Enhancement of Carrier Mobility in Multilayer InSe Transistors by van der Waals Integration.

Two-dimensional material indium selenide (InSe) holds great promise for applications in electronics and optoelectronics by virtue of its fascinating properties. However, most multilayer InSe-based transistors suffer from extrinsic scattering effects from interface disorders and the environment, which cause carrier mobility and density fluctuations and hinder their practical application. In this work, we employ the non-destructive method of van der Waals (vdW) integration to improve the electron mobility of back-gated multilayer InSe FETs. After introducing the hexagonal boron nitride (h-BN) as both an encapsulation layer and back-gate dielectric with the vdW interface, as well as graphene serving as a buffer contact layer, the electron mobilities of InSe FETs are substantially enhanced. The vdW-integrated devices exhibit a high electron mobility exceeding 103 cm2 V-1 s-1 and current on/off ratios of ~108 at room temperature. Meanwhile, the electron densities are found to exceed 1012 cm-2. In addition, the fabricated devices show an excellent stability with a negligible electrical degradation after storage in ambient conditions for one month. Electrical transport measurements on InSe FETs in different configurations suggest that a performance enhancement with vdW integration should arise from a sufficient screening effect on the interface impurities and an effective passivation of the air-sensitive surface.

Selective Chemical Vapor Deposition Growth of WS2/MoS2 Vertical and Lateral Heterostructures on Gold Foils.

Vertical and lateral heterostructures consisting of atomically layered two-dimensional (2D) materials exhibit intriguing properties, such as efficient charge/energy transfer, high photoresponsivity, and enhanced photocatalytic activities. However, the controlled fabrication of vertical or lateral heterojunctions on metal substrates remains challenging. Herein, we report a facile and controllable method for selective growth of WS2/MoS2 vertical or lateral heterojunctions on polycrystalline gold (Au) foil by tuning the gas flow rate of hydrogen (H2). We find that lateral growth is favored without H2, whereas vertical growth mode can be switched on by introducing 8-10 sccm H2. In addition, the areal coverage of the WS2/MoS2 vertical heterostructures is tunable in the range of 12-25%. Transmission electron microscopy (TEM) and selected area electron diffraction (SAED) results demonstrate the quality and absence of cross-contamination of the as-grown heterostructures. Furthermore, we investigate the effects of the H2 flow rate on the morphology of the heterostructures. These pave the way to develop unprecedented 2D heterostructures towards applications in (opto)electronic devices.

Ultrathin Single-Crystalline 2D Perovskite Photoconductor for High-Performance Narrowband and Wide Linear Dynamic Range Photodetection.

For next-generation Internet-of-Everything applications, for example, artificial-neural-network image sensors, artificial retina, visible light communication, on-chip light interconnection, and flexible devices, etc., high-performance microscale photodetectors are in urgent demands. 2D material (2DM) photodetectors have been researched and demonstrated impressive performances. However, they have not met the demands in filterless narrowband photoresponse, wide linear dynamic range (LDR), ultralow dark current, and large on/off ratio, which are key performances for these applications. 2D Ruddlesden-Popper perovskites (2D-RPPs) are recently highlighted photovoltaic and optoelectronic materials. Embedding ultrathin 2D-RPPs into 2DM photodetectors holds potentials to improve these performances. Herein, a single-crystalline ultrathin (PEA)2 PbI4 is integrated into a vertical-stacked graphene-(PEA)2 PbI4 -graphene micro photoconductor (V-PEPI-PC). V-PEPI-PC exhibits narrowband photoresponses at 517 nm with a full-width-at-half-maximum of 15 nm and a wide LDR of 122 dB. Due to the multiple quantum wells in (PEA)2 PbI4 , V-PEPI-PC demonstrates an ultralow dark current of 1.1 × 10-14 A (44 pA mm-2 ), a high specific detectivity of 1.2 × 1013 Jones, and a high on/off ratio of 1.6 × 106 . Owing to the short vertical channel, V-PEPI-PC shows a fast response rise time of 486 µs. Therefore, the vertical-stacked photodetectors based on hybrid 2D-RPPs and 2DMs may have great potentials in future optoelectronics.

