Asynchronous Distributed ADMM for Large-Scale Optimization- Part I: Algorithm and Convergence Analysis

Aiming at solving large-scale learning problems, this paper studies distributed optimization methods based on the alternating direction method of multipliers (ADMM). By formulating the learning problem as a consensus problem, the ADMM can be used to solve the consensus problem in a fully parallel fashion over a computer network with a star topology. However, traditional synchronized computation does not scale well with the problem size, as the speed of the algorithm is limited by the slowest workers. This is particularly true in a heterogeneous network where the computing nodes experience different computation and communication delays. In this paper, we propose an asynchronous distributed ADMM (AD-AMM) which can effectively improve the time efficiency of distributed optimization. Our main interest lies in analyzing the convergence conditions of the AD-ADMM, under the popular partially asynchronous model, which is defined based on a maximum tolerable delay of the network. Specifically, by considering general and possibly non-convex cost functions, we show that the AD-ADMM is guaranteed to converge to the set of Karush-Kuhn-Tucker (KKT) points as long as the algorithm parameters are chosen appropriately according to the network delay. We further illustrate that the asynchrony of the ADMM has to be handled with care, as slightly modifying the implementation of the AD-ADMM can jeopardize the algorithm convergence, even under a standard convex setting.Comment: 37 page

Electric-field-induced strong enhancement of electroluminescence in multilayer molybdenum disulfide.

The layered transition metal dichalcogenides have attracted considerable interest for their unique electronic and optical properties. While the monolayer MoS2 exhibits a direct bandgap, the multilayer MoS2 is an indirect bandgap semiconductor and generally optically inactive. Here we report electric-field-induced strong electroluminescence in multilayer MoS2. We show that GaN-Al2O3-MoS2 and GaN-Al2O3-MoS2-Al2O3-graphene vertical heterojunctions can be created with excellent rectification behaviour. Electroluminescence studies demonstrate prominent direct bandgap excitonic emission in multilayer MoS2 over the entire vertical junction area. Importantly, the electroluminescence efficiency observed in multilayer MoS2 is comparable to or higher than that in monolayers. This strong electroluminescence can be attributed to electric-field-induced carrier redistribution from the lowest energy points (indirect bandgap) to higher energy points (direct bandgap) in k-space. The electric-field-induced electroluminescence is general for other layered materials including WSe2 and can open up a new pathway towards transition metal dichalcogenide-based optoelectronic devices

Large area growth and electrical properties of p-type WSe2 atomic layers.

Transition metal dichacogenides represent a unique class of two-dimensional layered materials that can be exfoliated into single or few atomic layers. Tungsten diselenide (WSe(2)) is one typical example with p-type semiconductor characteristics. Bulk WSe(2) has an indirect band gap (∼ 1.2 eV), which transits into a direct band gap (∼ 1.65 eV) in monolayers. Monolayer WSe(2), therefore, is of considerable interest as a new electronic material for functional electronics and optoelectronics. However, the controllable synthesis of large-area WSe(2) atomic layers remains a challenge. The studies on WSe(2) are largely limited by relatively small lateral size of exfoliated flakes and poor yield, which has significantly restricted the large-scale applications of the WSe(2) atomic layers. Here, we report a systematic study of chemical vapor deposition approach for large area growth of atomically thin WSe(2) film with the lateral dimensions up to ∼ 1 cm(2). Microphotoluminescence mapping indicates distinct layer dependent efficiency. The monolayer area exhibits much stronger light emission than bilayer or multilayers, consistent with the expected transition to direct band gap in the monolayer limit. The transmission electron microscopy studies demonstrate excellent crystalline quality of the atomically thin WSe(2). Electrical transport studies further show that the p-type WSe(2) field-effect transistors exhibit excellent electronic characteristics with effective hole carrier mobility up to 100 cm(2) V(-1) s(-1) for monolayer and up to 350 cm(2) V(-1) s(-1) for few-layer materials at room temperature, comparable or well above that of previously reported mobility values for the synthetic WSe(2) and comparable to the best exfoliated materials

A Highly Active Star Decahedron Cu Nanocatalyst for Hydrocarbon Production at Low Overpotentials

