arXiv subjects

Bilu Liu

Publications and source records attributed to Bilu Liu.

34 records · Page 2Linked to original sources

arXiv2020

Modulating Electronic Structure of Monolayer Transition Metal Dichalcogenides by Substitutional Nb-Doping

Modulating electronic structure of monolayer transition metal dichalcogenides (TMDCs) is important for many applications and doping is an effective way towards this goal, yet is challenging to control. Here we report the in-situ substitutional doping of niobium (Nb) into TMDCs with tunable concentrations during chemical vapour deposition. Taking monolayer WS2 as an example, doping Nb into its lattice leads to bandgap changes in the range 1.98 eV to 1.65 eV. Noteworthy, electrical transport measurements and density functional theory calculations show that the 4d electron orbitals of the Nb dopants contribute to the density of states of Nb-doped WS2 around the Fermi level, resulting in an n to p-type conversion. Nb-doping also reduces the energy barrier of hydrogen absorption in WS2, leading to an improved electrocatalytic hydrogen evolution performance. These results highlight the effectiveness of controlled doping in modulating the electronic structure of TMDCs and their use in electronic related applications.

cond-mat.mtrl-sci↗

arXiv2020

High-Fidelity Transfer of 2D Bismuth Oxyselenide and its Mechanical Properties

Two-dimensional (2D) bismuth oxyselenide (Bi2O2Se) with high electron mobility is advantageous in future high-performance and flexible electronic and optoelectronic devices. However, transfer of thin Bi2O2Se flakes is rather challenging, restricting measurements of its mechanical properties and application exploration in flexible devices. Here, we develop a reliable and effective polydimethylsiloxane (PDMS)-mediated method that allows transferring thin Bi2O2Se flakes from grown substrates onto target substrates like micro-electro-mechanical system substrates. The high fidelity of the transferred thin flakes stems from the high adhesive energy and flexibility of PDMS film. For the first time, the mechanical properties of 2D Bi2O2Se are experimentally acquired with nanoindentation method. We found that few-layer Bi2O2Se exhibits a large intrinsic stiffness of 18-23 GPa among 2D semiconductors, and a Young' s modulus of 88.7 +- 14.4 GPa which is consistent with the theoretical values. Furthermore, few-layer Bi2O2Se can withstand a high radial strain of more than 3%, demonstrating excellent flexibility. The development of the reliable transfer method and documentation of mechanical properties of 2D Bi2O2Se jointly fill the gap between theoretical prediction and experimental verification of mechanical properties of this emerging material, and will promote flexible electronics and optoelectronics based on 2D Bi2O2Se.

cond-mat.mtrl-sci↗

arXiv2020

High-Throughput Production of Cheap Mineral-Based 2D Electrocatalysts for High-Current-Density Hydrogen Evolution

The high-throughput scalable production of cheap, efficient and durable electrocatalysts that work well at high current densities demanded by industry is a great challenge for the large-scale implementation of electrochemical technologies. Here we report the production of a 2D MoS2-based ink-type electrocatalyst by a scalable top-down exfoliation technique followed by a simple heat treatment. The catalyst shows a high current density of 1000 mA cm^-2 at an overpotential of 454 mV for the hydrogen evolution reaction (HER) without the need of iR correction, as well as good stability over 24 hours. Using the same method, we have, for the first time, produced a cheap MoS2 mineral-based catalyst and found that it had an excellent performance for high-current-density HER. Noteworthy, production rate of this MoS2-based catalyst is one to two orders of magnitude higher than those previously reported. In addition, the price of the MoS2 mineral is five orders of magnitude lower than commercial Pt catalysts, making the MoS2 mineral-based catalyst cheap, and the ink-type catalyst dispersions can be easily integrated with other technologies for large-scale catalyst electrode preparation. These advantages indicate the huge potentials of this method and mineral-based cheap and abundant natural resources as catalysts in the electrochemical technologies.

physics.app-ph↗

arXiv2020

Synthesis of ultrahigh-quality monolayer molybdenum disulfide through in-situ defect healing with thiol molecules

