure, resulting in a favorable synergistic environment. This method may stimulate the exploration of electrocatalysts by utilizing MOFs as precursors while realizing electronic modulation by multimetal doping.

Journal ArticleDOI
TL;DR: In this paper, chemical doping of graphene with elements like nitrogen and boron gives rise to useful band gap bands for a range of applications, such as medical applications and artificial intelligence.
Abstract: Chemical doping of graphene is necessary to generate a band gap that is valuable for a range of applications. Chemical doping of graphene with elements like nitrogen and boron gives rise to useful ...

Journal ArticleDOI
TL;DR: In this paper, the authors highlight the scientific and engineering challenges to enhance the conductivity of n-type polymer thermoelectric materials, including n-doping efficiency in N-type polymers, factors influencing charge carrier mobilities after doping, and stability of N-Type conducting polymers.
Abstract: In the past several decades, conducting polymers have achieved remarkable progress and have been widely applied as the active materials for optoelectronics. So far, p-type conducting polymers exhibit high conductivities over 1000 S cm–1 and thermoelectric performance comparable to that of inorganic materials; however, only a few n-type conducting polymers showed conductivities over 1 S cm–1 after doping. The low conductivity of n-type conducting polymers is considered as the major barrier for further enhancing their thermoelectric performances. In this perspective, we highlight the scientific and engineering challenges to enhance the conductivity of n-type polymer thermoelectric materials, including n-doping efficiency in n-type polymers, factors influencing charge carrier mobilities after doping, and stability of n-type conducting polymers. Recent development and strategies to address these issues and enhance the conductivity of n-type conjugated polymers are summarized and discussed, providing materials...

Journal ArticleDOI
TL;DR: This Perspective describes and classifies recent advances in understanding defect chemistry and avenues toward defect density reduction in perovskite NCs, and it does so in the context of the promise perceived in light-emitting devices.
Abstract: The large specific surface area of perovskite nanocrystals (NCs) increases the likelihood of surface defects compared to that of bulk single crystals and polycrystalline thin films. It is thus crucial to comprehend and control their defect population in order to exploit the potential of perovskite NCs. This Perspective describes and classifies recent advances in understanding defect chemistry and avenues toward defect density reduction in perovskite NCs, and it does so in the context of the promise perceived in light-emitting devices. Several pathways for decreasing the defect density are explored, including advanced NC syntheses, new surface-capping strategies, doping with metal ions and rare earths, engineering elemental compensation, and the translation of core-shell heterostructures into the perovskite materials family. We close with challenges that remain in perovskite NC defect research.

Journal ArticleDOI
16 Oct 2019-Joule
TL;DR: In this paper, the authors reported a high zT of ∼2.1 at 723 K in In and Bi co-doped GeTe along with an extremely high TE conversion efficiency of ∼12.3% in a single-leg thermoelectric generator for the temperature difference of 445 K.

Journal ArticleDOI
TL;DR: In this article, a facile one-pot solvothermal method was designed to synthesize porous 1T-MoS2 that is integrated with atomic doping of Cu atoms.
Abstract: Molybdenum sulfide (MoS2) has attracted great interest as a promising non-precious-metal catalyst candidate to replace the precious-metal Pt catalysts for the hydrogen evolution reaction (HER). Nevertheless, the catalytic efficiency of MoS2 is significantly restricted by its density of catalytic active sites and inert basal plane. In this work, we have designed a facile one-pot solvothermal method to synthesize porous 1T-MoS2 that is integrated with atomic doping of Cu atoms. The as-prepared Cu@MoS2 sample exhibits enhanced HER performance with a low overpotential of 131 mV at the current density of 10 mA/cm2, a small Tafel slope of 51 mV/dec and as well as a good long-term stability. Enhanced HER performance can be ascribed to the synergistic effect of 1T-MoS2 metallic phase, single atom Cu doping and numerous sulfur vacancies. Theoretical calculations indicates that the adsorption energy of Cu atom on 1T-MoS2 surface (−3.68 eV) is much higher than that on 2H-MoS2 surface (−1.94 eV), moreover, the Cu atom adsorbed on the surface of the 1T-MoS2 has larger charge transfer (−0.38e), which can be contributed to further enhance HER performance of 1T-MoS2.

Journal ArticleDOI
TL;DR: It is shown that the photoluminescence quantum yield of as-processed MoS2 and WS2 monolayers reaches near-unity when they are made intrinsic through electrostatic doping, without any chemical passivation.
Abstract: Defects in conventional semiconductors substantially lower the photoluminescence (PL) quantum yield (QY), a key metric of optoelectronic performance that directly dictates the maximum device efficiency. Two-dimensional (2D) transition metal dichalcogenides (TMDCs), such as monolayer MoS2, often exhibit low PL QY for as-processed samples, which has typically been attributed to a large native defect density. We show that the PL QY of as-processed MoS2 and WS2 monolayers reaches near-unity when they are made intrinsic by electrostatic doping, without any chemical passivation. Surprisingly, neutral exciton recombination is entirely radiative even in the presence of a high native defect density. This finding enables TMDC monolayers for optoelectronic device applications as the stringent requirement of low defect density is eased.


