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Showing papers on "Single crystal published in 2019"


Journal ArticleDOI
06 Jun 2019-Nature
TL;DR: The epitaxial growth of large single-crystal hexagonal boron nitride monolayers on low-symmetry copper foils is demonstrated and is expected to facilitate the wide application of 2D devices and lead to the epitaxials growth of broad non-centrosymmetric 2D materials, such as various transition-metal dichalcogenides20–23, to produce large single crystals.
Abstract: The development of two-dimensional (2D) materials has opened up possibilities for their application in electronics, optoelectronics and photovoltaics, because they can provide devices with smaller size, higher speed and additional functionalities compared with conventional silicon-based devices1. The ability to grow large, high-quality single crystals for 2D components—that is, conductors, semiconductors and insulators—is essential for the industrial application of 2D devices2–4. Atom-layered hexagonal boron nitride (hBN), with its excellent stability, flat surface and large bandgap, has been reported to be the best 2D insulator5–12. However, the size of 2D hBN single crystals is typically limited to less than one millimetre13–18, mainly because of difficulties in the growth of such crystals; these include excessive nucleation, which precludes growth from a single nucleus to large single crystals, and the threefold symmetry of the hBN lattice, which leads to antiparallel domains and twin boundaries on most substrates19. Here we report the epitaxial growth of a 100-square-centimetre single-crystal hBN monolayer on a low-symmetry Cu (110) vicinal surface, obtained by annealing an industrial copper foil. Structural characterizations and theoretical calculations indicate that epitaxial growth was achieved by the coupling of Cu step edges with hBN zigzag edges, which breaks the equivalence of antiparallel hBN domains, enabling unidirectional domain alignment better than 99 per cent. The growth kinetics, unidirectional alignment and seamless stitching of the hBN domains are unambiguously demonstrated using centimetre- to atomic-scale characterization techniques. Our findings are expected to facilitate the wide application of 2D devices and lead to the epitaxial growth of broad non-centrosymmetric 2D materials, such as various transition-metal dichalcogenides20–23, to produce large single crystals. The epitaxial growth of large single-crystal hexagonal boron nitride monolayers on low-symmetry copper foils is demonstrated.

363 citations


Journal ArticleDOI
TL;DR: Li et al. as mentioned in this paper proposed a 2D layered perovskite-like (NH4)3Bi2I9 device that provides unique anisotropic X-ray detecting performance with different crystal directions, effective suppression of ion migration and a low detection limit of 55'nGyair's−1.
Abstract: The effective detection of X-ray radiation with low threshold is essential to many medical and industrial applications. Three-dimensional (3D) organolead trihalide and double perovskites have been shown to be suitable for direct X-ray detection. However, the sensitivity and stability of 3D perovskite X-ray detectors are limited by ion motion, and there remains a demand to develop green and stable X-ray detectors with high sensitivity and low detection limit. The emerging low-dimensional perovskites have shown promising optoelectronic properties, featuring good intrinsic stability and reduced ion migration. Inspired by this, we show that our 2D layered perovskite-like (NH4)3Bi2I9 device provides unique anisotropic X-ray detecting performance with different crystal directions, effective suppression of ion migration and a low detection limit of 55 nGyair s−1. These results will motivate new strategies to achieve a high-performance X-ray detector by utilizing 2D layered perovskite or perovskite-like materials, without requiring toxic elements. Perovskite-like materials enable different X-ray detection performance along different crystal directions. A low detection limit of 55 nGyair s−1 is demonstrated.

