Vinod K. Sangwan

Emerging device applications for semiconducting two-dimensional transition metal dichalcogenides.

With advances in exfoliation and synthetic techniques, atomically thin films of semiconducting transition metal dichalcogenides have recently been isolated and characterized. Their two-dimensional structure, coupled with a direct band gap in the visible portion of the electromagnetic spectrum, suggests suitability for digital electronics and optoelectronics. Toward that end, several classes of high-performance devices have been reported along with significant progress in understanding their physical properties. Here, we present a review of the architecture, operating principles, and physics of electronic and optoelectronic devices based on ultrathin transition metal dichalcogenide semiconductors. By critically assessing and comparing the performance of these devices with competing technologies, the merits and shortcomings of this emerging class of electronic materials are identified, thereby providing a roadmap for future development.

Effective passivation of exfoliated black phosphorus transistors against ambient degradation.

Unencapsulated, exfoliated black phosphorus (BP) flakes are found to chemically degrade upon exposure to ambient conditions. Atomic force microscopy, electrostatic force microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy are employed to characterize the structure and chemistry of the degradation process, suggesting that O2 saturated H2O irreversibly reacts with BP to form oxidized phosphorus species. This interpretation is further supported by the observation that BP degradation occurs more rapidly on hydrophobic octadecyltrichlorosilane self-assembled monolayers and on H-Si(111) versus hydrophilic SiO2. For unencapsulated BP field-effect transistors, the ambient degradation causes large increases in threshold voltage after 6 h in ambient, followed by a ∼ 10(3) decrease in FET current on/off ratio and mobility after 48 h. Atomic layer deposited AlOx overlayers effectively suppress ambient degradation, allowing encapsulated BP FETs to maintain high on/off ratios of ∼ 10(3) and mobilities of ∼ 100 cm(2) V(-1) s(-1) for over 2 weeks in ambient conditions. This work shows that the ambient degradation of BP can be managed effectively when the flakes are sufficiently passivated. In turn, our strategy for enhancing BP environmental stability will accelerate efforts to implement BP in electronic and optoelectronic applications.

Carbon nanomaterials for electronics, optoelectronics, photovoltaics, and sensing

In the last three decades, zero-dimensional, one-dimensional, and two-dimensional carbon nanomaterials (i.e., fullerenes, carbon nanotubes, and graphene, respectively) have attracted significant attention from the scientific community due to their unique electronic, optical, thermal, mechanical, and chemical properties. While early work showed that these properties could enable high performance in selected applications, issues surrounding structural inhomogeneity and imprecise assembly have impeded robust and reliable implementation of carbon nanomaterials in widespread technologies. However, with recent advances in synthesis, sorting, and assembly techniques, carbon nanomaterials are experiencing renewed interest as the basis of numerous scalable technologies. Here, we present an extensive review of carbon nanomaterials in electronic, optoelectronic, photovoltaic, and sensing devices with a particular focus on the latest examples based on the highest purity samples. Specific attention is devoted to each class of carbon nanomaterial, thereby allowing comparative analysis of the suitability of fullerenes, carbon nanotubes, and graphene for each application area. In this manner, this article will provide guidance to future application developers and also articulate the remaining research challenges confronting this field.

Band-like transport in high mobility unencapsulated single-layer MoS 2 transistors

Ultra-thin MoS2 has recently emerged as a promising two-dimensional semiconductor for electronic and optoelectronic applications. Here, we report high mobility (>60 cm2/Vs at room temperature) field-effect transistors that employ unencapsulated single-layer MoS2 on oxidized Si wafers with a low level of extrinsic contamination. While charge transport in the sub-threshold regime is consistent with a variable range hopping model, monotonically decreasing field-effect mobility with increasing temperature suggests band-like transport in the linear regime. At temperatures below 100 K, temperature-independent mobility is limited by Coulomb scattering, whereas, at temperatures above 100 K, phonon-limited mobility decreases as a power law with increasing temperature.

Gate-tunable carbon nanotube–MoS2 heterojunction p-n diode

Significance The p-n junction diode is the most ubiquitous and fundamental building block of modern electronics, with far-reaching applications including integrated circuits, detectors, photovoltaics, and lasers. With the recent discovery and study of atomically thin materials, opportunities exist for adding new functionality to the p-n junction diode. Here we demonstrate that a p-n heterojunction diode based on atomically thin MoS2 and sorted semiconducting carbon nanotubes yields unprecedented gate tunability in both its electrical and optical properties, which is not observed in the case of bulk semiconductor devices. In addition to enabling advanced electronic and optoelectronic technologies, this p-n heterojunction diode provides new insight into charge transport and separation at atomically thin heterointerfaces. The p-n junction diode and field-effect transistor are the two most ubiquitous building blocks of modern electronics and optoelectronics. In recent years, the emergence of reduced dimensionality materials has suggested that these components can be scaled down to atomic thicknesses. Although high-performance field-effect devices have been achieved from monolayered materials and their heterostructures, a p-n heterojunction diode derived from ultrathin materials is notably absent and constrains the fabrication of complex electronic and optoelectronic circuits. Here we demonstrate a gate-tunable p-n heterojunction diode using semiconducting single-walled carbon nanotubes (SWCNTs) and single-layer molybdenum disulfide as p-type and n-type semiconductors, respectively. The vertical stacking of these two direct band gap semiconductors forms a heterojunction with electrical characteristics that can be tuned with an applied gate bias to achieve a wide range of charge transport behavior ranging from insulating to rectifying with forward-to-reverse bias current ratios exceeding 104. This heterojunction diode also responds strongly to optical irradiation with an external quantum efficiency of 25% and fast photoresponse <15 μs. Because SWCNTs have a diverse range of electrical properties as a function of chirality and an increasing number of atomically thin 2D nanomaterials are being isolated, the gate-tunable p-n heterojunction concept presented here should be widely generalizable to realize diverse ultrathin, high-performance electronics and optoelectronics.

