2D Indium Phosphorus Sulfide (In2 P3 S9 ): An Emerging van der Waals High-k Dielectrics.

2D van der Waals (vdW) semiconductors hold great potentials for more-than-Moore field-effect transistors (FETs), and the efficient utilization of their theoretical performance requires compatible high-k dielectrics to guarantee the high gate coupling efficiency. The deposition of traditional high-k dielectric oxide films on 2D materials usually generates interface concerns, thereby causing the carrier scattering and degeneration of device performance. Here, utilizing a space-confined epitaxy growth approach, the authors successfully obtained air-stable ultrathin indium phosphorus sulfide (In2 P3 S9 ) nanosheets, the thickness of which can be scaled down to monolayer limit (≈0.69 nm) due to its layered structure. 2D In2 P3 S9 exhibits excellent insulating properties, with a high dielectric constant (≈24) and large breakdown voltage (≈8.1 MV cm-1 ) at room temperature. Serving as gate insulator, ultrathin In2 P3 S9 nanosheet can be integrated into MoS2 FETs with high-quality dielectric/semiconductor interface, thus providing a competitive electrical performance of device with subthreshold swings (SS) down to 88 mV dec-1 and a high ON/OFF ratio of 105 . This study proves an important strategy to prepare 2D vdW high-k dielectrics, and greatly facilitates the ongoing research of 2D materials for functional electronics.

Mechanical Anisotropy in Two-Dimensional Selenium Atomic Layers.

Two-dimensional (2D) trigonal selenium (t-Se) has become a new member in 2D semiconducting nanomaterial families. It is composed of well-aligned one-dimensional Se atomic chains bonded via van der Waals (vdW) interaction. The contribution of this unique anisotropic nanostructure to its mechanical properties has not been explored. Here, for the first time, we combine experimental and theoretical analyses to study the anisotropic mechanical properties of individual 2D t-Se nanosheets. It was found that its fracture strength and Young's modulus parallel to the atomic chain direction are much higher than along the transverse direction, which was attributed to the weak vdW interaction between Se atomic chains as compared to the covalent bonding within individual chains. Additionally, two distinctive fracture modes along two orthogonal loading directions were identified. This work provides important insights into the understanding of anisotropic mechanical behaviors of 2D semiconducting t-Se and opens new possibilities for future applications.

Lowering the Contact Barriers of 2D Organic F16 CuPc Field-Effect Transistors by Introducing Van der Waals Contacts.

2D organic crystals exhibit efficient charge transport and field-effect characteristics, making them promising candidates for high-performance nanoelectronics. However, the strong Fermi level pinning (FLP) effect and large Schottky barrier between organic semiconductors and metals largely limit device performance. Herein, by carrying out temperature-dependent transport and Kelvin probe force microscopy measurements, it is demonstrated that the introducing of 2D metallic 1T-TaSe2 with matched band-alignment as electrodes for F16 CuPc nanoflake filed-effect transistors leads to enhanced field-effect characteristics, especially lowered Schottky barrier height and contact resistance at the contact and highly efficient charge transport within the channel, which are attributed to the significantly suppressed FLP effect and appropriate band alignment at the nonbonding van der Waals (vdW) hetero-interface. Moreover, by taking advantage of the improved contact behavior with 1T-TaSe2 contact, the optoelectronic performance of F16 CuPc nanoflake-based phototransistor is drastically improved, with a maximum photoresponsivity of 387 A W-1 and detectivity of 3.7 × 1014 Jones at quite a low Vds of 1 V, which is more competitive than those of the reported organic photodetectors and phototransistors. The work provides an avenue to improve the electrical and optoelectronic properties of 2D organic devices by introducing 2D metals with appropriate work function for vdW contacts.

Unraveling the Raman Enhancement Mechanism on 1T'-Phase ReS2 Nanosheets.

2D transition metal dichalcogenides materials are explored as potential surface-enhanced Raman spectroscopy substrates. Herein, a systematic study of the Raman enhancement mechanism on distorted 1T (1T') rhenium disulfide (ReS2 ) nanosheets is demonstrated. Combined Raman and photoluminescence studies with the introduction of an Al2 O3 dielectric layer unambiguously reveal that Raman enhancement on ReS2 materials is from a charge transfer process rather than from an energy transfer process, and Raman enhancement is inversely proportional while the photoluminescence quenching effect is proportional to the layer number (thickness) of ReS2 nanosheets. On monolayer ReS2 film, a strong resonance-enhanced Raman scattering effect dependent on the laser excitation energy is detected, and a detection limit as low as 10-9 m can be reached from the studied dye molecules such as rhodamine 6G and methylene blue. Such a high enhancement factor achieved through enhanced charge interaction between target molecule and substrate suggests that with careful consideration of the layer-number-dependent feature and excitation-energy-related resonance effect, ReS2 is a promising Raman enhancement platform for sensing applications.