318 citations


Journal ArticleDOI
TL;DR: In this article, a Ni-rich LiNi0.8Co0.1O2 secondary cathode material consisting of radially aligned single-crystal primary particles is proposed and synthesized.
Abstract: DOI: 10.1002/aenm.201803963 3.8 V (vs Li+/Li), making them a class of promising cathode material and attracting considerable attention. Nevertheless, the inferior cycling stability and poor rate capability of Ni-rich oxide cathode materials have to be overcome before they can compete in practical implementation.[2,4] These drawbacks are largely attributed to their spherical micrometer-sized secondary particles aggregated densely by many randomly oriented primary nanoparticles,[4–6] as shown in Figure 1a. On the one hand, concomitant with this structure, the surface of secondary particles is terminated with random crystal planes. As Li+ can only diffuse along the 2D {010} plane in the hexagonal-layer structure of NCM materials,[4,7] the randomly exposed crystal planes (not solely the active {010} plane) may substantially hinder the Li+ exchange at the electrode/electrolyte interface. Meanwhile, the randomly oriented primary nanoparticles induce a prolonged and mazy Li+ diffusion pathway inside the secondary particles, because Li+ ions have to migrate across the grain boundaries, especially between the grains with inconsistent crystal planes. On the other hand, the successive phase transition accompanied by repeated Li+ insertion/extraction would result in anisotropic variation of the lattice parameters, and such variation is severely aggravated with the increase of Ni content.[8] Accordingly, in the Ni-rich oxide cathode materials, the substantial anisotropic lattice expansion/contraction would result in drastic microstrains at the boundaries of randomly oriented primary particles due to the asynchronous volume Ni-rich Li[NixCoyMn1−x−y]O2 (x ≥ 0.8) layered oxides are the most promising cathode materials for lithium-ion batteries due to their high reversible capacity of over 200 mAh g−1. Unfortunately, the anisotropic properties associated with the α-NaFeO2 structured crystal grains result in poor rate capability and insufficient cycle life. To address these issues, a micrometersized Ni-rich LiNi0.8Co0.1Mn0.1O2 secondary cathode material consisting of radially aligned single-crystal primary particles is proposed and synthesized. Concomitant with this unique crystallographic texture, all the exposed surfaces are active {010} facets, and 3D Li+ ion diffusion channels penetrate straightforwardly from surface to center, remarkably improving the Li+ diffusion coefficient. Moreover, coordinated charge–discharge volume change upon cycling is achieved by the consistent crystal orientation, significantly alleviating the volume-change-induced intergrain stress. Accordingly, this material delivers superior reversible capacity (203.4 mAh g−1 at 3.0–4.3 V) and rate capability (152.7 mAh g−1 at a current density of 1000 mA g−1). Further, this structure demonstrates excellent cycling stability without any degradation after 300 cycles. The anisotropic morphology modulation provides a simple, efficient, and scalable way to boost the performance and applicability of Ni-rich layered oxide cathode materials.

259 citations


Journal ArticleDOI
TL;DR: A novel lead-free zero-dimensional (0D) indium-based perovskite (Cs2 InBr5 ⋅H2 O) single crystal that is red-luminescent with a high photoluminescence quantum yield (PLQY) of 33 %.
Abstract: Low-dimensional luminescent lead halide perovskites have attracted tremendous attention for their fascinating optoelectronic properties, while the toxicity of lead is still considered a drawback. Herein, we report a novel lead-free zero-dimensional (0D) indium-based perovskite (Cs2 InBr5 ⋅H2 O) single crystal that is red-luminescent with a high photoluminescence quantum yield (PLQY) of 33 %. Experimental and computational studies reveal that the strong PL emission might originate from self-trapping excitons (STEs) that result from an excited-state structural deformation. More importantly, the in situ transformation between hydrated Cs2 InBr5 ⋅H2 O and the dehydrated form is accompanied with a switchable dual emission, which enables it to act as a PL water-sensor in humidity detection or the detection of traces of water in organic solvents.

258 citations


Journal ArticleDOI
TL;DR: Low-energy electron microscopy enables controlled synthesis and characterization of (large) single-crystal borophene on metal substrates and substantiates the idea of boran allotrope as a model for development of artificial 2D materials.
Abstract: Borophene, a theoretically proposed two-dimensional (2D) boron allotrope1–3, has attracted much attention4,5 as a candidate material platform for high-speed, transparent and flexible electronics6–9. It was recently synthesized, on Ag(111) substrates10,11, and studied by tunnelling and electron spectroscopy12. However, the exact crystal structure is still controversial, the nanometre-size single-crystal domains produced so far are too small for device fabrication and the structural tunability via substrate-dependent epitaxy is yet to be proven. We report on the synthesis of borophene monitored in situ by low-energy electron microscopy, diffraction and scanning tunnelling microscopy (STM) and modelled by ab initio theory. We resolved the crystal structure and phase diagram of borophene on Ag(111), but found that the domains remain nanoscale for all growth conditions. However, by growing borophene on Cu(111) surfaces, we obtained large single-crystal domains, up to 100 μm2 in size. The crystal structure is a novel triangular network with a concentration of hexagonal vacancies of η = 1/5. Our experimental data, together with first principles calculations, indicate charge-transfer coupling to the substrate without significant covalent bonding. Our work sets the stage for fabricating borophene-based devices and substantiates the idea of borophene as a model for development of artificial 2D materials. Low-energy electron microscopy enables controlled synthesis and characterization of (large) single-crystal borophene on metal substrates.

