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Aerosol absorption profiling is crucial for radiative transfer calculations and climate modelling. Here, we utilize the synergy of lidar with sun-photometer measurements to derive the absorption coefficient and single scattering albedo profiles during the ACTRIS-2 campaigns held in Germany, Greece and Cyprus. The remote sensing techniques are compared with in situ measurements in order to harmonize and validate the different methodologies and reduce the absorption profiling uncertainties.

Carbonaceous particles, such as soot, make up a notable fraction of atmospheric particulate matter and contribute substantially to anthropogenic climate forcing, air pollution, and human health impacts. Thermal–optical analysis (TOA) is one of the most widespread methods used to speciate carbonaceous particles and divides total carbon (TC) into the operationally defined quantities of organic carbon (OC; carbon that has evolved during slow heating in an inert atmosphere) and elemental carbon (EC). While multiple studies have identified fundamental scientific reasons for uncertainty in distinguishing OC and EC, far fewer studies have reported on between-laboratory reproducibility. Moreover, existing reproducibility studies have focused on complex atmospheric samples. The real-time instruments used for regulatory measurements of the mass concentration of aircraft engine non-volatile particulate matter (nvPM) emissions are required to be calibrated to the mass of EC, as determined by TOA of the filter-sampled emissions of a diffusion flame combustion aerosol source (DFCAS). However, significant differences have been observed in the calibration factor for the same instrument based on EC content determined by different calibration laboratories. Here, we report on the reproducibility of TC, EC, and OC quantified using the same TOA protocol, instrument model (Model 5L, Sunset Laboratory), and software settings (auto-split-point: Calc405) across five different laboratories and instrument operators. Six unique data sets were obtained, with one laboratory operating two instruments. All samples were collected downstream of an aircraft engine after treatment with a catalytic stripper to remove volatile organics. Between-laboratory contributions made up a majority of the within-filter uncertainties for EC and TC, even for these relatively well-controlled samples. Overall, expanded (k = 2) uncertainties due to measurement reproducibility correspond to 17 %, 15 %, and 13 % of the nominal values for EC, OC, and TC, respectively, and 7.3 % in the EC / TC ratio. These values are lower than previous studies, including atmospheric samples without volatile organic removal; therefore, they likely represent lower limits for the uncertainties of the TOA method. [ABSTRACT FROM AUTHOR]

It is necessary to measure the mixing states of light-absorbing carbon (LAC) particles to reduce uncertainties in climate forcing due to particulate from wildfires and biomass combustion. For refractory LAC (normally called refractory black carbon; rBC), such measurements can be made using the single particle soot photometer (SP2). The SP2 measures the incandescent mass of individual particles heated by a 1064 nm laser. The SP2 also monitors single-particle light scattering from rBC plus internally mixed material (e.g., coatings of volatile particulate matter). rBC mixing states can be estimated from SP2 measurements by combining the scattering and incandescence signals. This is the basis of the published methods known as (i) scattering–incandescence lag-time, (ii) leading-edge only (LEO), and (iii) normalized derivative methods. More recently, the tandem centrifugal particle mass analyzer–single particle soot photometer (CPMA-SP2) method has been developed. The CPMA-SP2 method does not rely on the SP2 scattering signals and, therefore truly measures the rBC mass fraction, with no assumptions regarding particle composition or morphology. In this study, we provide the first quantitative comparison of the light-scattering and CPMA-SP2 methods for measuring mixing state. We discuss the upper and lower limits of detection (in terms of both rBC and coatings), temporal resolution, role of counting statistics, and errors associated with the measurements. We use a data set of atmospheric particles sampled at a regional background site (Kamloops about 350 km northeast of Vancouver, British Columbia, Canada), where the majority of rBC was emitted by seasonal wildfires. In the overall comparison of measurement methods, the CPMA-SP2 method is found to have significantly better systematic uncertainties than the light-scattering methods for wildfire smoke. For example, the light-scattering methods could not quantify coatings on half of the rBC particles, because their light-scattering signals were below the SP2 detection limit. Consequently, the bias in SP2-only estimates of rBC mixing states depends on the size distribution of the rBC particles. Although more accurate, CPMA-SP2 measurements require significantly more time to acquire, whereas SP2-only light-scattering analyses (both LEO and lag-time) can provide near real-time qualitative information representing large rBC particles. [ABSTRACT FROM AUTHOR]

Soot aggregates form as open, fractal-like structures, but aged atmospheric particles are often observed to be restructured into more-compact shapes due to internal mixing ("coating"). This compaction has a major effect on the radiative properties of the aggregates, and may also influence their aerosol-cloud interactions, toxicity, and deposition in human lungs. Recent laboratory studies have presented conflicting arguments on whether this compaction occurs during condensation or during the evaporation of coatings. In this three-part study, we combine theory and experiments to explain these conflicting results. First, we review the surface-science literature and identify explicit mechanisms for condensation-compaction as well as evaporation-compaction. We also identify a mechanism for avoiding compaction during condensation, based on heterogeneous nucleation theory and the kinetic barriers to capillary formation. Second, we review the soot-restructuring literature and find clear evidence for both condensation- and evaporation-compaction, with condensation-compaction being the norm. Third, we present new experimental results where the capillary forces due to anthracene coatings were "switched on" or "switched off" by using solid or liquid phases during coating addition and removal. Consequently, we demonstrate condensation-compaction, evaporation-compaction, and no compaction, for the same soot source. Overall, our study indicates that soot particles will typically undergo compaction when internal mixing occurs by the condensation of liquid coatings, while compaction may be avoided when internal mixing occurs through coagulation or the gas-to-particle formation of solid or highly viscous coatings. Copyright © 2022 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]