Advances in Heterostructures for Optoelectronic Devices: Materials, Properties, Conduction Mechanisms, Device Applications.

Atomically thin 2D transition metal dichalcogenides (TMDs) have recently been spotlighted for next-generation electronic and photoelectric device applications. TMD materials with high carrier mobility have superior electronic properties different from bulk semiconductor materials. 0D quantum dots (QDs) possess the ability to tune their bandgap by composition, diameter, and morphology, which allows for a control of their light absorbance and emission wavelength. However, QDs exhibit a low charge carrier mobility and the presence of surface trap states, making it difficult to apply them to electronic and optoelectronic devices. Accordingly, 0D/2D hybrid structures are considered as functional materials with complementary advantages that may not be realized with a single component. Such advantages allow them to be used as both transport and active layers in next-generation optoelectronic applications such as photodetectors, image sensors, solar cells, and light-emitting diodes. Here, recent discoveries related to multicomponent hybrid materials are highlighted. Research trends in electronic and optoelectronic devices based on hybrid heterogeneous materials are also introduced and the issues to be solved from the perspective of the materials and devices are discussed.

Probing Optical Multi-Level Memory Effects in Single Core-Shell Quantum Dots and Application Through 2D-0D Hybrid Inverters.

Challenges in the development of a multi-level memory (MM) device for multinary arithmetic computers have posed an obstacle to low-power, ultra-high-speed operation. For the effective transfer of a huge amount of data between arithmetic and storage devices, optical communication technology represents a compelling solution. Here, by replicating a floating gate architecture with CdSe/ZnS type-I core/shell quantum dots (QDs), a 2D-0D hybrid optical multi-level memory (OMM) device operated is demonstrated by laser pulses. In the device, laser pulses create linear optically trapped currents with MM characteristics, while conversely, voltage pulses reset all the trapped currents at once. Assuming electron transfer via the energy band alignment between MoS2 and CdSe, the study also establishes the mechanism of the OMM effect. Analysis of the designed device led to a new hypothesis that charge transfer is difficult for laterally adjacent QDs facing a double ZnS shell, which is tested by separately stimulating different positions on the 2D-0D hybrid structure with finely focused laser pulses. Results indicate that each laser pulse induced independent MM characteristics in the 2D-0D hybrid architecture. Based on this phenomenon, we propose a MM inverter to produce MM effects, such as programming and erasing, solely through the use of laser pulses. Finally, the feasibility of a fully optically-controlled intelligent system based on the proposed OMM inverters is evaluated through a CIFAR-10 pattern recognition task using a convolutional neural network.

Fermi-Level Pinning-Free WSe2 Transistors via 2D Van der Waals Metal Contacts and Their Circuits.

Precise control over the polarity of transistors is a key necessity for the construction of complementary metal-oxide-semiconductor circuits. However, the polarity control of 2D transistors remains a challenge because of the lack of a high-work-function electrode that completely eliminates Fermi-level pinning at metal-semiconductor interfaces. Here, a creation of clean van der Waals contacts is demonstrated, wherein a metallic 2D material, chlorine-doped SnSe2 (Cl-SnSe2 ), is used as the high-work-function contact, providing an interface that is free of defects and Fermi-level pinning. Such clean contacts made from Cl-SnSe2 can pose nearly ideal Schottky barrier heights, following the Schottky-Mott limit and thus permitting polarity-controllable transistors. With the integration of Cl-SnSe2 as contacts, WSe2 transistors exhibit pronounced p-type characteristics, which are distinctly different from those of the devices with evaporated metal contacts, where n-type transport is observed. Finally, this ability to control the polarity enables the fabrication of functional logic gates and circuits, including inverter, NAND, and NOR.

Multilayer WSe2 /MoS2 Heterojunction Phototransistors through Periodically Arrayed Nanopore Structures for Bandgap Engineering.

While 2D transition metal dichalcogenides (TMDs) are promising building blocks for various optoelectronic applications, limitations remain for multilayered TMD-based photodetectors: an indirect bandgap and a short carrier lifetime by strongly bound excitons. Accordingly, multilayered TMDs with a direct bandgap and an enhanced carrier lifetime are required for the development of various optoelectronic devices. Here, periodically arrayed nanopore structures (PANS) are proposed for improving the efficiency of multilayered p-WSe2 /n-MoS2 phototransistors. Density functional theory calculations as well as photoluminescence and time-resolved photoluminescence measurements are performed to characterize the photodetector figures of merit of multilayered p-WSe2 /n-MoS2 heterostructures with PANS. The characteristics of the heterojunction devices with PANS reveal an enhanced responsivity and detectivity measured under 405 nm laser excitation, which at 1.7 × 104 A W-1 and 1.7 × 1013 Jones are almost two orders of magnitude higher than those of pristine devices, 3.6 × 102 A W-1 and 3.6 × 1011 Jones, respectively. Such enhanced optical properties of WSe2 /MoS2 heterojunctions with PANS represent a significant step toward next-generation optoelectronic applications.

