Oxygen Self-Doping Bi2S3@C Spheric Successfully Enhanced Long-Term Performance in Lithium-Ion Batteries.

High theoretical capacity of Bi2S3 propels it toward an ideal anode material for lithium-ion batteries (LIBs); however, rapid capacity attenuation and poor long-term stability are major barriers to widespread application. In this work, an oxygen self-doping strategy was utilized to synthesize O-Bi2S3@C, significantly increasing the amount of active sites for lithium-ion storage. Meanwhile, sulfur vacancies were formed to improve the electrical conductivity and ionic transport efficiency, enhance the long-term stability, and accelerate the electrochemical kinetics of Bi2S3@C. O-BSC-S1:3 anode exhibits a reversible capacity of 673.1 mAh g-1 at 0.2 A g-1. It retains a long-term capacity of 596.3 mAh g-1 over 1100 cycles at a high density of 3 A g-1 in LIBs. Moreover, the installed O-Bi2S3@C//LiCoO2 full battery offers exceptional reversible capacity and remarkable cyclability (325.2 mAh g-1 after 200 cycles) at 0.2 A g-1. The combined strategy of oxygen self-doping and sulfur vacancy effectively enhances the reversible capacity and cycling life of Bi2S3, providing an approach for the design of high-performance transition metal sulfide anodes for LIBs.

Synergistically-mediated highly-efficient visible-light-driven hydrogen evolution activity using Ohmic/Schottky-type dual-junctions and sulfur vacancy.

Enabling highly-efficient multiplex-optimization photocatalysts is critical to overcome the bottlenecks of hydrogen evolution reaction efficiency and photostability. Herein, novel CoS/Sv-ZnIn2S4/MoS2 composites are successfully synthesized through an in situ technique. Taking advantage of the synergistic effect of sulfur vacancy, Schottky-type MoS2/Sv-ZnIn2S4 junction and Ohmic-type CoS/Sv-ZnIn2S4 junction, the light absorption, electron/hole separation efficiency, charge transfer rate and hydrogen reduction reaction dynamic can be significantly enhanced. As a result, an impressive photocatalytic hydrogen evolution rate of 18.43 mmol g-1 h-1 is achieved under the visible-light irradiation. Furthermore, apparent quantum efficiencies of 72.14 % and 9.91 % are also achieved under 350 and 420 nm monochromatic light irradiation. This work presents an in situ perspective to design multiplex-optimization photocatalytic system for highly-efficient hydrogen production.

Electrospun carbon nanofibers loaded with sulfur vacancy CoS2 as separator coating to accelerate sulfur conversion in Lithium-Sulfur batteries.

Lithium-sulfur batteries (LSBs) have been sought after by researchers owing to their high energy density; however, the inevitable capacity decay and slow reaction kinetics have hindered their advancement. Here, we prepare a Prussian blue analog, Co3[Co(CN)6]2 and synthesize carbon nanofibers/S vacancy CoS2-x (CNFs/CoS2-x) as electrocatalysts for separator coating via electrospinning, carbonization, sulfurization, and hydrogen reduction. CNFs/CoS2-x exhibits excellent electrocatalytic activity, wherein S vacancies induce the partial oxidation of Co2+ to Co3+ in CoS2 and CNFs provide long-range electron transport pathways. Various electrochemical tests, such as Tafel, ion diffusion coefficient, Li2S precipitation, and Li2S6 symmetric cells, further confirm the enhanced electrocatalytic activity. The LSBs with CNFs/CoS2-x modified separator delivers an initial discharge capacity of 1056.7 mAh g-1 at 0.2C, maintaining 840.8 mAh g-1 after 100 cycles at 0.2C. When S loading is increased to 4.42 mg cm-2, the battery retains a discharge capacity of 687.9 mAh g-1 (3.04 mAh cm-2) after 70 cycles at 0.1C. Our work can provide a reference for synthesizing anion-vacancy materials and designing anion-vacancy electrocatalytic composites for LSBs.