240 citations


Journal ArticleDOI
Richeng Lin1, Quanlin Guo1, Qun Zhu1, Yanming Zhu1, Wei Zheng1, Feng Huang1 
TL;DR: An all-inorganic lead-free CsCu2 I3 perovskite single crystal (SC) with stable and high photoluminescence quantum yield through strongly localized 1D exciton recombination is synthesized, which has great potential in energy-saving white lighting.
Abstract: Energy-saving white lighting from the efficient intrinsic emission of semiconductors is considered as a next-generation lighting source. Currently, white-light emission can be composited with a blue light-emitting diode and yellow phosphor. However, this solution has an inevitable light loss, which makes the improvement of the energy utilization efficiency more difficult. To deal with this problem, intrinsic white-light emission (IWE) in a single solid material gives a possibility. Here, an all-inorganic lead-free CsCu2 I3 perovskite single crystal (SC) with stable and high photoluminescence quantum yield (≈15.7%) IWE through strongly localized 1D exciton recombination is synthesized. In the CsCu2 I3 , the Cu-I octahedron, which provides most of electron states, is isolated by Cs atoms in two directions to form a 1D electronic structure, resulting a high radiation recombination rate of excitons. With this electronic structure design, the CsCu2 I3 SCs have great potential in energy-saving white lighting.

191 citations


Journal ArticleDOI
TL;DR: In this article, a low-temperature gradient crystallization (LTGC) method was proposed to obtain high-quality CH3NH3PbBr3 single crystals with lateral dimension as large as two inches.

170 citations


Journal ArticleDOI
TL;DR: One-dimensional (1D) ZnO nanorods were synthesized by a facile and effective hydrothermal method using the mixture of sodium dodecyl sulfate (SDS) and polyethylene glycol 400 (PEG400) with a molar ratio of 1:1 as the complex surfactant as mentioned in this paper.
Abstract: One-dimensional (1D) ZnO nanorods (ZNRs) were synthesized by a facile and effective hydrothermal method using the mixture of sodium dodecyl sulfate (SDS) and polyethylene glycol 400 (PEG400) with a molar ratio of 1:1 as the complex surfactant. The microstructure and morphology were characterized using of X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. The results demonstrated that the ZNRs are of a single crystal hexagonal wurtzite structure, having a larger length-to-diameter ratio with more regular surface morphology compared with the ZnO products obtained in the presence of only SDS or PEG400. A possible growth mechanism was proposed based the mediation reaction of the complex surfactant. Gas sensing measurements indicated that the ZNRs assisted by the complex surfactant demonstrated excellent ethanol sensing properties at an optimal operating temperature of 300 °C, which could be ascribed to their large length-to-diameter ratio, one-dimensional structure, and numerous surface defects of oxygen vacancies.

