Gate-Tunable van der Waals Photodiodes with an Ultrahigh Peak-to-Valley Current Ratio.

Photodetectors and imagers based on 2D layered materials are currently subject to a rapidly expanding application space, with an increasing demand for cost-effective and lightweight devices. However, the underlying carrier transport across the 2D homo- or heterojunction channel driven by the external electric field, like a gate or drain bias, is still unclear. Here, a visible-near infrared photodetector based on van der Waals stacked molybdenum telluride (MoTe2 ) and black phosphorus (BP) is reported. The type-I and type-II band alignment can be tuned by the gate and drain voltage combined showing a dynamic modulation of the conduction polarity and negative differential transconductance. The heterojunction devices show a good photoresponse to light illumination ranging from 520-2000 nm. The built-in potential at the MoTe2 /BP interface can efficiently separate photoexcited electron-hole pairs with a high responsivity of 290 mA W-1 , an external quantum efficiency of 70%, and a fast photoresponse of 78 µs under zero bias.

Fast near-infrared photodetectors from p-type SnSe nanoribbons.

Low-dimensional tin selenide nanoribbons (SnSe NRs) show a wide range of applications in optoelectronics fields such as optical switches, photodetectors, and photovoltaic devices due to the suitable band gap, strong light-matter interaction, and high carrier mobility. However, it is still challenging to grow high-quality SnSe NRs for high-performance photodetectors so far. In this work, we successfully synthesized high-quality p-type SnSe NRs by chemical vapor deposition and then fabricated near-infrared photodetectors. The SnSe NR photodetectors show a high responsivity of 376.71 A W-1, external quantum efficiency of 5.65 × 104%, and detectivity of 8.66 × 1011Jones. In addition, the devices show a fast response time with rise and fall time of up to 43µs and 57µs, respectively. Furthermore, the spatially resolved scanning photocurrent mapping shows very strong photocurrent at the metal-semiconductor contact regions, as well as fast generation-recombination photocurrent signals. This work demonstrated that p-type SnSe NRs are promising material candidates for broad-spectrum and fast-response optoelectronic devices.

Emerging Single-Photon Detectors Based on Low-Dimensional Materials.

Single-photon detectors (SPDs) that can sense individual photons are the most sensitive instruments for photodetection. Established SPDs such as conventional silicon or III-V compound semiconductor avalanche diodes and photomultiplier tubes have been used in a wide range of time-correlated photon-counting applications, including quantum information technologies, in vivo biomedical imaging, time-of-flight 3D scanners, and deep-space optical communications. However, further development of these fields requires more sophisticated detectors with high detection efficiency, fast response, and photon-number-resolving ability, etc. Thereby, significant efforts have been made to improve the performance of conventional SPDs and to develop new photon-counting technologies. In this review, the working mechanisms and key performance metrics of conventional SPDs are first summarized. Then emerging photon-counting detectors (in the visible to infrared range) based on 0D quantum dots, 1D quantum nanowires, and 2D layered materials are discussed. These low-dimensional materials exhibit many exotic properties due to the quantum confinement effect. And photodetectors built from these nD-materials (n = 0, 1, 2) can potentially be used for ultra-weak light detection. By reviewing the status and discussing the challenges faced by SPDs, this review aims to provide future perspectives on the research directions of emerging photon-counting technologies.

Post-CMOS Compatible Aluminum Scandium Nitride/2D Channel Ferroelectric Field-Effect-Transistor Memory.

Recent advances in oxide ferroelectric (FE) materials have rejuvenated the field of low-power, nonvolatile memories and made FE memories a commercial reality. Despite these advances, progress on commercial FE-RAM based on lead zirconium titanate has stalled due to process challenges. The recent discovery of ferroelectricity in scandium-doped aluminum nitride (AlScN) presents new opportunities for direct memory integration with logic transistors due to the low temperature of AlScN deposition (approximately 350 °C), making it compatible with back end of the line integration on silicon logic. Here, we present a FE-FET device composed of an FE-AlScN dielectric layer integrated with a two-dimensional MoS2 channel. Our devices show an ON/OFF ratio of ∼106, concurrent with a normalized memory window of 0.3 V/nm. The devices also demonstrate stable memory states up to 104 cycles and state retention up to 105 s. Our results suggest that the FE-AlScN/2D combination is ideal for embedded memory and memory-based computing architectures.