Monolayer transition metal dichalcogenides (TMDCs) are two-dimensional (2D) materials with many potential applications. Chemical vapour deposition (CVD) is a promising method to synthesize these materials. However, CVD-grown materials generally have poorer quality than mechanically exfoliated ones and contain more defects due to the difficulties in controlling precursors' distribution and concentration during growth where solid precursors are used. Here, we propose to use thiol as a liquid precursor for CVD growth of high quality and uniform 2D MoS2. Atomic-resolved structure characterizations indicate that the concentration of sulfur vacancies in the MoS2 grown from thiol is the lowest among all reported CVD samples. Low temperature spectroscopic characterization further reveals the ultrahigh optical quality of the grown MoS2. Density functional theory simulations indicate that thiol molecules could interact with sulfur vacancies in MoS2 and repair these defects during the growth of MoS2, resulting in high quality MoS2. This work provides a facile and controllable method for the growth of high-quality 2D materials with ultralow sulfur vacancies and high optical quality, which will benefit their optoelectronic applications.

cond-mat.mtrl-sci↗

arXiv2020

High Yield Growth and Doping of Black Phosphorus with Tunable Electronic Properties

Black phosphorus (BP) has recently attracted significant interest due to its unique electronic and optical properties. Doping is an effective strategy to tune a material's electronic structures, however, the direct and controllable growth of BP with a high yield and its doping remain a great challenge. Here we report an efficient short-distance transport (SDT) growth approach and achieve the controlled growth of high quality BP with the highest yield so far, where 98% of the red phosphorus is converted to BP. The doping of BP by As, Sb, Bi, Se and Te are also achieved by this SDT growth approach. Spectroscopic results show that doping systematically changes its electronic structures including band gap, work function, and energy band position. As a result, we have found that the air-stability of doped BP samples (Sb and Te-doped BP) improves compared with pristine BP, due to the downshift of the conduction band minimum with doping. This work develops a new method to grow BP and doped BP with tunable electronic structures and improved stability, and should extend the uses of these class of materials in various areas.

cond-mat.mtrl-sci↗

arXiv2020

Giant magneto-birefringence effect and tuneable colouration of 2D crystals' suspensions

One of the long sought-after goals in manipulation of light through light-matter interactions is the realization of magnetic-field-tuneable colouration, so-called magneto-chromatic effect, which holds great promise for optical, biochemical and medical applications due to its contactless and non-invasive nature. This goal can be achieved by magnetic-field controlled birefringence, where colours are produced by the interference between phase-retarded components of transmitted polarised light. Thus far birefringence-tuneable coloration has been demonstrated using electric field, material chirality and mechanical strain but magnetic field control remained elusive due to either weak magneto-optical response of transparent media or low transmittance to visible light of magnetically responsive media, such as ferrofluids. Here we demonstrate magnetically tuneable colouration of aqueous suspensions of two-dimensional cobalt-doped titanium oxide which exhibit an anomalously large magneto-birefringence effect. The colour of the suspensions can be tuned over more than two wavelength cycles in the visible range by moderate magnetic fields below 0.8 T. We show that such giant magneto-chromatic response is due to particularly large phase retardation (>3 pi) of the polarised light, which in its turn is a combined result of a large Cotton-Mouton coefficient (three orders of magnitude larger than for known liquid crystals), relatively high saturation birefringence (delta n = 2 x 10^-4) and high transparency of our suspensions to visible light. The work opens a new avenue to achieve tuneable colouration through engineered magnetic birefringence and can readily be extended to other magnetic 2D nanocrystals. The demonstrated effect can be used in a variety of magneto-optical applications, including magnetic field sensors, wavelength-tuneable optical filters and see-through printing.

physics.app-ph↗

arXiv2020

Vertical CVD Growth of Highly Uniform Transition Metal Dichalcogenides

Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have attracted great attention due to their physical and chemical properties that make them promising in electronics and optoelectronics. Because of the difficulties in controlling concentrations of solid precursors and spatially non-uniform growth dynamics, it is challenging to grow wafer-scale 2D TMDCs with good uniformity and reproducibility so far, which significantly hinders their practical use. Here we report a vertical chemical vapor deposition (VCVD) design to grow monolayer TMDCs with a uniform density and high quality over the whole wafer, and with excellent reproducibility. The use of such VCVD design can easily control the three key growth parameters of precursor concentration, gas flow and temperature, which cannot be done in currently widely-used horizontal CVD system. Statistical results show that VCVD-grown monolayer TMDCs including MoS2 and WS2 are of high uniformity and quality on substrates over centimeter size. We also fabricated multiple van der Waals heterostructures by the one-step transfer of VCVD-grown TMDC samples, owning to its good uniformity. This work opens a way to grow 2D materials with high uniformity and reproducibility on the wafer scale, which can be used for the scalable fabrication of 2D materials and their heterostructures.

