Layered black phosphorus has drawn much attention due to the existence of a band gap compared to the widely known graphene. However, environmental stability of black phosphorus is still a major issue, which hinders the realization of practical device applications. Here, we spatially Raman map exfoliated black phosphorus using confocal fast-scanning technique at different time intervals. We observe a Raman intensity modulation for , B2g, and modes. This Raman modulation is found to be caused by optical interference, which gives insights into the oxidation mechanism. Finally, we examine the fabrication compatible PMMA coating as a viable passivation layer. Our measurements indicate that PMMA passivated black phosphorus thin film flakes can stay pristine for a period of 19 days when left in a dark environment, allowing sufficient time for further nanofabrication processing. Our results shed light on black phosphorus degradation which can aid future passivation methods.
Glial fibrillary acidic protein (GFAP) is a discriminative blood biomarker for many neurological diseases, such as traumatic brain injury. Detection of GFAP in buffer solutions using biosensors has been demonstrated, but accurate quantification of GFAP in patient samples has not been reported, yet in urgent need. Herein, we demonstrate a robust on-chip graphene field-effect transistor (GFET) biosensing method for sensitive and ultrafast detection of GFAP in patient plasma. Patients with moderate–severe traumatic brain injuries, defined by the Mayo classification, are recruited to provide plasma samples. The binding of target GFAP with the specific antibodies that are conjugated on a monolayer GFET device triggers the shift of its Dirac point, and this signal change is correlated with the GFAP concentration in the patient plasma. The limit of detection (LOD) values of 20 fg/mL (400 aM) in buffer solution and 231 fg/mL (4 fM) in patient plasma have been achieved using this approach. In parallel, for the first time, we compare our results to the state-of-the-art single-molecule array (Simoa) technology and the classic enzyme-linked immunosorbent assay (ELISA) for reference. The GFET biosensor shows competitive LOD to Simoa (1.18 pg/mL) and faster sample-to-result time (<15 min), and also it is cheaper and more user-friendly. In comparison to ELISA, GFET offers advantages of total detection time, detection sensitivity, and simplicity. This GFET biosensing platform holds high promise for the point-of-care diagnosis and monitoring of traumatic brain injury in GP surgeries and patient homes.
Biosensors based on graphene field effect transistors (GFETs) have the potential to enable the development of point-of-care diagnostic tools for early stage disease detection. However, issues with reproducibility and manufacturing yields of graphene sensors, but also with Debye screening and unwanted detection of nonspecific species, have prevented the wider clinical use of graphene technology. Here, we demonstrate that our wafer-scalable GFETs array platform enables meaningful clinical results. As a case study of high clinical relevance, we demonstrate an accurate and robust portable GFET array biosensor platform for the detection of pancreatic ductal adenocarcinoma (PDAC) in patients’ plasma through specific exosomes (GPC-1 expression) within 45 min. In order to facilitate reproducible detection in blood plasma, we optimized the analytical performance of GFET biosensors via the application of an internal control channel and the development of an optimized test protocol. Based on samples from 18 PDAC patients and 8 healthy controls, the GFET biosensor arrays could accurately discriminate between the two groups while being able to detect early cancer stages including stages 1 and 2. Furthermore, we confirmed the higher expression of GPC-1 and found that the concentration in PDAC plasma was on average more than 1 order of magnitude higher than in healthy samples. We found that these characteristics of GPC-1 cancerous exosomes are responsible for an increase in the number of target exosomes on the surface of graphene, leading to an improved signal response of the GFET biosensors. This GFET biosensor platform holds great promise for the development of an accurate tool for the rapid diagnosis of pancreatic cancer.
Layered hafnium diselenide (HfSe2) is an emerging Van der Waals semiconductor in which a hafnium layer is sandwiched between two selenium layers. Owning to its indirect band gap with magnitudes close to silicon's band gap and high predicted carrier mobility, hafnium diselenide material is a strong candidate for device applications. Here, the effect of laser treatment on 2H‐ HfSe2 devices is shown in ambient conditions using µ‐Raman spectroscopy. It is shown that an emerging Raman peak evolves with increasing laser exposure time. It is also shown that top‐down fabricated 2H‐HfSe2 devices exhibit an anomalous p‐type behavior post laser treatment, with Ion/Ioff ratio as high as 103. This anomalous conductivity change can be observed after thermal and electrical annealing. For bottom‐up devices, it is observed that p‐type conductivity with remarkable Ion/Ioff ratio reaching 104. This conductivity switch can also be shown on 1T‐HfSe2 devices post laser irradiation and high Vds bias treatments. Based on the circuit model, this conductivity switch is attributed to contact doping caused by an increase in the Schottky barrier height at each contact, which shifts the Fermi energy closer to the valance band. These results demonstrate a unique conductivity switching mechanism for HfSe2‐FET devices.
Newly explored two-dimensional (2D) materials have shown promising optical properties, owning to the tunable band gap of the layered material with its thickness. A widely used method to achieve tunable light emission (or photoluminescence) is through thickness modulation, but this can only cover specific wavelengths. This approach limits the development of tunable optical devices with high spectral resolution over a wide range of wavelengths. Here, we report wideband tunable light emission of exfoliated black phosphorus nanosheets via a pulsed thermal annealing process in ambient conditions. Tunable anisotropic emission was observed between wavelengths of 590 and 720 nm with a spectral resolution of 5 nm. This emission can be maintained for at least 11 days when proper passivation coupled with adequate storage is applied. Using hyperspectral imaging X-ray photoelectron spectroscopy (i-XPS), this tunable emission is found to be strongly dependent on the level of oxidation. We finally discuss the underlying mechanism responsible for the observed tunable emission and show that tunable emission is only observed in nanosheets with thicknesses of (70–125 nm) ± 10 nm with the maximum range achieved for nanosheets with thicknesses of 125 ± 10 nm. Our results shed some light on an emerging class of 2D oxides with potential in optoelectronic applications.
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