Evolution of Local Structural Motifs in Colloidal Quantum Dot Semiconductor Nanocrystals Leading to Nanofaceting.

Colloidal nanocrystals (NCs) have shown remarkable promise for optoelectronics, energy harvesting, photonics, and biomedical imaging. In addition to optimizing quantum confinement, the current challenge is to obtain a better understanding of the critical processing steps and their influence on the evolution of structural motifs. Computational simulations and electron microscopy presented in this work show that nanofaceting can occur during nanocrystal synthesis from a Pb-poor environment in a polar solvent. This could explain the curved interfaces and the olivelike-shaped NCs observed experimentally when these conditions are employed. Furthermore, the wettability of the PbS NCs solid film can be further modified via stoichiometry control, which impacts the interface band bending and, therefore, processes such as multiple junction deposition and interparticle epitaxial growth. Our results suggest that nanofaceting in NCs can become an inherent advantage when used to modulate band structures beyond what is traditionally possible in bulk crystals.

Facile one-pot iodine gas phase doping on 2D MoS2/CuS FET at room temperature.

Electronic devices composed of semiconducting two-dimensional (2D) materials and ultrathin 2D metallic electrode materials, accompanying synergistic interactions and extraordinary properties, are becoming highly promising for future flexible and transparent electronic and optoelectronic device applications. Unlike devices with bulk metal electrode and 2D channel materials, devices with ultrathin 2D electrode and 2D channel are susceptible to chemical reactions in both channel and electrode surface due to the high surface to volume ratio of the 2D structures. However, so far, the effect of doping was primary concerned on the channel component, and there is lack of understanding in terms of how to modulate electrical properties of devices by engineering electrical properties of both the metallic electrode and the semiconducting channel. Here, we propose the novel, one-pot doping of the field-effect transistor (FET) based on 2D molybdenum disulfide (MoS2) channel and ultrathin copper sulfide (CuS) electrodes under mild iodine gas environment at room temperature, which simultaneously modulates electrical properties of the 2D MoS2channel and 2D CuS electrode in a facile and cost-effective way. After one-pot iodine doping, effective p-type doping of the channel and electrode was observed, which was shown through decreased off current level, improvedIon/Ioffratio and subthreshold swing value. Our results open up possibility for effectively and conveniently modulating electrical properties of FETs made of various 2D semiconductors and ultrathin contact materials without causing any detrimental damage.

Strain-Mediated Interlayer Coupling Effects on the Excitonic Behaviors in an Epitaxially Grown MoS2/WS2 van der Waals Heterobilayer.

van der Waals heterostructures composed of two different monolayer crystals have recently attracted attention as a powerful and versatile platform for studying fundamental physics, as well as having great potential in future functional devices because of the diversity in the band alignments and the unique interlayer coupling that occurs at the heterojunction interface. However, despite these attractive features, a fundamental understanding of the underlying physics accounting for the effect of interlayer coupling on the interactions between electrons, photons, and phonons in the stacked heterobilayer is still lacking. Here, we demonstrate a detailed analysis of the strain-dependent excitonic behavior of an epitaxially grown MoS2/WS2 vertical heterostructure under uniaxial tensile and compressive strain that enables the interlayer interactions to be modulated along with the electronic band structure. We find that the strain-modulated interlayer coupling directly affects the characteristic combined vibrational and excitonic properties of each monolayer in the heterobilayer. It is further revealed that the relative photoluminescence intensity ratio of WS2 to MoS2 in our heterobilayer increases monotonically with tensile strain and decreases with compressive strain. We attribute the strain-dependent emission behavior of the heterobilayer to the modulation of the band structure for each monolayer, which is dictated by the alterations in the band gap transitions. These findings present an important pathway toward designing heterostructures and flexible devices.

Recent development of piezoelectric biosensors for physiological signal detection and machine learning assisted cardiovascular disease diagnosis.

As cardiovascular disease stands as a global primary cause of mortality, there has been an urgent need for continuous and real-time heart monitoring to effectively identify irregular heart rhythms and to offer timely patient alerts. However, conventional cardiac monitoring systems encounter challenges due to inflexible interfaces and discomfort during prolonged monitoring. In this review article, we address these issues by emphasizing the recent development of the flexible, wearable, and comfortable piezoelectric passive sensor assisted by machine learning technology for diagnosis. This innovative device not only harmonizes with the dynamic mechanical properties of human skin but also facilitates continuous and real-time collection of physiological signals. Addressing identified challenges and constraints, this review provides insights into recent advances in piezoelectric cardiac sensors, from devices to circuit systems. Furthermore, this review delves into the integration of machine learning technologies, showcasing their pivotal role in facilitating continuous and real-time assessment of cardiac status. The synergistic combination of flexible piezoelectric sensor design and machine learning holds substantial potential in automating the detection of cardiac irregularities with minimal human intervention. This transformative approach has the power to revolutionize patient care paradigms.