Intercorrelated Ferroelectricity and Bulk Photovoltaic Effect in Two-Dimensional Sn2P2S6 Semiconductor for Polarization-Sensitive Photodetection.

A two-dimensional (2D) ferroelectric semiconductor, which is coupled with photosensitivity and room-temperature ferroelectricity, provides the possibility of coordinated conductance modulation by both electric field and light illumination and is promising for triggering the revolution of optoelectronics for monolithic multifunctional integration. Here, we report that semiconducting Sn2P2S6 crystals can be achieved in a 2D morphology using a chemical vapor transport approach with the assistant of space confinement and experimentally demonstrate the robust ferroelectricity in atomic-thin Sn2P2S6 nanosheet at room temperature. The intercorrelated programming of ferroelectric order along out-of-plane (OOP) and in-plane (IP) directions enables a tunable bulk photovoltaic (BPV) effect through multidirectional electrical control. By combining the capability of anisotropic in-plane optical absorption, a highly integrated Sn2P2S6 optoelectronic device vertically sandwiched with graphene electrodes yields the polarization-dependent open-circuit photovoltage with a dichroic ratio of 2.0 under 405 nm light illumination. The reintroduction of ferroelectric Sn2P2S6 to the 2D asymmetric semiconductor family provides possibilities to hardware implement of the self-powered polarization-sensitive photodetection and spotlights the promising applications for next-generation photovoltaic devices.

Synaptic plasticity realized by selective oxidation of TiS3 nanosheet for neuromorphic devices.

Memristive devices operating analogous to biology synapses demonstrate great potential for neuromorphic applications. Here, we reported the space-confined vapor synthesis of ultrathin titanium trisulfide (TiS3) nanosheets, and subsequent laser manufacturing of a TiS3-TiOx-TiS3 in-plane heterojunction for memristor applications. Due to the flux-controlled migration and aggregation of oxygen vacancies, the two-terminal memristor demonstrates reliable "analog" switching behaviors, in which the channel conductance can be incrementally adjusted by tuning the duration and sequence of programming voltage. The device allows the emulation of basic synaptic functions, featuring excellent linearity and symmetry in conductance change during long-term potentiation/depression processes. The small asymmetric ratio of 0.15 enables it to be integrated into a neural network for the pattern recognition task with a high accuracy of 90%. The results demonstrate the great potential of TiS3-based synaptic devices for neuromorphic applications.

Two-dimensional semiconducting SnP2Se6 with giant second-harmonic-generation for monolithic on-chip electronic-photonic integration.

Two-dimensional (2D) layered semiconductors with nonlinear optical (NLO) properties hold great promise to address the growing demand of multifunction integration in electronic-photonic integrated circuits (EPICs). However, electronic-photonic co-design with 2D NLO semiconductors for on-chip telecommunication is limited by their essential shortcomings in terms of unsatisfactory optoelectronic properties, odd-even layer-dependent NLO activity and low NLO susceptibility in telecom band. Here we report the synthesis of 2D SnP2Se6, a van der Waals NLO semiconductor exhibiting strong odd-even layer-independent second harmonic generation (SHG) activity at 1550 nm and pronounced photosensitivity under visible light. The combination of 2D SnP2Se6 with a SiN photonic platform enables the chip-level multifunction integration for EPICs. The hybrid device not only features efficient on-chip SHG process for optical modulation, but also allows the telecom-band photodetection relying on the upconversion of wavelength from 1560 to 780 nm. Our finding offers alternative opportunities for the collaborative design of EPICs.

Neuro-inspired optical sensor array for high-accuracy static image recognition and dynamic trace extraction.

Neuro-inspired vision systems hold great promise to address the growing demands of mass data processing for edge computing, a distributed framework that brings computation and data storage closer to the sources of data. In addition to the capability of static image sensing and processing, the hardware implementation of a neuro-inspired vision system also requires the fulfilment of detecting and recognizing moving targets. Here, we demonstrated a neuro-inspired optical sensor based on two-dimensional NbS2/MoS2 hybrid films, which featured remarkable photo-induced conductance plasticity and low electrical energy consumption. A neuro-inspired optical sensor array with 10 × 10 NbS2/MoS2 phototransistors enabled highly integrated functions of sensing, memory, and contrast enhancement capabilities for static images, which benefits convolutional neural network (CNN) with a high image recognition accuracy. More importantly, in-sensor trajectory registration of moving light spots was experimentally implemented such that the post-processing could yield a high restoration accuracy. Our neuro-inspired optical sensor array could provide a fascinating platform for the implementation of high-performance artificial vision systems.

A polarization-sensitive photothermoelectric photodetector based on mixed-dimensional SWCNT-MoS2 heterostructures.