physics.app-ph↗

arXiv2020

Unsaturated Single Atoms on Monolayer Transition Metal Dichalcogenides for Ultrafast Hydrogen Evolution

Large scale implementation of electrochemical water splitting for hydrogen evolution requires cheap and efficient catalysts to replace expensive platinum. Molybdenum disulfide is one of the most promising alternative catalysts but its intrinsic activity is still inferior to platinum. There is therefore a need to explore new active site origins in molybdenum disulfide with ultrafast reaction kinetics and to understand their mechanisms. Here, we report a universal cold hydrogen plasma reduction method for synthesizing different single atoms sitting on two-dimensional monolayers. In case of molybdenum disulfide, we design and identify a new type of active site, i.e., unsaturated Mo single atoms on cogenetic monolayer molybdenum disulfide. The catalyst shows exceptional intrinsic activity with a Tafel slope of 35.1 mV dec-1 and a turnover frequency of ~10^3 s-1 at 100 mV, based on single flake microcell measurements. Theoretical studies indicate that coordinately unsaturated Mo single atoms sitting on molybdenum disulfide increase the bond strength between adsorbed hydrogen atoms and the substrates through hybridization, leading to fast hydrogen adsorption/desorption kinetics and superior hydrogen evolution activity. This work shines fresh light on preparing highly-efficient electrocatalysts for water splitting and other electrochemical processes, as well as provides a general method to synthesize single atoms on two-dimensional monolayers.

cond-mat.mtrl-sci↗

arXiv2020

Dissolution-Precipitation Growth of Uniform and Clean Two Dimensional Transition Metal Dichalcogenides

Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have attracted much interest and shown promise in many applications. However, it is challenging to obtain uniform TMDCs with clean surfaces, because of the difficulties in controlling the way the reactants are supplied to the reaction in the current chemical vapor deposition (CVD) growth process. Here, we report a new growth approach called dissolution-precipitation (DP) growth, where the metal sources are sealed inside glass substrates to control their feeding to the reaction. Noteworthy, the diffusion of metal source inside glass to its surface provides a uniform metal source on the glass surface, and restricts the TMDC growth to only a surface reaction while eliminates unwanted gas-phase reaction. This feature gives rise to highly-uniform monolayer TMDCs with a clean surface on centimeter-scale substrates. The DP growth works well for a large variety of TMDCs and their alloys, providing a solid foundation for the controlled growth of clean TMDCs by the fine control of the metal source.

cond-mat.mtrl-sci↗

arXiv2020

Mass Production of Two-Dimensional Materials by Intermediate-Assisted Grinding Exfoliation

The scalable and high-efficiency production of two-dimensional (2D) materials is a prerequisite to their commercial use. Currently, only graphene and graphene oxide can be produced on a ton scale, and the inability to produce other 2D materials on such a large scale hinders their technological applications. Here we report a grinding exfoliation method that uses micro-particles as force intermediates to resolve applied compressive forces into a multitude of small shear forces, inducing the highly-efficient exfoliation of layer materials. The method, referred to as intermediate-assisted grinding exfoliation (iMAGE), can be used for the large-scale production of many 2D materials. As an example, we have exfoliated bulk h-BN into 2D h-BN with large flake sizes, high quality and structural integrity, with a high exfoliation yield of 67%, a high production rate of 0.3 g h-1 and a low energy consumption of 3.01x10^6 J g-1. The production rate and energy consumption are one to two orders of magnitude better than previous results. Besides h-BN, this iMAGE technology has been used to exfoliate various layer materials such as graphite, black phosphorus, transition metal dichalcogenides, and metal oxides, proving its universality. Molybdenite concentrate, a natural low-cost and abundant mineral, was used as a demo for the large-scale exfoliation production of 2D MoS2 flakes. Our work indicates the huge potential of the iMAGE method to produce large amounts of various 2D materials, which paves the way for their commercial application.