Synergistic manipulation of sulfur vacancies and palladium doping of In2S3 for enhanced photocatalytic H2 production.

In this study, a simple one-pot synthesis process is employed to introduce Pd dopant and abundant S vacancies into In2S3 nanosheets. The optimized Pd-doped In2S3 photocatalyst, with abundant S vacancies, demonstrates a significant enhancement in photocatalytic hydrogen evolution. The joint modification of Pd doping and rich S vacancies on the band structure of In2S3 result in an improvement in both the light absorption capacity and proton reduction ability. It is worth noting that photogenerated electrons enriched by S vacancies can rapidly migrate to adjacent Pd atoms through an efficient transfer path constructed by Pd-S bond, effectively suppressing the charge recombination. Consequently, the dual-defective In2S3 shows an efficient photocatalytic H2 production rate of 58.4 ± 2.0 µmol·h-1. Additionally, further work has been conducted on other ternary metal sulfide, ZnIn2S4. Our findings provide a new insight into the development of highly efficient photocatalysts through synergistic defect engineering.

Defect Density and Atomic Defect Recognition in the Middle Layer of a Trilayer MoS2 Stack.

Molybdenum disulfide (MoS2) is one of the most intriguing two-dimensional materials, and moreover, its single atomic defects can significantly alter the properties. These defects can be both imaged and engineered using spherical and chromatic aberration-corrected high-resolution transmission electron microscopy (CC/CS-corrected HRTEM). In a few-layer stack, several atoms are vertically aligned in one atomic column. Therefore, it is challenging to determine the positions of missing atoms and the damage cross-section, particularly in the not directly accessible middle layers. In this study, we introduce a technique for extracting subtle intensity differences in CC/CS-corrected HRTEM images. By exploiting the crystal structure of the material, our method discerns chalcogen vacancies even in the middle layer of trilayer MoS2. We found that in trilayer MoS2 the middle layer's damage cross-section is about ten times lower than that in the monolayer. Our findings could be essential for the application of few-layer MoS2 in nanodevices.

Ball-milled MoS2 with graphene shows enhanced catalytic activity for hydrogen evolution reaction.

The hydrogen evolution reaction (HER) is an important phenomenon in water splitting. Consequently, the development of an active, earth-abundant, and inexpensive HER catalyst is highly desired. MoS2 has drawn considerable interest as an HER catalyst because it is composed of non-precious metal and exhibits high catalytic activity in the nanosheet form. In this study, size-controlled MoS2 particles were synthesized by ball milling. The as-prepared samples exhibited significantly enhanced electrochemical and catalytic properties compared to those of pristine bulk MoS2. Furthermore, the HER activity improved further upon the introduction of graphene into the as-prepared ball-milled samples. In particular, the MoS2 sample ball-milled for 12 h mixed with graphene exhibited optimal performance, showing an overpotential (160 mV at 10 mA cm-2) that was ~ 335 mV lower than that of pristine bulk MoS2. The superior catalytic activity was ascribed to the exposed edge sites, sulfur vacancies, and 1T phase of MoS2, as well as the noteworthy fortifying effect of the electronically conductive flexible material, graphene. The results provide a promising strategy for its application as an efficient and stable HER catalyst.

Li et al. reported MoS₂-based electrocatalysts for the hydrogen evolution reaction. The superior catalytic activity was ascribed to exposed edge sites, sulfur vacancies, 1T phase, and the effect of graphene.

Phase Transformation on Multilayer 2M-WS2 for Improved Surface-enhanced Raman Scattering.

