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Long-term measurements of the mass concentration of black carbon (BC) in the atmosphere (MBC) with well-constrained accuracy are indispensable to quantify its emission, transport, and deposition. The aerosol light absorption coefficient (babs), usually measured by a filter-based absorption photometer, including an Aethalometer (AE), is often used to estimate MBC. The measured babs is converted to MBC by assuming a value for the mass absorption cross section (MAC). Previously, we derived the MAC for AE (MAC (AE)) from measured babs and independently measured MBC values at two sites in the Arctic. MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). The accuracy of the COSMOS-derived MBC (MBC (COSMOS)) was within about 15%. Here, we obtained additional MAC (AE) measurements to improve understanding of its variability and uncertainty. We measured babs (AE) and MBC (COSMOS) at Alert (2018–2020), Barrow (2012–2022), Ny-Ålesund (2012–2019), and Pallas (2019–2022). At Pallas, we also obtained four-wavelength photoacoustic aerosol absorption spectrometer (PAAS-4λ) measurements of babs. babs (AE) and MBC (COSMOS) were tightly correlated; the average MAC (AE) at the four sites was 11.4 ± 1.2 m2 g−1 (mean ± 1σ) at 590 nm and 7.76 ± 0.73 m2 g−1 at 880 nm. The spatial variability of MAC (AE) was about 11% (1σ), and its year-to-year variability was about 18%. We compared MAC (AE) in the Arctic with values at mid-latitudes, measured by previous studies, and with values obtained by using other types of filter-based absorption photometer, and PAAS-4λ. Copyright © 2024 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

Here, we used a modified single-particle soot photometer (SP2) coupled with a concentric pneumatic nebulizer to measure the size-resolved number and mass concentrations of light-absorbing iron oxide aerosols (FeOx) in liquid water (CNFeOx and CMFeOx, respectively). The SP2 could selectively detect individual FeOx particles in mixed wüstite–fullerene soot laboratory samples and melted Arctic snow samples. The nebulizer efficiency for FeOx particles was about 50% within the 70–650 nm diameter range, as derived from the ratio of the volume of ammonium sulfate before and after extraction by the nebulizer and the size-resolved transmission efficiency in the nebulizer–SP2 sampling line. Uncertainty from the boundary lines empirically drawn to discriminate the scatterplots of FeOx and black carbon in the mixed wüstite–fullerene soot suspensions and snow samples was approximately 3.0% and 10%, respectively. Overall uncertainty in total CNFeOx and CMFeOx (220–1400 nm) was approximately 19% and 18%, respectively. After storage at 4 °C for 16 months, the FeOx particle size distributions in melted Arctic snow had remained stable, and CNFeOx and CMFeOx had changed by less than 19% and 1.0%, on average, respectively. Most of the FeOx on dust particles measured by this system was estimated to be in the diameter range smaller than 1000 nm, considering the nebulizer efficiency for dust particles. The high accuracy of the CNFeOx and CMFeOx measurements will help to improve our quantitative understanding of the wet deposition of FeOx and provide more accurate estimates of the effects of FeOx on snow surface albedo. [ABSTRACT FROM AUTHOR]

Long-term measurements of black carbon (BC) aerosols by filter-based absorption photometers with a heated inlet (COSMOS) in different regions have been useful in elucidating spatial variations and radiative impacts of BC. Evaluations of mass concentrations of BC (MBC) measured by the COSMOS have been made by our previous studies through comparisons with other measurement techniques. However, how variations in the microphysical properties of BC and the co-existing light scattering aerosols affect the COSMOS measurements should be evaluated in more detail. In this study, we assessed these potential effects under various field environments in the Arctic and in the East Asia. From the slopes of the correlation plots between the MBC values measured by the COSMOS and a single-particle soot photometer, the average accuracy of the COSMOS was estimated as ∼10% in the MBC range 1–3000 ng m−3. On an hourly basis, the estimated sensitivity of the COSMOS MBC values to the changes in the BC size distributions was less than 10%, within the typical variabilities of BC size at individual observation sites. The COSMOS measurements depended little on the mixing states of BC and the concentrations of co-existing light scattering aerosols, except in the maritime air masses of East Asia, where the relative abundance of sea salt to BC was very high. The MBC measured by COSMOS also well agreed with elemental carbon measurements. Our results demonstrate the high reliability of COSMOS measurements under various environments. Copyright © 2019 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