2D Material and Perovskite Heterostructure for Optoelectronic Applications.

Optoelectronic devices are key building blocks for sustainable energy, imaging applications, and optical communications in modern society. Two-dimensional materials and perovskites have been considered promising candidates in this research area due to their fascinating material properties. Despite the significant progress achieved in the past decades, challenges still remain to further improve the performance of devices based on 2D materials or perovskites and to solve stability issues for their reliability. Recently, a novel concept of 2D material/perovskite heterostructure has demonstrated remarkable achievements by taking advantage of both materials. The diverse fabrication techniques and large families of 2D materials and perovskites open up great opportunities for structure modification, interface engineering, and composition tuning in state-of-the-art optoelectronics. In this review, we present comprehensive information on the synthesis methods, material properties of 2D materials and perovskites, and the research progress of optoelectronic devices, particularly solar cells and photodetectors which are based on 2D materials, perovskites, and 2D material/perovskite heterostructures with future perspectives.

Room Temperature Wafer-Scale Synthesis of Highly Transparent, Conductive CuS Nanosheet Films via a Simple Sulfur Adsorption-Corrosion Method.

The development of highly conductive electrodes with robust mechanical durability and clear transmittance in the visible to IR spectral range is of great importance for future wearable/flexible electronic applications. In particular, low resistivity, robust flexibility, and wide spectral transparency have a significant impact on optoelectronic performance. Herein, we introduce a new class of covellite copper monosulfide (CuS) nanosheet films as a promising candidate for soft transparent conductive electrodes (TCEs). An atmospheric sulfur adsorption-corrosion phenomenon represents a key approach in our work for the achievement of wafer-scale CuS nanosheet films through systematic control of the neat Cu layer thickness ranging from 2 to 10 nm multilayers at room temperature. These nanosheet films provide outstanding conductivity (∼25 Ω sq-1) and high transparency (> 80%) in the visible to infrared region as well as distinct flexibility and long stability under air exposure, yielding a high figure-of-merit (∼60) that is comparable to that of conventional rigid metal oxide material-based TCEs. Our unique room temperature synthesis process delivers high quality CuS nanosheets on any arbitrary substrates in a short time (< 1 min) scale, thus guaranteeing the widespread use of highly producible and scalable device fabrication.

Electrode-Induced Self-Healed Monolayer MoS2 for High Performance Transistors and Phototransistors.

Contact engineering for monolayered transition metal dichalcogenides (TMDCs) is considered to be of fundamental challenge for realizing high-performance TMDCs-based (opto) electronic devices. Here, an innovative concept is established for a device configuration with metallic copper monosulfide (CuS) electrodes that induces sulfur vacancy healing in the monolayer molybdenum disulfide (MoS2 ) channel. Excess sulfur adatoms from the metallic CuS electrodes are donated to heal sulfur vacancy defects in MoS2 that surprisingly improve the overall performance of its devices. The electrode-induced self-healing mechanism is demonstrated and analyzed systematically using various spectroscopic analyses, density functional theory (DFT) calculations, and electrical measurements. Without any passivation layers, the self-healed MoS2 (photo)transistor with the CuS contact electrodes show outstanding room temperature field effect mobility of 97.6 cm2 (Vs)-1 , On/Off ratio > 108 , low subthreshold swing of 120 mV per decade, high photoresponsivity of 1 × 104  A W-1 , and detectivity of 1013 jones, which are the best among back-gated transistors that employ 1L MoS2 . Using ultrathin and flexible 2D CuS and MoS2 , mechanically flexible photosensor is also demonstrated, which shows excellent durability under mechanical strain. These findings demonstrate a promising strategy in TMDCs or other 2D material for the development of high performance and functional devices including self-healable sulfide electrodes.

Balanced Charge Carrier Transport Mediated by Quantum Dot Film Post-organization for Light-Emitting Diode Applications.