158 citations


Journal ArticleDOI
TL;DR: In this paper, the magnetic structure of MnBi$_2$Te$_4$ below T$_N$ was determined by powder and single crystal neutron diffraction measurements, which indicated that the magnetic order in Mn-Te layer has negligible effect on the electronic band structure.
Abstract: Millimeter-sized MnBi$_2$Te$_4$ single crystals are grown out of Bi-Te flux and characterized by measuring magnetic and transport properties, scanning tunneling microscope (STM) and spectroscopy (STS). The magnetic structure of MnBi$_2$Te$_4$ below T$_N$ is determined by powder and single crystal neutron diffraction measurements. Below T$_N$=24\,K, Mn$^{2+}$ moments order ferromagnetically in the \textit{ab} plane but antiferromagnetically along the crystallographic \textit{c} axis. The ordered moment is 4.04(13) $\mu_{B}$/Mn at 10\,K and aligned along the crystallographic \textit{c}-axis. The electrical resistivity drops upon cooling across T$_N$ or when going across the metamagnetic transition in increasing fields below T$_N$. A critical scattering effect was observed in the vicinity of T$_N$ in the temperature dependence of thermal conductivity. However, A linear temperature dependence was observed for thermopower in the temperature range 2K-300K without any anomaly around T$_N$. These indicate that the magnetic order in Mn-Te layer has negligible effect on the electronic band structure, which makes possible the realization of proposed topological properties in MnBi$_2$Te$_4$ after fine tuning of the electronic band structure.

151 citations


Journal ArticleDOI
TL;DR: A novel lead-free luminescent material with a unique zero-dimensional structure constituted by 3- octahedral and tetrahedral units, which exhibits broadband photoluminescence (PL) almost spanning the whole visible spectrum with a lifetime of 3.2 μs is reported.
Abstract: Low-dimensional lead halide perovskite materials recently have drawn much attention owing to the intriguing broadband emissions; however, the toxicity of lead will hinder their future development. Now, a lead-free (C4 H14 N2 )2 In2 Br10 single crystal with a unique zero-dimensional (0D) structure constituted by [InBr6 ]3- octahedral and [InBr4 ]- tetrahedral units is described. The single crystal exhibits broadband photoluminescence (PL) that spans almost the whole visible spectrum with a lifetime of 3.2 μs. Computational and experimental studies unveil that an excited-state structural distortion in [InBr6 ]3- octahedral units enables the formation of intrinsic self-trapped excitons (STEs) and thus contributing the broad emission. Furthermore, femtosecond transient absorption (fs-TA) measurement reveals that the ultrafast STEs formation together with an efficient intersystem crossing has made a significant contribution to the long-lived and broad STE-based emission behavior.

150 citations


Journal ArticleDOI
20 Mar 2019-Joule
TL;DR: In this article, an oxide-removal strategy was employed for polycrystalline hole-doped tin selenide (SnSe) alloyed with 5% lead selenides.

Journal ArticleDOI
TL;DR: In this article, a solid-state method was used to synthesize single crystals of perovskite-phase cesium lead iodide (γ-CsPbI3) that are kinetically stable at room temperature.
Abstract: We use a solid-state method to synthesize single crystals of perovskite-phase cesium lead iodide (γ-CsPbI3) that are kinetically stable at room temperature. Single crystal X-ray diffraction charact...

Journal ArticleDOI
TL;DR: In this paper, multi-particle nano-single crystal coalesced PtCu NSs are designed and successfully synthesized by a cost-effective aqueous solution method, which exhibits a superior hydrogen evolution reaction (HER) electrocatalytic activity with an ultralow onset potential of 18mV at the current density of 2mV and high mass activity of 1.08mV.

Journal ArticleDOI
TL;DR: In this paper, the thermal explosion technique was combined with selective laser melting (SLM) to synthesize the highly textured p-type Bi0.4Sb1.6Te3 bulk material.
Abstract: While zone-melted (ZM) Bi2Te3 is a standard commercially available thermoelectric (TE) material, it suffers from not being sufficiently mechanically robust due to the presence of the van der Waals bonded Te–Te layers that reduce the product yield and compromise operational reliability. Polycrystalline materials prepared by powder metallurgy techniques exhibit improved mechanical properties but usually lose the desired texture exhibited by ZM ingots, and this affects their TE performance. It is highly desirable to be able to fabricate Bi2Te3-based bulk materials with anisotropies similar to a single crystal, yet being mechanically strong as the polycrystalline specimens. Herein, we combine for the first time the thermal explosion technique with selective laser melting (SLM) to synthesize the highly textured p-type Bi0.4Sb1.6Te3 bulk material. Structural analysis (FESEM and XRD) indicates that the slender columnar grains grew along the building direction (BD) of the structure and the orientation factor reached up to 0.9, close to that representing a single crystal. TEM images revealed a high density of dislocations inside the grains. Since the printed compound has a high degree of texture, the TE and mechanical properties exhibit a highly anisotropic behavior. The maximum ZT of annealed samples parallel to the BD was 1.1, similar to that of the single crystal. However, the compressive strength of the structure reached up to 91 MPa, some 2.5 times the strength of a typical single crystal (37 MPa), and even higher than that of Spark Plasma Sintered (SPS) polycrystalline samples (80 MPa). Meanwhile, the mechanical cutting performance was much superior compared to that of the ZM ingot, and TE legs could be cut to sizes as small as 0.2 mm. A micro-TE module assembled using SLM-printed high performance p-type BiSbTe and SPS-compacted n-type BiTeSe materials showed the maximum cooling temperature difference of 62 °C. The work provides a facile and effective solution for preparation of Bi2Te3-based materials with high texture, robust mechanical properties, and excellent TE performance. As such, it lays a solid foundation for rapid in situ 3D printing of Bi2Te3-based micro-TE devices.

