Fast and Highly Sensitive Ionic‐Polymer‐Gated WS2–Graphene Photodetectors

The combination of graphene with semiconductor materials in heterostructure photodetectors enables amplified detection of femtowatt light signals using micrometer‐scale electronic devices. Presently, long‐lived charge traps limit the speed of such detectors, and impractical strategies, e.g., the use of large gate‐voltage pulses, have been employed to achieve bandwidths suitable for applications such as video‐frame‐rate imaging. Here, atomically thin graphene–WS₂ heterostructure photodetectors encapsulated in an ionic polymer are reported, which are uniquely able to operate at bandwidths up to 1.5 kHz whilst maintaining internal gain as large as 10⁶. Highly mobile ions and the nanometer‐scale Debye length of the ionic polymer are used to screen charge traps and tune the Fermi level of the graphene over an unprecedented range at the interface with WS₂. Responsivity R = 10⁶ A W^?1 and detectivity D* = 3.8 × 10¹¹ Jones are observed, approaching that of single‐photon counters. The combination of both high responsivity and fast response times makes these photodetectors suitable for video‐frame‐rate imaging applications.     

Low‐Temperature Heteroepitaxy of 2D PbI2/Graphene for Large‐Area Flexible Photodetectors

Heterostructures based on graphene and other 2D atomic crystals exhibit fascinating properties and intriguing potential in flexible optoelectronics, where graphene films function as transparent electrodes and other building blocks are used as photoactive materials. However, large‐scale production of such heterostructures with superior performance is still in early stages. Herein, for the first time, the preparation of a submeter‐sized, vertically stacked heterojunction of lead iodide (PbI₂)/graphene on a flexible polyethylene terephthalate (PET) film by vapor deposition of PbI₂ on graphene/PET substrate at a temperature lower than 200 °C is demonstrated. This film is subsequently used to fabricate bendable graphene/PbI₂/graphene sandwiched photodetectors, which exhibit high responsivity (45 A W^?1 cm^?2), fast response (35 µs rise, 20 µs decay), and high‐resolution imaging capability (1 µm). This study may pave a facile pathway for scalable production of high‐performance flexible devices.     

Solution‐Processed 3D RGO–MoS2/Pyramid Si Heterojunction for Ultrahigh Detectivity and Ultra‐Broadband Photodetection

Molybdenum disulfide (MoS₂), a typical 2D metal dichalcogenide (2DMD), has exhibited tremendous potential in optoelectronic device applications, especially in photodetection. However, due to the weak light absorption of planar mono‐/multilayers, limited cutoff wavelength edge, and lack of high‐quality junctions, most reported MoS₂‐based photodetectors show undesirable performance. Here, a structurized 3D heterojunction of RGO–MoS₂/pyramid Si is demonstrated via a simple solution‐processing method. Owing to the improved light absorption by the pyramid structure, the narrowed bandgap of the MoS₂ by the imperfect crystallinity, and the enhanced charge separation/transportation by the inserted reduced graphene oxide (RGO), the assembled photodetector exhibits excellent performance in terms of a large responsivity of 21.8 A W^?1, extremely high detectivity up to 3.8 × 10¹⁵ Jones (Jones = cm Hz^1/2 W^?1) and ultrabroad spectrum response ranging from 350 nm (ultraviolet) to 4.3 µm (midwave infrared). These device parameters represent the best results for MoS₂‐based self‐driven photodetectors, and the detectivity value sets a new record for the 2DMD‐based photodetectors reported thus far. Prospectively, the design of novel 3D heterojunction can be extended to other 2DMDs, opening up the opportunities for a host of high‐performance optoelectronic devices.     

