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High-precision artificial synaptic devices compatible with existing CMOS technology are essential for realizing robust neuromorphic hardware systems with reliable parallel analogue computation beyond the von Neumann serial digital computing architecture. However, critical issues related to reliability and variability, such as nonlinearity and asymmetric weight updates, have been great challenges in the implementation of artificial synaptic devices in practical neuromorphic hardware systems. Herein, a robust three-terminal two-dimensional (2D) MoS

We investigated chemical vapor-deposited (CVD) two-dimensional (2D) niobium diselenide (NbSe2) material for the resistive switching and synaptic characteristics. Three different atomic switch devices with Ag/HfO2/Pt, Ag/Ti/HfO2/Pt, and Ag/NbSe2/HfO2/Pt were studied as both memory and neuromorphic devices. Both the inserted Ti and NbSe2 buffer layers effectively control the stochastic Ag-ion diffusion, leading to suppressed variation of switching characteristics, which is a critical issue in an atomic switch device. Especially, the device with the 2D NbSe2 buffer layer strikingly enhanced the device reliability in both endurance and retention. In conjunction with scanning transmission electron microscopy (STEM) and energy-dispersive spectrometry (EDS) analysis of the control of the Ag-ion migration, it was understood that filament connection is interrelated with the SET and RESET processes. Besides resistive behaviors in the memory device, various synapse functions such as spike-rate-dependent plasticity (SRDP), forgetting curve, potentiation, and depression were demonstrated with an atomic switch with the 2D NbSe2 buffer layer. Furthermore, the emulated long-term synaptic property was simulated using the MNIST 28 × 28 pixel database. Using adopting a CVD 2D NbSe2 blocking layer, the stochastic Ag-ion diffusion behavior is well-controlled and therefore stable switching and synapse functions are attained.

Atomic two-dimensional (2D) transition metal dichalcogenides (TMDs) have attracted significant attention for application in various optoelectronic devices such as image sensors, biomedical imaging systems, and consumer electronics and in diverse spectroscopic analyses. However, a complicated fabrication process, involving transfer and alignment of as-synthesized 2D layers onto flexible target substrates, hinders the development of flexible high-performance heterojunction-based photodetectors. Herein, an ultra-flexible 2D-MoS2/Si heterojunction-based photodetector is successfully fabricated through atmospheric-pressure plasma enhanced chemical vapor deposition, which enables the direct deposition of multi-layered MoS2 onto a flexible Si substrate at low temperature (

Transparent hydrogenated amorphous silicon thin-film solar modules are fabricated using oxide-metal-oxide (OMO) electrodes as the back electrode for building-integrated photovoltaic applications. The outer aluminum-doped zinc oxide and inner silver layers constitute a thin OMO electrode (~110 nm thick), exhibiting a sheet resistance of 6.8 Ω/□ and an average transmittance of ~88% in the visible range of 400–800 nm. The external quantum efficiency and average transmittance of the cell were investigated for the absorber-layer thickness using the finite-difference time-domain method, and it was found that the optical loss in the cell was mainly due to the absorption of the front electrode in the ultra-violet region and free-carrier absorption of the OMO in the infrared region. Fabrication issues are introduced for a 532 nm short-pulse high-power laser patterning process for transparent modules with thin OMO electrodes. Optimization of the laser power for the P2 and P3 laser processes is demonstrated by observing the profiles and measuring the shunt resistance of the laser-patterned edges. Furthermore, the cell width is optimized based on an equivalent circuit model using PSpice simulation. The highest module efficiency and average transparency achieved in the range of 500–800 nm were 5.6% and 15.2%, respectively. The short-circuit current density, fill factor, and open-circuit voltage per cell of the module were found to be 10.8 mA/cm2, 62.7%, and 0.830 V, respectively.

A major problem in the application of mesoporous TiO2 as an electron transport layer for flexible perovskite solar cells is that a high-temperature sintering process is required to remove organic a...

