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  • 1
    In: Nature Communications, Springer Science and Business Media LLC, Vol. 14, No. 1 ( 2023-07-10)
    Abstract: Real-time surveillance of airborne SARS-CoV-2 virus is a technological gap that has eluded the scientific community since the beginning of the COVID-19 pandemic. Offline air sampling techniques for SARS-CoV-2 detection suffer from longer turnaround times and require skilled labor. Here, we present a proof-of-concept pathogen Air Quality (pAQ) monitor for real-time (5 min time resolution) direct detection of SARS-CoV-2 aerosols. The system synergistically integrates a high flow (~1000 lpm) wet cyclone air sampler and a nanobody-based ultrasensitive micro-immunoelectrode biosensor. The wet cyclone showed comparable or better virus sampling performance than commercially available samplers. Laboratory experiments demonstrate a device sensitivity of 77–83% and a limit of detection of 7-35 viral RNA copies/m 3 of air. Our pAQ monitor is suited for point-of-need surveillance of SARS-CoV-2 variants in indoor environments and can be adapted for multiplexed detection of other respiratory pathogens of interest. Widespread adoption of such technology could assist public health officials with implementing rapid disease control measures.
    Type of Medium: Online Resource
    ISSN: 2041-1723
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2023
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  • 2
    In: Nature Geoscience, Springer Science and Business Media LLC, Vol. 16, No. 8 ( 2023-08), p. 683-688
    Abstract: Wildfires emit large amounts of black carbon and light-absorbing organic carbon, known as brown carbon, into the atmosphere. These particles perturb Earth’s radiation budget through absorption of incoming shortwave radiation. It is generally thought that brown carbon loses its absorptivity after emission in the atmosphere due to sunlight-driven photochemical bleaching. Consequently, the atmospheric warming effect exerted by brown carbon remains highly variable and poorly represented in climate models compared with that of the relatively nonreactive black carbon. Given that wildfires are predicted to increase globally in the coming decades, it is increasingly important to quantify these radiative impacts. Here we present measurements of ensemble-scale and particle-scale shortwave absorption in smoke plumes from wildfires in the western United States. We find that a type of dark brown carbon contributes three-quarters of the short visible light absorption and half of the long visible light absorption. This strongly absorbing organic aerosol species is water insoluble, resists daytime photobleaching and increases in absorptivity with night-time atmospheric processing. Our findings suggest that parameterizations of brown carbon in climate models need to be revised to improve the estimation of smoke aerosol radiative forcing and associated warming.
    Type of Medium: Online Resource
    ISSN: 1752-0894 , 1752-0908
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2023
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    SSG: 16,13
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 15 ( 2021-08-09), p. 11843-11856
    Abstract: Abstract. Organic aerosol (OA) emissions from biomass burning have been the subject of intense research in recent years, involving a combination of field campaigns and laboratory studies. These efforts have aimed at improving our limited understanding of the diverse processes and pathways involved in the atmospheric processing and evolution of OA properties, culminating in their accurate parameterizations in climate and chemical transport models. To bring closure between laboratory and field studies, wildfire plumes in the western United States were sampled and characterized for their chemical and optical properties during the ground-based segment of the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field campaign. Using a custom-developed multiwavelength integrated photoacoustic-nephelometer spectrometer in conjunction with a suite of instruments, including an oxidation flow reactor equipped to generate hydroxyl (OH⚫) or nitrate (NO3⚫) radicals to mimic daytime or nighttime oxidative aging processes, we investigated the effects of multiple equivalent hours of OH⚫ or NO3⚫ exposure on the chemical composition and mass absorption cross-sections (MAC(λ)) at 488 and 561 nm of OA emitted from wildfires in Arizona and Oregon. We found that OH⚫ exposure induced a slight initial increase in absorption corresponding to short timescales; however, at longer timescales, the wavelength-dependent MAC(λ) decreased by a factor of 0.72 ± 0.08, consistent with previous laboratory studies and reports of photobleaching. On the other hand, NO3⚫ exposure increased MAC(λ) by a factor of up to 1.69 ± 0.38. We also noted some sensitivity of aerosol aging to different fire conditions between Arizona and Oregon. The MAC(λ) enhancement following NO3⚫ exposure was found to correlate with an enhancement in CHO1N and CHOgt1N ion families measured by an Aerodyne aerosol mass spectrometer.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2092549-9