Mixed-dimensional van der Waals (vdW) integration has been demonstrated to be effective for the modulation of the physical properties of homogeneous materials. Herein, we reported the enhancement of photothermal conversion and decrease of thermal conductivity in metallic single-walled carbon nanotube (SWCNT) films with the integration of chemical vapor deposition-grown monolayer MoS2 films. The induced temperature gradient in SWCNT-MoS2 hybrid films drives carrier diffusion to generate photocurrent via the photothermoelectric (PTE) effect, and a self-powered photodetector working in the visible band range from 405 to 785 nm was demonstrated. The maximum responsivity of the device increases by 6 times compared to that of the SWCNT counterpart. More importantly, the mixed-dimensional device exhibits polarization-dependent photogeneration, showing a large anisotropy ratio of 1.55. This work paves a way for developing high-performance, polarization-sensitive photodetectors by mixed-dimensional integration.

2D-1D mixed-dimensional heterostructures: progress, device applications and perspectives.

Two-dimensional (2D) materials have attracted broad interests and been extensively exploited for a variety of functional applications. Moreover, one-dimensional (1D) atomic crystals can also be integrated into 2D templates to create mixed-dimensional heterostructures, and the versatility of combinations provides 2D-1D heterostructures plenty of intriguing physical properties, making them promising candidate to construct novel electronic and optoelectronic nanodevices. In this review, we first briefly present an introduction of relevant fabrication methods and structural configurations for 2D-1D heterostructures integration. We then discuss the emerged intriguing physics, including high optical absorption, efficient carrier separation, fast charge transfer and plasmon-exciton interconversion. Their potential applications such as electronic/optoelectronic devices, photonic devices, spintronic devices and gas sensors, are also discussed. Finally, we provide a brief perspective for the future opportunities and challenges in this emerging field.

Anisotropic Signal Processing with Trigonal Selenium Nanosheet Synaptic Transistors.

Hardware implementation of an artificial neural network requires neuromorphic devices to process information with low energy consumption and high heterogeneity. Here we demonstrate an electrolyte-gated synaptic transistor (EGT) based on a trigonal selenium (t-Se) nanosheet. Due to the intrinsic low conductivity of the Se channel, the t-Se synaptic transistor exhibits ultralow energy consumption, less than 0.1 pJ per spike. More importantly, the intrinsic low symmetry of t-Se offers a strong anisotropy along its c- and a-axis in electrical conductance with a ratio of up to 8.6. The multiterminal EGT device exhibits an anisotropic response of filtering behavior to the same external stimulus, which enables it to mimic the heterogeneous signal transmission process of the axon-multisynapse biostructure in the human brain. The proof-of-concept device in this work represents an important step to develop neuromorphic electronics for processing complex signals.

Photoresponse Enhancement in Monolayer ReS2 Phototransistor Decorated with CdSe-CdS-ZnS Quantum Dots.

ReS2 films are considered as a promising candidate for optoelectronic applications due to their direct band gap character and optical/electrical anisotropy. However, the direct band gap in a narrow spectrum and the low absorption of atomically thin flakes weaken the prospect for light-harvesting applications. Here, we developed an efficient approach to enhance the performance of a ReS2-based phototransistor by coupling CdSe-CdS-ZnS core-shell quantum dots. Under 589 nm laser irradiation, the responsivity of the ReS2 phototransistor decorated with quantum dots could be enhanced by more than 25 times (up to ∼654 A/W) and the rising and recovery time can be also reduced to 3.2 and 2.8 s, respectively. The excellent optoelectronic performance is originated from the coupling effect of quantum dots light absorber and cross-linker ligands 1,2-ethanedithiol. Photoexcited electron-hole pairs in quantum dots can separate and transfer efficiently due to the type-II band alignment and charge exchange process at the interface. Our work shows that the simple hybrid zero- and two-dimensional hybrid system can be employed for photodetection applications.

Chemical Vapor Deposition Growth of Degenerate p-Type Mo-Doped ReS2 Films and Their Homojunction.

Substitutional doping of transition metal dichalcogenide two-dimensional materials has proven to be effective in tuning their intrinsic properties, such as band gap, transport characteristics, and magnetism. In this study, we realized substitutional doping of monolayer rhenium disulfide (ReS2) with Mo via chemical vapor deposition. Scanning transmission electron microscopy demonstrated that Mo atoms are successfully doped into ReS2 by substitutionally replacing Re atoms in the lattice. Electrical measurements revealed the degenerate p-type semiconductor behavior of Mo-doped ReS2 field effect transistors, in agreement with density functional theory calculations. The p-n diode device based on a doped ReS2 and ReS2 homojunction exhibited gate-tunable current rectification behaviors, and the maximum rectification ratio could reach up to 150 at Vd = -2/+2 V. The successful synthesis of p-type ReS2 in this study could largely promote its application in novel electronic and optoelectronic devices.