Reduced interface effect of proton beam irradiation on the electrical properties of WSe2/hBN field effect transistors.

Two-dimensional transition metal dichalcogenide (TMDC) semiconductors are emerging as strong contenders for electronic devices that can be used in highly radioactive environments such as outer space where conventional silicon-based devices exhibit nonideal characteristics for such applications. To address the radiation-induced interface effects of TMDC-based electronic devices, we studied high-energy proton beam irradiation effects on the electrical properties of field-effect transistors (FETs) made with tungsten diselenide (WSe2) channels and hexagonal boron-nitride (hBN)/SiO2gate dielectrics. The electrical characteristics of WSe2FETs were measured before and after the irradiation at various proton beam doses of 1013, 1014, and 1015cm-2. In particular, we demonstrated the dependence of proton irradiation-induced effects on hBN layer thickness in WSe2FETs. We observed that the hBN layer reduces the WSe2/dielectric interface effect which would shift the transfer curve of the FET toward the positive direction of the gate voltage. Also, this interface effect was significantly suppressed when a thicker hBN layer was used. This phenomenon can be explained by the fact that the physical separation of the WSe2channel and SiO2dielectric by the hBN interlayer prevents the interface effects originating from the irradiation-induced positive trapped charges in SiO2reaching the interface. This work will help improve our understanding of the interface effect of high-energy irradiation on TMDC-based nanoelectronic devices.

Key research development by Prof Mark Reed in molecular electronic devices.

In memory of Professor Mark Reed, who passed away on May 5, 2021, this article summarizes a series of his past groundbreaking developments in molecular electronic devices. Specifically, three key reports are summarized; measurement of the electrical conductance of molecular junctions using the mechanically controlled break junction technique and demonstration of negative differential resistance and orbital gating effect observed in molecular junctions. Also, a brief outlook on molecular electronics research field is addressed.

Highly sensitive, scalable, and rapid SARS-CoV-2 biosensor based on In2O3 nanoribbon transistors and phosphatase.

Developing convenient and accurate SARS-CoV-2 antigen test and serology test is crucial in curbing the global COVID-19 pandemic. In this work, we report an improved indium oxide (In2O3) nanoribbon field-effect transistor (FET) biosensor platform detecting both SARS-CoV-2 antigen and antibody. Our FET biosensors, which were fabricated using a scalable and cost-efficient lithography-free process utilizing shadow masks, consist of an In2O3 channel and a newly developed stable enzyme reporter. During the biosensing process, the phosphatase enzymatic reaction generated pH change of the solution, which was then detected and converted to electrical signal by our In2O3 FETs. The biosensors applied phosphatase as enzyme reporter, which has a much better stability than the widely used urease in FET based biosensors. As proof-of-principle studies, we demonstrate the detection of SARS-CoV-2 spike protein in both phosphate-buffered saline (PBS) buffer and universal transport medium (UTM) (limit of detection [LoD]: 100 fg/mL). Following the SARS-CoV-2 antigen tests, we developed and characterized additional sensors aimed at SARS-CoV-2 IgG antibodies, which is important to trace past infection and vaccination. Our spike protein IgG antibody tests exhibit excellent detection limits in both PBS and human whole blood ((LoD): 1 pg/mL). Our biosensors display similar detection performance in different mediums, demonstrating that our biosensor approach is not limited by Debye screening from salts and can selectively detect biomarkers in physiological fluids. The newly selected enzyme for our platform performs much better performance and longer shelf life which will lead our biosensor platform to be capable for real clinical diagnosis usage. Electronic Supplementary Material: Supplementary material (materials and methods for device fabrication, functionalization of In2O3 devices, photographs of the liquid gate measurement setup, mobilities of the nine devices labeled in Fig. 1(b), family curves of I DS-V DS with the liquid gate setup and current change after bubbling the substrate solution (current vs. time curve for S1 antigen detection)) is available in the online version of this article at 10.1007/s12274-022-4190-0.

Gate-tunable plasmons in mixed-dimensional van der Waals heterostructures.