Gate-Tunable Semiconductor Heterojunctions from 2D/3D van der Waals Interfaces.

van der Waals (vdW) semiconductors are attractive for highly scaled devices and heterogeneous integration as they can be isolated into self-passivated, two-dimensional (2D) layers that enable superior electrostatic control. These attributes have led to numerous demonstrations of field-effect devices ranging from transistors to triodes. By exploiting the controlled, substitutional doping schemes in covalently bonded, three-dimensional (3D) semiconductors and the passivated surfaces of 2D semiconductors, one can construct devices that can exceed performance metrics of "all-2D" vdW heterojunctions. Here, we demonstrate 2D/3D semiconductor heterojunctions using MoS2 as the prototypical 2D semiconductor laid upon Si and GaN as the 3D semiconductor layers. By tuning the Fermi levels in MoS2, we demonstrate devices that concurrently exhibit over 7 orders of magnitude modulation in rectification ratios and conductance. Our results further suggest that the interface quality does not necessarily affect Fermi level tuning at the junction, opening up possibilities for novel 2D/3D heterojunction device architectures.

Single Pixel Black Phosphorus Photodetector for Near-Infrared Imaging.

Infrared imaging systems have wide range of military or civil applications and 2D nanomaterials have recently emerged as potential sensing materials that may outperform conventional ones such as HgCdTe, InGaAs, and InSb. As an example, 2D black phosphorus (BP) thin film has a thickness-dependent direct bandgap with low shot noise and noncryogenic operation for visible to mid-infrared photodetection. In this paper, the use of a single-pixel photodetector made with few-layer BP thin film for near-infrared imaging applications is demonstrated. The imaging is achieved by combining the photodetector with a digital micromirror device to encode and subsequently reconstruct the image based on compressive sensing algorithm. Stationary images of a near-infrared laser spot (λ = 830 nm) with up to 64 × 64 pixels are captured using this single-pixel BP camera with 2000 times of measurements, which is only half of the total number of pixels. The imaging platform demonstrated in this work circumvents the grand challenges of scalable BP material growth for photodetector array fabrication and shows the efficacy of utilizing the outstanding performance of BP photodetector for future high-speed infrared camera applications.

Surface Plasmon-Enhanced Photodetection in Few Layer MoS2 Phototransistors with Au Nanostructure Arrays.

2D Molybdenum disulfide (MoS2 ) is a promising candidate material for high-speed and flexible optoelectronic devices, but only with low photoresponsivity. Here, a large enhancement of photocurrent response is obtained by coupling few-layer MoS2 with Au plasmonic nanostructure arrays. Au nanoparticles or nanoplates placed onto few-layer MoS2 surface can enhance the local optical field in the MoS2 layer, due to the localized surface plasmon (LSP) resonance. After depositing 4 nm thick Au nanoparticles sparsely onto few-layer MoS2 phototransistors, a doubled increase in the photocurrent response is observed. The photocurrent of few-layer MoS2 phototransistors exhibits a threefold enhancement with periodic Au nanoarrays. The simulated optical field distribution confirms that light can be trapped and enhanced near the Au nanoplates. These findings offer an avenue for practical applications of high performance MoS2 -based optoelectronic devices or systems in the future.

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 × 10(2), 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.

Giant intrinsic photovoltaic effect in one-dimensional van der Waals grain boundaries.

The photovoltaic effect lies at the heart of eco-friendly energy harvesting. However, the conversion efficiency of traditional photovoltaic effect utilizing the built-in electric effect in p-n junctions is restricted by the Shockley-Queisser limit. Alternatively, intrinsic/bulk photovoltaic effect (IPVE/BPVE), a second-order nonlinear optoelectronic effect arising from the broken inversion symmetry of crystalline structure, can overcome this theoretical limit. Here, we uncover giant and robust IPVE in one-dimensional (1D) van der Waals (vdW) grain boundaries (GBs) in a layered semiconductor, ReS2. The IPVE-induced photocurrent densities in vdW GBs are among the highest reported values compared with all kinds of material platforms. Furthermore, the IPVE-induced photocurrent is gate-tunable with a polarization-independent component along the GBs, which is preferred for energy harvesting. The observed IPVE in vdW GBs demonstrates a promising mechanism for emerging optoelectronics applications.

