Ionic Glass–Gated 2D Material–Based Phototransistor: MoSe2 over LaF3 as Case Study

Modulating the carrier density of 2D materials is pivotal to tailor their electrical properties, with novel physical phenomena expected to occur at a higher doping level. Here, the use of ionic glass as a high capacitance gate is explored to develop a 2D material–based phototransistor operated with a higher carrier concentration up to 5 × 10¹³ cm^?2, using MoSe₂ over LaF₃ as an archetypal system. Ion glass gating reveals to be a powerful technique combining the high carrier density of electrolyte gating methods while enabling direct optical addressability impeded with usual electrolyte technology. The phototransistor demonstrates I_ON/I_OFF ratio exceeding five decades and photoresponse times down to 200 µs, up to two decades faster than MoSe₂ phototransistors reported so far. Careful phototransport analysis reveals that ionic glass gating of 2D materials allows tuning the nature of the carrier recombination processes, while annihilating the traps' contribution in the electron injection regime. This remarkable property results in a photoresponse that can be modulated electrostatically by more than two orders of magnitude, while at the same time increasing the gain bandwidth product. This study demonstrates the potential of ionic glass gating to explore novel photoconduction processes and alternative architectures of devices.     

Machine Vision Based on an Ultra-Wide Bandgap 2D Semiconductor AsSbO3

Facing the future development trend of miniaturization and intelligence of electronic devices, solar-blind photodetectors based on ultrawide-bandgap 2D semiconductors have the advantages of low dark current, and high signal-to-noise ratio, as well as the features of micro-nanometer miniaturization and multi-functionalization of 2D material devices, which have potential applications in the photoelectric sensor part of high-performance machine vision systems. This study reports a 2D oxide semiconductor, AsSbO₃, with an ultrawide bandgap (4.997 eV for monolayer and 4.4 eV for multilayer) to be used to fabricate highly selective solar-blind UV photodetectors, of which the dark current as low as 100 fA and rejection ratio of UV-C and UV-A reaches 7.6 × 10³. Under 239 nm incident light, the responsivity is 105 mA W⁻¹ and the detectivity is 7.58 × 10¹² Jones. Owing to the remarkable anisotropic crystal structure, AsSbO₃ also shows significant linear dichroism and nonlinear optical properties. Finally, a simple machine vision system is simulated by combining the real-time imaging function in solar-blind UV with a convolutional neural network. This study enriches the material system of ultrawide-bandgap 2D semiconductors and provides insight into the future development of high-performance solar-blind UV optoelectronic devices.     

Vertical-type 3D/Quasi-2D n-p Heterojunction Perovskite Photodetector

This research demonstrates a state-of-the-art vertical-transport photodetector with an n-type 3D MAPbI₃/p-type quasi-2D (Q-2D) BA₂MA₂Pb₃I₁₀ perovskite heterojunction. This structure introduces a ≈0.6 V built-in electric field at the n-p junction that greatly improves the characteristics of the perovskite photodetector, and the presence of Q-2D perovskite on the surface improves the life. The electrical polarities of the 3D and the Q-2D perovskite layers are simply controlled by self-constituent doping, making clearly defined n-p characteristics. Doctor-blade coating is used to fabricate the photodetector with a large area. The Q-2D materials with highly oriented (040) Q-2D (n = 2,3) planes are near the surface, and the (111) preferred planes mixed with high index Q-2D materials (n = 4,5) are found near the 3D/Q-2D interface. The stacking and interface are beneficial for carrier extraction and transport, yielding an external quantum efficiency of 77.9%, a carrier lifetime long as 295.7 ns, and a responsibility of 0.41 A W⁻¹. A low dark current density of 6.2 × 10⁻⁷ mA cm⁻² and a high detectivity of 2.82 × 10¹³ Jones are obtained. Rise time and fall time are fast as 1.33 and 10.1 µs, respectively. The results show the application potential of 3D/Q-2D n-p junction perovskite photodetectors.     