Initial reversibility and excellent capacity retention are the key requirements for the success of high-capacity electrode materials in high-performance Li-ion batteries and pose a number of challenges to development. Silicon has been regarded as a promising anode material because of its outstanding theoretical capacity. However, it suffers from colossal volume change and continuous formation of unstable solid electrolyte interphases during lithiation/delithiation processes, which eventually result in low initial Coulombic efficiency (ICE) and severe capacity decay. To circumvent these challenges, a new sandwich Si anode (SiO

In this study, we aimed to develop semitransparent solar cells (STSCs) using hydrogenated amorphous silicon (a-Si:H) at a low temperature of 150 °C to support the fabrication of flexible solar modules, applicable in building-integrated photovoltaics (BIPV). To compensate for the presumable loss of device performance at such a low processing temperature, careful control of the p/i interface is proposed. We fabricated buffer layers with hydrogen (H 2 )/silane (SiH 4 ) gas flow ratios (R) ranging from 4 to 16 (R 4 –R 16 ) to investigate their characteristics and incorporate them at the p/i interface by considering energy band matching. By employing this buffer, the power conversion efficiency (PCE) of a STSC was improved from 4.83% to 5.57% which is the best record in a-Si:H STSCs processed at a low temperature of 150 °C. This p/i interfacial buffer can support the realization of flexible a-Si:H-based BIPV systems using plastic- or polymer-based substrates.

We focused on developing penetration-type semitransparent thin-film solar cells (STSCs) using hydrogenated amorphous Si (a-Si:H) for a building-integrated photovoltaic (BIPV) window system. Instead of conventional p-type a-Si:H, p-type hydrogenated microcrystalline Si oxide (p-μc-SiOx:H) was introduced for a wide-bandgap and conductive window layer. For these purposes, we tuned the CO2/SiH4 flow ratio (R) during p-μc-SiOx:H deposition. The film crystallinity decreased from 50% to 13% as R increased from 0.2 to 1.2. At the optimized R of 0.6, the quantum efficiency was improved under short wavelengths by the suppression of p-type layer parasitic absorption. The series resistance was well controlled to avoid fill factor loss at R = 0.6. Furthermore, we introduced dual buffers comprising p-a-SiOx:H/i-a-Si:H at the p/i interface to alleviate interfacial energy-band mismatch. The a-Si:H STSCs with the suggested window and dual buffers showed improvements in transmittance and efficiency from 22.9% to 29.3% and from 4.62% to 6.41%, respectively, compared to the STSC using a pristine p-a-Si:H window.

We investigated chemical vapor-deposited (CVD) two-dimensional (2D) niobium diselenide (NbSe

Atomic two-dimensional (2D) transition metal dichalcogenides (TMDs) have attracted significant attention for application in various optoelectronic devices such as image sensors, biomedical imaging systems, and consumer electronics and in diverse spectroscopic analyses. However, a complicated fabrication process, involving transfer and alignment of as-synthesized 2D layers onto flexible target substrates, hinders the development of flexible high-performance heterojunction-based photodetectors. Herein, an ultra-flexible 2D-MoS2/Si heterojunction-based photodetector is successfully fabricated through atmospheric-pressure plasma enhanced chemical vapor deposition, which enables the direct deposition of multi-layered MoS2 onto a flexible Si substrate at low temperature (200 °C). The photodetector is responsive to near infrared light (λ = 850 nm), showing responsivity of 10.07 mA W-1 and specific detectivity (D*) of 4.53 × 1010 Jones. The measured photocurrent as a function of light intensity exhibits good linearity with a power law exponent of 0.84, indicating negligible trapping/de-trapping of photo-generated carriers at the heterojunction interface, which facilitates photocarrier collection. Furthermore, the photodetectors can be bent with a small bending radius (5 mm) and wrapped around a glass rod, showing excellent photoresponsivity under various bending radii. Hence, the device exhibits excellent flexibility, rollability, and durability under harsh bending conditions. This photodetector has significant potential for use in next-generation flexible and patchable optoelectronic devices.