In recent years, two-dimensional (2D) transition metal dichalcogenides (TMDCs) have been widely recognized as an ideal platform for surface-enhanced Raman scattering (SERS). Given their rich structural phases, phase transformation in 2D TMDCs is an efficient strategy to tailor their SERS performance. In this paper, we present the great SERS performance of multilayer 2M-WS2 and then investigate the effect of its phase transformation on SERS performance. It is observed that multilayer 2M-WS2 nanosheets undergo a thermally induced single-crystal phase transition from 2M-WS2 to 2H-WS2 upon thermal annealing or laser treatment. Distinguishing from the commercially available pure 2H-WS2 (P-2H-WS2), 2H-WS2 obtained by annealing and laser treatment still retain SERS properties comparable to those of 2M-WS2, among which the detection limits for CV molecules (10-8 M) are 3 orders of magnitude lower than that of P-2H-WS2 and the Raman intensity enhancements are ∼10-37 times higher. In contrast to the charge transfer (CT) mechanism governed by the Fermi level in metallic-phase 2M-WS2, 2H-WS2 obtained by phase transition exhibits accelerated CT facilitated by the bandgap reduction and reorganization resulting from the abundance of vacancies. This study introduces an interesting perspective and potential avenue for enhancing SERS through metal-to-semiconductor phase transitions in 2D TMDCs materials.

Sulfur-Vacancy Engineering Accelerates Rapid Surface Reconstruction in Ni-Co Bimetal Sulfide Nanosheet for Urea Oxidation Electrocatalysis.

Developing a highly efficient catalyst for electrocatalytic urea oxidation reaction (UOR) is not only beneficial for the degradation of urea pollutants in wastewater but also provides a benign route for hydrogen production. Herein, a sulfur-vacancy (Sv) engineering is proposed to accelerate the formation of metal (oxy)hydroxide on the surface of Ni-Co bimetal sulfide nanosheet arrays on nickel foam (Sv-CoNiS@NF) for boosting the urea oxidation electrocatalysis. As a result, the obtained Sv-CoNiS@NF demonstrates an outstanding electrocatalytic UOR performance, which requires a low potential of only 1.397 V versus the reversible hydrogen electrode to achieve the current density of 100 mA cm-2. The ex situ Raman spectra and density functional theory calculations reveal the key roles of the Sv site and Co9S8 in promoting the electrocatalytic UOR performance. This work provides a new strategy for accelerating the transformation of electrocatalysts to active metallic (oxy)hydroxide for urea electrolysis via engineering the surface vacancies.

Additive-Assisted Hydrothermal Growth Enabling Defect Passivation and Void Remedy in Antimony Selenosulfide Solar Cells.

Antimony selenosulfide (Sb2(S,Se)3) has recently emerged as a promising light-absorbing material, attributed to its tunable photovoltaic properties, low toxicity, and robust environmental stability. However, despite these advantages, the current record efficiency for Sb2(S,Se)3 solar cells significantly lags behind their Shockley-Queisser limit, especially when compared to other well-established chalcogenide-based thin-film solar cells, such as CdTe and Cu(In,Ga)Se2. This underperformance primarily arises from the formation of unfavorable defects, predominately located at deep energy levels, which act as recombination centers, thereby limiting the potential for performance enhancement in Sb2(S,Se)3 solar cells. Specifically, deep-level defects, such as sulfur vacancy (VS), have a lower formation energy, leading to severe non-radiative recombination and compromising device performance. To address this challenge, thioacetamide (TA), a sulfur-containing additive is introduced, into the precursor solution for the hydrothermal deposition of Sb2(S,Se)3. This results indicate that the incorporation of TA helps in passivating deep-level defects such as sulfur vacancies and in suppressing the formation of large voids within the Sb2(S,Se)3 absorber. Consequently, Sb2(S,Se)3 solar cells, with reduced carrier recombination and improved film quality, achieved a power conversion efficiency of 9.04%, with notable improvements in open-circuit voltage and fill factor. This work provides deeper insights into the passivation of deep-level donor-like VS defects through the incorporation of a sulfur-containing additive, highlighting pathways to enhance the photovoltaic performance of Sb2(S,Se)3 solar cells.

Engineering sulfur defective Bi2S3@C with remarkably enhanced electrochemical kinetics of lithium-ion batteries.