We developed an improved technique for measuring the size distribution of black carbon (BC) particles suspended in liquid water to facilitate quantitative studies of the wet deposition of BC. The measurement system, which consists of a nebulizer and a single-particle soot photometer, incorporates two improvements into the system that we developed earlier. First, we extended the upper limit of the detectable BC size from 0.9 μm to about 4.0 μm by modifying the photo-detector for measuring the laser-induced incandescence signal. Second, we introduced a pneumatic nebulizer (Marin-5) with a high extraction efficiency (∼50.0%) that was independent of particle diameter up to 2.0 μm. For BC mass concentrations less than 70 μg L−1, we experimentally showed that the diameters of BC particles did not appreciably change during the Marin-5 extraction process, consistent with theoretical calculations. Finally, we demonstrated by laboratory experiments that the size distributions of ambient BC particles changed little during their growth into cloud droplets under supersaturation of water vapor. Using our improved system, we measured the size distributions of BC particles simultaneously in air and rainwater in Tokyo during summer 2014. We observed that the size distributions of BC particles in rainwater shifted to larger sizes compared with those observed in ambient air, indicating that larger BC particles in air were removed more efficiently by precipitation. Copyright © 2016 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

Copyright © 2016 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

Accurate and time-resolved measurement of the size of water droplets is a prerequisite for the study of the microphysical processes of cloud formation by using an expansion chamber. We developed a droplet sizing method that uses color images of coronae observed under illumination of a white-light beam, also known as the corona-imaging colorimetry (CIC) method. In the CIC method, RGB data from images obtained by a commercial digital camera are converted into standard colorimetric parameters. The droplet size is estimated by optimizing the agreement of the measured colorimetric parameters with those estimated from Mie theory. For polystyrene latex spheres suspended in water, the particles size estimated by the CIC method agrees to within 2% of the predetermined value. We apply this method to the time-resolved measurement of the size of water droplets formed in an expansion chamber. The CIC method is technically simple and enables accurate and instantaneous measurements of the size of droplets with diameters larger than about 10 μm, which is the typical size of cloud droplets that form in the atmosphere. Copyright 2013 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

We conducted a detailed evaluation of a method for measuring the mass concentrations and size distributions of black carbon (BC) particles in rainwater and snow. The method uses an ultrasonic nebulizer (USN) and a single particle soot photometer (SP2). The USN disperses sample water into micron-size droplets at a constant rate and then dries them to release BC particles into the air. The masses of individual BC particles are measured by the SP2, using the laser-induced incandescence technique. The loss of BC particles during the extraction from liquid water to air depends on their sizes. We determined the size-dependent extraction efficiency using polystyrene latex (PSL) spheres with 12 different diameters between 107 and 1025 nm. The PSL concentrations in water were measured by the light extinction at 532 nm. The extraction efficiency of the USN showed a broad maximum of about 10% in the diameter range 200–500 nm and decreased substantially at larger sizes. The accuracy and reproducibility of the measured mass concentration of BC in sample water after long-term storage were about ±25% and ±35%, respectively. We tested the method by analyzing rainwater and surface snow samples collected in Okinawa and Sapporo, respectively. The measured number size distributions of BC in these samples showed negligible contributions of BC particles larger than 300 nm to the total number of BC particles. A dominant fraction of BC mass in these samples was observed in the diameter range 100–500 nm. Copyright 2013 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

Reducing uncertainties associated with measurements of black carbon (BC) particles is critical for improved quantification of their impacts on climate and health. We compared BC measurements using a continuous soot-monitoring system (COSMOS) and a multi-angle absorption photometer (MAAP) to assess their uncertainties. We found that measurements by COSMOS and MAAP instruments correlate strongly to each other, and their hourly ratio showed minimal temporal variations, but the MAAP values were systematically higher by a factor of 1.56 ± 0.19 (1σ), based on simultaneous observations on Fukue, a remote island in Japan, for about a year. This factor was almost independent of the air mass origins and seasons. Measurements in central Tokyo for about 2 months also yielded a similar relationship, with a systematic difference factor of ∼1.8. It is likely that the systematic differences are caused by differences in the conditions/protocols in the thermal/optical BC determinations used for calibration of each optical instrument. Based on results from the COSMOS instrument calibrated using an elemental carbon and organic carbon analyzer with thermal/optical transmittance correction, the MAAP absorption cross section (6.6 m2 g−1) needs to be systematically increased to 10.3 m2 g−1 at 639 nm for Fukue when b abs values derived from the built-in software are used. Small temporal fluctuations in the ratios of MAAP-derived BC to COSMOS-derived BC were possibly caused by humidity effects and temporal variations in the optical properties of the measured particles. For MAAP, we also found that low filter-transmittance (0.2–0.5) could either increase or decrease the BC reading. The current best recommendations with the MAAP instrument are to use an increased cross section, to use data with high filter-transmittance (>0.5) only, and to control humidity. Copyright 2012 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