In light-emitting diodes (LEDs), balanced electron and hole transport is of particular importance to achieve high rates of radiative recombination. Most quantum dot (QD)-based LEDs, however, employ infinitesimal core-shell QDs which inherently have different electron and hole mobilities. As QDs are the core building blocks of QD-LEDs, the inherent mobility difference in the core-shell QDs causes significantly unbalanced charge carrier transport, resulting in detrimental effects on performances of QD-LEDs. Herein, we introduce a post-chemical treatment to reconstruct the QD films through the solvent-mediated self-organization process. The treatment using various poly-alkyl alcohol groups enables QD ensembles to transform from disordered solid dispersion into an ordered superlattice and effectively modulate electron and hole mobilities, which leads to the balanced charge carrier transport. In particular, ethanol-treated QD films exhibit enhanced charge carrier lifetime and reduced hysteresis due to the balanced charge carrier transport, which is attributed to the preferential-facet-oriented QD post-organization. As a result, 63, 78, and 54% enhancements in the external quantum efficiency were observed in red, green, and blue QD-LEDs, respectively. These results are of fundamental importance to understand both solvent-mediated QD film reconstruction and the effect of balanced electron and hole transport in QD-LEDs.

Direct Epitaxial Synthesis of Selective Two-Dimensional Lateral Heterostructures.

Two-dimensional (2D) heterostructured or alloyed monolayers composed of transition metal dichalcogenides (TMDCs) have recently emerged as promising materials with great potential for atomically thin electronic applications. However, fabrication of such artificial TMDC heterostructures with a sharp interface and a large crystal size still remains a challenge because of the difficulty in controlling various growth parameters simultaneously during the growth process. Here, a facile synthetic protocol designed for the production of the lateral TMDC heterostructured and alloyed monolayers is presented. A chemical vapor deposition approach combined with solution-processed precursor deposition makes it possible to accurately control the sequential introduction time and the supersaturation levels of the vaporized precursors and thus reliably and exclusively produces selective and heterogeneous epitaxial growth of TMDC monolayer crystals. In addition, TMDC core/shell heterostructured (MoS2/alloy, alloy/WS2) or alloyed (Mo1-xWxS2) monolayers are also easily obtained with precisely controlled growth parameters, such as sulfur introduction timing and growth temperature. These results represent a significant step toward the development of various 2D materials with interesting properties.

Electronic Skin to Feel "Pain": Detecting "Prick" and "Hot" Pain Sensations.

An artificial tactile system has attracted tremendous interest and intensive study, since it can be applied as a new functional interface between humans and electronic devices. Unfortunately, most previous works focused on improving the sensitivity of sensors. However, humans also respond to psychological feelings for sensations such as pain, softness, or roughness, which are important factors for interacting with others and objects. Here, we present an electronic skin concept that generates a "pain" warning signal, specifically, to sharp "prick" and "hot" sensations. To simplify the sensor structure for these two feelings, a single-body tactile sensor design is proposed. By exploiting "hot" feeling based on the Seebeck effect instead of the pyroelectric property, it is possible to distinguish points registering a "hot" feeling from those generating a "prick" feeling, which is based on the piezoelectric effect. The control of free carrier concentration in nanowire induced the appropriate level of Seebeck current, which enabled the sensor system to be more reliable. The first derivatives of the piezo and Seebeck output signals are the key factors for the signal processing of the "pain" feeling. The main idea can be applied to mimic other psychological tactile feelings.

Surface functionalization-induced photoresponse characteristics of monolayer MoS2 for fast flexible photodetectors.

Monolayered, semiconducting molybdenum disulfide (MoS2) is of considerable interest for its potential applications in next-generation flexible, wearable, and transparent photodetectors because it has outstanding physical properties coupled with unique atomically thin dimensions. However, there is still a lack of understanding in terms of the underlying mechanisms responsible for the photoresponse dynamics, which makes it difficult to identify the appropriate device design strategy for achieving a fast photoresponse time in MoS2 photodetectors. In this study, we investigate the importance of surface functionalization on controlling the charge carrier densities in a MoS2 monolayer and in turn the corresponding behavior of the photoresponse in relation to the position of the Fermi-level and the energy band structure. We find that the p-doping and n-doping, which is achieved through the surface functionalization of the MoS2 monolayer, leads to devices with different photoresponse behavior. Specifically, the MoS2 devices with surface functional groups contributing to p-doping exhibited a faster response time as well as higher sensitivity compared to that observed for the MoS2 devices with surface functional groups contributing to n-doping. We attribute this difference to the degree of bending in the energy bands at the metal-semiconductor junction as a result of shifting in the Fermi-level position, which influences the optoelectronic transport properties as well as the recombination dynamics leading to a low dark and thus high detectivity and fast decay time. Based upon these findings, we have also demonstrated the broad applicability of surface functionalization by fabricating a flexible MoS2 photodetector that shows an outstanding decay time of 0.7 s, which is the fastest response time observed in flexible MoS2 detectors ever reported.