Introducing the appropriate vacancies to augment the active sites and improve the electrochemical kinetics while maintaining high cyclability is a major challenge for its widespread application in electrochemical energy storage. Here, core-shell structured Bi2S3@C with sulfur vacancies was prepared by hydrothermal method and one-step carbonization/sulfuration process, which significantly improves the intrinsic electrical conductivity and ion transport efficiency of Bi2S3. Additionally, the uniform protective carbon layer around surface of composite maintains structural stability and effectively alleviates volume expansion during alloying/dealloying. As a result, the BSC-500 anode exhibits a brilliant reversible capacity of 636 mAh/g at 0.2 A/g and a long-term stable capacity of 524 mAh/g for 500 cycles at a high current density of 3 A/g in lithium-ion batteries. In addition, the assembled Bi2S3@C//LiCoO2 full cell delivered a capacity of 184 mAh/g at 1 A/g and excellent cyclability (125 mAh/g after 1000 cycles). The proposed strategy of combining sulfur vacancies with a core-shell structure to improve the electrochemical kinetics of Bi2S3 in lithium-ion batteries off the prospect for practical applications of transition metal sulfide anodes.

Sulfur Vacancies in Pyrite Trigger the Path to Nonradical Singlet Oxygen and Spontaneous Sulfamethoxazole Degradation: Unveiling the Hidden Potential in Sediments.

Pharmaceutical residues in sediments are concerning as ubiquitous emerging contaminants. Pyrite is the most abundant sulfide minerals in the estuarine and coastal sediments, making it a major sink for pharmaceutical pollutants such as sulfamethoxazole (SMX). However, research on the adsorption and redox behaviors of SMX on the pyrite surface is limited. Here, we investigated the impact of the nonphotochemical process of pyrite on the fate of coexisting SMX. Remarkably, sulfur vacancies (SVs) on pyrite promoted the generation of nonradical species (hydrogen peroxide, H2O2 and singlet oxygen, 1O2), thereby exhibiting prominent SMX degradation performance under darkness. Nonradical 1O2 contributed approximately 73.1% of the total SMX degradation. The SVs with high surrounding electron density showed an advanced affinity for adsorbing O2 and then initiated redox reactions in the sediment electron-storing geobattery pyrite, resulting in the extensive generation of H2O2 through a two-electron oxygen reduction pathway. Surface Fe(III) (hydro)oxides on pyrite facilitated the decomposition of H2O2 to 1O2 generation. Distinct nonradical products were observed in all investigated estuarine and coastal samples with the concentrations of H2O2 ranging from 1.96 to 2.94 µM, while the concentrations of 1O2 ranged from 4.63 × 10-15 to 8.93 × 10-15 M. This dark-redox pathway outperformed traditional photochemical routes for pollutant degradation, broadening the possibilities for nonradical species use in estuarine and coastal sediments. Our study highlighted the SV-triggered process as a ubiquitous yet previously overlooked source of nonradical species, which offered fresh insights into geochemical processes and the dynamics of pollutants in regions of frequent redox oscillations and sulfur-rich sediments.

Enhanced Hydrogen Evolution Catalysis of Pentlandite due to the Increases in Coordination Number and Sulfur Vacancy during Cubic-Hexagonal Phase Transition.

The search for new phases is an important direction in materials science. The phase transition of sulfides results in significant changes in catalytic performance, such as MoS2 and WS2. Cubic pentlandite [cPn, (Fe, Ni)9S8] can be a functional material in batteries, solar cells, and catalytic fields. However, no report about the material properties of other phases of pentlandite exists. In this study, the unit-cell parameters of a new phase of pentlandite, sulfur-vacancy enriched hexagonal pentlandite (hPn), and the phase boundary between cPn and hPn are determined for the first time. Compared to cPn, the hPn shows a high coordination number, more sulfur vacancies, and high conductivity, which result in significantly higher hydrogen evolution performance of hPn than that of cPn and make the non-nano rock catalyst hPn superior to other most known nanosulfide catalysts. The increase of sulfur vacancies during phase transition provides a new approach to designing functional materials.