Gate-tunable memristive phenomena mediated by grain boundaries in single-layer MoS2

Continued progress in high-speed computing depends on breakthroughs in both materials synthesis and device architectures. The performance of logic and memory can be enhanced significantly by introducing a memristor, a two-terminal device with internal resistance that depends on the history of the external bias voltage. State-of-the-art memristors, based on metal-insulator-metal (MIM) structures with insulating oxides, such as TiO₂, are limited by a lack of control over the filament formation and external control of the switching voltage. Here, we report a class of memristors based on grain boundaries (GBs) in single-layer MoS₂ devices. Specifically, the resistance of GBs emerging from contacts can be easily and repeatedly modulated, with switching ratios up to ∼10(3) and a dynamic negative differential resistance (NDR). Furthermore, the atomically thin nature of MoS₂ enables tuning of the set voltage by a third gate terminal in a field-effect geometry, which provides new functionality that is not observed in other known memristive devices.

Low-frequency electronic noise in single-layer MoS2 transistors.

Ubiquitous low-frequency 1/f noise can be a limiting factor in the performance and application of nanoscale devices. Here, we quantitatively investigate low-frequency electronic noise in single-layer transition metal dichalcogenide MoS2 field-effect transistors. The measured 1/f noise can be explained by an empirical formulation of mobility fluctuations with the Hooge parameter ranging between 0.005 and 2.0 in vacuum (<10(-5) Torr). The field-effect mobility decreased, and the noise amplitude increased by an order of magnitude in ambient conditions, revealing the significant influence of atmospheric adsorbates on charge transport. In addition, single Lorentzian generation-recombination noise was observed to increase by an order of magnitude as the devices were cooled from 300 to 6.5 K.

Fundamental Performance Limits of Carbon Nanotube Thin-Film Transistors Achieved Using Hybrid Molecular Dielectrics

In the past decade, semiconducting carbon nanotube thin films have been recognized as contending materials for wide-ranging applications in electronics, energy, and sensing. In particular, improvements in large-area flexible electronics have been achieved through independent advances in postgrowth processing to resolve metallic versus semiconducting carbon nanotube heterogeneity, in improved gate dielectrics, and in self-assembly processes. Moreover, controlled tuning of specific device components has afforded fundamental probes of the trade-offs between materials properties and device performance metrics. Nevertheless, carbon nanotube transistor performance suitable for real-world applications awaits understanding-based progress in the integration of independently pioneered device components. We achieve this here by integrating high-purity semiconducting carbon nanotube films with a custom-designed hybrid inorganic-organic gate dielectric. This synergistic combination of materials circumvents conventional design trade-offs, resulting in concurrent advances in several transistor performance metrics such as transconductance (6.5 μS/μm), intrinsic field-effect mobility (147 cm(2)/(V s)), subthreshold swing (150 mV/decade), and on/off ratio (5 × 10(5)), while also achieving hysteresis-free operation in ambient conditions.

Investigation of Band-Offsets at Monolayer–Multilayer MoS2 Junctions by Scanning Photocurrent Microscopy

The thickness-dependent band structure of MoS2 implies that discontinuities in energy bands exist at the interface of monolayer (1L) and multilayer (ML) thin films. The characteristics of such heterojunctions are analyzed here using current versus voltage measurements, scanning photocurrent microscopy, and finite element simulations of charge carrier transport. Rectifying I-V curves are consistently observed between contacts on opposite sides of 1L/ML junctions, and a strong bias-dependent photocurrent is observed at the junction. Finite element device simulations with varying carrier concentrations and electron affinities show that a type II band alignment at single layer/multilayer junctions reproduces both the rectifying electrical characteristics and the photocurrent response under bias. However, the zero-bias junction photocurrent and its energy dependence are not explained by conventional photovoltaic and photothermoelectric mechanisms, indicating the contributions of hot carriers.

Large‐Area, Electronically Monodisperse, Aligned Single‐Walled Carbon Nanotube Thin Films Fabricated by Evaporation‐Driven Self‐Assembly

By varying the evaporation conditions and the nanotube and surfactant concentrations, large-area, aligned single-walled carbon nanotube (SWCNT) thin films are fabricated from electronically monodisperse SWCNT solutions by evaporation-driven self-assembly with precise control over the thin film growth geometry. Tunability is possible from 0.5 μm stripes to continuous thin films. The resulting SWCNT thin films possess highly anisotropic electrical and optical properties that are well suited for transparent conductor applications.