Journal ArticleDOI
TL;DR: In this article, a controlled evaporation process was used to grow large-size 2D hybrid perovskite (PEA) single crystal wafer with high mu-tau (μτ) product, superior environmental stability and irradiation resistance.
Abstract: Two-dimensional (2D) metal halide perovskites have shown great potential in high performance optoelectronic applications due to their intrinsic quantum well structure, enhanced moisture- and photo-stability. Unfortunately, there is still no effective method to produce large-size 2D hybrid perovskite single crystals, and consequently there is lack of research on its optoelectronic applications. Herein, we report the utilization of a controlled evaporation process to grow well-defined large-size (>200 mm2) 2D (PEA)2PbBr4 (C6H5CH2CH2NH3+, PEA+) single crystals. Upon careful examination of the crystal growth kinetics, it was found that the optimum temperature for the growth of (PEA)2PbBr4 single crystal wafer was 23 ± 0.5 °C. The wafers that were harvested showed high mu-tau (μτ) product, superior environmental stability and irradiation resistance. Furthermore, an array of planar-type UV photodetectors were designed and fabricated with extremely low dark current (∼10−13 A), large ON/OFF current ratio (∼105), very high specific detectivity (∼1013 cm Hz1/2 W−1) and fast response rate (∼0.4 ms). All the above performance data are among the best achieved compared to those of the state-of-the-art materials including ZnO, TiO2 and GaN in the field. It makes us believe that the availability of these materials may pave the way for ultrafast optical computing and optical communications.


Journal ArticleDOI
TL;DR: In a search for Pb-free photovoltaic materials, a double perovskite Cs2AgSbBr6 with an indirect optical bandgap of 1.64 eV has been synthesized, suggesting that the dark colour arises from the Sb3+-Sb5+ charge transfer.

Journal ArticleDOI
TL;DR: This work sys-tematically study the early stages of electrochemical oxidation of Cu(111) and polycrystalline Cu surfaces in different pH electro-lytes using in situ shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS).
Abstract: Investigating the chemical nature of the adsorbed intermediate species on well-defined Cu single crystal substrates is crucial in understanding many electrocatalytic reactions. Herein, we systemati...


Journal ArticleDOI
TL;DR: Results clearly indicate that both in reduced ceria powders as well as in reduced single crystal ceria films hydrogen may form hydroxyls at the surface and hydride species below the surface.
Abstract: The interaction of hydrogen with reduced ceria (CeO2-x ) powders and CeO2-x (111) thin films was studied using several characterization techniques including TEM, XRD, LEED, XPS, RPES, EELS, ESR, and TDS. The results clearly indicate that both in reduced ceria powders as well as in reduced single crystal ceria films hydrogen may form hydroxyls at the surface and hydride species below the surface. The formation of hydrides is clearly linked to the presence of oxygen vacancies and is accompanied by the transfer of an electron from a Ce3+ species to hydrogen, which results in the formation of Ce4+ , and thus in oxidation of ceria.