Surface plasmons, collective electromagnetic excitations coupled to conduction electron oscillations, enable the manipulation of light-matter interactions at the nanoscale. Plasmon dispersion of metallic structures depends sensitively on their dimensionality and has been intensively studied for fundamental physics as well as applied technologies. Here, we report possible evidence for gate-tunable hybrid plasmons from the dimensionally mixed coupling between one-dimensional (1D) carbon nanotubes and two-dimensional (2D) graphene. In contrast to the carrier density-independent 1D Luttinger liquid plasmons in bare metallic carbon nanotubes, plasmon wavelengths in the 1D-2D heterostructure are modulated by 75% via electrostatic gating while retaining the high figures of merit of 1D plasmons. We propose a theoretical model to describe the electromagnetic interaction between plasmons in nanotubes and graphene, suggesting plasmon hybridization as a possible origin for the observed large plasmon modulation. The mixed-dimensional plasmonic heterostructures may enable diverse designs of tunable plasmonic nanodevices.

Narrower Nanoribbon Biosensors Fabricated by Chemical Lift-off Lithography Show Higher Sensitivity.

Wafer-scale nanoribbon field-effect transistor (FET) biosensors fabricated by straightforward top-down processes are demonstrated as sensing platforms with high sensitivity to a broad range of biological targets. Nanoribbons with 350 nm widths (700 nm pitch) were patterned by chemical lift-off lithography using high-throughput, low-cost commercial digital versatile disks (DVDs) as masters. Lift-off lithography was also used to pattern ribbons with 2 µm or 20 µm widths (4 or 40 µm pitches, respectively) using masters fabricated by photolithography. For all widths, highly aligned, quasi-one-dimensional (1D) ribbon arrays were produced over centimeter length scales by sputtering to deposit 20 nm thin-film In2O3 as the semiconductor. Compared to 20 µm wide microribbons, FET sensors with 350 nm wide nanoribbons showed higher sensitivity to pH over a broad range (pH 5 to 10). Nanoribbon FETs functionalized with a serotonin-specific aptamer demonstrated larger responses to equimolar serotonin in high ionic strength buffer than those of microribbon FETs. Field-effect transistors with 350 nm wide nanoribbons functionalized with single-stranded DNA showed greater sensitivity to detecting complementary DNA hybridization vs 20 µm microribbon FETs. In all, we illustrate facile fabrication and use of large-area, uniform In2O3 nanoribbon FETs for ion, small-molecule, and oligonucleotide detection where higher surface-to-volume ratios translate to better detection sensitivities.

Flexible Multiplexed In2O3 Nanoribbon Aptamer-Field-Effect Transistors for Biosensing.

Flexible sensors are essential for advancing implantable and wearable bioelectronics toward monitoring chemical signals within and on the body. Developing biosensors for monitoring multiple neurotransmitters in real time represents a key in vivo application that will increase understanding of information encoded in brain neurochemical fluxes. Here, arrays of devices having multiple In2O3 nanoribbon field-effect transistors (FETs) were fabricated on 1.4-µm-thick polyethylene terephthalate (PET) substrates using shadow mask patterning techniques. Thin PET-FET devices withstood crumpling and bending such that stable transistor performance with high mobility was maintained over >100 bending cycles. Real-time detection of the small-molecule neurotransmitters serotonin and dopamine was achieved by immobilizing recently identified high-affinity nucleic-acid aptamers on individual In2O3 nanoribbon devices. Limits of detection were 10 fM for serotonin and dopamine with detection ranges spanning eight orders of magnitude. Simultaneous sensing of temperature, pH, serotonin, and dopamine enabled integration of physiological and neurochemical data from individual bioelectronic devices.

Tunneling Spectroscopy in Carbon Nanotube-Hexagonal Boron Nitride-Carbon Nanotube Heterojunctions.

Electron tunneling spectroscopy is a powerful technique to probe the unique physical properties of one-dimensional (1D) single-walled carbon nanotubes (SWNTs), such as the van Hove singularities in the density of states or the power-law tunneling probability of a Luttinger liquid. However, little is known about the tunneling behavior between two 1D SWNTs over a large energy spectrum. Here, we investigate the electron tunneling behavior between two crossed SWNTs across a wide spectral window up to 2 eV in the unique carbon nanotube-hexagonal boron nitride-carbon nanotube heterojunctions. We observe many sharp resonances in the differential tunneling conductance at different bias voltages applied between the SWNTs. These resonances can be attributed to elastic tunneling into the van Hove singularities of different 1D subbands in both SWNTs, and they allow us to determine the quasi-particle bandgaps and higher-lying 1D subbands in SWNTs on the insulating substrate.

Red-phosphorus-impregnated carbon nanofibers for sodium-ion batteries and liquefaction of red phosphorus.