Modeling Electrical Percolation to optimize the Electromechanical Properties of CNT/Polymer Composites in Highly Stretchable Fiber Strain Sensors.

A simulation model of electrical percolation through a three-dimensional network of curved CNTs is developed in order to analyze the electromechanical properties of a highly stretchable fiber strain sensor made of a CNT/polymer composite. Rigid-body movement of the curved CNTs within the polymer matrix is described analytically. Random arrangements of CNTs within the composite are generated by a Monte-Carlo simulation method and a union-find algorithm is utilized to investigate the network percolation. Consequently, the strain-induced resistance change curves are obtained in a wide strain range of the composite. In order to compare our model with experimental results, two CNT/polymer composite fibers were fabricated and tested as strain sensors. Their effective CNT volume fractions are estimated by comparing the experimental data with our simulation model. The results confirm that the proposed simulation model reproduces well the experimental data and is useful for predicting and optimizing the electromechanical characteristics of highly stretchable fiber strain sensors based on CNT/polymer composites.

Consecutive Junction-Induced Efficient Charge Separation Mechanisms for High-Performance MoS2/Quantum Dot Phototransistors.

Phototransistors that are based on a hybrid vertical heterojunction structure of two-dimensional (2D)/quantum dots (QDs) have recently attracted attention as a promising device architecture for enhancing the quantum efficiency of photodetectors. However, to optimize the device structure to allow for more efficient charge separation and transfer to the electrodes, a better understanding of the photophysical mechanisms that take place in these architectures is required. Here, we employ a novel concept involving the modulation of the built-in potential within the QD layers for creating a new hybrid MoS2/PbS QDs phototransistor with consecutive type II junctions. The effects of the built-in potential across the depletion region near the type II junction interface in the QD layers are found to improve the photoresponse as well as decrease the response times to 950 µs, which is the faster response time (by orders of magnitude) than that recorded for previously reported 2D/QD phototransistors. Also, by implementing an electric-field modulation of the MoS2 channel, our experimental results reveal that the detectivity can be as large as 1 × 1011 jones. This work demonstrates an important pathway toward designing hybrid phototransistors and mixed-dimensional van der Waals heterostructures.

Balancing Charge Carrier Transport in a Quantum Dot P-N Junction toward Hysteresis-Free High-Performance Solar Cells.

In a quantum dot solar cell (QDSC) that has an inverted structure, the QD layers form two different junctions between the electron transport layer (ETL) and the other semiconducting QD layer. Recent work on an inverted-structure QDSC has revealed that the junction between the QD layers is the dominant junction, rather than the junction between the ETL and the QD layers, which is in contrast to the conventional wisdom. However, to date, there have been a lack of systematic studies on the role and importance of the QD heterojunction structure on the behavior of the solar cell and the resulting device performance. In this study, we have systematically controlled the structure of the QD junction to balance charge transport, which demonstrates that the position of the junction has a significant effect on the hysteresis effect, fill factor, and solar cell performance and is attributed to balanced charge transport.

Monolayer optical memory cells based on artificial trap-mediated charge storage and release.

Monolayer transition metal dichalcogenides are considered to be promising candidates for flexible and transparent optoelectronics applications due to their direct bandgap and strong light-matter interactions. Although several monolayer-based photodetectors have been demonstrated, single-layered optical memory devices suitable for high-quality image sensing have received little attention. Here we report a concept for monolayer MoS2 optoelectronic memory devices using artificially-structured charge trap layers through the functionalization of the monolayer/dielectric interfaces, leading to localized electronic states that serve as a basis for electrically-induced charge trapping and optically-mediated charge release. Our devices exhibit excellent photo-responsive memory characteristics with a large linear dynamic range of ∼4,700 (73.4 dB) coupled with a low OFF-state current (<4 pA), and a long storage lifetime of over 104 s. In addition, the multi-level detection of up to 8 optical states is successfully demonstrated. These results represent a significant step toward the development of future monolayer optoelectronic memory devices.

Dataset on electro-optically tunable smart-supercapacitors based on oxygen-excess nanograin tungsten oxide thin film.

The dataset presented here is related to the research article entitled "Highly Efficient Electro-optically Tunable Smart-supercapacitors Using an Oxygen-excess Nanograin Tungsten Oxide Thin Film" (Akbar et al., 2017) [9] where we have presented a nanograin WO3 film as a bifunctional electrode for smart supercapacitor devices. In this article we provide additional information concerning nanograin tungsten oxide thin films such as atomic force microscopy, Raman spectroscopy, and X-ray diffraction spectroscopy. Moreover, their electrochemical properties such as cyclic voltammetry, electrochemical supercapacitor properties, and electrochromic properties including coloration efficiency, optical modulation and electrochemical impedance spectroscopy are presented.