All-Inorganic CsPbBr3 Perovskite Nanocrystals/2D Non-Layered Cadmium Sulfide Selenide for High-Performance Photodetectors by Energy Band Alignment Engineering

Perovskites have attracted intensive attention as promising materials for the application in various optoelectronic devices due to their large light absorption coefficient, high carrier mobility, and long charge carrier diffusion length. However, the performance of the pure perovskite nanocrystals-based device is extremely restricted by the limited charge transport capability due to the existence of a large number of the grain boundary between perovskite nanocrystals. To address these issues, a high-performance photodetector based on all-inorganic CsPbBr₃ perovskite nanocrystals/2D non-layered cadmium sulfide selenide heterostructure has been demonstrated through energy band engineering with designed typed-II heterostructure. The photodetector exhibits an ultra-high light-to-dark current ratio of 1.36 × 10⁵, a high responsivity of 2.89 × 10² A W⁻¹, a large detectivity of 1.28 × 10¹⁴ Jones, and the response/recovery time of 0.53s/0.62 s. The enhancement of the optoelectronic performance of the heterostructure photodetector is mainly attributed to the efficient charge carrier transfer ability between the all-inorganic CsPbBr₃ perovskites and 2D cadmium sulfide selenide resulting from energy band alignment engineering. The charge carriers’ transfer dynamics and the mechanism of the CsPbBr₃ perovskites/2D non-layered nanosheets interfaces have also been studied by state-state PL spectra, fluorescence lifetime imaging microscopy, time-resolved photoluminescence spectroscopy, and Kelvin probe force microscopy measurements.     

Gate-Controlled Polarity-Reversible Photodiodes with Ambipolar 2D Semiconductors

A photosensor with an amplitude-tunable and polarity-reversible response under gate modulation has potential as a computational photosensor, which can provide more recognition degree of data to enhance signal processing efficiency. Although, the ambipolar 2D semiconductors possess unique gate-tunable properties, the question of how to utilize this property to design polarity-reversible photodiodes for intelligent applications remains unanswered. Here, gate-controllable polarity-reversible photodiodes based on ambipolar 2D semiconductors with an asymmetrically metal-contacted architecture are proposed. By controlling the gate-field, the local carrier type and density profile can be manipulated in the channel due to the partial shielding feature of the asymmetrically metal-contacted architecture, resulting in a polarity-reversible photodiode. The reported WSe₂-based photodiode possesses excellent rectifying behavior with a rectification ratio over 10⁵, photovoltaic performance with 90% external quantum efficiency, and 2.3% power conversion efficiency under gate regulation. Meanwhile, the device exhibits reversible polarity of photovoltage from a negative to positive state under gate control. By utilizing the reversible photovoltage of the WSe₂ photodiode, an optoelectronic switch with a photovoltage polarity signal is demonstrated without a bias voltage. This photovoltage-reversible homodiode paves the way to develop 2D devices with multiple operation modes for potential applications in high-efficiency photovoltaics, intelligent vision sensors, and logic optoelectronics.     

Large‐Area Chemical Vapor Deposited MoS2 with Transparent Conducting Oxide Contacts toward Fully Transparent 2D Electronics

2D semiconductors are poised to revolutionize the future of electronics and photonics, much like transparent oxide conductors and semiconductors have revolutionized the display industry. Herein, these two types of materials are combined to realize fully transparent 2D electronic devices and circuits. Specifically, a large‐area chemical vapor deposition process is developed to grow monolayer MoS₂ continuous films, which are, for the first time, combined with transparent conducting oxide (TCO) contacts. Transparent conducting aluminum doped zinc oxide contacts are deposited by atomic layer deposition, with composition tuning to achieve optimal conductivity and band‐offsets with MoS₂. The optimized process gives fully transparent TCO/MoS₂ 2D electronics with average visible‐range transmittance of 85%. The transistors show high mobility (4.2 cm² V^?1 s^?1), fast switching speed (0.114 V dec^?1), very low threshold voltage (0.69 V), and large switching ratio (4 × 10⁸). To our knowledge, these are the lowest threshold voltage and subthreshold swing values reported for monolayer chemical vapor deposition MoS₂ transistors. The transparent inverters show fast switching properties with a gain of 155 at a supply voltage of 10 V. The results demonstrate that transparent conducting oxides can be used as contact materials for 2D semiconductors, which opens new possibilities in 2D electronic and photonic applications.     