Red phosphorus offers a high theoretical sodium capacity and has been considered as a candidate anode for sodium-ion batteries. Similar to silicon anodes for lithium-ion batteries, the electrochemical performance of red phosphorus is plagued by the large volume variation upon sodiation. Here we perform in situ transmission electron microscopy analysis of the synthesized red-phosphorus-impregnated carbon nanofibers with the corresponding chemo-mechanical simulation, revealing that, the sodiated red phosphorus becomes softened with a "liquid-like" mechanical behaviour and gains superior malleability and deformability against pulverization. The encapsulation strategy of the synthesized red-phosphorus-impregnated carbon nanofibers has been proven to be an effective method to minimize the side reactions of red phosphorus in sodium-ion batteries, demonstrating stable electrochemical cycling. Our study provides a valid guide towards high-performance red-phosphorus-based anodes for sodium-ion batteries.

Nonlinear Luttinger liquid plasmons in semiconducting single-walled carbon nanotubes.

Interacting electrons confined in one dimension are generally described by the Luttinger liquid formalism, where the low-energy electronic dispersion is assumed to be linear and the resulting plasmonic excitations are non-interacting. Instead, a Luttinger liquid in one-dimensional materials with nonlinear electronic bands is expected to show strong plasmon-plasmon interactions, but an experimental demonstration of this behaviour has been lacking. Here, we combine infrared nano-imaging and electronic transport to investigate the behaviour of plasmonic excitations in semiconducting single-walled carbon nanotubes with carrier density controlled by electrostatic gating. We show that both the propagation velocity and the dynamic damping of plasmons can be tuned continuously, which is well captured by the nonlinear Luttinger liquid theory. These results contrast with the gate-independent plasmons observed in metallic nanotubes, as expected for a linear Luttinger liquid. Our findings provide an experimental demonstration of one-dimensional electron dynamics beyond the conventional linear Luttinger liquid paradigm and are important for understanding excited-state properties in one dimension.

Metallic Carbon Nanotube Nanocavities as Ultracompact and Low-loss Fabry-Perot Plasmonic Resonators.

Plasmonic resonators enable deep subwavelength manipulation of light matter interactions and have been intensively studied both in fundamental physics as well as for potential technological applications. While various metallic nanostructures have been proposed as plasmonic resonators, their performances are rather limited at mid- and far-infrared wavelengths. Recently, highly confined and low-loss Luttinger liquid plasmons in metallic single-walled carbon nanotubes (SWNTs) have been observed at infrared wavelengths. Here, we tailor metallic SWNTs into ultraclean nanocavities by advanced scanning probe lithography and investigate plasmon modes in these individual nanocavities by infrared nanoimaging. The dependence of mode evolutions on cavity length and excitation wavelength can be captured by a Fabry-Perot resonator model of a plasmon nanowaveguide terminated by highly reflective ends. Plasmonic resonators based on SWNT nanocavities approach the ultimate plasmon confinement limit and open the door to the strong light-matter coupling regime, which may enable various nanophotonic applications.

Tellurene Photodetector with High Gain and Wide Bandwidth.

Two-dimensional (2D) semiconductors have been extensively explored as a new class of materials with great potential. In particular, black phosphorus (BP) has been considered to be a strong candidate for applications such as high-performance infrared photodetectors. However, the scalability of BP thin film is still a challenge, and its poor stability in the air has hampered the progress of the commercialization of BP devices. Herein, we report the use of hydrothermal-synthesized and air-stable 2D tellurene nanoflakes for broadband and ultrasensitive photodetection. The tellurene nanoflakes show high hole mobilities up to 458 cm2/V·s at ambient conditions, and the tellurene photodetector presents peak extrinsic responsivity of 383 A/W, 19.2 mA/W, and 18.9 mA/W at 520 nm, 1.55 µm, and 3.39 µm light wavelength, respectively. Because of the photogating effect, high gains up to 1.9 × 103 and 3.15 × 104 are obtained at 520 nm and 3.39 µm wavelength, respectively. At the communication wavelength of 1.55 µm, the tellurene photodetector exhibits an exceptionally high anisotropic behavior, and a large bandwidth of 37 MHz is obtained. The photodetection performance at different wavelength is further supported by the corresponding quantum molecular dynamics (QMD) simulations. Our approach has demonstrated the air-stable tellurene photodetectors that fully cover the short-wave infrared band with ultrafast photoresponse.

Dynamically controllable polarity modulation of MoTe2 field-effect transistors through ultraviolet light and electrostatic activation.