Journal ArticleDOI
TL;DR: Bulk single crystals of Co3Sn2S2 are synthesized that naturally hosts the band structure of a topological semimetal, guaranteeing the existence of robust TSS from the Co atoms, and emphasize the importance of tailoring TSS for the rational design of high-activity electrocatalysts.
Abstract: The band inversion in topological phase matters bring exotic physical properties such as the topologically protected surface states (TSS). They strongly influence the surface electronic structures of the materials and could serve as a good platform to gain insight into the surface reactions. Here we synthesized high-quality bulk single crystals of Co3Sn2S2 that naturally hosts the band structure of a topological semimetal. This guarantees the existence of robust TSS from the Co atoms. Co3Sn2S2 crystals expose their Kagome lattice that constructed by Co atoms and have high electrical conductivity. They serves as catalytic centers for oxygen evolution process (OER), making bonding and electron transfer more efficient due to the partially filled orbital. The bulk single crystal exhibits outstanding OER catalytic performance, although the surface area is much smaller than that of Co-based nanostructured catalysts. Our findings emphasize the importance of tailoring TSS for the rational design of high-activity electrocatalysts.

Journal ArticleDOI
TL;DR: In this paper, the authors synthesize high-quality bulk single crystals of the topological semimetal Co$_3$Sn$_2$S $_2$.
Abstract: The band inversion in topological phase matters bring exotic physical properties such as the emergence of a topologically protected surface states. They strongly influence the surface electronic structures of the investigated materials and could serve as a good platform to gain insight into the catalytic mechanism of surface reactions. Here we synthesized high-quality bulk single crystals of the topological semimetal Co$_3$Sn$_2$S$_2$. We found that at room temperature, Co$_3$Sn$_2$S$_2$ naturally hosts the band structure of a topological semimetal. This guarantees the existence of robust surface states from the Co atoms. Bulk single crystal of Co$_3$Sn$_2$S$_2$ exposes their Kagome lattice that constructed by Co atoms and have high electrical conductivity. They serves as catalytic centers for oxygen evolution process (OER), making bonding and electron transfer more efficient due to the partially filled $e_g$ orbital. The bulk single crystal exhibits outstanding OER catalytic performance, although the surface area is much smaller than that of Co-based nanostructured catalysts. Our findings emphasize the importance of tailoring topological non-trivial surface states for the rational design of high-activity electrocatalysts.

Journal ArticleDOI
TL;DR: Here, it is discussed how the effects of the elastic and plastic deformation of molecular crystals on the diffraction signature give primary evidence of their degree of crystallinity.
Abstract: The mention of the word "crystal" invokes images of minerals, gems, and rocks, all of which are inevitably solid, hard, and durable entities with well-defined smooth faces and straight edges. With the discovery in the first half of the 20th century that many molecular crystals are soft and can be deformed in a similar way as rubber or plastic, this perception is changing, and both the concept and formal definition of what a crystal is may require reinterpretation. The seemingly naive question posed in the title of this Minireview does not have a simple answer. Here, we discuss how the effects of the elastic and plastic deformation of molecular crystals on the diffraction signature give primary evidence of their degree of crystallinity. In most cases, the definition of a crystal holds for both elastically and plastically deformed crystals and, unless there is significant or complete physical separation of the crystal during the deformation, they can safely be considered (deformed) single crystals with a high concentration of defects.

Journal ArticleDOI
TL;DR: This work provides the first layered noncentrosymmetric semiconductor of edge-sharing MoS6 octahedra for the research of nonlinear optics.
Abstract: Noncentrosymmetric MoS2 semiconductors (1H, 3R) possess not only novel electronic structures of spin-orbit coupling (SOC) and valley polarization but also remarkable nonlinear optical effects. A more interesting noncentrosymmetric structure, the so-called 1T‴-MoS2 layers, was predicted to be built up from [MoS6] octahedral motifs by theoreticians, but the bulk 1T‴ MoS2 or its single crystal structure has not been reported yet. Here, we have successfully harvested 1T‴ MoS2 single crystals by a topochemical method. The new layered structure is determined from single-crystal X-ray diffraction. The crystal crystallizes in space group P31m with a cell of a = b = 5.580(2) A and c = 5.957(2) A, which is a √3 a × √3 a superstructure of 1T MoS2 with corner-sharing Mo3 triangular trimers observed by the STEM. 1T‴ MoS2 is verified to be semiconducting and possesses a band gap of 0.65 eV, different from metallic nature of 1T or 1T' MoS2. More surprisingly, the 1T‴ MoS2 does show strong optical second-harmonic generation signals. This work provides the first layered noncentrosymmetric semiconductor of edge-sharing MoS6 octahedra for the research of nonlinear optics.