Visible to near-infrared photodetector with novel optoelectronic performance based on graphene/S-doped InSe heterostructure on h-BN substrate.

van der Waals heterostructures of two-dimensional (2D) materials have attracted considerable attention due to their flexibility in the design of new functional devices. Despite numerous studies on graphene/2D semiconductor heterostructures, their optoelectronic applications are significantly hindered because of several disadvantages, such as large band gaps and chemical instability. In this work, we demonstrate the fabrication of graphene/S-doped InSe heterostructure photodetectors with excellent photoresponse performance, and this is attributed to the moderate band gap and band gap engineering by element doping of InSe as well as the high carrier mobility of graphene. In particular, the graphene/InSe0.9S0.1 device achieves an ultrahigh photoresponsivity of ∼4.9 × 106 A W-1 at 700 nm and an EQE of 8.7 × 108%, and it exhibits broadband photodetection (visible to near-infrared). More importantly, by virtue of the interaction between n-type graphene arising from the influence of h-BN as a dielectric layer and S-doped InSe with a high work-function, our devices always exhibited positive photocurrent when the polarity of the gate voltage is adjusted, and is different from that the previously reported graphene/2D semiconductor photodetectors. This work not only provides a promising platform for highly efficient broadband photodetectors but also sheds light on tuning the optoelectronic performance through band gap engineering and designing novel heterostructures-based various 2D materials.

Continuously Tuning Electronic Properties of Few-Layer Molybdenum Ditelluride with in Situ Aluminum Modification toward Ultrahigh Gain Complementary Inverters.

Semiconducting molybdenum ditelluride (2H-MoTe2), a two-dimensional (2D) transition metal dichalcogenide, has attracted extensive research attention due to its favorable physical properties for future electronic devices, such as appropriate bandgap, ambipolar transport characteristic, and good chemical stability. The rational tuning of its electronic properties is a key point to achieve MoTe2-based complementary electronic and optoelectronic devices. Herein, we demonstrate the dynamic and effective control of the electronic properties of few-layer MoTe2, through the in situ surface modification with aluminum (Al) adatoms, with a view toward high-performance complementary inverter devices. MoTe2 is found to be significantly electron doped by Al, exhibiting a continuous transport transition from p-dominated ambipolar to n-type unipolar with enhanced electron mobility. Using a spatially controlled Al doping technique, both p- and n-channels are established on a single MoTe2 nanosheet, which gives complementary inverters with a record-high gain of ∼195, which stands out in the 2D family of materials due to the balanced p- and n-transport in Al-modified MoTe2. Our studies coupled with the tunable nature of in situ modification enable MoTe2 to be a promising candidate for high-performance complementary electronics.

Unraveling High-Yield Phase-Transition Dynamics in Transition Metal Dichalcogenides on Metallic Substrates.

2D transition metal dichalcogenides (2D-TMDs) and their unique polymorphic features such as the semiconducting 1H and quasi-metallic 1T' phases exhibit intriguing optical and electronic properties, which can be used in novel electronic and photonic device applications. With the favorable quasi-metallic nature of 1T'-phase 2D-TMDs, the 1H-to-1T' phase engineering processes are an immensely vital discipline exploited for novel device applications. Here, a high-yield 1H-to-1T' phase transition of monolayer-MoS2 on Cu and monolayer-WSe2 on Au via an annealing-based process is reported. A comprehensive experimental and first-principles study is performed to unravel the underlying mechanism and derive the general trends for the high-yield phase transition process of 2D-TMDs on metallic substrates. While each 2D-TMD possesses different intrinsic 1H-1T' energy barriers, the option of metallic substrates with higher chemical reactivity plays a significantly pivotal role in enhancing the 1H-1T' phase transition yield. The yield increase is achieved via the enhancement of the interfacial hybridizations by the means of increased interfacial binding energy, larger charge transfer, shorter interfacial spacing, and weaker bond strength. Fundamentally, this study opens up the field of 2D-TMD/metal-like systems to further scientific investigation and research, thereby creating new possibilities for 2D-TMDs-based device applications.

Fabry-Perot Cavity-Enhanced Optical Absorption in Ultrasensitive Tunable Photodiodes Based on Hybrid 2D Materials.