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  • 4
    Online Resource
    Online Resource
    Copernicus GmbH ; 2019
    In:  Atmospheric Measurement Techniques Vol. 12, No. 2 ( 2019-02-28), p. 1365-1373
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 12, No. 2 ( 2019-02-28), p. 1365-1373
    Abstract: Abstract. Mass absorption cross section (MAC) measurements of atmospherically relevant aerosols are required to quantify their effect on Earth's radiative budget. Estimating aerosol light absorption from transmittance and/or reflectance measurements through filter deposits is an attractive option because of their ease of deployment in field settings, low cost, and the ability to revisit previously analyzed samples. These measurements suffer from artifacts that depend on a given filter measurement system and aerosol optics. Empirical correction algorithms are available for commercial instruments equipped with optically thick fiber filters, but optically thin filter media have not been characterized in detail. Here, we present empirical relationships between particle light absorption optical depth – measured using multiwavelength integrated photoacoustic spectrometers – and filter optical depth measurements for polytetrafluoroethylene (PTFE) membrane filter samples of carbonaceous aerosols generated from combustion of diverse biomass fuels and kerosene (surrogate for fossil fuel combustion). Through radiative transfer modeling, we assessed the suitability of three measures of filter-based optical depth for robustly describing particulate-phase light absorption over a range of single scattering albedo (SSA) values: (1) ODs – a measure of transmission of the fraction of incident radiation that is not backscattered by the filter system – which utilizes transmittance and reflectance of the sample side of the filter; (2) the commonly used ODc, which uses transmittance and reflectance of the clean side of the filter; and (3) ATN or the Beer–Lambert attenuation. Modeling results were also validated experimentally, with ODs showing the least variability around the mean in this multidimensional parameter space. We establish a simple, wavelength-independent formulation for calculating aerosol MAC and absorption coefficients from measurements of ODs. We find the ratio between in situ particulate absorption optical depth and ODs to be inversely proportional to aerosol SSA. Our findings underscore that ODs is a better optical depth measure than ODc for applying appropriate correction factors when estimating particle-phase light absorption from filter-based techniques.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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  • 5
    Online Resource
    Online Resource
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 13 ( 2019-07-11), p. 8817-8830
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 13 ( 2019-07-11), p. 8817-8830
    Abstract: Abstract. Recent studies have shown that organic aerosol (OA) could have a nontrivial role in atmospheric light absorption at shorter visible wavelengths. Good estimates of OA light absorption are therefore necessary to better estimate radiative forcing due to these aerosols in climate models. One of the common techniques used to measure OA light absorption is the solvent extraction technique from filter samples which involves the use of a spectrophotometer to measure bulk absorbance by the solvent-soluble organic fraction of particulate matter. Measured solvent-phase absorbance is subsequently converted to particle-phase absorption coefficient using scaling factors. The conventional view is to apply a correction factor of 2 to absorption coefficients obtained from solvent-extracted OA based on Mie calculations. The appropriate scaling factors are a function of biases due to incomplete extraction of organic carbon (OC) by solvents and size-dependent absorption properties of OA. The range for these biases along with their potential dependence on burn conditions is an unexplored area of research. Here, we performed a comprehensive laboratory study involving three solvents (water, methanol, and acetone) to investigate the bias in absorption coefficients obtained from solvent-extraction-based photometry techniques as compared to in situ particle-phase absorption for freshly emitted OA from biomass burning. We correlated the bias with OC∕TC (total carbon) mass ratio and single scattering albedo (SSA) and observed that the conventionally used correction factor of 2 for water and methanol-extracted OA might not be extensible to all systems, and we suggest caution while using such correction factors to estimate particle-phase OA absorption coefficients. Furthermore, a linear correlation between SSA and the OC∕TC ratio was also established. Finally, from the spectroscopic data, we analyzed the differences in absorption Ångström exponents (AÅE) obtained from solution- and particulate-phase measurements. We noted that AÅE from solvent-phase measurements could deviate significantly from their OA counterparts.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 6
