Scaffold‐guided formation of neuronal‐like networks, especially under electrical stimulation, can be an appealing avenue toward functional restoration of injured nervous systems. Here, 3D conductive scaffolds are fabricated based on printed microfiber constructs using near‐field electrostatic printing (NFEP) and graphene oxide (GO) coating. Various microfiber patterns are obtained from poly(
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Partial laser treatment is introduced to carbon‐based microfibers to generate excellent photon sensing capability without bias. This treatment brings about a Seebeck coefficient distribution along the sample's length, out of which a photovoltage with no external bias is generated and sensed. Using a line‐shaped laser spot, carbon microfiber (CMF), graphene microfiber (GMF), and graphene aerogel fiber (GAF) are investigated for their response to µm‐scale photon irradiation. A higher sensitivity for the incident photon is found for the GAF with no position sensitivity. More Seebeck coefficient variation is also observed for the GAF considering the amount of laser power used for the laser treatment. A weaker Seebeck coefficient spatial variation is observed for the GMF compared with the GAF. However, its photovoltage shows an abrupt magnitude change from the laser‐treated region to the non‐treated one. Despite the low spatial variation of the Seebeck coefficient for the CMF, it features an excellent and accurate position‐sensitive photoresponse with polarization change over a distance of ≈100 µm. Such unique capability prompts novel applications in using partially annealed CMF for sensing the position of optical beams at the microscale.
more » « less- Award ID(s):
- 1930866
- NSF-PAR ID:
- 10485704
- Publisher / Repository:
- Wiley
- Date Published:
- Journal Name:
- Advanced Optical Materials
- ISSN:
- 2195-1071
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract l ‐lactic acid‐co ‐caprolactone) (PLCL) using NFEP and complexity is achieved via modulating the fiber overlay angles (45°, 60°, 75°, 90°), fiber diameters (15 to 148 µm), and fiber spatial organization (spider web and tubular structure). Upon coating GO onto PLCL microfibers via a layer‐by‐layer (L‐b‐L) assembly technique and in situ reduction into reduced GO (rGO), the obtained conductive scaffolds, with 25–50 layers of rGO, demonstrate superior conductivity (≈0.95 S cm−1) and capability of inducing neuronal‐like network formation along the conductive microfibers under electrical stimulation (100–150 mV cm−1). Both electric field (0–150 mV cm−1) and microfiber diameter (17–150 µm) affect neurite outgrowth (PC‐12 cells and primary mouse hippocampal neurons) and the formation of orientated neuronal‐like networks. With further demonstration of such guidance to neuronal cells, these conductive scaffolds may see versatile applications in nerve regeneration and neural engineering. -
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The temperature coefficient of resistivity (θT) of carbon-based materials is a critical property that directly determines their electrical response upon thermal impulses. It could have metal- (positive) or semiconductor-like (negative) behavior, depending on the combined temperature dependence of electron density and electron scattering. Its distribution in space is very difficult to measure and is rarely studied. Here, for the first time, we report that carbon-based micro/nanoscale structures have a strong non-uniform spatial distribution of θT. This distribution is probed by measuring the transient electro-thermal response of the material under extremely localized step laser heating and scanning, which magnifies the local θT effect in the measured transient voltage evolution. For carbon microfibers (CMFs), after electrical current annealing, θT varies from negative to positive from the sample end to the center with a magnitude change of >130% over <1 mm. This θT sign change is confirmed by directly testing smaller segments from different regions of an annealed CMF. For micro-thick carbon nanotube bundles, θT is found to have a relative change of >125% within a length of ∼2 mm, uncovering strong metallic to semiconductive behavior change in space. Our θT scanning technique can be readily extended to nm-thick samples with μm scanning resolution to explore the distribution of θT and provide a deep insight into the local electron conduction.
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Neurotransmitters are small molecules involved in neuronal signaling and can also serve as stress biomarkers.1Their abnormal levels have been also proposed to be indicative of several neurological diseases such as Alzheimer’s disease, Parkinson’s disease, Huntington disease, among others. Hence, measuring their levels is highly important for early diagnosis, therapy, and disease prognosis. In this work, we investigate facile functionalization methods to tune and enhance sensitivity of printed graphene sensors to neurotransmitters. Sensors based on direct laser scribing and screen-printed graphene ink are studied. These printing methods offer ease of prototyping and scalable fabrication at low cost.