Journal ArticleDOI
TL;DR: Wafer-size growth of a single-crystal Bi2O2Se film, which is a novel air-stable 2D semiconductor with high mobility, was achieved on insulating perovskite oxide substrates and provides an alternative platform of oxide heterostructure to investigate novel physical phenomena.
Abstract: Emerging two-dimensional (2D) semiconducting materials serve as promising alternatives for next-generation digital electronics and optoelectronics. However, large-scale 2D semiconductor films synthesized so far are typically polycrystalline with defective grain boundaries that could degrade their performance. Here, for the first time, wafer-size growth of a single-crystal Bi2O2Se film, which is a novel air-stable 2D semiconductor with high mobility, was achieved on insulating perovskite oxide substrates [SrTiO3, LaAlO3, (La, Sr)(Al, Ta)O3]. The layered Bi2O2Se epilayer exhibits perfect lattice matching and strong interaction with perovskite oxide substrates, which enable unidirectional alignment and seamless mergence of multiple seeds into single-crystal continuous films free of detrimental grain boundaries. The single-crystal Bi2O2Se thin films show excellent spatial homogeneity over the entire wafer and allow for the batch fabrication of high-performance field-effect devices with high mobilities of ∼150...

Journal ArticleDOI
27 Sep 2019-ACS Nano
TL;DR: This study opens a new way to synthesize uniform PtSe2 monolayers and other Pt-based heterostructures and shed considerable lights on optoelectronics in vdW solids consisting of weak and strong interlayer coupled materials.
Abstract: PtSe2, a layered two-dimensional transition-metal dichalcogenide (TMD), has drawn intensive attention owing to its layer-dependent band structure, high air stability, and spin-layer locking effect which can be used in various applications for next-generation optoelectronic and electronic devices or catalysis applications. However, synthesis of PtSe2 is highly challenging due to the low chemical reactivity of Pt sources. Here, we report the chemical vapor deposition of monolayer PtSe2 single crystals on MoSe2. The periodic Moire patterns from the vertically stacked heterostructure (PtSe2/MoSe2) are clearly identified via annular dark-field scanning transmission electron microscopy. First-principles calculations show a type II band alignment and reveal interface states originating from the strong-weak interlayer coupling (SWIC) between PtSe2 and MoSe2 monolayers, which is supported by the electrostatic force microscopy imaging. Ultrafast hole transfer between PtSe2 and MoSe2 monolayers is observed in the PtSe2/MoSe2 heterostructure, matching well with the theoretical results. Our study will shed light on the synthesis of Pt-based TMD heterostructures and boost the realization of SWIC-based optoelectronic devices.

Journal ArticleDOI
TL;DR: It is found that the amount of subsurface carbon in Cu foils directly correlates with the extent of adlayer growth, and high-performance field-effect transistors are readily fabricated in the large regions between adjacent parallel folds in the adlayer-free single crystal graphene film.
Abstract: To date, thousands of publications have reported chemical vapor deposition growth of "single layer" graphene, but none of them has described truly single layer graphene over large area because a fraction of the area has adlayers. It is found that the amount of subsurface carbon (leading to additional nuclei) in Cu foils directly correlates with the extent of adlayer growth. Annealing in hydrogen gas atmosphere depletes the subsurface carbon in the Cu foil. Adlayer-free single crystal and polycrystalline single layer graphene films are grown on Cu(111) and polycrystalline Cu foils containing no subsurface carbon, respectively. This single crystal graphene contains parallel, centimeter-long ≈100 nm wide "folds," separated by 20 to 50 µm, while folds (and wrinkles) are distributed quasi-randomly in the polycrystalline graphene film. High-performance field-effect transistors are readily fabricated in the large regions between adjacent parallel folds in the adlayer-free single crystal graphene film.