An Asymmetry Field-Effect Phototransistor for Solving Large Exciton Binding Energy of 2D TMDCs.

The probing of fundamental photophysics is a key prerequisite for the construction of diverse optoelectronic devices and circuits. To date, though, photocarrier dynamics in 2D materials remains unclear, plagued primarily by two issues: a large exciton binding energy, and the lack of a suitable system that enables the manipulation of excitons. Here, a WSe2 -based phototransistor with an asymmetric split-gate configuration is demonstrated, which is named the "asymmetry field-effect phototransistor" (AFEPT). This structure allows for the effective modulation of the electric-field profile across the channel, thereby providing a standard device platform for exploring the photocarrier dynamics of the intrinsic WSe2 layer. By controlling the electric field, this work the spatial evolution of the photocurrent is observed, notably with a strong signal over the entire WSe2 channel. Using photocurrent and optical spectroscopy measurements, the physical origin of the novel photocurrent behavior is clarified and a room-temperature exciton binding energy of 210 meV is determined with the device. In the phototransistor geometry, lateral p-n junctions serve as a simultaneous pathway for both photogenerated electrons and holes, reducing their recombination rate and thus enhancing photodetection. The study establishes a new device platform for both fundamental studies and technological applications.

Near-Infrared Self-Powered Linearly Polarized Photodetection and Digital Incoherent Holography Using WSe2/ReSe2 van der Waals Heterostructure.

Polarization-sensitive photodetection has attracted considerable attention as an emerging technology for future optoelectronic applications such as three-dimensional (3D) imaging, quantum optics, and encryption. However, traditional photodetectors based on Si or III-V InGaAs semiconductors cannot directly detect polarized light without additional optical components. Herein, we demonstrate a self-powered linear-polarization-sensitive near-infrared (NIR) photodetector using a two-dimensional WSe2/ReSe2 van der Waals heterostructure. The WSe2/ReSe2 heterojunction photodiode with semivertical geometry exhibits excellent performance: an ideality factor of 1.67, a broad spectral photoresponse of 405-980 nm with a significant photovoltaic effect, outstanding linearity with a linear dynamic range wider than 100 dB, and rapid photoswitching behavior with a cutoff frequency up to 100 kHz. Strongly polarized excitonic transitions around the band edge in ReSe2 lead to significant 980 nm NIR linear-polarization-dependent photocurrent. This linear polarization sensitivity remains stable even after exposure to air for longer than five months. Furthermore, by leveraging the NIR (980 nm)-selective linear polarization detection of this photodiode under photovoltaic operation, we demonstrate digital incoherent holographic 3D imaging.

Frequency Doubler and Universal Logic Gate Based on Two-Dimensional Transition Metal Dichalcogenide Transistors with Low Power Consumption.

Two-dimensional transition metal dichalcogenide semiconductors are very promising candidates for future electronic applications with low power consumption due to a low leakage current and high on-off current ratio. In this study, we suggest a complementary circuit consisting of ambipolar WSe2 and n-MoS2 field-effect transistors (FETs), which demonstrate dual functions of a frequency doubler and single inversion AND (SAND) logic gate. In order to reduce the power consumption, a high-quality thin h-BN single crystal is used as a gate dielectric that leads to a low operating voltage of less than 5 V. By combining the low operating voltage with a low operating current in the complementary circuit, a low power consumption of 300 nW (a minimum of 10 pW) has been achieved, which is a significant improvement compared to the tens of µW consumed by a graphene channel. The complementary circuit shows the effective frequency doubling of the input with a dynamic range from 20 to 100 Hz. Furthermore, this circuit satisfies all the truth tables of a SAND logic gate that can be used as a universal logic gate like NAND. Considering that the NAND logic gate generally consists of four transistors, it is significantly advantageous to implement the equivalent circuit SAND logic gate with only two FETs. Our results open up possibilities for analog- and logic-circuit applications based on low-dimensional semiconductors.