High‐Responsivity Graphene/InAs Nanowire Heterojunction Near‐Infrared Photodetectors with Distinct Photocurrent On/Off Ratios

Graphene is a promising candidate material for high‐speed and ultra‐broadband photodetectors. However, graphene‐based photodetectors suffer from low photoreponsivity and I_light/I_dark ratios due to their negligible‐gap nature and small optical absorption. Here, a new type of graphene/InAs nanowire (NW) vertically stacked heterojunction infrared photodetector is reported, with a large photoresponsivity of 0.5 AW^?1 and I_light/I_dark ratio of 5 × 10², while the photoresponsivity and I_light/I_dark ratio of graphene infrared photodetectors are 0.1 mAW^?1 and 1, respectively. The Fermi level (E_F ) of graphene can be widely tuned by the gate voltage owing to its 2D nature. As a result, the back‐gated bias can modulate the Schottky barrier (SB) height at the interface between graphene and InAs NWs. Simulations further demonstrate the rectification behavior of graphene/InAs NW heterojunctions and the tunable SB controls charge transport across the vertically stacked heterostructure. The results address key challenges for graphene‐based infrared detectors, and are promising for the development of graphene electronic and optoelectronic applications.     

Multifunctional MoS2 Transistors with Electrolyte Gel Gating

MoS₂, one of the most valued 2D materials beyond graphene, shows potential for future applications in postsilicon digital electronics and optoelectronics. However, achieving hole transport in MoS₂, which is dominated by electron transport, is always a challenge. Here, MoS₂ transistors gated by electrolyte gel exhibit the characteristics of hole and electron transport, a high on/off ratio over 10⁵, and a low subthreshold swing below 50 mV per decade. Due to the electrolyte gel, the density of electrons and holes in the MoS₂ channel reaches ≈9 × 10¹³ and 8.85 × 10¹³ cm^?2, respectively. The electrolyte gel‐assisted MoS₂ phototransistor exhibits adjustable positive and negative photoconductive effects. Additionally, the MoS₂ p–n homojunction diode affected by electrolyte gel shows high performance and a rectification ratio over 10⁷. These results demonstrate that modifying the conductance of MoS₂ through electrolyte gel has great potential in highly integrated electronics and optoelectronic photodetectors.     

Lowering the Schottky Barrier Height by Graphene/Ag Electrodes for High‐Mobility MoS2 Field‐Effect Transistors

2D transition metal dichalcogenides (TMDCs) have emerged as promising candidates for post‐silicon nanoelectronics owing to their unique and outstanding semiconducting properties. However, contact engineering for these materials to create high‐performance devices while adapting for large‐area fabrication is still in its nascent stages. In this study, graphene/Ag contacts are introduced into MoS₂ devices, for which a graphene film synthesized by chemical vapor deposition (CVD) is inserted between a CVD‐grown MoS₂ film and a Ag electrode as an interfacial layer. The MoS₂ field‐effect transistors with graphene/Ag contacts show improved electrical and photoelectrical properties, achieving a field‐effect mobility of 35 cm² V^?1 s^?1, an on/off current ratio of 4 × 10⁸, and a photoresponsivity of 2160 A W^?1, compared to those of devices with conventional Ti/Au contacts. These improvements are attributed to the low work function of Ag and the tunability of graphene Fermi level; the n‐doping of Ag in graphene decreases its Fermi level, thereby reducing the Schottky barrier height and contact resistance between the MoS₂ and electrodes. This demonstration of contact interface engineering with CVD‐grown MoS₂ and graphene is a key step toward the practical application of atomically thin TMDC‐based devices with low‐resistance contacts for high‐performance large‐area electronics and optoelectronics.     

Highly Flexible and Transparent Multilayer MoS2 Transistors with Graphene Electrodes

A highly flexible and transparent transistor is developed based on an exfoliated MoS₂ channel and CVD‐grown graphene source/drain electrodes. Introducing the 2D nanomaterials provides a high mechanical flexibility, optical transmittance (～74%), and current on/off ratio (>10⁴) with an average field effect mobility of ～4.7 cm² V^?1 s^?1, all of which cannot be achieved by other transistors consisting of a MoS₂ active channel/metal electrodes or graphene channel/graphene electrodes. In particular, a low Schottky barrier (～22 meV) forms at the MoS₂/graphene interface, which is comparable to the MoS₂/metal interface. The high stability in electronic performance of the devices upon bending up to ±2.2 mm in compressive and tensile modes, and the ability to recover electrical properties after degradation upon annealing, reveal the efficacy of using 2D materials for creating highly flexible and transparent devices.     