physics.app-ph↗

arXiv2019

Anisotropic Moiré Optical Transitions in Twisted Monolayer/bilayer Phosphorene Heterostructures

Moiré superlattices of van der Waals heterostructures provide a powerful new way to engineer the electronic structures of two-dimensional (2D) materials. Many novel quantum phenomena have emerged in different moiré heterostructures, such as correlated insulators, superconductors, and Chern insulators in graphene systems and moiré excitons in transition metal dichalcogenide (TMDC) systems. Twisted phosphorene offers another attractive system to explore moiré physics because phosphorene features an anisotropic rectangular lattice, different from the isotropic hexagonal lattice in graphene and TMDC. Here we report emerging anisotropic moiré optical transitions in twisted monolayer/bilayer phosphorene. The optical resonances in phosphorene moiré superlattice depend sensitively on the twist angle between the monolayer and bilayer. Surprisingly, even for a twist angle as large as 19° the moiré heterostructure exhibits optical resonances completely different from those in the constituent monolayer and bilayer phosphorene. The new moiré optical resonances exhibit strong linear polarization, with the principal axis lying close to but different from the optical axis of bilayer phosphorene. Our ab initio calculations reveal that the Γ-point direct bandgap and the rectangular lattice of phosphorene, unlike the K-point bandgap of hexagonal lattice in graphene and TMDC, give rise to the remarkably strong moiré physics in large-twist-angle phosphorene heterostructures. Our results highlight the exciting opportunities to explore moiré physics in phosphorene and other van der Waals heterostructures with different lattice configurations.

cond-mat.mes-hall↗

arXiv2016

High Performance WSe2 Field-Effect Transistors via Controlled Formation of In-Plane Heterojunctions

Monolayer WSe2 is a two dimensional (2D) semiconductor with a direct bandgap, and it has been recently explored as a promising material for electronics and optoelectronics. Low field effect mobility is the main constraint preventing WSe2 from becoming one of the competing channel materials for field-effect transistors (FETs). Recent results have demonstrated that chemical treatments can modify the electrical properties of transition metal dichalcogenides (TMDCs) including MoS2 and WSe2. Here, we report that controlled heating in air significantly improves device performance of WSe2 FETs in terms of on-state currents and field-effect mobilities. Specifically, after heating at optimized conditions, chemical vapor deposition grown monolayer WSe2 FETs showed an average FET mobility of 31 cm2/Vs and on/off current ratios up to 5*108. For few-layer WSe2 FETs, after the same treatment applied, we achieved a high mobility up to 92 cm2/Vs. These values are significantly higher than FETs fabricated using as-grown WSe2 flakes without heating treatment, demonstrating the effectiveness of air heating on the performance improvements of WSe2 FETs. The underlying chemical processes involved during air heating and the formation of in-plane heterojunctions of WSe2 and WO3-x, which is believed to be the reason for the improved FET performance, were studied by spectroscopy and transmission electron microscopy. We further demonstrated that by combining air heating method developed in this work with supporting 2D materials on BN substrate, we achieved a noteworthy field effect mobility of 83 cm2/Vs for monolayer WSe2 FETs. This work is a step towards controlled modification of the properties of WSe2 and potentially other TMDCs, and may greatly improve device performance for future applications of 2D materials in electronics and optoelectronics.

cond-mat.mtrl-sci↗

arXiv2015

Black Arsenic-Phosphorus: Layered Anisotropic Infrared Semiconductors with Highly Tunable Compositions and Properties

Two-dimensional (2D) layered materials with diverse properties have attracted significant interest in the past decade. The layered materials discovered so far have covered a wide, yet discontinuous electromagnetic spectral range from semimetallic graphene, insulating boron nitride, to semiconductors with bandgaps from middle infrared to visible light. Here, we introduce new layered semiconductors, black arsenic-phosphorus (b-AsP), with highly tunable chemical compositions and electronic and optical properties. Transport and infrared absorption studies demonstrate the semiconducting nature of b-AsP with tunable bandgaps, ranging from 0.3 to 0.15 eV. These bandgaps fall into long-wavelength infrared (LWIR) regime and cannot be readily reached by other layered materials. Moreover, polarization-resolved infrared absorption and Raman studies reveal in-plane anisotropic properties of b-AsP. This family of layered b-AsP materials extend the electromagnetic spectra covered by 2D layered materials to the LWIR regime, and may find unique applications for future all 2D layered material based devices.