Room-temperature low-threshold avalanche effect in stepwise van-der-Waals homojunction photodiodes.

Avalanche or carrier-multiplication effect, based on impact ionization processes in semiconductors, has a great potential for enhancing the performance of photodetector and solar cells. However, in practical applications, it suffers from high threshold energy, reducing the advantages of carrier multiplication. Here, we report on a low-threshold avalanche effect in a stepwise WSe2 structure, in which the combination of weak electron-phonon scattering and high electric fields leads to a low-loss carrier acceleration and multiplication. Owing to this effect, the room-temperature threshold energy approaches the fundamental limit, Ethre ≈ Eg, where Eg is the bandgap of the semiconductor. Our findings offer an alternative perspective on the design and fabrication of future avalanche and hot-carrier photovoltaic devices.

Reconfigurable, non-volatile neuromorphic photovoltaics.

The neural network image sensor-which mimics neurobiological functions of the human retina-has recently been demonstrated to simultaneously sense and process optical images. However, highly tunable responsivity concurrent with non-volatile storage of image data in the neural network would allow a transformative leap in compactness and function of these artificial neural networks. Here, we demonstrate a reconfigurable and non-volatile neuromorphic device based on two-dimensional semiconducting metal sulfides that is concurrently a photovoltaic detector. The device is based on a metal-semiconductor-metal (MSM) two-terminal structure with pulse-tunable sulfur vacancies at the M-S junctions. By modulating sulfur vacancy concentrations, the polarities of short-circuit photocurrent can be changed with multiple stable magnitudes. The bias-induced motion of sulfur vacancies leads to highly reconfigurable responsivities by dynamically modulating the Schottky barriers. A convolutional neuromorphic network is finally designed for image processing and object detection using the same device. The results demonstrated that neuromorphic photodetectors can be the key components of visual perception hardware.

Study of the growth mechanism of a self-assembled and ordered multi-dimensional heterojunction at atomic resolution.

Multi-dimensional heterojunction materials have attracted much attention due to their intriguing properties, such as high efficiency, wide band gap regulation, low dimensional limitation, versatility and scalability. To further improve the performance of materials, researchers have combined materials with various dimensions using a wide variety of techniques. However, research on growth mechanism of such composite materials is still lacking. In this paper, the growth mechanism of multi-dimensional heterojunction composite material is studied using quasi-two-dimensional (quasi-2D) antimonene and quasi-one-dimensional (quasi-1D) antimony sulfide as examples. These are synthesized by a simple thermal injection method. It is observed that the consequent nanorods are oriented along six-fold symmetric directions on the nanoplate, forming ordered quasi-1D/quasi-2D heterostructures. Comprehensive transmission electron microscopy (TEM) characterizations confirm the chemical information and reveal orientational relationship between Sb2S3 nanorods and the Sb nanoplate as substrate. Further density functional theory calculations indicate that interfacial binding energy is the primary deciding factor for the self-assembly of ordered structures. These details may fill the gaps in the research on multi-dimensional composite materials with ordered structures, and promote their future versatile applications.

Graphene/MoS2-xOx/graphene photomemristor with tunable non-volatile responsivities for neuromorphic vision processing.

Conventional artificial intelligence (AI) machine vision technology, based on the von Neumann architecture, uses separate sensing, computing, and storage units to process huge amounts of vision data generated in sensory terminals. The frequent movement of redundant data between sensors, processors and memory, however, results in high-power consumption and latency. A more efficient approach is to offload some of the memory and computational tasks to sensor elements that can perceive and process the optical signal simultaneously. Here, we proposed a non-volatile photomemristor, in which the reconfigurable responsivity can be modulated by the charge and/or photon flux through it and further stored in the device. The non-volatile photomemristor has a simple two-terminal architecture, in which photoexcited carriers and oxygen-related ions are coupled, leading to a displaced and pinched hysteresis in the current-voltage characteristics. For the first time, non-volatile photomemristors implement computationally complete logic with photoresponse-stateful operations, for which the same photomemristor serves as both a logic gate and memory, using photoresponse as a physical state variable instead of light, voltage and memresistance. The polarity reversal of photomemristors shows great potential for in-memory sensing and computing with feature extraction and image recognition for neuromorphic vision.