3D/2D Perovskite Single Crystals Heterojunction for Suppressed Ions Migration in Hard X-Ray Detection

Halide perovskites exhibit diverse properties depending on their compositions. However, integrating desired properties into one material is still challenging. Here, a facile solution-processed epitaxial growth method to grow 2D perovskite single crystal on top of 3D perovskite single crystal, which can passivate the surface defects for improved device performance is reported. Short formamidine (FA⁺) ions are replaced by long organic cations, which can fully align and cover the single crystal surface to prevent the ions migration or short FA⁺ ions volatilization. The thickness of epitaxial layer can be finely adjusted by controlling the growth time. The defect density of single crystals heterojunction is only 3.18 × 10⁹ cm⁻³, and the carrier mobility is 80.43 cm² V⁻¹ s⁻¹, which is greater than that of the control 3D perovskite single crystal. This study for the first time realized large area 3D/2D perovskite single crystals heterojunction, which suppressed ions migration and exhibited advanced performance in hard X-rays detection applications. This strategy also provides a way to grow large area 2D perovskite single crystal from solution processes.     

Electrical Interrogation of Thickness-Dependent Multiferroic Phase Transitions in the 2D Antiferromagnetic Semiconductor NiI2

2D magnetic materials hold promise for quantum and spintronic applications. 2D antiferromagnetic materials are of particular interest due to their relative insensitivity to external magnetic fields and higher switching speeds compared to 2D ferromagnets. However, their lack of macroscopic magnetization impedes detection and control of antiferromagnetic order, thus motivating magneto-electrical measurements for these purposes. Additionally, many 2D magnetic materials are ambient-reactive and electrically insulating or highly resistive below their magnetic ordering temperatures, which imposes severe constraints on electronic device fabrication and characterization. Herein, these issues are overcome via a fabrication protocol that achieves electrically conductive devices from the ambient-reactive 2D antiferromagnetic semiconductor NiI₂. The resulting gate-tunable transistors show band-like electronic transport below the antiferromagnetic and multiferroic transition temperatures of NiI₂, revealing a Hall mobility of 15 cm² V⁻¹ s⁻¹ at 1.7 K. These devices also allow direct electrical probing of the thickness-dependent multiferroic phase transition temperature of NiI₂ from 59 K (bulk) to 28 K (monolayer).     

Visualizing Piezoelectricity on 2D Crystals Nanobubbles

2D crystals with noncentrosymmetric structures exhibit piezoelectric properties that show great potential for applications in energy conversion and electromechanical devices. Quantitative visualization of piezoelectric field spatial distribution is expected to offer a better understanding of macroscopic piezoelectricity, yet remains to be realized. Here, a technique of mapping piezoelectric potential on 2D materials bubbles based on the measurements of surface potential using kelvin probe force microscope is reported. By using odd number of layers hexagonal boron nitride and MoS₂ nanobubbles, strain-induced piezoelectric potential profiles are quantitatively visualized on the bubbles. The obtained piezoelectric coefficient is 3.4 ± 1.2 × 10⁻¹⁰ C m⁻¹ and 3.3 ± 0.2 × 10⁻¹⁰ C m⁻¹ for hBN and MoS₂, in agreement with the values reported. On the contrary, homogeneous distribution of surface potential is measured on even number of layers crystals bubbles where the crystal's inversion symmetry is restored. Using such technique, in situ visualization of photogenerated charge carrier separation under piezoelectric potential is also achieved, which offers a platform of investigating the coupling between piezoelectricity and photoelectric effect, and an approach of tuning piezoelectric field. The present work should aid the understanding of local piezoelectric potential and its various affecting factors including substrate doping and external stimuli, and give insights for designing piezoelectric nanodevices based on 2D nanobubbles.     

Large-Size Ultrathin α-Ga2S3 Nanosheets toward High-Performance Photodetection

Following the extensive researches of graphene, 2D layered semiconductors have attracted widespread attention for their intriguing physical properties. 2D α-Ga₂S₃ as an important member of group III_A–VI_A semiconductors has outstanding optoelectronic properties. However, the controllable large-size synthesis of ultrathin α-Ga₂S₃ nanosheets still remains a huge challenge. In this paper, a large-size ultrathin nanosheets of hexagonal Ga₂S₃ is prepared via an improved chemical vapor deposition method. High-performance photodetectors based on the ultrathin Ga₂S₃ nanosheets is demonstrated. The device shows a high photosensitivity/detectivity (9.2 A W⁻¹/1.4 × 10¹² Jones) and a fast response time (rise/fall time of <4/3 ms), respectively. Strikingly, wearable flexible photodetectors based on Ga₂S₃ nanosheets are fabricated accordingly and demonstrate great response performance and stability. This work provides a new direction for 2D semiconductors to apply in next-generation nanoscale smart optoelectronics.     

