Machine learning (ML) is becoming an effective tool for studying 2D materials. Taking as input computed or experimental materials data, ML algorithms predict the structural, electronic, mechanical, ...and chemical properties of 2D materials that have yet to be discovered. Such predictions expand investigations on how to synthesize 2D materials and use them in various applications, as well as greatly reduce the time and cost to discover and understand 2D materials. This tutorial review focuses on the understanding, discovery, and synthesis of 2D materials enabled by or benefiting from various ML techniques. We introduce the most recent efforts to adopt ML in various fields of study regarding 2D materials and provide an outlook for future research opportunities. The adoption of ML is anticipated to accelerate and transform the study of 2D materials and their heterostructures.
The ability to detect low‐abundance proteins in human body fluids plays a critical role in proteomic research to achieve a comprehensive understanding of protein functions and early‐stage disease ...diagnosis to reduce mortality rates. Ultrasensitive (sub‐fM), rapid, simple “mix‐and‐read” plasmonic colorimetric biosensing of large‐size (≈180 kDa) proteins in biofluids using an ultralow‐noise multilayer molybdenum disulfide (MoS2) photoconducting channel is reported here. With its out‐of‐plane structure optimized to minimize carrier scattering, the multilayer MoS2 channel operated under near‐infrared illumination enables the detection of a subtle plasmonic extinction shift caused by antigen‐induced nanoprobe aggregation. The demonstrated biosensing strategy allows quantifying carcinoembryonic antigen in unprocessed whole blood with a dynamic range of 106, a sample‐to‐answer time of 10 min, and a limit of detection of 0.1–3 pg mL−1, which is ≈100‐fold more sensitive than the clinical‐standard enzyme‐linked immunosorbent assays. The biosensing methodology can be broadly used to realize timely personalized diagnostics and physiological monitoring of diseases in point‐of‐care settings.
A plasmonic colorimetric biosensing platform for rapid and ultrasensitive detection of cancer biomarkers in biofluids is developed using an ultralow‐noise multilayer molybdenum disulfide (MoS2) photoconducting channel. Near‐infrared operation of the multilayer MoS2 channel coupled with a nanoparticle aggregation‐based assay enables user‐friendly homogeneous on‐chip immunosensing that is poised for point‐of‐care testing.
Field-effect transistors made from MoS2 and other emerging layered semiconductors have been demonstrated to be able to serve as ultrasensitive biosensors. However, such nanoelectronic sensors still ...suffer seriously from a series of challenges associated with the poor compatibility between electronic structures and liquid analytes. These challenges hinder the practical biosensing applications that demand rapid, low-noise, highly specific biomolecule quantification at femtomolar levels. To address such challenges, we study a cyclewise process for operating MoS2 transistor biosensors, in which a series of reagent fluids are delivered to the sensor in a time-sequenced manner and periodically set the sensor into four assay-cycle stages, including incubation, flushing, drying, and electrical measurement. Running multiple cycles of such an assay can acquire a time-dependent sensor response signal quantifying the reaction kinetics of analyte-receptor binding. This cyclewise detection approach can avoid the liquid-solution-induced electrochemical damage, screening, and nonspecific adsorption to the sensor and therefore improves the transistor sensor’s durability, sensitivity, specificity, and signal-to-noise ratio. These advantages in combination with the inherent high sensitivity of MoS2 biosensors allow for rapid biomolecule quantification at femtomolar levels. We have demonstrated the cyclewise quantification of Interleukin-1β in pure and complex solutions (e.g., serum and saliva) with a detection limit of ∼1 fM and a total detection time ∼23 min. This work leverages the superior properties of layered semiconductors for biosensing applications and advances the techniques toward realizing fast real-time immunoassay for low-abundance biomolecule detection.
Memristors based on 2D layered materials could provide biorealistic ionic interactions and potentially enable construction of energy-efficient artificial neural networks capable of faithfully ...emulating neuronal interconnections in human brains. To build reliable 2D-material-based memristors suitable for constructing working neural networks, the memristive switching mechanisms in such memristors need to be systematically analyzed. Here, we present a study on the switching characteristics of the few-layer MoS2 memristors made by mechanical printing. First, two types of dc-programmed switching characteristics, termed rectification-mediated and conductance-mediated behaviors, are observed among different MoS2 memristors, which are attributed to the modulation of MoS2/metal Schottky barriers and redistribution of vacancies, respectively. We also found that an as-fabricated MoS2 memristor initially exhibits an analog pulse-programmed switching behavior, but it can be converted to a quasi-binary memristor with an abrupt switching behavior through an electrical stress process. Such a transition of switching characteristics is attributed to field-induced agglomeration of vacancies at MoS2/metal interfaces. The additional Kelvin probe force microscopy, Auger electron spectroscopy analysis, and electronic characterization results support this hypothesis. Finally, we fabricated a testing device consisting of two adjacent MoS2 memristors and demonstrated that these two memristors can be ionically coupled to each other. This device interconnection scheme could be exploited to build neural networks for emulating ionic interactions among neurons. This work advances the device physics for understanding the memristive properties of 2D-material-based memristors and serves as a critical foundation for building biorealistic neuromorphic computing systems based on such memristors.
Directly identifying the presence of the virus in infected hosts with an appropriate speed and sensitivity permits early epidemic management even during the presymptomatic incubation period of ...infection. Here, we synthesize a bioinspired plasmo-virus (BPV) particle for rapid and sensitive point-of-care (POC) detection of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) via a self-assembled plasmonic nanoprobe array on spike proteins. The BPV enables strong near-infrared (NIR) extinction peaks caused by plasmonic nanogaps. We quantify SARS-CoV-2 in viral transport medium (VTM) at low titers within 10 min with a limit of detection (LOD) of 1.4 × 101 pfu/mL, which is 103 times more sensitive than the current gold-standard method. The high-sensitivity and high-speed POC detection may be widely used for the timely, individualized diagnosis of infectious agents in low-resource settings.