Monolayer two-dimensional (2D) transition metal dichalcogenides (TMDs) show interesting optical and electrical properties because of their direct bandgap. However, the low absorption of atomically thin TMDs limits their applications. Here, we report enhanced absorption and optoelectronic properties of monolayer molybdenum disulfide (MoS2) by using an asymmetric Fabry-Perot cavity. The cavity is based on a hybrid structure of MoS2/ hexagonal boron nitride (BN)/Au/SiO2 realized through layer-by-layer vertical stacking. Photoluminescence (PL) intensity of monolayer MoS2 is enhanced over 2 orders of magnitude. Theoretical calculations show that the strong absorption of MoS2 comes from photonic localization on the top of the microcavity at optimal BN spacer thickness. The n/n+ MoS2 homojunction photodiode incorporating this asymmetric Fabry-Perot cavity exhibits excellent current rectifying behavior with an ideality factor of 1 and an ultrasensitive and gate-tunable external photo gain and specific detectivity. Our work offers an effective method to achieve uniform enhanced light absorption by monolayer TMDs, which has promising applications for highly sensitive optoelectronic devices.

Surface Functionalization of Black Phosphorus via Potassium toward High-Performance Complementary Devices.

Two-dimensional black phosphorus configured field-effect transistor devices generally show a hole-dominated ambipolar transport characteristic, thereby limiting its applications in complementary electronics. Herein, we demonstrate an effective surface functionalization scheme on few-layer black phosphorus, through in situ surface modification with potassium, with a view toward high performance complementary device applications. Potassium induces a giant electron doping effect on black phosphorus along with a clear bandgap reduction, which is further corroborated by in situ photoelectron spectroscopy characterizations. The electron mobility of black phosphorus is significantly enhanced to 262 (377) cm2 V-1 s-1 by over 1 order of magnitude after potassium modification for two-terminal (four-terminal) measurements. Using lithography technique, a spatially controlled potassium doping technique is developed to establish high-performance complementary devices on a single black phosphorus nanosheet, for example, the p-n homojunction-based diode achieves a near-unity ideality factor of 1.007 with an on/off ratio of ∼104. Our findings coupled with the tunable nature of in situ modification scheme enable black phosphorus as a promising candidate for further complementary electronics.

Molecular Alignment and Electronic Structure of N,N'-Dibutyl-3,4,9,10-perylene-tetracarboxylic-diimide Molecules on MoS2 Surfaces.

The molecular orientation of organic semiconductors on a solid surface could be an indispensable factor to determine the electrical performance of organic-based devices. Despite its fundamental prominence, a clear description of the emergent two-dimensional layered material-organic interface is not fully understood yet. In this study, we reveal the molecular alignment and electronic structure of thermally deposited N,N'-dibutyl-3,4,9,10-perylene-dicarboximide (PTCDI-C4) molecules on natural molybdenum disulfide (MoS2) using near-edge X-ray absorption fine structure spectroscopy (NEXAFS). The average tilt angle determination reveals that the anisotropy in the π* symmetry transition of the carbon K-edge (284-288 eV range) is present at the sub-monolayer regime. Supported by ultraviolet photoelectron spectroscopy (UPS), X-ray photoelectron spectroscopy (XPS), and resonant photoemission spectroscopy (RPES) measurements, we find that our spectroscopic measurements indicate a weak charge transfer established at the PTCDI-C4/MoS2 interface. Sterical hindrance due to the C4 alkyl chain caused tilting of the molecular plane at the initial thin film deposition. Our result shows a tunable interfacial alignment of organic molecules on transition metal dichalcogenide surfaces effectively enhancing the electronic properties of hybrid organic-inorganic heterostructure devices.

Plasmon-free SERS self-monitoring of catalysis reaction on Au nanoclusters/TiO2 photonic microarray.

Here, using the (Au/TiO2)-catalyzed reduction of 4-nitrothiophenol as a probe reaction, a catalysis/SERS bifunctional composite fabricated by uniformly dispersing catalysis-active Au nanoclusters (∼2 nm) on a SERS-active TiO2 photonic microarray was successfully applied to the non-plasmonic SERS self-monitoring of a catalytic reaction for the first time, which is superiorly sensitive and interference-free.

Improved SERS sensitivity on plasmon-free TiO2 photonic microarray by enhancing light-matter coupling.

Highly sensitive surface-enhanced Raman scattering (SERS) detection was achieved on plasmon-free TiO2 photonic artificial microarray, which can be quickly recovered under simulated solar light irradiation and repeatedly used. The sensitive detection performance is attributed to the enhanced matter-light interaction through repeated and multiple light scattering in photonic microarray. Moreover, the SERS sensitivity is unprecedentedly found to be dependent on the different light-coupling performance of microarray with various photonic band gaps, where microarray with band gap center near to laser wavelength shows a lower SERS signal due to depressed light propagation, while those with band gap edges near to laser wavelength show higher sensitivity due to slow light effect.