Geometry-asymmetric photodetectors from metal-semiconductor-metal van der Waals heterostructures.

The functional diversities of two-dimensional (2D) material devices with simple architectures are ultimately limited by immature doping techniques. An alternative strategy is to use geometry-asymmetric metal-semiconductor-metal (GA-MSM) structures, which enable the basic functions of semiconductor junctions such as rectification and photovoltaics. Here, the mixed-dimensional van der Waals heterostructures (MDvdWHs) based on the separation and self-assembly of p-type SnS layered nanosheets (NSs) and n-type SnS2 nanoparticles (NPs) are obtained using an aqueous phase exfoliation (APE) method. Due to the surface charge transfer doping, the carrier transport mechanism of devices based on MDvdWHs turns from thermionic field emission (TFE) to thermionic emission (TE), with the rectification factor (Iforward/Ireverse) changing from 0.7 to 3. To further illustrate the experimental results, the generic current transport models of GA-MSM devices have been established based on the TE and TFE mechanisms in which the TE and TFE mechanisms lead to opposite rectification phenomena in good agreement with the experimental results. The GA-MSM devices show a photovoltaic effect with a high responsivity of 35 A W-1 and detectivity of 3.4 × 1011 cm Hz1/2 W-1. This study not only provides a novel strategy to design photovoltaic devices with MDvdWHs, but more importantly, we have established fundamental models for the rectification behavior of GA-MSM devices.

Momentum-matching and band-alignment van der Waals heterostructures for high-efficiency infrared photodetection.

Two-dimensional (2D) infrared photodetectors always suffer from low quantum efficiency (QE) because of the limited atomically thin absorption. Here, we reported 2D black phosphorus (BP)/Bi2O2Se van der Waals (vdW) photodetectors with momentum-matching and band-alignment heterostructures to achieve high QE. The QE was largely improved by optimizing the generation, suppressing the recombination, and improving the collection of photocarriers. Note that momentum-matching BP/Bi2O2Se heterostructures in k-space lead to the highly efficient generation and transition of photocarriers. The recombination process can be largely suppressed by lattice mismatching-immune vdW interfaces. Furthermore, type II BP/Bi2O2Se vdW heterostructures could also assist fast transport and collection of photocarriers. By constructing momentum-matching and band-alignment heterostructures, a record-high QE of 84% at 1.3 micrometers and 76.5% at 2 micrometers have been achieved in BP/Bi2O2Se vdW photodetectors.

Direct Optoelectronic Imaging of 2D Semiconductor-3D Metal Buried Interfaces.

The semiconductor-metal junction is one of the most critical factors for high-performance electronic devices. In two-dimensional (2D) semiconductor devices, minimizing the voltage drop at this junction is particularly challenging and important. Despite numerous studies concerning contact resistance in 2D semiconductors, the exact nature of the buried interface under a three-dimensional (3D) metal remains unclear. Herein, we report the direct measurement of electrical and optical responses of 2D semiconductor-metal buried interfaces using a recently developed metal-assisted transfer technique to expose the buried interface, which is then directly investigated using scanning probe techniques. We characterize the spatially varying electronic and optical properties of this buried interface with <20 nm resolution. To be specific, potential, conductance, and photoluminescence at the buried metal/MoS2 interface are correlated as a function of a variety of metal deposition conditions as well as the type of metal contacts. We observe that direct evaporation of Au on MoS2 induces a large strain of ∼5% in the MoS2 which, coupled with charge transfer, leads to degenerate doping of the MoS2 underneath the contact. These factors lead to improvement of contact resistance to record values of 138 kΩ µm, as measured using local conductance probes. This approach was adopted to characterize MoS2-In/Au alloy interfaces, demonstrating contact resistance as low as 63 kΩ µm. Our results highlight that the MoS2/metal interface is sensitive to device fabrication methods and provide a universal strategy to characterize buried contact interfaces involving 2D semiconductors.