cond-mat.mtrl-sci↗

arXiv2015

Chemical Vapor Deposition Growth of Monolayer WSe2 with Tunable Device Characteristics and Growth Mechanism Study

Semiconducting transition metal dichalcogenides (TMDCs) have attracted a lot of attention recently, because of their interesting electronic, optical, and mechanical properties. Among large numbers of TMDCs, monolayer of tungsten diselenides (WSe2) is of particular interest since it possesses a direct band gap and tunable charge transport behaviors, which make it suitable for a variety of electronic and optoelectronic applications. Direct synthesis of large domains of monolayer WSe2 and their growth mechanism studies are important steps toward applications of WSe2. Here, we report systematical studies on ambient pressure chemical vapor deposition (CVD) growth of monolayer and few layer WSe2 flakes directly on silica substrates. The WSe2 flakes were characterized using optical microscopy, atomic force microscopy, Raman spectroscopy, and photoluminescence spectroscopy. We investigated how growth parameters, with emphases on growth temperatures and durations, affect the sizes, layer numbers, and shapes of as-grown WSe2 flakes. We also demonstrated that transport properties of CVD-grown monolayer WSe2, similar to mechanically-exfoliated samples, can be tuned into either p-type or ambipolar electrical behavior, depending on the types of metal contacts. These results deepen our understandings on the vapor phase growth mechanism of WSe2, and may benefit the uses of these CVD-grown monolayer materials in electronic and optoelectronics.

cond-mat.mtrl-sci↗

arXiv2014

Nearly Exclusive Growth of Small Diameter Semiconducting Single-Wall Carbon Nanotubes from Organic Chemistry Synthetic End-Cap Molecules

The inability to synthesize single-wall carbon nanotubes (SWCNTs) possessing uniform electronic properties and chirality represents the major impediment to their widespread applications. Recently, there is growing interest to explore and synthesize well-defined carbon nanostructures, including fullerenes, short nanotubes, and sidewalls of nanotubes, aiming for controlled synthesis of SWCNTs. One noticeable advantage of such processes is that no metal catalysts are used, and the produced nanotubes will be free of metal contamination. Many of these methods, however, suffer shortcomings of either low yield or poor controllability of nanotube uniformity. Here, we report a brand new approach to achieve high efficiency metal-free growth of nearly pure SWCNT semiconductors, as supported by extensive spectroscopic characterization, electrical transport measurements, and density functional theory calculations. Our strategy combines bottom-up organic chemistry synthesis with vapour phase epitaxy elongation. We identify a strong correlation between the electronic properties of SWCNTs and their diameters in nanotube growth. This study not only provides material platforms for electronic applications of semiconducting SWCNTs, but also contributes to fundamental understanding of the growth mechanism and controlled synthesis of SWCNTs.

cond-mat.mtrl-sci↗

arXiv2014

Screw-Dislocation-Driven Growth of Two-Dimensional Few-Layer and Pyramid-Like WSe2 by Sulfur-Assisted Chemical Vapor Deposition

Two-dimensional (2D) layered tungsten diselenides (WSe2) material has recently drawn a lot of attention due to its unique optoelectronic properties and ambipolar transport behavior. However, direct chemical vapor deposition (CVD) synthesis of 2D WSe2 is not as straightforward as other 2D materials due to the low reactivity between reactants in WSe2 synthesis. In addition, the growth mechanism of WSe2 in such CVD process remains unclear. Here we report the observation of a screw-dislocation-driven (SDD) spiral growth of 2D WSe2 flakes and pyramid-like structures using a sulfur-assisted CVD method. Few-layer and pyramid-like WSe2 flakes instead of monolayer were synthesized by introducing a small amount of sulfur as a reducer to help the selenization of WO3, which is the precursor of tungsten. Clear observations of steps, helical fringes, and herring-bone contours under atomic force microscope characterization reveal the existence of screw dislocations in the as-grown WSe2. The generation and propagation mechanisms of screw dislocations during the growth of WSe2 were discussed. Back-gated field-effect transistors were made on these 2D WSe2 materials, which show on/off current ratios of 106 and mobility up to 44 cm2/Vs.

cond-mat.mtrl-sci↗