Uniform, well-ordered sub-20 nm patterns can be generated by the templated self-assembly of block copolymers (BCPs) with a high Flory-Huggins interaction parameter (χ). However, the self-assembled BCP monolayers remain limited in the possible structural geometries. Here, we introduce a multiple self-assembly method which uses di-BCPs to produce diverse morphologies, such as dot, dot-in-honeycomb, line-on-dot, double-dot, pondering, dot-in-pondering, and line-on-pondering patterns. To improve the diversity of BCP morphological structures, we employed sphere-forming and cylinder-forming poly(styrene-block-dimethylsiloxane) (PS-b-PDMS) BCPs with a high χ. The self-assembled mono-layer and double-layer SiOx dot patterns were modified at a high temperature (∼800 °C), showing hexagonally arranged (dot) and double-hexagonally arranged (pondering) SiOx patterns, respectively. We successfully obtained additional new nanostructures (big-dot, dot-in-honeycomb, line-on-dot, pondering, dot-in-pondering, and line-on-pondering types) through a second self-assembly of cylinder-forming BCPs using the dot and pondering patterns as guiding templates. This simple approach can likely be extended to the multiple self-assembly of many other BCPs with good functionality, significantly contributing to the development of various nanodevices.

A major problem in the application of mesoporous TiO

We focused on fabricating all p-i-n layer hydrogenated amorphous silicon oxide (a-SiOx:H) thin film solar cells in order to improve their transmittance in visible ranges of 500–800 nm for application in building integrated photovoltaics system. We varied CO2/SiH4 (R) gas flow ratio from 0 to 0.6 for i-layer to investigate an effect of oxygen addition. When the R ratio increased, the transmittance of devices improved due to the enhancement in optical bandgap of the absorber. However, power conversion efficiency (PCE) decreased owing to the increase in defects and recombination rate which might be ascribed to back bonding of oxygen atoms with Si atoms. Unlike other R flow ratio, however, the PCE of a-SiOx:H solar cell at the R ratio of 0.2 was slightly improved by the increase in open circuit voltage as indicated by the wide band gap and the increase in quantum efficiency within short-wavelengths (300–500 nm). We introduced a figure of merit (FOM), multiplication of PCE and average transmittance in range of 500–800 nm, in order to assess the performance of transparent solar cells. The a-SiOx:H solar cell at the R ratio of 0.2 achieved the highest FOM, which was better than conventional amorphous silicon solar cell.

We developed a transparent oxide–metal–oxide (OMO) structure using aluminum-doped zinc oxide and oxidized silver (AgOx) as a transparent electrode of a hydrogenated amorphous silicon (a-Si:H) thin-film solar cell for use in building-integrated photovoltaic (BIPV) windows. The oxygen (O2) addition (O2 flow rate) was optimized for a metal-to-dielectric intermediate-phase AgOx OMO to have high transparency and high conductivity, which were confirmed by finite-difference time-domain simulation. Using the AgOx OMO as a rear electrode, transparent a-Si:H solar cells were fabricated for BIPV window application. The performance of the fabricated cells showed highest bifacial efficiency (b-η) of 7.87% at AgOx OMO of 1 sccm, and highest average transmittance (T500–800, i.e., wavelength range: 500–800 nm) of 21.9% at AgOx OMO of 3 sccm, i.e., improvements from b-η = 7.42% and T500–800 = 18.8% at Ag OMO of 0 sccm. The cell with the optimized AgOx OMO (3 sccm) achieved b-η = 7.69% and the best figure of merit (product of b-η and T500–800) of 169%, i.e., 30% higher than the Ag OMO cell (139%). The developed AgOx OMO electrodes could be used in BIPV windows or in other optical devices requiring both high transparency and high conductivity.