Controllable Doping in 2D Layered Materials.

For each generation of semiconductors, the issue of doping techniques is always placed at the top of the priority list since it determines whether a material can be used in the electronic and optoelectronic industry or not. When it comes to 2D materials, significant challenges have been found in controllably doping 2D semiconductors into p- or n-type, let alone developing a continuous control of this process. Here, a unique self-modulated doping characteristic in 2D layered materials such as PtSSe, PtS0.8 Se1.2 , PdSe2 , and WSe2 is reported. The varying number of vertically stacked-monolayers is the critical factor for controllably tuning the same material from p-type to intrinsic, and to n-type doping. Importantly, it is found that the thickness-induced lattice deformation makes defects in PtSSe transit from Pt vacancies to anion vacancies based on dynamic and thermodynamic analyses, which leads to p- and n-type conductance, respectively. By thickness-modulated doping, WSe2 diode exhibits a high rectification ratio of 4400 and a large open-circuit voltage of 0.38 V. Meanwhile, the PtSSe detector overcomes the shortcoming of large dark-current in narrow-bandgap optoelectronic devices. All these findings provide a brand-new perspective for fundamental scientific studies and applications.

Recent Progress on Electrical and Optical Manipulations of Perovskite Photodetectors.

Photodetectors built from conventional bulk materials such as silicon, III-V or II-VI compound semiconductors are one of the most ubiquitous types of technology in use today. The past decade has witnessed a dramatic increase in interest in emerging photodetectors based on perovskite materials driven by the growing demands for uncooled, low-cost, lightweight, and even flexible photodetection technology. Though perovskite has good electrical and optical properties, perovskite-based photodetectors always suffer from nonideal quantum efficiency and high-power consumption. Joint manipulation of electrons and photons in perovskite photodetectors is a promising strategy to improve detection efficiency. In this review, electrical and optical characteristics of typical types of perovskite photodetectors are first summarized. Electrical manipulations of electrons in perovskite photodetectors are discussed. Then, artificial photonic nanostructures for photon manipulations are detailed to improve light absorption efficiency. By reviewing the manipulation of electrons and photons in perovskite photodetectors, this review aims to provide strategies to achieve high-performance photodetectors.

Blackbody-sensitive room-temperature infrared photodetectors based on low-dimensional tellurium grown by chemical vapor deposition.

Blackbody-sensitive room-temperature infrared detection is a notable development direction for future low-dimensional infrared photodetectors. However, because of the limitations of responsivity and spectral response range for low-dimensional narrow bandgap semiconductors, few low-dimensional infrared photodetectors exhibit blackbody sensitivity. Here, highly crystalline tellurium (Te) nanowires and two-dimensional nanosheets were synthesized by using chemical vapor deposition. The low-dimensional Te shows high hole mobility and broadband detection. The blackbody-sensitive infrared detection of Te devices was demonstrated. A high responsivity of 6650 A W-1 (at 1550-nm laser) and the blackbody responsivity of 5.19 A W-1 were achieved. High-resolution imaging based on Te photodetectors was successfully obtained. All the results suggest that the chemical vapor deposition-grown low-dimensional Te is one of the competitive candidates for sensitive focal-plane-array infrared photodetectors at room temperature.

Hybrid exciton-plasmon-polaritons in van der Waals semiconductor gratings.

Van der Waals materials and heterostructures that manifest strongly bound exciton states at room temperature also exhibit emergent physical phenomena and are of great promise for optoelectronic applications. Here, we demonstrate that nanostructured, multilayer transition metal dichalcogenides (TMDCs) by themselves provide an ideal platform for excitation and control of excitonic modes, paving the way to exciton-photonics. Hence, we show that by patterning the TMDCs into nanoresonators, strong dispersion and avoided crossing of exciton, cavity photons and plasmon polaritons with effective separation energy exceeding 410 meV can be controlled with great precision. We further observe that inherently strong TMDC exciton absorption resonances may be completely suppressed due to excitation of hybrid light-matter states and their interference. Our work paves the way to the next generation of integrated exciton optoelectronic nano-devices and applications in light generation, computing, and sensing.