The electrochemical carbon dioxide reduction reaction (CO_2RR) presents a viable approach to recycle CO_2 gas into low carbon fuels. Thus, the development of highly active catalysts at low overpotential is desired for this reaction. Herein, a high‐yield synthesis of unique star decahedron Cu nanoparticles (SD‐Cu NPs) electrocatalysts, displaying twin boundaries (TBs) and multiple stacking faults, which lead to low overpotentials for methane (CH_4) and high efficiency for ethylene (C_2H_4) production, is reported. Particularly, SD‐Cu NPs show an onset potential for CH_4 production lower by 0.149 V than commercial Cu NPs. More impressively, SD‐Cu NPs demonstrate a faradaic efficiency of 52.43% ± 2.72% for C_2H_4 production at −0.993 ± 0.0129 V. The results demonstrate that the surface stacking faults and twin defects increase CO binding energy, leading to the enhanced CO_2RR performance on SD‐Cu NPs

Gate-induced insulator to band-like transport transition in organolead halide perovskite

Understanding the intrinsic charge transport in organolead halide perovskites is essential for the development of high-efficiency photovoltaics and other optoelectronic devices. Despite the rapid advancement of the organolead halide perovskite in photovoltaic and optoelectronic applications, the intrinsic charge carrier transport in these materials remains elusive partly due to the difficulty of fabricating electrical devices and obtaining good electrical contact. Here, we report the fabrication of organolead halide perovskite microplates with monolayer graphene as low barrier electrical contact. A systematic charge transport studies reveal an insulator to band-like transport transition. Our studies indicate that the insulator to band-like transport transition depends on the orthorhombic-to-tetragonal phase transition temperature and defect densities of the organolead halide perovskite microplates. Our findings are not only important for the fundamental understanding of charge transport behavior but also offer valuable practical implications for photovoltaics and optoelectronic applications based on the organolead halide perovskite.Comment: 18 pages, 5 figure

Enhanced interlayer neutral excitons and trions in trilayer van der Waals heterostructures

Vertically stacked van der Waals heterostructures constitute a promising platform for providing tailored band alignment with enhanced excitonic systems. Here we report observations of neutral and charged interlayer excitons in trilayer WSe2-MoSe2-WSe2 van der Waals heterostructures and their dynamics. The addition of a WSe2 layer in the trilayer leads to significantly higher photoluminescence quantum yields and tunable spectral resonance compared to its bilayer heterostructures at cryogenic temperatures. The observed enhancement in the photoluminescence quantum yield is due to significantly larger electron-hole overlap and higher light absorbance in the trilayer heterostructure, supported via first-principle pseudopotential calculations based on spin-polarized density functional theory. We further uncover the temperature- and power-dependence, as well as time-resolved photoluminescence of the trilayer heterostructure interlayer neutral excitons and trions. Our study elucidates the prospects of manipulating light emission from interlayer excitons and designing atomic heterostructures from first-principles for optoelectronics.Comment: 25 pages, 5 figures(Maintext). 9 pages, 7 figures(Supplementary Information). - Accepted for publication in npg: 2D materials and applications and reformatted to its standard. - Updated co-authors and references. - Title and abstract are modified for clarity. - Errors have been corrected, npg: 2D materials and applications (2018

Electroluminescence and photocurrent generation from atomically sharp WSe2/MoS2 heterojunction p-n diodes

The p-n diodes represent the most fundamental device building block for diverse optoelectronic functions, but are difficult to achieve in atomically thin transition metal dichalcogenides (TMDs) due to the inability to selectively dope them into p- or n-type semiconductors. Here we report the first demonstration of an atomically thin and atomically sharp heterojunction p-n diode by vertically stacking p-type monolayer tungsten diselenide (WSe2) and n-type few-layer molybdenum disulfide (MoS2). Electrical measurement demonstrates excellent diode characteristics with well-defined current rectification behaviour and an ideality factor of 1.2. Photocurrent mapping shows fast photoresponse over the entire overlapping region with a highest external quantum efficiency up to 12 %. Electroluminescence studies show prominent band edge excitonic emission and strikingly enhanced hot electron luminescence. A systematic investigation shows distinct layer-number dependent emission characteristics and reveals important insight about the origin of hot-electron luminescence and the nature of electron-orbital interaction in TMDs. We believe that these atomically thin heterojunction p-n diodes represent an interesting system for probing the fundamental electro-optical properties in TMDs, and can open up a new pathway to novel optoelectronic devices such as atomically thin photodetectors, photovoltaics, as well as spin-/valley-polarized light emitting diodes and on-chip lasers.Comment: 27 pages, 7 figure