Structure and function analysis of a type III preQ1-I riboswitch from Escherichia coli reveals direct metabolite sensing by the Shine-Dalgarno sequence
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Polymer nanocomposites offer design solutions to control and tune optical, conductive, topological, and thermomechanical properties of advanced and multifunctional materials. Because of their ubiquitous nature, methodologies to diagnose failure or structural changes in the nanocomposites are of significant interest. Herein, we report a nanocomposite system loaded with quantum dots and coumarin-modified carbon nanotubes that transduce mechanical force into fluorescence at a strain, for the first time, as low as 7.5%. Our comprehensive studies detail the optical, morphological, and thermomechanical properties of these nanocomposites to establish the fundamental reason behind the activation of fluorescence. Here our results indicate that bare carbon nanotubes can irreversibly quench the fluorescence from quantum dots and that the coumarin-modified carbon nanotubes mitigate the quenching through Förster Resonance Energy Transfer. Next, the application of force to the sample changes the quantum dot-carbon nanotube spacing as well as the carbon nanotube morphology to activate fluorescence in the nanocomposite. Overall, this force activation of fluorescence can serve as a general strategy for the development of a new class of mechano-responsive nanocomposites that impart polymeric materials with desirable functionalities including damage sensing and mechanical strength.
This work proposes a spectral convolutional neural network (CNN) operating on laser induced breakdown spectroscopy (LIBS) signals to learn to (1) disentangle spectral signals from the sources of sensor uncertainty (i.e., pre-process) and (2) get qualitative and quantitative measures of chemical content of a sample given a spectral signal (i.e., calibrate). Once the spectral CNN is trained, it can accomplish either task through a single feed-forward pass, with real-time benefits and without any additional side information requirements including dark current, system response, temperature and detector-to-target range. Our experiments demonstrate that the proposed method outperforms the existing approaches used by the Mars Science Lab for pre-processing and calibration for remote sensing observations from the Mars rover, ‘Curiosity’.
In this work, we demonstrate a simple and robust method for measuring the shape- and orientation-dependent optical scattering of various plasmonic nanostructures adsorbed onto a solid surface using polarized dark-field microscopy. By analyzing the dark-field scattering images of gold nanostructures using grazing incidence polarized light with a bench-top microscope, we are able to correlate optical scattering from the individual nanostructures with their shape and orientation. Depending on the size, shape, and orientation of the plasmonic nanostructures, they exhibit characteristic angle- and polarization-dependent scattering signals. Extracting the red, green, and blue channels of the scattering signals from a color-imaging detector as a function of azimuthal angle provides a polar plot of color intensity values that is characteristic of the underlying nanostructure. Examples are presented for various nanostructures, including spherical nanoparticles, nanotriangles, and nanorods. Experimental results are complemented by numerical calculations of the scattering spectra of representative model nanostructures. We demonstrate that the polarization- and orientation-dependent scattering behavior is a consequence of various localized surface plasmon modes existing in the nanostructures and can be used to verify the shape of individual objects as well as quickly identify the orientation of numerous objects on a densely populated substrate. We anticipate that this method will provide a rapid and efficient complement to the typical structural analysis of nanoparticles that is achieved by electron microscopy as well as providing a simple method for generating detailed information of the optical scattering of various types of individual plasmonic nanostructures.
The evaluation of epigenetic features such as DNA methylation is becoming increasingly important in many biochemical processes like gene expression and transcription as well as in several diseases like schizophrenia or diabetes. Here, in this work, we report that self-assembled nanomechanical resonators entirely composed of DNA molecules can be used to explore gross changes in DNA methylation levels (0–25–50%), while careful control of tensile stress is needed to reduce the variability of resonance frequency for rigorous quantification. The effect of the tensile stress retained by the suspended DNA nanoresonators on the application of the technique is extensively explored using a combination of laser Doppler vibrometry and atomic force spectroscopy. DNA nanoresonators are real-time, label-free sensors and could avoid chemical functionalization and sample amplification. Therefore, they may represent in the future a key complementary routine tool for global DNA methylation analysis needed to evaluate the consequences of environmental stresses on the human genome.
Porous Li-ion electrodes contain active particles, ion transporting electrolyte, and carbon-binder networks. While macrohomogeneous models are often used to predict electrode behavior, accurate predictions remain challenging, owing to the incomplete understanding of the critical role of carbon-binder networks and how they affect the electrochemical response. The present study systematically characterizes these effects in terms of effective properties by utilizing macrohomogeneous models to analyze the measured responses for electrodes with different carbon-binder content, electrode thickness, and porosity but with identical materials. We find that the impact of the carbon-binder network is more severe than previously thought. Even for low carbon-binder content (5 %wt. dry electrode), the presence of the network decreases the reaction area and increases the ion transport resistance, negatively impacting electrode performance. These effects scale with not just porosity or active material volume but also with carbon-binder content. The findings underscore the importance of connecting all effective properties to electrode specifications in a full factorial sense to transform the electrode design paradigm.