High Detectivity and Transparent Few‐Layer MoS2/Glassy‐Graphene Heterostructure Photodetectors

Layered van der Waals heterostructures have attracted considerable attention recently, due to their unique properties both inherited from individual two‐dimensional (2D) components and imparted from their interactions. Here, a novel few‐layer MoS₂/glassy‐graphene heterostructure, synthesized by a layer‐by‐layer transfer technique, and its application as transparent photodetectors are reported for the first time. Instead of a traditional Schottky junction, coherent ohmic contact is formed at the interface between the MoS₂ and the glassy‐graphene nanosheets. The device exhibits pronounced wavelength selectivity as illuminated by monochromatic lights. A responsivity of 12.3 mA W^?1 and detectivity of 1.8 × 10¹⁰ Jones are obtained from the photodetector under 532 nm light illumination. Density functional theory calculations reveal the impact of specific carbon atomic arrangement in the glassy‐graphene on the electronic band structure. It is demonstrated that the band alignment of the layered heterostructures can be manipulated by lattice engineering of 2D nanosheets to enhance optoelectronic performance.     

Asymmetrically Encapsulated Vertical ITO/MoS2/Cu2O Photodetector with Ultrahigh Sensitivity

Strong light absorption, coupled with moderate carrier transport properties, makes 2D layered transition metal dichalcogenide semiconductors promising candidates for low intensity photodetection applications. However, the performance of these devices is severely bottlenecked by slow response with persistent photocurrent due to long lived charge trapping, and nonreliable characteristics due to undesirable ambience and substrate effects. Here ultrahigh specific detectivity (D*) of 3.2 × 10¹⁴ Jones and responsivity (R) of 5.77 × 10⁴ A W^?1 are demonstrated at an optical power density (P_op) of 0.26 W m^?2 and external bias (V_ext) of ?0.5 V in an indium tin oxide/MoS₂/copper oxide/Au vertical multi‐heterojunction photodetector exhibiting small carrier transit time. The active MoS₂ layer being encapsulated by carrier collection layers allows us to achieve repeatable characteristics over large number of cycles with negligible trap assisted persistent photocurrent. A large D* > 10¹⁴ Jones at zero external bias is also achieved due to the built‐in field of the asymmetric photodetector. Benchmarking the performance against existing reports in literature shows a viable pathway for achieving reliable and highly sensitive photodetectors for ultralow intensity photodetection applications.     

2D In2S3 Nanoflake Coupled with Graphene toward High‐Sensitivity and Fast‐Response Bulk‐Silicon Schottky Photodetector

Silicon‐based electronic devices, especially graphene/Si photodetectors (Gr/Si PDs), have triggered tremendous attention due to their simple structure and flexible integration of the Schottky junction. However, due to the relatively poor light–matter interaction and mobility of silicon, these Gr/Si PDs typically suffer an inevitable compromise between photoresponsivity and response speed. Herein, a novel strategy for coupling 2D In₂S₃ with Gr/Si PDs is demonstrated. The introduction of the double‐heterojunction design not only strengthens the light absorption of graphene/Si but also combines the advantages of the photogating effect and photovoltaic effect, which suppresses the dark current, accelerates the separation of photogenerated carriers, and brings photoconductive gain. As a result, In₂S₃/graphene/Si devices present an ultrahigh photoresponsivity of 4.53 × 10⁴ A W^?1 and fast response speed less than 40 µs, simultaneously. These parameters are an order of magnitude higher than pristine Gr/Si PDs and among the best values compared with reported 2D materials/Si heterojunction PDs. Furthermore, the In₂S₃/graphene/Si PD expresses outstanding long‐term stability, with negligible performance degradation even after 1 month in air or 1000 cycles of operation. These findings highlight a simple and novel strategy for constructing high‐sensitivity and ultrafast Gr/Si PDs for further optoelectronic applications.     