Electrically Dynamic Configurable WSe2 Transistor and the Applications in Photodetector

Non-destructive and reversible modulations of polarity and carrier concentration in transistors are essential for complementary devices. The fabricated multi-gated WSe₂ devices obtain dynamic electrostatic field induced electrically configurable functions and demonstrate as diode with high rectification ratio of 4.1 × 10⁵, as well as n- and p-type inverter with voltage gain of 19.9 and 12.1, respectively. Benefiting from the continuous band alignment induced modulation of channel underneath the dual gates, the devices exhibit high-performance photodetection in wide spectral range. The devices yield high photo-responsivity (5.16 A W⁻¹) and large I_light/I_dark ratio (1 × 10⁵). Besides, the local gate fields accelerate the separation of photo-induced carriers, leading to fast response without persistent current. This strategy takes the advantage of the simplified design and continues to deliver integrated circuits with high density. The superior electrical and photodetection characteristics exhibit great potency in the domain of future optoelectronics.     

High-Resolution and Stable Ruddlesden–Popper Quasi-2D Perovskite Flexible Photodetectors Arrays for Potential Applications as Optical Image Sensor

The development of an efficient fabrication route to achieve high-resolution perovskite pixel array is key for large-scale flexible image sensor devices. Herein, a high-resolution and stable 10 × 10 flexible PDs array based on formamidinium(FA⁺) and phenylmethylammonium (PMA⁺) quasi-2D (PMA)₂FAPb₂I₇ (n = 2) perovskite is demonstrated by developing SiO₂-assisted hydrophobic and hydrophilic treatment process on polyethylene terephthalate substrate. By introducing Au nanoparticles (Au NPs),  the perovskite film quality is improved and grain boundaries are reduced. The mechanism by which Au NPs upgrade the photoelectric quality of perovskite is mainly revealed by glow discharge-optical emission spectroscopy (GD-OES) and grazing-incidence wide-angle X-ray scattering (GIWAXS). To further improve the photoelectric performance of the devices, a post-treatment strategy with formamidinium chloride (FACl) is used . The optimized flexible PDs arrays show excellent optoelectronic properties with a high responsivity of 4.7 A W⁻¹, a detectivity of 6.3 × 10¹² Jones, and a broad spectral sensitivity. The device also exhibits excellent electrical stability even under severe bending and excellent flexural strength, as well as excellent environmental stability. Finally, the integrated flexible PDs arrays are used as sensor pixels in an imaging system to obtain high-resolution imaging patterns, demonstrating the imaging capability of the PDs arrays.     

Graphene-Enhanced Metal Transfer Printing for Strong van der Waals Contacts between 3D Metals and 2D Semiconductors

2D semiconductors have shown great potentials for ultra-short channel field-effect transistors (FETs) in next-generation electronics. However, because of intractable surface states and interface barriers, it is challenging to realize high-quality contacts with low contact resistances for both p- and n- 2D FETs. Here, a graphene-enhanced van der Waals (vdWs) integration approach is demonstrated, which is a multi-scale (nanometer to centimeter scale) and reliable (≈100% yield) metal transfer strategy applicable to various metals and 2D semiconductors. Scanning transmission electron microscopy imaging shows that 2D/2D/3D semiconductor/graphene/metal interfaces are atomically flat, ultraclean, and defect-free. First principles calculations indicate that the sandwiched graphene monolayer can eliminate gap states induced by 3D metals in 2D semiconductors. Through this approach, Schottky barrier-free contacts are realized on both p- and n-type 2D FETs, achieving p-type MoTe₂, p-type black phosphorus and n-type MoS₂ FETs with on-state current densities of 404, 1520, and 761 µA µm⁻¹, respectively, which are among the highest values reported in literature.     