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 15, No. 15 ( 2022-08-12), p. 4569-4583
    Abstract: Abstract. Measurement of light absorption of solar radiation by aerosols is vital for assessing direct aerosol radiative forcing, which affects local and global climate. Low-cost and easy-to-operate filter-based instruments, such as the Particle Soot Absorption Photometer (PSAP), that collect aerosols on a filter and measure light attenuation through the filter are widely used to infer aerosol light absorption. However, filter-based absorption measurements are subject to artifacts that are difficult to quantify. These artifacts are associated with the presence of the filter medium and the complex interactions between the filter fibers and accumulated aerosols. Various correction algorithms have been introduced to correct for the filter-based absorption coefficient measurements toward predicting the particle-phase absorption coefficient (Babs). However, the inability of these algorithms to incorporate into their formulations the complex matrix of influencing parameters such as particle asymmetry parameter, particle size, and particle penetration depth results in prediction of particle-phase absorption coefficients with relatively low accuracy. The analytical forms of corrections also suffer from a lack of universal applicability: different corrections are required for rural and urban sites across the world. In this study, we analyzed and compared 3 months of high-time-resolution ambient aerosol absorption data collected synchronously using a three-wavelength photoacoustic absorption spectrometer (PASS) and PSAP. Both instruments were operated on the same sampling inlet at the Department of Energy's Atmospheric Radiation Measurement program's Southern Great Plains (SGP) user facility in Oklahoma. We implemented the two most commonly used analytical correction algorithms, namely, Virkkula (2010) and the average of Virkkula (2010) and Ogren (2010)–Bond et al. (1999) as well as a random forest regression (RFR) machine learning algorithm to predict Babs values from the PSAP's filter-based measurements. The predicted Babs was compared against the reference Babs measured by the PASS. The RFR algorithm performed the best by yielding the lowest root mean square error of prediction. The algorithm was trained using input datasets from the PSAP (transmission and uncorrected absorption coefficient), a co-located nephelometer (scattering coefficients), and the Aerosol Chemical Speciation Monitor (mass concentration of non-refractory aerosol particles). A revised form of the Virkkula (2010) algorithm suitable for the SGP site has been proposed; however, its performance yields approximately 2-fold errors when compared to the RFR algorithm. To generalize the accuracy and applicability of our proposed RFR algorithm, we trained and tested it on a dataset of laboratory measurements of combustion aerosols. Input variables to the algorithm included the aerosol number size distribution from the Scanning Mobility Particle Sizer, absorption coefficients from the filter-based Tricolor Absorption Photometer, and scattering coefficients from a multiwavelength nephelometer. The RFR algorithm predicted Babs values within 5 % of the reference Babs measured by the multiwavelength PASS during the laboratory experiments. Thus, we show that machine learning approaches offer a promising path to correct for biases in long-term filter-based absorption datasets and accurately quantify their variability and trends needed for robust radiative forcing determination.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
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  • 7
    In: ACS Sensors, American Chemical Society (ACS), Vol. 8, No. 8 ( 2023-08-25), p. 3023-3031
    Type of Medium: Online Resource
    ISSN: 2379-3694 , 2379-3694
    Language: English
    Publisher: American Chemical Society (ACS)
    Publication Date: 2023
    detail.hit.zdb_id: 2843497-3
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  • 8
    In: Journal of Quantitative Spectroscopy and Radiative Transfer, Elsevier BV, Vol. 206 ( 2018-02), p. 392-398
    Type of Medium: Online Resource
    ISSN: 0022-4073
    Language: English
    Publisher: Elsevier BV
    Publication Date: 2018
    detail.hit.zdb_id: 1491916-3
    SSG: 11
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  • 9
    Online Resource
    Online Resource
    Informa UK Limited ; 2021
    In:  Aerosol Science and Technology Vol. 55, No. 5 ( 2021-05-04), p. 539-551
    In: Aerosol Science and Technology, Informa UK Limited, Vol. 55, No. 5 ( 2021-05-04), p. 539-551
    Type of Medium: Online Resource
    ISSN: 0278-6826 , 1521-7388
    Language: English
    Publisher: Informa UK Limited
    Publication Date: 2021
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    detail.hit.zdb_id: 787246-X
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