A Full-Spectrum ZnS Photocatalyst with Gradient Distribution of Atomic Copper Dopants and Concomitant Sulfur Vacancies for Highly Efficient Hydrogen Evolution.

A rarely discussed phenomenon in the realm of photocatalytic materials involves the presence of gradient distributed dopants and defects from the interior to the surface. This intriguing characteristic has been successfully achieved in the case of ZnS through the incorporation of atomic monovalent copper ions (Cu+) and concurrent sulfur vacancies (Vs), resulting in a photocatalyst denoted as G-CZS1-x. Through the cooperative action of these atomic Cu dopants and Vs, G-CZS1-x significantly extends its photoabsorption range to encompass the full spectrum (200-2100 nm), which improves the solar utilization ability. This alteration enhances the efficiency of charge separation and optimizes Δ(H*) (free energy of hydrogen adsorption) to approach 0 eV for the hydrogen evolution reaction (HER). It is noteworthy that both surface-exposed atomic Cu and Vs act as active sites for photocatalysis. G-CZS1-x exhibits a significant H2 evolution rate of 1.01 mmol h-1 in the absence of a cocatalyst. This performance exceeds the majority of previously reported photocatalysts, exhibiting approximately 25-fold as ZnS, and 5-fold as H-CZS1-x with homogeneous distribution of equal content Cu dopants and Vs. In contrast to G-CZS1-x, the H adsorption on Cu sites for H-CZS1-x (ΔG(H*) = -1.22 eV) is excessively strong to inhibit the H2 release, and the charge separation efficiency for H-CZS1-x is relatively sluggish, revealing the positive role of a gradient distribution model of dopants and defects on activity enhancement. This work highlights the synergy of atomic dopants and defects in advancing photoactivity, as well as the significant benefit of the controllable distribution model of dopants and defects for photocatalysis.

MoS2 Field-Effect Transistor Performance Enhancement by Contact Doping and Defect Passivation via Fluorine Ions and Its Cyclic Field-Assisted Activation.

MoS2-based field-effect transistors (FETs) and, in general, transition metal dichalcogenide channels are fundamentally limited by high contact resistance (RC) and intrinsic defects, which results in low drive current and lower carrier mobilities, respectively. This work addresses these issues using a technique based on CF4 plasma treatment in the contacts and further cyclic field-assisted drift and activation of the fluorine ions (F-), which get introduced into the contact region during the CF4 plasma treatment. The F- ions are activated using cyclic pulses applied across the source-drain (S/D) contacts, which leads to their migration to the contact edges via the channel. Further, using ab initio molecular dynamics and density functional theory simulations, these F- ions are found to bond at sulfur (S) vacancies, resulting in their passivation and n-type doping in the channel and near the S/D contacts. An increase in doping results in the narrowing of the Schottky barrier width and a reduction in RC by ∼90%. Additionally, the passivation of S vacancies in the channel enhances the mobility of the FET by ∼150%. The CF4 plasma treatment in contacts and further cyclic field-assisted activation of F- ions resulted in an ON-current (ION) improvement by ∼90% and ∼480% for exfoliated and CVD-grown MoS2, respectively. Moreover, this improvement in ION has been achieved without any deterioration in the ION/IOFF, which was found to be >7-8 orders.

Sulfur vacancy-rich (α/ß-CdS)/SiO2 photocatalysts for enhanced visible-light-driven photocatalytic degradation of rhodamine B.