Near‐Infrared Photodetectors Based on MoTe2/Graphene Heterostructure with High Responsivity and Flexibility

2D transition metal dichalcogenides (TMDCs) have attracted considerable attention due to their impressively high performance in optoelectronic devices. However, efficient infrared (IR) photodetection has been significantly hampered because the absorption wavelength range of most TMDCs lies in the visible spectrum. In this regard, semiconducting 2D MoTe₂ can be an alternative choice owing to its smaller band gap ≈1 eV from bulk to monolayer and high carrier mobility. Here, a MoTe₂/graphene heterostructure photodetector is demonstrated for efficient near‐infrared (NIR) light detection. The devices achieve a high responsivity of ≈970.82 A W^?1 (at 1064 nm) and broadband photodetection (visible‐1064 nm). Because of the effective photogating effect induced by electrons trapped in the localized states of MoTe₂, the devices demonstrate an extremely high photoconductive gain of 4.69 × 10⁸ and detectivity of 1.55 × 10¹¹ cm Hz^1/2 W^?1. Moreover, flexible devices based on the MoTe₂/graphene heterostructure on flexible substrate also retains a good photodetection ability after thousands of times bending test (1.2% tensile strain), with a high responsivity of ≈60 A W^?1 at 1064 nm at V _DS = 1 V, which provides a promising platform for highly efficient, flexible, and low cost broadband NIR photodetectors.     

17% Efficient Organic Solar Cells Based on Liquid Exfoliated WS2 as a Replacement for PEDOT:PSS

The application of liquid‐exfoliated 2D transition metal disulfides (TMDs) as the hole transport layers (HTLs) in nonfullerene‐based organic solar cells is reported. It is shown that solution processing of few‐layer WS₂ or MoS₂ suspensions directly onto transparent indium tin oxide (ITO) electrodes changes their work function without the need for any further treatment. HTLs comprising WS₂ are found to exhibit higher uniformity on ITO than those of MoS₂ and consistently yield solar cells with superior power conversion efficiency (PCE), improved fill factor (FF), enhanced short‐circuit current (J_SC), and lower series resistance than devices based on poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) and MoS₂. Cells based on the ternary bulk‐heterojunction PBDB‐T‐2F:Y6:PC₇₁BM with WS₂ as the HTL exhibit the highest PCE of 17%, with an FF of 78%, open‐circuit voltage of 0.84 V, and a J_SC of 26 mA cm^?2. Analysis of the cells' optical and carrier recombination characteristics indicates that the enhanced performance is most likely attributed to a combination of favorable photonic structure and reduced bimolecular recombination losses in WS₂‐based cells. The achieved PCE is the highest reported to date for organic solar cells comprised of 2D charge transport interlayers and highlights the potential of TMDs as inexpensive HTLs for high‐efficiency organic photovoltaics.     

High‐Performance Photovoltaic Detector Based on MoTe2/MoS2 Van der Waals Heterostructure

Van der Waals heterostructures based on 2D layered materials have received wide attention for their multiple applications in optoelectronic devices, such as solar cells, light‐emitting devices, and photodiodes. In this work, high‐performance photovoltaic photodetectors based on MoTe₂/MoS₂ vertical heterojunctions are demonstrated by exfoliating‐restacking approach. The fundamental electric properties and band structures of the junction are revealed and analyzed. It is shown that this kind of photodetectors can operate under zero bias with high on/off ratio (>10⁵) and ultralow dark current (≈3 pA). Moreover, a fast response time of 60 µs and high photoresponsivity of 46 mA W^?1 are also attained at room temperature. The junctions based on 2D materials are expected to constitute the ultimate functional elements of nanoscale electronic and optoelectronic applications.     

Roll‐to‐Roll Production of Layer‐Controlled Molybdenum Disulfide: A Platform for 2D Semiconductor‐Based Industrial Applications