We make detailed evaluations of a method of measuring the mass concentration and size distribution of black carbon (BC) particles suspended in water for the purpose of application to rainwater samples. Water samples were aerosolized with an ultrasonic nebulizer. Generated water droplets were dried in order to extract airborne BC particles. The mass of each BC particle was then measured by a Single Particle Soot Photometer (SP2), based on the laser-induced incandescence technique. Under the optimized operating conditions of our measurement system, the overall efficiency of the extraction of BC particles from rainwater was determined to be 11.4% ± 0.83% by mass, resulting in a total uncertainty of about ±20% for the measurement of the BC concentration in rainwater. The change in efficiency due to water-soluble species was found to be negligibly small for rainwater samples analyzed in this study. The determination of the efficiency by using standard BC solutions was necessary at an appropriate frequency because changes in the overall conditions of the system lead to changes in the efficiency in the long term. The size of BC particles in rainwater can be overestimated because of the coagulation of BC particles in the process of extraction by the nebulizer. This effect increased with the increase in BC concentration in rainwater. The effect can be minimized by dilution of rainwater samples by pure water. The volume of a rainwater sample required for BC measurement was less than 5 mL, enabling measurement for weak rain or highly time-resolved measurements during each rain event. [ABSTRACT FROM AUTHOR]

We used a single-particle soot photometer (SP2) to measure the mass of individual black carbon (BC) particles down to ∼ 0.5 fg by means of laser-induced incandescence with an intra-cavity, continuous-wave laser. The incandescence of nine different types of BC samples was investigated to provide a physical basis for choosing appropriate BC materials for SP2 calibration. We estimated the vaporization temperatures of these BC samples from the spectral dependence of incandescence at the limit of the small size parameter x, for which spectral dependence of emissivity is known a priori. The vaporization temperatures differed by less than 2.2% among the samples. For the x < 1 regime of particle size, the peak amplitude of the incandescence signal measured by the SP2 was linearly proportional to the particle mass. The slopes of such linear proportionality were positively correlated with | (m2-1)/(m2+2)|, where the m is the complex refractive index of the BC particle. For particles in which x > 1, the rate of increase in the peak amplitude of the incandescence signal with increasing particle mass was negatively correlated with the compactness of particle shape, consistent with the theoretical prediction of emissivity, which accounts for particle shape. The incandescence-BC mass relationships were similar between fullerene soot and ambient soot sampled in Tokyo, thus suggesting that fullerene soot is a suitable calibration standard for SP2 measurements of ambient soot. [ABSTRACT FROM AUTHOR]

Laboratory experiments and theoretical calculations were made to characterize the performance of a Single Particle Soot Photometer (SP2) manufactured by Droplet Measurement Technologies (DMT), which was designed to measure the mass and the mixing state of individual black carbon (BC) or elemental carbon (EC) particles, based on the laser-induced incandescence (LII) technique. In this study, graphite was used as a surrogate of EC. Graphite particles with mass equivalent diameters of 110-200 nm were layered with organic liquids (glycerol and oleic acid) to produce coated graphite with diameters up to 650-800 nm. These were sampled by the SP2 to measure the waveforms (i.e., time development) of the LII and scattering signals. The peak temperature and the peak LII signal of graphite particles were independent of the coating thickness or the coating material to within experimental errors. These results indicate that the mass of EC can be measured by using peak LII signal without interference by the coating conditions. It was also shown that the difference between the times of the scattering and LII peaks can be used as an indicator of coating on EC with thicknesses larger than about 100-200 nm. LII and scattering waveforms were calculated using a newly developed theoretical model that takes into account the physical processes controlling the temperature and evaporation rate of the coated graphite particle in the laser beam. The calculations reproduced the general features of observed waveforms of LII and scattering signals, providing a firm theoretical basis for the interpretation of the SP2 data. [ABSTRACT FROM AUTHOR]