Probing the Importance of Charge Balance and Noise Current in WSe2/WS2/MoS2 van der Waals Heterojunction Phototransistors by Selective Electrostatic Doping.

Heterojunction structures using 2D materials are promising building blocks for electronic and optoelectronic devices. The limitations of conventional silicon photodetectors and energy devices are able to be overcome by exploiting quantum tunneling and adjusting charge balance in 2D p-n and n-n junctions. Enhanced photoresponsivity in 2D heterojunction devices can be obtained with WSe2 and BP as p-type semiconductors and MoS2 and WS2 as n-type semiconductors. In this study, the relationship between photocurrent and the charge balance of electrons and holes in van der Waals heterojunctions is investigated. To observe this phenomenon, a p-WSe2/n-WS2/n-MoS2 heterojunction device with both p-n and n-n junctions is fabricated. The device can modulate the charge carrier balance between heterojunction layers to generate photocurrent upon illumination by selectively applying electrostatic doping to a specific layer. Using photocurrent mapping, the operating transition zones for the device is demonstrated, allowing to accurately identify the locations where photocurrent generates. Finally, the origins of flicker and shot noise at the different semiconductor interfaces are analyzed to understand their effect on the photoresponsivity and detectivity of unit active area (2.5 µm2, λ = 405 nm) in the p-WSe2/n-WS2/n-MoS2 heterojunction device.

Realizing Long-Term Stability and Thickness Control of Black Phosphorus by Ambient Thermal Treatment.

Few-layer black phosphorus (BP) has shown great potential for next-generation electronics with tunable band gap and high carrier mobility. For the electronic applications, the thickness modulation of a BP flake is essential due to its thickness-dependent electronic properties. However, controlling the precise thickness of few-layer BP is a challenge for the high-performance device applications. In this study, we demonstrate that thermal treatment under ambient condition precisely controls the thickness of BP flake. The thermal etching method utilizes the chemical reactivity of BP surface with oxygen and water molecules by the repeated formation and evaporation of phosphoric acid during thermal annealing. Field-effect transistor of the thickness-modulated BP sheet by thermal etching method shows a high hole mobility of ∼576 cm2 V-1 s-1 and a high on-off ratio of ∼105. The stability of the BP devices remained for 1 month under ambient condition without an additional protecting layer, resulting from the preservation of active BP layers below native surface phosphorus oxide.

Hybrid Black Phosphorus/Zero-Dimensional Quantum Dot Phototransistors: Tunable Photodoping and Enhanced Photoresponsivity.

Recently, black phosphorus (BP) with direct band gap exhibited excellent potential for optoelectronic applications because of its high charge carrier mobility and low dark current as well as the variable band gap of 0.3-1.5 eV depending on the number of layers. However, few-layer BP-based phototransistors (photo-FETs) have been limited in sensitivity and wavelength selectivity. To overcome the drawback of these photo-FETs, we studied hybrid photo-FETs combined with the novel properties of the two materials between the channel and sensitizer layers. By combining a strong absorbance of a quantum dot (QD) layer and a two-dimensional layer material with high carrier mobility, the hybrid photo-FETs are expected to produce high-performance photodetectors that can effectively control the responsivity, detectivity, and response time. In this study, we demonstrate that the photogenerated carriers formed from QD sensitizer layers migrate to the BP transport layer with high charge mobility and not only improve the photodetector performance but also enhance the photodoping effect of the BP transport layer with an ambipolar characteristic by electrons transferred from n-type CdSe QDs or holes injected from p-type PbS QDs. The responsivity and detectivity of hybrid BP/0D photo-FETs exhibit 1.16 × 109 A W-1 and 7.53 × 1016 Jones for the BP/CdSe QD photo-FET and 5.36 × 108 A W-1 and 1.89 × 1016 Jones for the BP/PbS QD photo-FET, respectively. The photocurrent rise (τrise) and decay (τdecay) times were τrise = 0.406 s and τdecay = 0.815 s for BP/CdSe QD photo-FET and τrise = 0.576 s and τdecay = 0.773 s for BP/PbS QD photo-FET, respectively.

Dual-Gate Black Phosphorus Field-Effect Transistors with Hexagonal Boron Nitride as Dielectric and Passivation Layers.