Energy band engineering is of fundamental importance in nanoelectronics. Compared to chemical approaches such as doping and surface functionalization, electrical and optical methods provide greater flexibility that enables continuous, reversible, and in situ band tuning on electronic devices of various kinds. In this report, we demonstrate highly effective band modulation of MoTe2 field-effect transistors through the combination of electrostatic gating and ultraviolet light illumination. The scheme can achieve reversible doping modulation from deep n-type to deep p-type with ultrafast switching speed. The treatment also enables noticeable improvement in field-effect mobility by roughly 30 and 2 times for holes and electrons, respectively. The doping scheme also provides good spatial selectivity and allows the building of a photo diode on a single MoTe2 flake with excellent photo detection and photovoltaic performances. The findings provide an effective and generic doping approach for a wide variety of 2D materials.

Photoinduced Doping To Enable Tunable and High-Performance Anti-Ambipolar MoTe2/MoS2 Heterotransistors.

van der Waals (vdW) p-n heterojunctions formed by two-dimensional nanomaterials exhibit many physical properties and deliver functionalities to enable future electronic and optoelectronic devices. In this report, we demonstrate a tunable and high-performance anti-ambipolar transistor based on MoTe2/MoS2 heterojunction through in situ photoinduced doping. The device demonstrates a high on/off ratio of 105 with a large on-state current of several micro-amps. The peak position of the drain-source current in the transfer curve can be adjusted through the doping level across a large dynamic range. In addition, we have fabricated a tunable multivalue inverter based on the heterojunction that demonstrates precise control over its output logic states and window of midlogic through source-drain bias adjustment. The heterojunction also exhibits excellent photodetection and photovoltaic performances. Dynamic and precise modulation of the anti-ambipolar transport properties may inspire functional devices and applications of two-dimensional nanomaterials and their heterostructures of various kinds.

Fully Printed All-Solid-State Organic Flexible Artificial Synapse for Neuromorphic Computing.

Nonvolatile, flexible artificial synapses that can be used for brain-inspired computing are highly desirable for emerging applications such as human-machine interfaces, soft robotics, medical implants, and biological studies. Printed devices based on organic materials are very promising for these applications due to their sensitivity to ion injection, intrinsic printability, biocompatibility, and great potential for flexible/stretchable electronics. Herein, we report the experimental realization of a nonvolatile artificial synapse using organic polymers in a scalable fabrication process. The three-terminal electrochemical neuromorphic device successfully emulates the key features of biological synapses: long-term potentiation/depression, spike timing-dependent plasticity learning rule, paired-pulse facilitation, and ultralow energy consumption. The artificial synapse network exhibits an excellent endurance against bending tests and enables a direct emulation of logic gates, which shows the feasibility of using them in futuristic hierarchical neural networks. Based on our demonstration of 100 distinct, nonvolatile conductance states, we achieved a high accuracy in pattern recognition and face classification neural network simulations.

Logarithm Diameter Scaling and Carrier Density Independence of One-Dimensional Luttinger Liquid Plasmon.

Quantum-confined electrons in one-dimensional (1D) metals are described by a Luttinger liquid. The collective charge excitations (i.e., plasmons) in a Luttinger liquid can behave qualitatively different from their conventional counterparts. For example, the Luttinger liquid plasmon velocity is uniquely determined by the electron-electron interaction, which scales logarithmly with the diameter of the 1D material. In addition, the Luttinger liquid plasmon is predicted to be independent of the carrier concentration. Here, we report the observation of such unusual Luttinger liquid plasmon behaviors in metallic single-walled carbon nanotubes, a model system featuring strong electron quantum confinement. We systematically investigate the plasmon propagation in over 30 metallic carbon nanotubes of different diameters using infrared nanoscopy. We establish that the plasmon velocity has a weak logarithm dependence on the nanotube diameter, as predicted by the Luttinger liquid theory. We further study the plasmon excitation as a function of the carrier density in electrostatically gated metallic carbon nanotubes and demonstrate that the plasmon velocity is completely independent of the carrier density. These behaviors are in striking contrast to conventional plasmons in 1D metallic shells, where the plasmon dispersion changes dramatically with the metal electron density and the 1D diameter. The unusual behaviors of Luttinger liquid plasmon may enable novel nanophotonic applications based on carbon nanotubes.

Carbon Nanotubes and Related Nanomaterials: Critical Advances and Challenges for Synthesis toward Mainstream Commercial Applications.