Journal ArticleDOI
TL;DR: This work highlights the approaches to overcome the drawbacks of WO3 photoanodes, including the manipulation of nanostructured WO1 photoanode to decrease the nanoparticle size to promote hole migration to the WO2/electrolyte interface which benefits the charge separation and controlling the crystal phase via annealing to reduce defects.
Abstract: Hydrogen production from photoelectrochemical (PEC) water splitting using semiconductor photocatalysts has attracted great attention to realize clean and renewable energy from solar energy. The visible light response of WO3 with a long hole diffusion length (∼150 nm) and good electron mobility (∼12 cm2 V-1 s-1) makes it suitable as the photoanode. However, WO3 suffers from issues including rapid recombination of photoexcited electron-hole pairs, photo-corrosion during the photocatalytic process due to the formation of peroxo-species, sluggish kinetics of photogenerated holes, and slow charge transfer at the semiconductor/electrolyte interface. This work highlights the approaches to overcome these drawbacks of WO3 photoanodes, including: (i) the manipulation of nanostructured WO3 photoanodes to decrease the nanoparticle size to promote hole migration to the WO3/electrolyte interface which benefits the charge separation; (ii) doping or introducing oxygen vacancies to improve electrical conductivity; exposing high energy crystal surfaces to promote the consumption of photogenerated holes on the high-active crystal face, thereby suppressing the recombination of photogenerated electrons and holes; (iii) decorating with co-catalysts to reduce the overpotential which inhibits the formation of peroxo-species; (iv) other methods such as coupling with narrow band semiconductors to accelerate the charge separation and controlling the crystal phase via annealing to reduce defects. These approaches are reviewed with detailed examples.

Journal ArticleDOI
TL;DR: In this article, the properties of Er3+-doped gallium lanthanum sulphide thin films were studied as a function of process temperature, showing that by increasing the substrate temperature, the deposited layer thickness increases and the crystallinity of the films changes.
Abstract: The properties of Er3+-doped gallium lanthanum sulphide thin films prepared on a silicon substrate by femtosecond pulsed laser deposition were studied as a function of process temperature. The films were characterised using transition electron microscopy imaging, X-ray diffractometry, Raman spectroscopy, fluorescence spectroscopy, and UV–Vis–NIR spectroscopy. The results show that by increasing the substrate temperature, the deposited layer thickness increases and the crystallinity of the films changes. The room temperature photoluminescence and lifetimes of the 4I13/2→4I15/2 transition of Er3+ are reported in the paper.

Journal ArticleDOI
TL;DR: The authors' results in Sb3+ doped Cs2SnCl6 materials provides insights into the machanisms of doping-induced emission centers, and it extends the existing knowledge of optical properties of doped halide NCs for further studies.
Abstract: Doped halide perovskite nanocrystals (NCs) have opened new opportunities for the emerging optical and optoelectronic applications. Here, we describe a hot-injection synthesis of all-inorganic lead-free Cs2SnCl6 and Sb3+ doped Cs2SnCl6 NCs. Cs2SnCl6 NCs present a blue emission peak at 438 nm, whereas a new broad-band emission peak appears at 615 nm for the Sb3+ doped NCs. Comparative structural and spectral characterizations of Sb3+ doped Cs2SnCl6 NCs with micrometer-sized undoped and Sb3+ doped crystals show that the formation of broad-band orange emission is originted from triplet self-trapped excitons, attributed to the 3Pn-1S0 transitions (n = 0, 1, 2). Our results in Sb3+ doped Cs2SnCl6 materials provide insights into the machanisms of doping-induced emission centers, and it extends the existing knowledge of optical properties of doped halide NCs for further studies.

Journal ArticleDOI
TL;DR: It is discovered that electrons are transferred from the R3P+ O- σ-bond to the peripheral tin atoms other than the directly interacted ones at the surface of SnO2, which accounts for the enhancement of conductivity and the decline of work function ofsnO2.
Abstract: Molecular doping of inorganic semiconductors is a rising topic in the field of organic/inorganic hybrid electronics. However, it is difficult to find dopant molecules which simultaneously exhibit strong reducibility and stability in ambient atmosphere, which are needed for n-type doping of oxide semiconductors. Herein, successful n-type doping of SnO2 is demonstrated by a simple, air-robust, and cost-effective triphenylphosphine oxide molecule. Strikingly, it is discovered that electrons are transferred from the R3P+ O- σ-bond to the peripheral tin atoms other than the directly interacted ones at the surface. That means those electrons are delocalized. The course is verified by multi-photophysical characterizations. This doping effect accounts for the enhancement of conductivity and the decline of work function of SnO2 , which enlarges the built-in field from 0.01 to 0.07 eV and decreases the energy barrier from 0.55 to 0.39 eV at the SnO2 /perovskite interface enabling an increase in the conversion efficiency of perovskite solar cells from 19.01% to 20.69%.