A facile methodology for the large‐scale production of layer‐controlled MoS₂ layers on an inexpensive substrate involving a simple coating of single source precursor with subsequent roll‐to‐roll‐based thermal decomposition is developed. The resulting 50 cm long MoS₂ layers synthesized on Ni foils possess excellent long‐range uniformity and optimum stoichiometry. Moreover, this methodology is promising because it enables simple control of the number of MoS₂ layers by simply adjusting the concentration of (NH₄)₂MoS₄. Additionally, the capability of the MoS₂ for practical applications in electronic/optoelectronic devices and catalysts for hydrogen evolution reaction is verified. The MoS₂‐based field effect transistors exhibit unipolar n‐channel transistor behavior with electron mobility of 0.6 cm² V^?1 s^?1 and an on‐off ratio of ≈10³. The MoS₂‐based visible‐light photodetectors are fabricated in order to evaluate their photoelectrical properties, obtaining an 100% yield for active devices with significant photocurrents and extracted photoresponsivity of ≈22 mA W^?1. Moreover, the MoS₂ layers on Ni foils exhibit applicable catalytic activity with observed overpotential of ≈165 mV and a Tafel slope of 133 mV dec^?1. Based on these results, it is envisaged that the cost‐effective methodology will trigger actual industrial applications, as well as novel research related to 2D semiconductor‐based multifaceted applications.     

A Dual‐Gate MoS2 Photodetector Based on Interface Coupling Effect

2D transition metal dichalcogenides (TMDs) based photodetectors have shown great potential for the next generation optoelectronics. However, most of the reported MoS₂ photodetectors function under the photogating effect originated from the charge‐trap mechanism, which is difficult for quantitative control. Such devices generally suffer from a poor compromise between response speed and responsivity (R) and large dark current. Here, a dual‐gated (DG) MoS₂ phototransistor operating based on the interface coupling effect (ICE) is demonstrated. By simultaneously applying a negative top‐gate voltage (V_TG) and positive back‐gate voltage (V_BG) to the MoS₂ channel, the photogenerated holes can be effectively trapped in the depleted region under TG. An ultrahigh R of ≈10⁵ A W^?1 and detectivity (D*) of ≈10¹⁴ Jones are achieved in several devices with different thickness under P_in of 53 µW cm^?2 at V_TG = ?5 V. Moreover, the response time of the DG phototransistor can also be modulated based on the ICE. Based on these systematic measurements of MoS₂ DG phototransistors, the results show that the ICE plays an important role in the modulation of photoelectric performances. The results also pave the way for the future optoelectrical application of 2D TMDs materials and prompt for further investigation in the DG structured phototransistors.     

Ultrasensitive 2D Bi2O2Se Phototransistors on Silicon Substrates

2D materials are considered as intriguing building blocks for next‐generation optoelectronic devices. However, their photoresponse performance still needs to be improved for practical applications. Here, ultrasensitive 2D phototransistors are reported employing chemical vapor deposition (CVD)‐grown 2D Bi₂O₂Se transferred onto silicon substrates with a noncorrosive transfer method. The as‐transferred Bi₂O₂Se preserves high quality in contrast to the serious quality degradation in hydrofluoric‐acid‐assisted transfer. The phototransistors show a responsivity of 3.5 × 10⁴ A W^?1, a photoconductive gain of more than 10⁴, and a time response in the order of sub‐millisecond. With back gating of the silicon substrate, the dark current can be reduced to several pA. This yields an ultrahigh sensitivity with a specific detectivity of 9.0 × 10¹³ Jones, which is one of the highest values among 2D material photodetectors and two orders of magnitude higher than that of other CVD‐grown 2D materials. The high performance of the phototransistor shown here together with the developed unique transfer technique are promising for the development of novel 2D‐material‐based optoelectronic applications as well as integrating with state‐of‐the‐art silicon photonic and electronic technologies.     

Direct Laser‐Patterned Micro‐Supercapacitors from Paintable MoS2 Films

Micrometer‐sized electrochemical capacitors have recently attracted attention due to their possible applications in micro‐electronic devices. Here, a new approach to large‐scale fabrication of high‐capacitance, two‐dimensional MoS₂ film‐based micro‐supercapacitors is demonstrated via simple and low‐cost spray painting of MoS₂ nanosheets on Si/SiO₂ chip and subsequent laser patterning. The obtained micro‐supercapacitors are well defined by ten interdigitated electrodes (five electrodes per polarity) with 4.5 mm length, 820 μm wide for each electrode, 200 μm spacing between two electrodes and the thickness of electrode is ～0.45 μm. The optimum MoS₂‐based micro‐supercapacitor exhibits excellent electrochemical performance for energy storage with aqueous electrolytes, with a high area capacitance of 8 mF cm^?2 (volumetric capacitance of 178 F cm^?3) and excellent cyclic performance, superior to reported graphene‐based micro‐supercapacitors. This strategy could provide a good opportunity to develop various micro‐/nanosized energy storage devices to satisfy the requirements of portable, flexible, and transparent micro‐electronic devices.     