Red green blue emissive lead sulfide quantum dots: heterogeneous synthesis and applications.

Visible emission colloidal quantum dots (QDs) have shown promise in optical and optoelectronic applications. These QDs are typically composed of relatively expensive elements in the form of indium, cadmium, and gallium since alternative candidate materials exhibiting similar properties are yet to be realized. Herein, for the first time, we report red green blue (RGB) photoluminescences with quantum yields of 18% from earth-abundant lead sulfide (PbS) QDs. The visible emissive property is mainly attributed to a high degree of crystallinity even for the extremely small QD sizes (1-3 nm), which is realized by employing a heterogeneous reaction methodology at high growth temperatures (>170 °C). We demonstrate that the proposed heterogeneous synthetic method can be extended to the synthesis of other metal chalcogenide QDs, such as zinc sulfide and zinc selenide, which are promising for future industrial applications. More importantly, benefiting from the enlarged band gaps, the as-prepared PbS solar cells show an impressive open circuit voltage (∼0.8 V) beyond that reported to date.

Thermodynamically Stable Synthesis of Large-Scale and Highly Crystalline Transition Metal Dichalcogenide Monolayers and their Unipolar n-n Heterojunction Devices.

Transition metal dichalcogenide (TMDC) monolayers are considered to be potential materials for atomically thin electronics due to their unique electronic and optical properties. However, large-area and uniform growth of TMDC monolayers with large grain sizes is still a considerable challenge. This report presents a simple but effective approach for large-scale and highly crystalline molybdenum disulfide monolayers using a solution-processed precursor deposition. The low supersaturation level, triggered by the evaporation of an extremely thin precursor layer, reduces the nucleation density dramatically under a thermodynamically stable environment, yielding uniform and clean monolayer films and large crystal sizes up to 500 µm. As a result, the photoluminescence exhibits only a small full-width-half-maximum of 48 meV, comparable to that of exfoliated and suspended monolayer crystals. It is confirmed that this growth procedure can be extended to the synthesis of other TMDC monolayers, and robust MoS2 /WS2 heterojunction devices are easily prepared using this synthetic procedure due to the large-sized crystals. The heterojunction device shows a fast response time (≈45 ms) and a significantly high photoresponsivity (≈40 AW-1 ) because of the built-in potential and the majority-carrier transport at the n-n junction. These findings indicate an efficient pathway for the fabrication of high-performance 2D optoelectronic devices.

Highly Monodispersed PbS Quantum Dots for Outstanding Cascaded-Junction Solar Cells.

High-performance cascaded-junction quantum dot solar cells (CJQDSCs) are fabricated from as-prepared highly monodispersed lead sulfide QDs. The cells have a high power conversion of 9.05% and a short-circuit current density of 32.51 mA cm-2. A reliable and effective stratagem for fabricating high-quality lead sulfide quantum dots (QD) is explored through a "monomer" concentration-controlled experiment. Robust QDSC performances with different band gaps are demonstrated from the as-proposed synthesis and processing stratagems. Various potential CJQDSCs can be envisioned from the band edge evolution of the QDs as a function of size and ligands reported here.

Synergistic Effects of a Multifunctional Graphene Based Interlayer on Electrochemical Behavior and Structural Stability.

The ability to rationally design and manipulate the interfacial structure in lithium ion batteries (LIBs) is of utmost technological importance for achieving desired performance requirements as it provides synergistic effects to the electrochemical properties and cycling stability of electrode materials. However, despite considerable efforts and progress made in recent years through the interface engineering based on active electrode materials, relatively little attention has been devoted to address the physical aspects of the interface and interfacial layer between the anode materials layer and the current collector. Here, we propose and successfully grow unique graphene directly on a Cu current collector as an ideal interfacial layer using the modified chemical vapor deposition (CVD). The anode with an engineered graphene interlayer exhibits remarkably improved electrochemical performances, such as large reversible specific capacity (921.4 mAh g(-1) at current density of 200 mA g(-1)), excellent Coulombic efficiency (close to approximately 96%), and superior cycling capacity retention and rate properties compared to the bare Cu. These excellent electrochemical features are discussed in terms of multiple beneficial effects of graphene on interfacial stability and adhesion between the anode and the collector, oxidation or corrosion resistance of the graphene grown Cu current collector, and electrical contact conductance during the charge/discharge process.