The development of highly efficient photocatalysts for visible-light-driven degradation of organic pollution is of great interest for wastewater purification. In this work, a sulfur vacancy-rich (α/ß-CdS)/SiO2 (α: hexagonal & ß: cubic) photocatalyst with a high catalytic activity was novelly synthesized on a nano-SiO2 carrier by the reaction of Cd2+ with a CS2 storage material (CS2SM) as sulfur source and crystalline modifiers. The dispersion of α/ß-CdS on the nano-SiO2 carrier significantly enhanced the visible-light-driven catalytic activity of (α/ß-CdS)/SiO2 photocatalyst, and 93.37 % rhodamine B (RhB) conversion was determined over 50 mg (α/ß-CdS)/SiO2 photocatalyst for 30 mL 400 mg/L RhB solution at light intensity of 150 mW/cm2 and 298.15 K. After five cycle tests, the (α/ß-CdS)/SiO2 photocatalyst still owned excellent visible-light-driven catalytic degradation stability (>90 %). The characterizations of morphology, functional groups, and photo-electrochemistry of (α/ß-CdS)/SiO2 photocatalyst demonstrated that nano-SiO2 as a carrier played meaningful role in dispersing α/ß-CdS and reducing agglomeration, thus increasing the active site of photocatalytic degradation reaction, and the presence of α/ß hetero-phase junctions and sulfur vacancies allows the rapid separation of photo-generated carriers and inhibits photo-generated electron-holes recombination. Meanwhile, the electron paramagnetic resonance (EPR) and free radical masking test have also proved that the main active species is ·O2- for the oxidation of RhB. Therefore, the work is providing a new reference to the visible-light-driven degradation of wastewater with high RhB concentration at room temperature.

Trifunctional L-Cysteine Assisted Construction of MoO2/MoS2/C Nanoarchitecture Toward High-Rate Sodium Storage.

The volume collapse and slow kinetics reaction of anode materials are two key issues for sodium ion batteries (SIBs). Herein, an "embryo" strategy is proposed for synthesis of nanorod-embedded MoO2/MoS2/C network nanoarchitecture as anode for SIBs with high-rate performance. Interestingly, L-cysteine which plays triple roles including sulfur source, reductant, and carbon source can be utilized to produce the sulfur vacancy-enriched heterostructure. Specifically, L-cysteine can combine with metastable monoclinic MoO3 nanorods at room temperature to encapsulate the "nutrient" of MoOx analogues (MoO2.5(OH)0.5 and MoO3·0.5H2O) and hydrogen-deficient L-cysteine in the "embryo" precursor affording for subsequent in situ multistep heating treatment. The resultant MoO2/MoS2/C presents a high-rate capability of 875 and 420 mAh g-1 at 0.5 and 10 A g-1, respectively, which are much better than the MoS2-based anode materials reported by far. Finite element simulation and analysis results verify that the volume expansion can be reduced to 42.8% from 88.8% when building nanorod-embedded porous network structure. Theoretical calculations reveal that the sulfur vacancies and heterointerface engineering can promote the adsorption and migration of Na+ leading to highly enhanced thermodynamic and kinetic reaction. The work provides an efficient approach to develop advanced electrode materials for energy storage.

Edge sulfur vacancies riched MoS2 nanosheets assist PEDOT:PSS flexible film ammonia sensing enhancement for wireless greenhouse vegetables monitoring.

Poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) is a promising NH3 sensing material owing to its super high electrical conductivity, excellent environmental stability, and reversible doping/dedoping nature. However, the low sensitivity and sluggish recovery rate limit its further application in gas sensors. Herein, exfoliated layered MoS2 nanosheets with large-specific surface area and abundant edge sulfur (S) vacancies are utilized to assist PEDOT:PSS and achieve ideal improvement in NH3 sensing performance at room temperature (RT), including high response values, fast response/recovery ability, and excellent sensing stability in complex environment. MoS2 nanosheets are combined with PEDOT:PSS to construct p-n heterojunction, the S vacancies can improve carrier transfer rate and serve as conductive bridge, effective active sites for NH3 adsorption, this series of performance improvement strategies is the significance of this work. Meanwhile, the density-functional theory (DFT), current-voltage (I-V), and in-situ FITR are firstly employed to discuss the sensing mechanisms in detail. Furthermore, integrating MoS2/PEDOT:PSS flexible sensor into a designed printed circuit board to intelligent, visual, and wireless real-time monitoring the NH3 resistance information in a simulated greenhouse vegetables equipment through the smartphone APP has also been successfully implemented.