A multifunctional fiber-reinforced composite with passive self-sensing, energy-harvesting, and damage detection capabilities is presented. In this work, barium titanate piezoelectric microparticles are deposited on basalt fibers by a scalable, low-cost, environmentally friendly continuous feed-through process. The resulting composite derives a superior interlaminar shear strength from the microparticle-modified fiber–matrix interfaces. The composite also demonstrates passive self-sensing capabilities that produce electrical signals proportional to various dynamic loading events. Vibration and strain-controlled experiments are performed on composite beams to quantify the sensitivity and power output as a function of input acceleration and strain. Furthermore, these composite-generated electrical signals are used to identify in situ damage initiation for structural health monitoring to inform composite damage prior to structural failure. In brief, this truly multifunctional composite simultaneously displays a sensitivity of 0.5–2.6 mV g -1 at a resolution of 0.045–0.20g (g = gravitational acceleration), energy harvesting in the range of nW cc -1 , and prediction of early damage by exhibiting 0.017–1.17 mV peaks in voltage–time history profiles while assuring ≈20% improved interlaminar shear strength.
Metal–organic frameworks (MOFs) NU-1000 and UiO-66 are herein exposed to two different gamma irradiation doses and dose rates and analyzed to determine the structural features that affect their stability in these environments. MOFs have shown promise for the capture and sensing of off-gases at civilian nuclear energy reprocessing sites, nuclear waste repositories, and nuclear accident locations. However, little is understood about the structural features of MOFs that contribute to their stability levels under the ionizing radiation conditions present at such sites. This study is the first of its kind to explore the structural features of MOFs that contribute to their radiolytic stability. Both NU-1000 and UiO-66 are MOFs that contain Zr metal-centers with the same metal absorption cross section. However, the two MOFs exhibit different linker connectivities, linker aromaticities, node densities, node connectivities, and interligand separations. In this study, NU-1000 and UiO-66 were exposed to high (423.3 Gy/min, 23 min, and 37 s) and low (0.78 Gy/min, 4320 min) dose rates of 60 Co gamma irradiation. NU-1000 displayed insignificant radiation damage under both dose rates due to its high linker connectivity, low node density, and low node connectivity. However, low radiation dose rates caused considerable damage to UiO-66, a framework with lower aromaticity and smaller interligand separation. Finally, results suggest that chronic, low-radiation environments are more detrimental to Zr MOF stability than acute, high-radiation conditions.
We report high temperature surface acoustic wave (SAW) gas sensors with conducting sensing layers require tuning of the sheet conductivity for optimal response. Conducting metal oxides are attractive sensing materials for their tunable electronic properties and high thermal stability, amongst others. Here, we have investigated the application of indium oxide (IO) and indium tin oxide (ITO) films on langasite (LGS)-based SAW reflective delay line sensor devices for monitoring hydrogen at 350 °C. Specifically, we modeled the effect of the IO and ITO sensing layer thickness on the wave velocity, attenuation, and effective electromechanical coefficient. This was followed by an experimental demonstration of tuning of the ITO film sheet conductivity by controlling the dopant concentration and yielding an improvement in the sensor sensitivity. The current study provides a pathway towards the development of conductivity-based sensing layers for high temperature SAW gas sensors with improved sensitivity.
Fabrication of porous materials from the standard sacrificial template method allows metal oxide nanostructures to be produced and have several applications in energy, filtration and constructing sensing devices. However, the low surface area of these nanostructures is a significant drawback for most applications. Here, we report the synthesis of ZnO/carbon composite monoliths in which carbon is used as a sacrificial template to produce zinc oxide (ZnO) porous nanostructures with a high specific surface area. The synthesized porous oxides of ZnO with a specific surface area of 78 m2/g are at least one order of magnitude higher than that of the ZnO nanotubes reported in the literature. The crucial point to achieving this remarkable result was the usage of a novel ZnO/carbon template where the carbon template was removed by simple heating in the air. As a high surface area porous nanostructured ZnO, these synthesized materials can be useful in various applications including catalysis, photocatalysis, separation, sensing, solar energy harvest and Zn-ion battery and as supercapacitors for energy storage.
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Plasmids play significant roles in microbial adaptation to ecosystems, yet their dynamics remain poorly understood due to identification challenges. We present the Global Soil Plasmidome Resource (GSPR), a comprehensive dataset of 98,728 plasmid sequences amassed from 6860 terrestrial microbial communities and isolates. We explore this resource through various computational approaches, including phylogenetic diversity analysis, host prediction, and extensive functional annotation, to understand the contribution of plasmids to the genetic and functional diversity in soil, correlating these findings with sample type, as well as the soil habitat they were retrieved from. Our analysis reveals insights into plasmid-encoded functions such as effector modules, quorum sensing, and stress resistance, which may contribute to their persistence and microbial adaptation in soil. Furthermore, CRISPR analysis suggests a prevalent role of these elements related to intra-plasmid competition. By contrasting plasmids from cultivated and uncultivated organisms, we identify important functions that expand existing knowledge of plasmid roles in these habitats. This study represents a notable step forward in elucidating plasmid diversity and function within soil microbiomes and establishes a foundational framework for exploring their roles in natural environments.