The effect of functionalization of laser induced graphene (LIG) by electrodeposition and solution-based deposition of TMDs (molybdenum disulfide2and tungsten disulfide) and metal nanoparticles is studied. For different processing methods, electrochemical characteristics (such as electrochemically active surface area: ECSA and heterogenous electron transfer rate: k0) are extracted and correlated to surface chemistry and defect density obtained respectively using X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. These functionalization methods are observed to directly impact the sensitivity and limit of detection (LOD) of the graphene sensors for the studied neurotransmitters. For example, as compared to bare LIG, it is observed that electrodeposition of MoS2on LIG improves ECSA by 3 times and k0by 1.5 times.3Electrodeposition of MoS2also significantly reduces LOD of serotonin and dopamine in saliva, enabling detection of their physiologically relevant concentrations (in pM-nM range). In addition, chemical treatment of LIG sensors is carried out in the form of acetic acid treatment. Acetic acid treatment has been shown previously to improve C-C bonds improving the conductivity of LIG sensors.4In our work, in particular, acetic acid treatment leads to larger improvement of LOD of norepinephrine compared to MoS2electrodeposition.
In addition, we investigate the effect of plasma treatment to tune the sensor response by modifying the defect density and chemistry. For example, we find that oxygen plasma treatment of screen-printed graphene ink greatly improves LOD of norepinephrine up to three orders of magnitude, which may be attributed to the increased defects and oxygen functional groups on the surface as evident by XPS measurements. Defects are known to play a key role in enhancing the sensitivity of 2D materials to surface interactions, and have been explored in tuning/enhancing the sensor sensitivity.5Building on our previous work,3we apply a custom machine learning-based data processing method to further improve that sensitivity and LOD, and also to automatically benchmark different molecule-material pairs.
Future work includes expanding the plasma chemistry and conditions, studying the effect of precursor mixture in laser-induced solution-based functionalization, and understanding the interplay between molecule-material system. Work is also underway to improve the machine learning model by using nonlinear learning models such as neural networks to improve the sensor sensitivity, selectivity, and robustness.
References A. J. Steckl, P. Ray, (2018), doi:10.1021/acssensors.8b00726.
Y. Lei, D. Butler, M. C. Lucking, F. Zhang, T. Xia, K. Fujisawa, T. Granzier-Nakajima, R. Cruz-Silva, M. Endo, H. Terrones, M. Terrones, A. Ebrahimi,
Sci. Adv. 6 , 4250–4257 (2020).V. Kammarchedu, D. Butler, A. Ebrahimi,
Anal. Chim. Acta .1232 , 340447 (2022).H. Yoon, J. Nah, H. Kim, S. Ko, M. Sharifuzzaman, S. C. Barman, X. Xuan, J. Kim, J. Y. Park,
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Adv. Mater. 31 , 1–12 (2019). -
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m −1cm−2and an ultra‐low limit of detection of 0.079 µm . The sensor can also detect pH and exhibit extraordinary stability to maintain more than 91% sensitivity over 21 days in ambient conditions. Taken together with a temperature sensor based on the same material system, the dual glucose and pH sensor integrated with a flexible microfluidic sweat sampling network further results in accurate continuous on‐body glucose detection calibrated by the simultaneously measured pH and temperature. The low‐cost, highly sensitive, and long‐term stable platform could facilitate the early identification and continuous monitoring of different biomarkers for non‐invasive disease diagnosis and treatment evaluation. -
Abstract The accurate, continuous analysis of healthcare-relevant gases such as nitrogen oxides (NO x ) in a humid environment remains elusive for low-cost, stretchable gas sensing devices. This study presents the design and demonstration of a moisture-resistant, stretchable NO x gas sensor based on laser-induced graphene (LIG). Sandwiched between a soft elastomeric substrate and a moisture-resistant semipermeable encapsulant, the LIG sensing and electrode layer is first optimized by tuning laser processing parameters such as power, image density, and defocus distance. The gas sensor, using a needlelike LIG prepared with optimal laser processing parameters, exhibits a large response of 4.18‰ ppm −1 to NO and 6.66‰ ppm −1 to NO 2 , an ultralow detection limit of 8.3 ppb to NO and 4.0 ppb to NO 2 , fast response/recovery, and excellent selectivity. The design of a stretchable serpentine structure in the LIG electrode and strain isolation from the stiff island allows the gas sensor to be stretched by 30%. Combined with a moisture-resistant property against a relative humidity of 90%, the reported gas sensor has further been demonstrated to monitor the personal local environment during different times of the day and analyze human breath samples to classify patients with respiratory diseases from healthy volunteers. Moisture-resistant, stretchable NO x gas sensors can expand the capability of wearable devices to detect biomarkers from humans and exposed environments for early disease diagnostics.more » « less