Two-dimensional black phosphorus (BP) has attracted much attention recently because of its applicability in high-performance electronic and optoelectronic devices. BP field-effect transistors (FETs) with a tunable band gap (0.3-1.5 eV) have demonstrated a high on-off current ratio and a high hole mobility with an ambipolar behavior in global-gated devices. However, local-gated BP FETs for integrated circuits have been reported with only p-type behaviors and a low on-current compared with global-gated BP FETs. Furthermore, BP, which is not stable in air, forms sharp spikes on its surface when exposed to humid air. This phenomenon plays a role in accelerating the degradation of the electrical properties of BP devices, which can occur even within a day. In this paper, we first demonstrate the origin of transport limitations of local-gated BP FETs by comparing the transport properties of hexagonal boron nitride (h-BN)-based device architectures with those of a bottom-gated BP FET on a Si/SiO2 substrate. By using h-BN as passivation and dielectric layers, BP FETs with a low gate operating voltage were fabricated with two different transistor geometries: top-gated and bottom-gated FETs. The highest mobility extracted from the global-gated BP FETs was 249 cm2 V-1 s-1 with a subthreshold swing of 848 mV dec-1.

Recovery Mechanism of Degraded Black Phosphorus Field-Effect Transistors by 1,2-Ethanedithiol Chemistry and Extended Device Stability.

Black phosphorus (BP) has drawn enormous attention for both intriguing material characteristics and electronic and optoelectronic applications. In spite of excellent advantages for semiconductor device applications, the performance of BP devices is hampered by the formation of phosphorus oxide on the BP surface under ambient conditions. It is thus necessary to resolve the oxygen-induced degradation on the surface of BP to recover the characteristics and stability of the devices. To solve this problem, it is demonstrated that a 1,2-ethanedithiol (EDT) treatment is a simple and effective way to remove the bubbles formed on the BP surface. The device characteristics of the degraded BP field-effect transistor (FET) are completely recovered to the level of the pristine cases by the EDT treatment. The underlying principle of bubble elimination on the BP surface by the EDT treatment is systematically analyzed by density functional theory calculation, atomic force microscopy, and X-ray photoelectron spectroscopy analysis. In addition, the performance of the hexagonal boron nitride-protected BP FET is completely retained without changing device characteristics even when exposed to 30 d or more in air. The EDT-induced recovering effect will allow a new route for the optimization of electronic and optoelectronic devices based on BP.

A hybrid MoS2 nanosheet-CdSe nanocrystal phototransistor with a fast photoresponse.

2-Dimensional (2D) and 0-dimensional (0D) hybrid nanostructures have been reported as promising new systems for highly-sensitive and wavelength-tunable photodetectors. Although the performance of hybrid photodetectors was enhanced by charge injection from 0D nanocrystals (NCs) to 2D nanosheets (NSs), the response time of hybrid photodetectors is still very slow due to the trapping and leakage of residual carriers at the interfaces of the hybrid materials. Here, we demonstrate a MoS2/CdSe hybrid phototransistor with enhanced responsivity of 2.5 × 105 A W-1 and detectivity of 1.24 × 1014 Jones. In addition, the device exhibited a fast rise (τrise) and decay time (τdecay) of 60 ms, respectively. The mechanism for the improved photoresponse time has been discussed using a charge injection model in an n-n type heterojunction energy band diagram of hybrid materials.

Bandgap tunable colloidal Cu-based ternary and quaternary chalcogenide nanosheets via partial cation exchange.

Copper based ternary and quaternary semiconductor nanostructures are of great interest for the fabrication of low cost photovoltaics. Although well-developed syntheses are available for zero dimensional (0D) nanoparticles, colloidal synthesis of two dimensional (2D) nanosheets remains a big challenge. Here we report, for the first time, a simple and reproducible cation exchange approach for 2D colloidal Cu2GeSe3, Cu2ZnGeSe4 and their alloyed Cu2GeS(x)Se(3-x), Cu2ZnGeS(x)Se(4-x) nanosheets using pre-synthesized Cu(2x)Se nanosheets as a template. A mechanism for the formation of Cu(2-x)Se nanosheets has been studied in detail. In situ oxidation of Cu(+) ions to form a CuSe secondary phase facilitates the formation of Cu(2-x)Se NSs. The obtained ternary and quaternary nanosheets have average lateral size in micrometers and thickness less than 5 nm. This method is general and can be extended to produce other important ternary semiconductor nanosheets such as CuIn(1-x)Ga(x)Se2. The optical band gap of these nanosheets is tuned from 1 to 1.48 eV, depending on their composition.