An atmospheric-pressure plasma deposition system was developed and used to deposit intrinsic hydrogenated microcrystalline silicon (μc-Si:H) thin films for μc-Si:H thin film solar cells. The helium (He) gas concentration in plasma increased Raman crystallinity (Xc) of μc-Si:H, which was a critical parameter to determine photovoltaic performance. In addition, dependence of Xc on the He concentration is shown to be closely related to the atomic hydrogen flux during film growth, which is evidenced by plasma diagnostics derived from in situ optical emission spectroscopy measurements. Those analysis contributed to achieve impressive photovoltaic performance – namely, a power conversion efficiency of 4.60%, an open-circuit voltage of 0.52 V, a short-circuit current density of 13.62 mA/cm2, and a fill factor of 0.65, which is the first experimental demonstration of μc-Si:H thin film solar cells fabricated with the atmospheric-pressure plasma deposition under very high working-pressure regime at 13.3 kPa.

A memristor based on emerging resistive random-access memory (RRAM) is a promising candidate for use as a next-generation neuromorphic computing device which overcomes the von Neumann bottleneck. Meanwhile, due to their unique properties, including atomically thin layers and surface smoothness, two-dimensional (2D) materials are being widely studied for implementation in the development of new information-processing electronic devices. However, inherent drawbacks concerning operational uniformities, such as device-to-device variability, device yield, and reliability, are huge challenges in the realization of concrete memristor hardware devices. In this study, we fabricated Ta2O5-based memristor devices, where a 2D-MoS2 buffer layer was directly inserted between the Ta2O5 switching layer and the Ag metal electrode to improve uniform switching characteristics in terms of switching voltage, the distribution of resistance states, endurance, and retention. A 2D-MoS2 layered buffer film with a 5 nm thickness was directly grown on the Ta2O5 switching layer by the atomic-pressure plasma-enhanced chemical vapor deposition (AP-PECVD) method, which is highly uniform and provided a superior yield of 2D-MoS2 film. It was observed that the switching operation was dramatically stabilized via the introduction of the 2D-MoS2 buffer layer compared to a pristine device without the buffer layer. It was assumed that the difference in mobility and reduction rates between Ta2O5 and MoS2 caused the narrow localization of ion migration, inducing the formation of more stable conduction filament. In addition, an excellent yield of 98% was confirmed while showing cell-to-cell operation uniformity, and the extrinsic and intrinsic variabilities in operating the device were highly uniform. Thus, the introduction of a MoS2 buffer layer could improve highly reliable memristor device switching operation.

Silicon oxide films were deposited by high-working-pressure plasma-enhanced chemical vapor deposition using hexamethyldisiloxane and O 2 /He plasma as the precursor and the reactant, respectively. As the O 2 flow rate increased during the process, the plasma density of O 2 and He decreased due to reduction in the partial pressure of He, which affected the composition of O/Si in the silicon oxide films. Consequently, we found out that the compositional ratio of SiO 2 /SiO could be modulated by O 2 flow conditions during the high-working-pressure plasma-enhanced chemical vapor deposition process. Additionally, it was observed that the water vapor transmission rate reduced with an increase in the O 2 flow rate because of a compositional change in the silicon oxide films.

Composition-modulated niobium oxide thin films were deposited by plasma-enhanced atomic layer deposition using NbF 5 , hydrogen plasma and ozone as the precursor, a reducing agent and an oxidant, respectively. For composition control of the niobium oxide thin films, a super-cycle was adopted, which was composed of n cycles of the metal deposition step and one cycle of the oxidation step. NbO 2 and Nb 2 O 5 phase components coexisted in the NbO x thin films, and the phase composition ratio of Nb 2 O 5 and NbO 2 could be modulated from approximately 80:20 to 40:60 through control of the cycle ratio. Furthermore, the optical bandgap and electrical resistivity decreased from 3.91eV to 2.19 eV and from 6.5×10 4 Ω cm to 3.1×10 −1 Ω cm with increasing the cycle count for the Nb metal deposition step, respectively. Consequently, we could effectively modulate the electrical properties of NbO x thin films via compositional modulation.