Highly Sensitive Self-Powered 2D Perovskite Photodiodes with Dual Interface Passivations

2D perovskites have attracted intensive attention by virtue of their excellent optical and electrical properties along with good stabilities. Herein, a highly sensitive self-powered photodiode based on (PEA)₂(MA)₄Pb₅I₁₆ (PEA=C₆H₅(CH₂)NH₃, MA=CH₃NH₃) 2D perovskite is demonstrated by dual interface passivations. The Al₂O₃ bottom passivation can reduce the pinhole defects in the 2D perovskite film and suppress the trap-related recombination loss, bringing forward much reduced dark current and increased photocurrent. The poly (methyl methacrylate) (PMMA) top passivation can encapsulate the 2D perovskite film and thus improve the stability of the device. These results show that the 2D perovskite-based photodiode with dual interface passivations exhibits a large photo-to-dark current ratio of 10⁷, a fast response speed of 597 ns and a linear dynamic range of 160 dB without bias. Responsivity (R) and detectivity (D*) respectively reach 0.36 A W⁻¹ and 5.4 × 10¹² Jones under 532 nm laser illumination at a power density of 1.5 nW cm⁻². Moreover, the dual interface passivated device exhibits good stabilities. This study paves the road for developing low-cost, low-power, solution processed image sensors.     

All-Dielectric Nanostructure Fabry–Pérot-Enhanced Mie Resonances Coupled with Photogain Modulation toward Ultrasensitive In2S3 Photodetector

As the fresh blood of 2D family, non-layered 2D materials (2DNLMs) have demonstrated great potential in the application of next-generation optoelectronic devices. However, stemming from the weak light absorption brought by atomically thin thickness and the interfacial recombination brought by surface dangling bonds, traditional 2DNLM photodetectors are always accompanied by limited performance. Herein, a structure that integrates Si nanopillar array and non-layered 2D In₂S₃ to construct an ultrasensitive photodetector is designed. In particular, periodically Si nanopillars can act as Fabry–Pérot-enhanced Mie resonators that can effectively control and enhance the light absorption of 2D In₂S₃. On the other hand, a vertical built-in electric field is introduced in the In₂S₃ channel to capture photogenerated holes and leave electrons recycling in In₂S₃, obtaining a high photogain. Benefiting from these two mechanisms, this proposed photodetector presents a high responsivity of 4812 A W⁻¹ and short rise/decay time of 5.2/4.0 ms at the wavelength of 405 nm. Especially, a high light on–off ratio greater than 10⁶ and a record-high detectivity of 5.4 × 10¹⁵ Jones are achieved, representing one of the most sensitive photodetectors based on 2D materials. This deliberate device design concept suggests an effective scheme to construct high-performance 2DNLM optoelectronic devices.     

High‐Performance Solid Polymer Electrolytes Filled with Vertically Aligned 2D Materials

Solid state lithium metal batteries are the most promising next‐generation power sources owing to their high energy density and safety. Solid polymer electrolytes (SPE) have gained wide attention due to the excellent flexibility, manufacturability, lightweight, and low‐cost processing. However, fatal drawbacks of the SPE such as the insufficient ionic conductivity and Li⁺ transference number at room temperature restrict their practical application. Here vertically aligned 2D sheets are demonstrated as an advanced filler for SPE with enhanced ionic conductivity, Li⁺ transference number, mechanical modulus, and electrochemical stability, using vermiculite nanosheets as an example. The vertically aligned vermiculite sheets (VAVS), prepared by the temperature gradient freezing, provide aligned, continuous, run‐through polymer‐filler interfaces after infiltrating with polyethylene oxide (PEO)‐based SPE. As a result, ionic conductivity as high as 1.89 × 10^?4 S cm^?1 at 25 °C is achieved with Li⁺ transference number close to 0.5. Along with their enhanced mechanical strength, Li|Li symmetric cells using VAVS–CSPE are stable over 1300 h with a low overpotential. LiFePO₄ in all‐solid‐state lithium metal batteries with VAVS–CSPE could deliver a specific capacity of 167 mAh g^?1 at 0.1 C at 35 °C and 82% capacity retention after 200 cycles at 0.5 C.     

PdPSe: Component-Fusion-Based Topology Designer of Two-Dimensional Semiconductor

Novel 2D semiconductors play an increasingly important role in modern nanoelectronics and optoelectronics. Herein, a novel topology designer based on component fusion is introduced, featured by the submolecular component integration and properties inheritance. As expected, a new air-stable 2D semiconductor PdPSe with a tailored puckered structure is successfully designed and synthesized via this method. Notably, the monolayer of PdPSe is constructed by two sublayers via P P bonds, different from 2D typical transition metal materials with sandwich-structured monolayers. With the expected orthorhombic symmetry and intralayer puckering, PdPSe displays a strong Raman anisotropy. The field-effect transistors and photodetectors based on few-layer PdPSe demonstrate good electronic properties with high carrier mobility of ≈35 cm² V⁻¹ s⁻¹ and a high on/off ratio of 10⁶, as well as excellent optoelectronic performance, including high photoresponsivity, photogain, and detectivity with values up to 1.06 × 10⁵ A W⁻¹, 2.47 × 10⁷%, and 4.84 × 10¹⁰ Jones, respectively. These results make PdPSe a promising air-stable 2D semiconductor for various electronic and optoelectronic applications. This work suggests that the component-fusion-based topology designer is a novel approach to tailor 2D materials with expected structures and interesting properties.     