Journal ArticleDOI
TL;DR: In this article, the first spectroscopic alpha particle detection based on CsPbBr 3 detectors with asymmetric contacts was reported, which demonstrated excellent gamma ray resolving capability with a full width at half maximum (FWHM) of ∼ 5.9 keV for the 57Co 122 keV γ ray.
Abstract: Here we report the first spectroscopic alpha particle detection based on CsPbBr 3 detectors with asymmetric contacts. The CsPbBr3 single crystal was grown from the melt using Bridgman method and then fabricated into detectors with different contacts. The In/CsPbBr 3/Au detector presented a low dark current density ( ∼ 100 nA/cm2 ) and temporal stable performance under high electric field (1000 V/cm). Such detector demonstrated excellent gamma ray resolving capability with a full-width at half maximum (FWHM) of ∼ 5.9 keV for the 57Co 122 keV γ ray. The CsPbBr3 detector was capable of simultaneously resolving both the alpha particle (5.5 MeV) and γ ray (59.5 keV) peaks from 241Am radioactive isotope. The transport properties of CsPbBr3 were then determined based on the alpha particle spectra and corresponding rise time distributions. The equivalent values of electron and hole mobilities were indicated as 63 and 49 cm2/(V ⋅ s) respectively. The calculated electron and hole mobility-lifetime products were 4.5 × 10−4 and 9.5 × 10−4 cm2/V, respectively, demonstrating superior transport properties of holes over electrons in CsPbBr3 . This work widens the scope of perovskite detectors to encompass charged radiation as well as high energy X/ γ rays, and will significantly promote and guide further studies on perovskite materials for radiation detection applications.

Journal ArticleDOI
TL;DR: Solid-state methods are used to synthesize single crystals of perovskite-phase cesium lead iodide (γ-CsPbI3) that are kinetically stable at room temperature and provide vital parameters for theoretical and experimental investigations into perovswrite-phase CsPbi3 that will the guide the design and synthesis of atmospherically stable inorganic halide perovSKites.
Abstract: We use solid-state methods to synthesize single crystals of perovskite-phase cesium lead iodide (${\gamma}$-CsPbI3) that are kinetically stable at room temperature. Single crystal X-ray diffraction characterization shows that the compound is orthorhombic with the GdFeO3 structure at room temperature. Unlike conventional semiconductors, the optical absorption and the joint density-of-states of bulk ${\gamma}$-CsPbI3 is greatest near the band edge and decreases beyond Eg for at least 1.9 eV. Bulk ${\gamma}$-CsPbI3 does not show an excitonic resonance and has an optical band gap of 1.63(3) eV, ~90 meV smaller than has been reported in thin films; these and other differences indicate that previously-measured thin film ${\gamma}$-CsPbI3 shows signatures of quantum confinement. By flowing gases over ${\gamma}$-CsPbI3 during in situ powder X-ray diffraction measurements, we confirm that ${\gamma}$-CsPbI3 is stable to oxygen but rapidly and catalytically converts to non-perovskite ${\delta}$-CsPbI3 in the presence of moisture. Our results on bulk ${\gamma}$-CsPbI3 provide vital parameters for theoretical and experimental investigations into perovskite-phase CsPbI3 that will the guide the design and synthesis of atmospherically stable inorganic halide perovskites.

Journal ArticleDOI
TL;DR: In this article, the phase transition from Bernal bilayer graphene to single-layer diamond was studied and verified by X-ray photoelectron, ultraviolet photoelectRON, Raman, UV-Vis, electron energy loss spectroscopies, transmission electron microscopy, and DFT calculations.
Abstract: Notwithstanding numerous density functional studies on the chemically induced transformation of multilayer graphene into a diamond-like film, a comprehensive convincing experimental proof of such a conversion is still lacking. We show that the fluorination of graphene sheets in Bernal (AB)-stacked bilayer graphene (AB-BLG) grown by chemical vapor deposition on a single crystal CuNi(111) surface triggers the formation of interlayer carbon-carbon bonds, resulting in a fluorinated diamond monolayer (F-diamane). Induced by fluorine chemisorption, the phase transition from AB-BLG to single layer diamond was studied and verified by X-ray photoelectron, ultraviolet photoelectron, Raman, UV-Vis, electron energy loss spectroscopies, transmission electron microscopy, and DFT calculations.