Despite extensive investigations of a wide variety of artificial synapse devices aimed at realizing a neuromorphic hardware system, the identification of a physical parameter that modulates synaptic plasticity is still required. In this context, a novel two-dimensional architecture consisting of a NbSe2/WSe2/Nb2O5 heterostructure placed on an SiO2/p+ Si substrate was designed to overcome the limitations of the conventional silicon-based complementary metal-oxide semiconductor technology. NbSe2, WSe2, and Nb2O5 were used as the metal electrode, active channel, and conductance-modulating layer, respectively. Interestingly, it was found that the post-synaptic current was successfully modulated by the thickness of the interlayer Nb2O5, with a thicker interlayer inducing a higher synapse spike current and a stronger interaction in the sequential pulse mode. Introduction of the Nb2O5 interlayer can facilitate the realization of reliable and controllable synaptic devices for brain-inspired integrated neuromorphic systems.

Here, we report that Nb doping of two-dimensional (2D) MoSe2 layered nanomaterials is a promising approach to improve their gas sensing performance. In this study, Nb atoms were incorporated into a 2D MoSe2 host matrix, and the Nb doping concentration could be precisely controlled by varying the number of Nb2O5 deposition cycles in the plasma enhanced atomic layer deposition process. At relatively low Nb dopant concentrations, MoSe2 showed enhanced device durability as well as NO2 gas response, attributed to its small grains and stabilized grain boundaries. Meanwhile, an increase in the Nb doping concentration deteriorated the NO2 gas response. This might be attributed to a considerable increase in the number of metallic NbSe2 regions, which do not respond to gas molecules. This novel method of doping 2D transition metal dichalcogenide-based nanomaterials with metal atoms is a promising approach to improve the performance such as stability and gas response of 2D gas sensors.

Enhancing light–matter interactions is essential to improving nanophotonic and optoelectronic device performance. In the present work, we developed a new design for 3D plasmonic nanostructures with enhanced near-field interactions among the plasmonic nanomaterials. The 3D plasmonic nanostructures consisted of multilayered bottom Ag/polydimethylsiloxane (PDMS) nanostructures, an alumina middle layer, and top Ag nanoparticles (NPs). High areal density PDMS nanoprotrusions were self-organized by a simple maskless plasma etching process. The conformal deposition of alumina using atomic layer deposition and Ag deposition produced 3D plasmonic nanostructures. These structures induced multiple near-field interactions between the ultrahigh-areal-density (1400 μm−2) top Ag NPs and the underlying Ag nanostructures, and among the top Ag NPs themselves. The high density of hot spots across the 3D space yielded highly efficient and widely tunable plasmonic responses across the entire visible range. The SERS signal enhancement measured at the 3D plasmonic nanostructures was 3.9 times the signal measured at the 2D multilayered structures and 48.0 times the signal measured at a Ag NP layer deposited onto a Si substrate. Finally, the 3D plasmonic nanostructures exhibited excellent uniformity with a variation of 6.8%, based on a microscale Raman mapping analysis. The excellent Raman signal uniformity can be attributed to the ultrahigh areal density of the Ag NPs and the uniform thickness of the alumina spacing layer.

Herein, a simple interference lithographic technique to design omniphobic surface-enhanced Raman scattering active surfaces composed of stacked-disk nanotower arrays is reported. To create the nanotower arrays in a highly reproducible fashion, the authors use a single laser exposure onto the photoresist-on-dielectric mirror using a phase mask. The interference by the phase shift produces a nanotower array with a submicrometer periodicity, whereas the standing wave effect by reflection from the mirror defines the stacked-disk structure at each nanotower at sub-100 nm periodicity. The stacked-disk nanotowers with silver outer-coating provide a strong electric field localization at the vertically integrated nanogaps on the side wall. At the same time, the series of reentrant geometry on the side walls can efficiently pin the liquid–air interface for a variety of liquids, including water and toluene, thereby providing omniphobic surface property. The molecules dissolved in either water or toluene at low concentration can be enriched in the drop on the surface in a course of evaporation, which are finally deposited onto a tiny spot. Raman spectra of the molecules are further amplified by the strong electric field at the nanogaps on the side walls of the nanotowers. Therefore, the surfaces provide high sensitivity of Raman analysis for both polar and nonpolar molecules.