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To explore aggregate-induced emission (AIE) properties, this study adopts a one-pot hydrothermal route for synthesizing polyethylene glycol (PEG)-coated graphene quantum dot (GQD) clusters, enabling the emission of highly intense photoluminescence under blue light illumination. The hydrothermal synthesis was performed at 300 °C using o-phenylenediamine as the nitrogen and carbon sources in the presence of PEG. Three different solvents, propylene glycol methyl ether acetate (PGMEA), ethanol, and water, were used for dispersing the PEG-coated GQDs, where extremely high fluorescent emission was achieved at 530–550 nm. It was shown that the quantum yield (QY) of PEG-coated GQD suspensions is strongly dependent on the solvent type. The pristine GQD suspension tends to be quenched (i.e., QY: ~1%) when dispersed in PGMEA (aggregation-caused quenching). However, coating GQD nanoparticles with polyethylene glycol results in substantial enhancement of the quantum yield. When investigating the photoluminescence emission from PEG-coated GQD clusters, the surface tension of the solvents was within the range of from 26.9 to 46.0 mN/m. This critical index can be tuned for assessing the transition point needed to activate the AIE mechanism which ultimately boosts the fluorescence intensity. The one-pot hydrothermal route established in this study can be adopted to engineer PEG-coated GQD clusters with solid-state PL emission capabilities, which are needed for next-generation optical, bio-sensing, and energy storage/conversion devices.
The Annual Site Environmental Report (ASER) from a U.S. Department of Energy (DOE) Site summarizes environmental data; environmental management performance; compliance with applicable DOE, federal, state, and local regulations; and restoration and surveillance monitoring programs. The Savannah River Site (SRS) produces ASERs that include results of monitoring mercury levels in fish samples obtained in the vicinity of SRS. Mercury is a toxic trace metal and the methylated organic form is a neurotoxin that bioaccumulates in the food web, endangering humans and other organisms. In United States, power plants are the largest source of mercury emissions. Research Objective: To determine the patterns of mercury levels in fish samples reported in the SRS environmental monitoring reports. We developed box plot visualizations to make sense of the data as well as identify fish species, dates and location with outlier mercury content. The integration and visual representation of multi-year datasets can support decision making processes on environmental compliance and environmental sustainability conducted at U.S. DOE Sites. We are constructing datasets from textual, image and multivariable data sources in the multi-year ASERs of the U.S. DOE Savannah River Site (SRS https://www.srs.gov/general/pubs/ERsum/index.html). The Fish Surveillance for mercury presents a case study for the intersection of food, energy and water systems. The dataset of 864 records (2008 and 2009) of mercury levels includes water location of fish, fish species, collection date and mercury content of fish sample. The patterns of mercury levels in the fish species as well as locations provide knowledge for further investigations. A research area for future studies is the composition of microbial communities in fish guts of varying levels of mercury.
As an abundant and cheap fossil energy source, natural gas has become a significant energy supply to support the United States’ economy. However, the large-scale extraction and utilization of natural gas also impose significant challenges on methane leakage. This problem is exacerbated by aging gas utility delivery systems, including interstate high-pressure pipelines, storage, and transmission facilities. This project aims to develop a cost-effective fiber optical sensing method that can perform multi-parameter real-time measurements of natural gas pipelines across long interrogation distances up to 100 km with 1-meter spatial resolution. This sensing tool can evaluate overall pipeline efficiency and reduce methane emissions for mid-stream methane infrastructures. To accomplish this objective, research and development efforts funded by this project have resulted in the following accomplishments: This project successfully has developed new functional sensory polymer materials using Metal-Organic Frameworks (MOFs) that can be coated on optical fiber through the reel-to-reel coating process. Functional polymer-coated optical fibers can perform sensitive methane detection through evanescence wave interaction and strain-based measurements to achieve 1% detection sensitivities. The new sensors fibers support both distributed measurements and multiplexed fiber sensors array for multi-point measurements. This project developed and optimized a new multi-core optical fiber that supports simultaneous and distributed measurements of strain and temperatures with 1-meter spatial resolutions across up to 100-km interrogation distance. This new fiber, combined with sensory polymercoated fiber, could perform both distributed temperature and methane detections. This project developed a new artificial intelligence big data algorithm approach that can effectively analyze high-resolution data harnessed by distributed fiber sensors to protect natural gas pipelines against external threats and detect internal defects induced by corrosion. Working with our industry partner, this project developed new optical fibers that support fiber sensor fabrications through polymer coating after the fibers are drawn. These new fibers eliminate the need for direct sensor fabrication when the fiber is fabricated on a fiber draw tower, which drastically expands fiber sensors' applicability. This research project has significantly advanced the distributed fiber sensing technology. It will dramatically increase the applicability and adaptability of distributed fiber sensors for a wide array of applications in energy, sustainability, and environmental science, including structural health monitoring of natural gas pipelines, oil infrastructures, hydrogen facilities, and environmental monitoring of carbon storage sites, water supply systems, and others.
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