The rapid emergence of air-mediated diseases in a micro-climate demands on-site monitoring of airborne microparticles. The on-site detection of airborne microparticles becomes more challenging as the ...particles are highly localized and change dynamically over time. However, most existing monitoring systems rely on time-consuming sample collection and centralized off-site analysis. Here, we report a smartphone-based integrated microsystem for on-site collection and detection that enables real-time detection of indoor airborne microparticles with high sensitivity. The collection device, inspired by the Venturi effect, was designed to collect airborne microparticles without requiring an additional power supply. Our systematic analysis showed that the collection device was able to collect microparticles with consistent negative pressure, regardless of the particle concentration in the air sample. By incorporating a microfluidic-biochip based on inertial force to trap particles and an optoelectronic photodetector into a miniaturized device with a smartphone, we demonstrate real-time and sensitive detection of the collected airborne microparticles, such as Escherichia coli, Bacillus subtilis, Micrococcus luteus, and Staphylococcus with a particle-density dynamic range of 103-108 CFU mL-1. Because of its capabilities of minimal-power sample collection, high sensitivity, and rapid detection of airborne microparticles, this integrated platform can be readily adopted by the government and industrial sectors to monitor indoor air contamination and improve human healthcare.
Monitoring of the time-varying immune status of a diseased host often requires rapid and sensitive detection of cytokines. Metallic nanoparticle-based localized surface plasmon resonance (LSPR) ...biosensors hold promise to meet this clinical need by permitting label-free detection of target biomolecules. These biosensors, however, continue to suffer from relatively low sensitivity as compared to conventional immunoassay methods that involve labeling processes. Their response speeds also need to be further improved to enable rapid cytokine quantification for critical care in a timely manner. In this paper, we report an immunobiosensing device integrating a biotunable nanoplasmonic optical filter and a highly sensitive few-layer molybdenum disulfide (MoS2) photoconductive component, which can serve as a generic device platform to meet the need of rapid cytokine detection with high sensitivity. The nanoplasmonic filter consists of anticytokine antibody-conjugated gold nanoparticles on a SiO2 thin layer that is placed 170 μm above a few-layer MoS2 photoconductive flake device. The principle of the biosensor operation is based on tuning the delivery of incident light to the few-layer MoS2 photoconductive flake thorough the nanoplasmonic filter by means of biomolecular surface binding-induced LSPR shifts. The tuning is dependent on cytokine concentration on the nanoplasmonic filter and optoelectronically detected by the few-layer MoS2 device. Using the developed optoelectronic biosensor, we have demonstrated label-free detection of IL-1β, a pro-inflammatory cytokine, with a detection limit as low as 250 fg/mL (14 fM), a large dynamic range of 106, and a short assay time of 10 min. The presented biosensing approach could be further developed and generalized for point-of-care diagnosis, wearable bio/chemical sensing, and environmental monitoring.
Heterogeneous nucleation could be an effective approach to producing an array of transition metal dichalco-genides (TMDs) at controlled locations on a substrate. In this study, we prepared Pt mesa ...structures on the substrate to induce heterogeneous nucleation of MoS2 during chemical vapor deposition (CVD) and investigated the adsorption of nuclei using Monte Carlo (MC) simulations. The MC simulations suggest that the site-selectivity of MoS2 dramatically drops when the CVD growth time goes beyond the critical time at which nuclei fully cover the Pt mesas, and such critical time can be delayed when the size of Pt mesas increases. Our experimental observations on a clean array of MoS2 successfully synthesized on 10 um-width square Pt mesas but not on 4 um -width square Pt mesas support the MC simulation. We further designed a simple method employing dummy substrates to increase the yield of the site-selective MoS2 array. Computational fluid dynamics (CFD) simulation reveals that such dummy substrates restrict the precursor concentration and provide a confined channel for the precursors to react slowly, which benefits producing large-area and site-selective MoS2. Furthermore, compared with conventional CVD, the total coverage of site-selective MoS2 has enlarged by seven times using dummy substrates.
Two-dimensional nanomaterials such as reduced graphene oxide (rGO) have captured significant attention in the realm of field-effect transistor (FET) sensors due to their inherent high sensitivity and ...cost-effective manufacturing. Despite their attraction, a comprehensive understanding of rGO–solution interfaces (specifically, electrochemical interfacial properties influenced by linker molecules and surface chemistry) remains challenging, given the limited capability of analytical tools to directly measure intricate solution interface properties. In this study, we introduce an analytical tool designed to directly measure the surface charge density of the rGO–solution interface leveraging the remote floating-gate FET (RFGFET) platform. Our methodology involves characterizing the electrochemical properties of rGO, which are influenced by adhesion layers between SiO2 and rGO, such as (3-aminopropyl)trimethoxysilane (APTMS) and hexamethyldisilazane (HMDS). The hydrophilic nature of APTMS facilitates the acceptance of oxygen-rich rGO, resulting in a noteworthy pH sensitivity of 56.8 mV/pH at the rGO–solution interface. Conversely, hydrophobic HMDS significantly suppresses the pH sensitivity from the rGO–solution interface, attributed to the graphitic carbon-rich surface of rGO. Consequently, the carbon-rich surface facilitates a denser arrangement of 1-pyrenebutyric acid N-hydroxysuccinimide ester linkers for functionalizing capturing probes on rGO, resulting in an enhanced sensitivity of lead ions by 32% in our proof-of-concept test.