Advances in the synthesis and scalable manufacturing of single-walled carbon nanotubes (SWCNTs) remain critical to realizing many important commercial applications. Here we review recent breakthroughs in the synthesis of SWCNTs and highlight key ongoing research areas and challenges. A few key applications that capitalize on the properties of SWCNTs are also reviewed with respect to the recent synthesis breakthroughs and ways in which synthesis science can enable advances in these applications. While the primary focus of this review is on the science framework of SWCNT growth, we draw connections to mechanisms underlying the synthesis of other 1D and 2D materials such as boron nitride nanotubes and graphene.

Correlation of Electron Tunneling and Plasmon Propagation in a Luttinger Liquid.

Quantum-confined electrons in one dimension behave as a Luttinger liquid. However, unambiguous demonstration of Luttinger liquid phenomena in single-walled carbon nanotubes (SWNTs) has been challenging. Here we investigate well-defined SWNT cross junctions with a point contact between two Luttinger liquids and combine electrical transport and optical nanoscopy measurements to correlate completely different physical properties (i.e., the electron tunneling and the plasmon propagation) in the same Luttinger liquid system. The suppressed electron tunneling at SWNT junctions exhibits a power-law scaling, which yields a Luttinger liquid interaction parameter that agrees quantitatively with that independently determined from the plasmon velocity based on the near-field optical nanoscopy.

Room-Temperature Pressure Synthesis of Layered Black Phosphorus-Graphene Composite for Sodium-Ion Battery Anodes.

Sodium-ion batteries offer an attractive option for grid-level energy storage due to the high natural abundance of sodium and low material cost of sodium compounds. Phosphorus (P) is a promising anode material for sodium-ion batteries, with a theoretical capacity of 2596 mAh/g. The red phosphorus (RP) form has worse electronic conductivity and lower initial Coulombic efficiency than black phosphorus (BP), but high material cost and limited production capacity have slowed the development of BP anodes. To address these challenges, we have developed a simple and scalable method to synthesize layered BP/graphene composite (BP/rGO) by pressurization at room temperature. A carbon-black-free and binder-free BP/rGO anode prepared with this method achieved specific charge capacities of 1460.1, 1401.2, 1377.6, 1339.7, 1277.8, 1123.78, and 720.8 mAh/g in a rate capability test at charge and discharge current densities of 0.1, 0.5, 1, 5, 10, 20, and 40 A/g, respectively. In a cycling performance test, after 500 deep cycles, the capacity of BP/rGO anodes stabilized at 1250 and 640 mAh/g at 1 and 40 A/g, respectively, which marks a significant performance improvement for sodium-ion battery anodes.

Hierarchical Carbon-Coated Ball-Milled Silicon: Synthesis and Applications in Free-Standing Electrodes and High-Voltage Full Lithium-Ion Batteries.

Lithium-ion batteries have been regarded as one of the most promising energy storage devices, and development of low-cost batteries with high energy density is highly desired so that the cost per watt-hour ($/Wh) can be minimized. In this work, we report using ball-milled low-cost silicon (Si) as the starting material and subsequent carbon coating to produce low-cost hierarchical carbon-coated (HCC) Si. The obtained particles prepared from different Si sources all show excellent cycling performance of over 1000 mAh/g after 1000 cycles. Interestingly, we observed in situ formation of porous Si, and it is well confined in the carbon shell based on postcycling characterization of the hierarchical carbon-coated metallurgical Si (HCC-M-Si) particles. In addition, lightweight and free-standing electrodes consisting of the HCC-M-Si particles and carbon nanofibers were fabricated, which achieved 1015 mAh/g after 100 cycles based on the total mass of the electrodes. Compared with conventional electrodes, the lightweight and free-standing electrodes significantly improve the energy density by 745%. Furthermore, LiCoO2 and LiNi0.5Mn1.5O4 cathodes were used to pair up with the HCC-M-Si anode to fabricate full cells. With LiNi0.5Mn1.5O4 as cathode, an energy density up to 547 Wh/kg was achieved by the high-voltage full cell. After 100 cycles, the full cell with a LiNi0.5Mn1.5O4 cathode delivers 46% more energy density than that of the full cell with a LiCoO2 cathode. The systematic investigation on low-cost Si anodes together with their applications in lightweight free-standing electrodes and high-voltage full cells will shed light on the development of high-energy Si-based lithium-ion batteries for real applications.