We first report that two-dimensional (2D) metal (NbSe2)-semiconductor (WSe2)-based flexible, wearable, and launderable gas sensors can be prepared through simple one-step chemical vapor deposition of prepatterned WO3 and Nb2O5. Compared to a control device with a Au/WSe2 junction, gas-sensing performance of the 2D NbSe2/WSe2 device was significantly enhanced, which might have resulted from the formation of a NbxW1-xSe2 transition alloy junction lowering the Schottky barrier height. This would make it easier to collect charges of channels induced by molecule adsorption, improving gas response characteristics toward chemical species including NO2 and NH3. 2D NbSe2/WSe2 devices on a flexible substrate provide gas-sensing properties with excellent durability under harsh bending. Furthermore, the device stitched on a T-shirt still performed well even after conventional cleaning with a laundry machine, enabling wearable and launderable chemical sensors. These results could pave a road toward futuristic gas-sensing platforms based on only 2D materials.

Manufacturing high-quality, two-dimensional (2D), layered materials with crystal-growth techniques is an important challenge for the advancement of 2D communication technologies. In this study, a simple method was developed for synthesizing 2D nanocrystals based on the model system of SnS2. The method involves the sulfurization of a metal oxide to a metal chalcogenide, which subsequently acts as a source of vapors for the growth of 2D crystals. The effect of the annealing conditions on the thermal sulfurization of SnO2 powder was investigated. The results showed that pure SnS2 powder could be obtained in a N2 atmosphere at 700 °C. SnS2 nanocrystals were successfully synthesized from the as-prepared SnS2 powder by the vapor transport method. The synthesized SnS2 nanocrystals had a 2D layered structure with hexagonal symmetry and exhibited typical n-type semiconducting characteristics, with an optical band gap of 2.05 eV. This novel method, which uses a preferentially prepared source for vapor transport, co...

Highly roughened Au-decorated 3D ZnO nano-structures were prepared using a combination of prism holographic lithography and atomic layer deposition techniques. Prism holographic lithography is a simple and rapid method for fabricating ordered 3D nanostructures using the optical interference effects of multiple beams derived from a specially designed prism. Highly ordered reproducible surface-enhanced Raman scattering (SERS) substrates are needed for the reliable calibration of target analyte concentrations. A high density of Au nanoparticles separated by nanoscale gaps was generated on the Au-coated ZnO inverse structures. The nanogaps may function as strong hot spots for highly sensitive SERS-based chemical/biological sensors. The optimized SERS intensity from the prepared Au-coated 3D ZnO inverse structures was 20 times the intensity obtained from an Au-coated flat glass control substrate. The surfaces could be reused after the photocatalytic degradation and removal of adsorbates in the presence of ZnO. The Au-coated 3D ZnO structures described here offer an alternative to traditional single-use SERS substrates.

Vanadium oxide (V 2 O 5-x ) thin films with a thickness of about 4 nm were prepared by atomic layer deposition (ALD) to be used as a hole-transporting layer in an amorphous silicon solar cell. The ALD growth characteristics (growth rate, crystallinity, and surface morphology) of the V 2 O 5-x films were investigated while exposed to different pulse times of ozone (O 3 ), which was used as an oxidant. The effect of the different ozone pulse times, used in the V 2 O 5 layer, on the device performance was also investigated. At the ozone pulse time of 1 s, the maximum value of power conversion efficiency (PCE), i.e., 5.35%, was achieved, whereas at the ozone pulse time of 5 s, the PCE was 4.18%. Ultraviolet photoelectron spectroscopy (UPS) and X-ray photoelectron spectroscopy (XPS) analyses confirmed that increasing the proportion of crystalline phase in the V 2 O 4 films with lower work function of V 2 O 5 resulted in decreased open-circuit voltage and conversion efficiency as the ozone pulse time increased.