Enhanced Field‐Emission Behavior of Layered MoS2 Sheets

Field emission studies are reported for the first time on layered MoS₂ sheets at the base pressure of ～1 × 10^?8 mbar. The turn‐on field required to draw a field emission current density of 10 μA/cm² is found to be 3.5 V/μm for MoS₂ sheets. The turn‐on values are found to be significantly lower than the reported MoS₂ nanoflowers, graphene, and carbon nanotube‐based field emitters due to the high field enhancement factor (～1138) associated with nanometric sharp edges of MoS₂ sheet emitter surface. The emission current–time plots show good stability over a period of 3 h. Owing to the low turn‐on field and planar (sheetlike) structure, the MoS₂ could be utilized for future vacuum microelectronics/nanoelectronic and flat panel display applications.     

Vertically Aligned Graphene–Carbon Fiber Hybrid Electrodes with Superlong Cycling Stability for Flexible Supercapacitors

Graphene electrode–based supercapacitors are in high demand due to their superior electrochemical characteristics. A major bottleneck of using the supercapacitors for commercial applications lies in their inferior electrode cycle life. Herein, a simple and facile method to fabricate highly efficient supercapacitor electrodes using pristine graphene sheets vertically stacked and electrically connected to the carbon fibers which can result in vertically aligned graphene–carbon fiber nanostructure is developed. The vertically aligned graphene–carbon fiber electrode prepared by electrophoretic deposition possesses a mesoporous 3D architecture which enabled faster and efficient electrolyte‐ion diffusion with a gravimetric capacitance of 333.3 F g^?1 and an areal capacitance of 166 mF cm^?2. The electrodes displayed superlong electrochemical cycling stability of more than 100 000 cycles with 100% capacitance retention hence promising for long‐lasting supercapacitors. Apart from the electrochemical double layer charge storage, the oxygen‐containing surface moieties and α‐Ni(OH)₂ present on the graphene sheets enhance the charge storage by faradaic reactions. This enables the assembled device to provide an excellent gravimetric energy density of 76 W h kg^?1 with a 100% capacitance retention even after 1000 bending cycles. This study opens the door for developing high‐performing flexible graphene electrodes for wearable energy storage applications.     

Flexible and High‐Performance All‐2D Photodetector for Wearable Devices

Emerging novel applications at the forefront of innovation horizon raise new requirements including good flexibility and unprecedented properties for the photoelectronic industry. On account of diversity in transport and photoelectric properties, 2D layered materials have proven as competent building blocks toward next‐generation photodetectors. Herein, an all‐2D Bi₂Te₃‐SnS‐Bi₂Te₃ photodetector is fabricated with pulsed‐laser deposition. It is sensitive to broadband wavelength from ultraviolet (370 nm) to near‐infrared (808 nm). In addition, it exhibits great durability to bend, with intact photoresponse after 100 bend cycles. Upon 370 nm illumination, it achieves a high responsivity of 115 A W^?1, a large external quantum efficiency of 3.9 × 10⁴%, and a superior detectivity of 4.1 × 10¹¹ Jones. They are among the best figures‐of‐merit of state‐of‐the‐art 2D photodetectors. The synergistic effect of SnS's strong light–matter interaction, efficient carrier separation of Bi₂Te₃–SnS interface, expedite carrier injection across Bi₂Te₃–SnS interface, and excellent carrier collection of Bi₂Te₃ topological insulator electrodes accounts for the superior photodetection properties. In summary, this work depicts a facile all‐in‐one fabrication strategy toward a Bi₂Te₃‐SnS‐Bi₂Te₃ photodetector. More importantly, it reveals a novel all‐2D concept for construction of flexible, broadband, and high‐performance photoelectronic devices by integrating 2D layered metallic electrodes and 2D layered semiconducting channels.