Gate‐Induced Massive and Reversible Phase Transition of VO2 Channels Using Solid‐State Proton Electrolytes

The use of gate bias to control electronic phases in VO₂, an archetypical correlated oxide, offers a powerful method to probe their underlying physics, as well as for the potential to develop novel electronic devices. Up to date, purely electrostatic gating in 3‐terminal devices with correlated channel shows the limited electrostatic gating efficiency due to insufficiently induced carrier density and short electrostatic screening length. Here massive and reversible conductance modulation is shown in a VO₂ channel by applying gate bias V_G at low voltage by a solid‐state proton (H⁺) conductor. By using porous silica to modulate H⁺ concentration in VO₂, gate‐induced reversible insulator‐to‐metal (I‐to‐M) phase transition at low voltage, and unprecedented two‐step insulator‐to‐metal‐to‐insulator (I‐to‐M‐to‐I) phase transition at high voltage are shown. V_G strongly and efficiently injects H⁺ into the VO₂ channel without creating oxygen deficiencies; this H⁺‐induced electronic phase transition occurs by giant modulation (≈7%) of out‐of‐plane lattice parameters as a result of H⁺‐induced chemical expansion. The results clarify the role of H⁺ on the electronic state of the correlated phases, and demonstrate the potentials for electronic devices that use ionic/electronic coupling.     

High Ionic Conductivity Motivated by Multiple Ion-Transport Channels in 2D MOF-Based Lithium Solid State Battery

Metal-organic frameworks (MOFs) have been proposed as novel fillers for constructing polymer solid electrolytes based composite electrolytes. However, MOFs are generally used as passive fillers, in-depth revealing the binding mode between MOFs and polyethylene oxide (PEO), the critical role of MOFs in facilitating Li⁺ transport in solid electrolytes is full of challenges. Herein, inspired by density functional theory (DFT) the 2D-MOF with rich unsaturated metal coordination sites that can bind the O atom in PEO through the metal–oxygen bond,  anchor TFSI⁻ to release Li⁺, resulting in a remarkable Li⁺ transference number of 0.58, is reported according well with the experimental results and molecular dynamics (MD) simulation. Impressively, after the introduction of the 2D-MOF, the Li⁺ can rapidly hop along the benzene ring center within the 2D-MOF plane, and the interface between the benzene ring and PEO can also serve as a fast Li⁺ migration pathway, delivering multiple ion-transport channels, which present a high ion conductivity of 4.6 × 10⁻⁵ S cm⁻¹ (25 °C). The lithium symmetric battery is stable for 1300 h at 60 °C, 0.1 mA cm⁻². The assembled lithium metal solid state battery maintains high capacity of 162.8 mAh g⁻¹ after 500 cycles at 60 °C and 0.5 C. This multiple ion-transport channels approach brings new ideas for designing advanced solid electrolytes.     

Controllable p-Type Doping of 2D WSe2 via Vanadium Substitution

Scalable substitutional doping of 2D transition metal dichalcogenides is a prerequisite to developing next-generation logic and memory devices based on 2D materials. To date, doping efforts are still nascent. Here, scalable growth and vanadium (V) doping of 2D WSe₂ at front-end-of-line and back-end-of-line compatible temperatures of 800 and 400 °C, respectively, is reported. A combination of experimental and theoretical studies confirm that vanadium atoms substitutionally replace tungsten in WSe₂, which results in p-type doping via the introduction of discrete defect levels that lie close to the valence band maxima. The p-type nature of the V dopants is further verified by constructed field-effect transistors, where hole conduction becomes dominant with increasing vanadium concentration. Hence, this study presents a method to precisely control the density of intentionally introduced impurities, which is indispensable in the production of electronic-grade wafer-scale extrinsic 2D semiconductors.