Vacancy-Rich CoSx@LDH@Co-NC Catalytic Membrane for Antibiotic Degradation with Mechanistic Insights.

Improving the wettability of carbon-based catalysts and overcoming the rate-limiting step of the Mn+1/Mn+ cycle are effective strategies for activating peroxymonosulfate (PMS). In this study, the coupling of Co-NC, layered double hydroxide (LDH), and CoSx heterostructure (CoSx@LDH@Co-NC) was constructed to completely degrade ofloxacin (OFX) within 10 min via PMS activation. The reaction rate of 1.07 min-1 is about 1-2 orders of magnitude higher than other catalysts. The interfacial effect of confined Co-NC and layered double hydroxide (LDH) not only enhanced the wettability of catalysts but also increased the vacancy concentration; it facilitated easier contact with the interface reactive oxygen species (ROS). Simultaneously, reduced sulfur species (CoSx) accelerated the Co3+/Co2+ cycle, acquiring long-term catalytic activity. The catalytic mechanism revealed that the synergistic effect of hydroxyl groups and reduced sulfur species promoted the formation of 1O2, with a longer lifespan and a longer migration distance, and resisted the influence of nontarget background substances. Moreover, considering the convenience of practical application, the CoSx@LDH@Co-NC-based catalytic membrane was prepared, which had zero discharge of OFX and no decay in continuous operation for 5.0 h. The activity of the catalytic membrane was also verified in actual wastewater. Consequently, this work not only provides a novel strategy for designing excellent catalysts but also is applicable to practical organic wastewater treatment.

One-Step Passivation of Both Sulfur Vacancies and SiO2 Interface Traps of MoS2 Device.

Transition metal dichalcogenides (TMDs) benefit electrical devices with spin-orbit coupling and valley- and topology-related properties. However, TMD-based devices suffer from traps arising from defect sites inside the channel and the gate oxide interface. Deactivating them requires independent treatments, because the origins are dissimilar. This study introduces a single treatment to passivate defects in a multilayer MoS2 FET. By applying back-gate bias, protons from an H-TFSI droplet are injected into the MoS2, penetrating deeply enough to reach the SiO2 gate oxide. The characterizations employing low-temperature transport and deep-level transient spectroscopy (DLTS) studies reveal that the trap density of S vacancies in MoS2 drops to the lowest detection level. The temperature-dependent mobility plot on the SiO2 substrate resembles that of the h-BN substrate, implying that dangling bonds in SiO2 are passivated. The carrier mobility on the SiO2 substrate is enhanced by approximately 2200% after the injection.

Approaching Ohmic Contacts for Ideal Monolayer MoS2 Transistors Through Sulfur-Vacancy Engineering.

Field-effect transistors (FETs) made of monolayer 2D semiconductors (e.g., MoS2 ) are among the basis of the future modern wafer chip industry. However, unusually high contact resistances at the metal-semiconductor interfaces have seriously limited the improvement of monolayer 2D semiconductor FETs so far. Here, a high-scale processable strategy is reported to achieve ohmic contact between the metal and monolayer MoS2 with a large number of sulfur vacancies (SVs) by using simple sulfur-vacancy engineering. Due to the successful doping of the contact regions by introducing SVs, the contact resistance of monolayer MoS2 FET is as low as 1.7 kΩ·µm. This low contact resistance enables high-performance MoS2 FETs with ultrahigh carrier mobility of 153 cm2 V-1 s-1 , a large on/off ratio of 4 × 109 , and high saturation current of 342 µA µm-1 . With the comprehensive investigation of different SV concentrations by adjusting the plasma duration, it is also demonstrated that the SV-increased electron doping, with its resulting reduced Schottky barrier, is the dominant factor driving enhanced electrical performance. The work provides a simple method to promote the development of industrialized atomically thin integrated circuits.