The third phase of the Fifth International Ice Nucleation Workshop (FIN-03) was conducted at the Storm Peak Laboratory in Steamboat Springs, Colorado, in September 2015 to facilitate the intercomparison of instruments measuring ice-nucleating particles (INPs) in the field. Instruments included two online and four offline measurement systems for INPs, which are a subset of those utilized in the laboratory study that comprised the second phase of FIN (FIN-02). The composition of the total aerosols was characterized using the Particle Analysis by Laser Mass Spectrometry (PALMS) and Wideband Integrated Bioaerosol Sensor (WIBS) instruments, and aerosol size distributions were measured by a laser aerosol spectrometer (LAS). The dominant total particle compositions present during FIN-03 were composed of sulfates, organic compounds, and nitrates, as well as particles derived from biomass burning. Mineral-dust-containing particles were ubiquitous throughout and represented 67 % of supermicron particles. Total WIBS fluorescing particle concentrations for particles with diameters of > 0.5 mu m were 0.04 +/- 0.02 cm-3 (0.1 cm-3 highest; 0.02 cm-3 lowest), typical of the warm season in this region and representing approximate to 9 % of all particles in this size range as a campaign average. The primary focus of FIN-03 was the measurement of INP concentrations via immersion freezing at temperatures > -33 degrees C. Additionally, some measurements were made in the deposition nucleation regime at these same temperatures, representing one of the first efforts to include both mechanisms within a field campaign. INP concentrations via immersion freezing agreed within factors ranging from nearly 1 to 5 times on average between matched (time and temperature) measurements, and disagreements only rarely exceeded 1 order of magnitude for sampling times coordinated to within 3 h. Comparisons were restricted to temperatures lower than -15 degrees C due to the limits of detection related to sample volumes and very low INP concentrations. Outliers of up to 2 orders of magnitude occurred between -25 and -18 degrees C; a better agreement was seen at higher and lower temperatures. Although the 5-10 factor agreement of INP measurements found in FIN-03 aligned with the results of the FIN-02 laboratory comparison phase, giving confidence in progress of this measurement field, this level of agreement still equates to temperature uncertainties of 3.5 to 5 degrees C that may not be sufficient for numerical cloud modeling applications that utilize INP information. INP activity in the immersion-freezing mode was generally found to be an order of magnitude or more, making it more efficient than in the deposition regime at 95 %-99 % water relative humidity, although this limited data set should be augmented in future efforts. To contextualize the study results, an assessment was made of the composition of INPs during the late-summer to early-fall period of this study inferred through comparison to existing ice nucleation parameterizations and through measurement of the influence of thermal and organic carbon digestion treatments on immersion-freezing ice nucleation activity. Consistent with other studies in continental regions, biological INPs dominated at temperatures of > -20 degrees C and sometimes colder, while arable dust-like or other organic-influenced INPs were inferred to dominate below -20 degrees C.

Atmospheric brown carbon (BrC) from wildfires is a key component of light-absorbing carbon that significantly contributes to global radiative forcing, but its atmospheric evolution and lifetime remain poorly understood. In this study, we investigate BrC evolution by synthesizing data from one laboratory campaign and four aircraft campaigns spanning diverse spatial scales across North America. To estimate initial conditions for evaluating plume evolution, we develop a method to parametrize the emission ratios of BrC and other species using commonly measured inert tracers, acetonitrile and hydrogen cyanide. The evolution of BrC absorption in the free troposphere is characterized as a function of hydroxyl radical (OH) exposure, yielding an effective photochemical rate constant of 9.7-1.6+4.8 × 10-12 cm3 molecule-1 s-1. The relatively slow reaction rate results in small BrC decay within the first few hours after emission, making it difficult to distinguish from source variability. This helps explain the absence of clear evolutionary trends in near-field studies. Assuming an OH concentration of 1.26 × 106 molecules cm-3, this rate constant corresponds to an e-folding lifetime of approximately 23 h. After extensive photooxidation (OH exposure ∼1012 molecules cm-3 s), 4 ± 2% of the emitted BrC persists, representing a recalcitrant fraction with potential long-term climate impacts. These results improve our understanding of BrC variability and photochemical processing and provide critical constraints for modeling its impacts on climate.

The effect of food texture on the development of schedule-induced polydipsia was examined in six groups of rats (n = 8), each receiving one of six grades of food granulation. A seventh group received pellets. By the end of 15 sessions of FT 60-sec food delivery, rats receiving pellets and the coarser granulations had developed polydipsia. The volume of water drunk at asymptote by the remaining groups declined with decreased coarseness of the food. Ethological analyses of the behavioral repertoire of the rats during the fifteenth session showed that the polydipsic groups sustained their drinking throughout the session, rather than turning from ingestive to exploratory behaviors near the end of the session, as was the case with animals receiving finer granulations. The enhanced drinking induced by the coarser food texture was reciprocally related to the amount of time the animal spent with its head in the feeder hole during the period of maximum drinking. The results support the conclusion that the schedule-induced polydipsia traditionally demonstrated with pellets as the reinforcer is critically dependent on the fact that pellets are coarse in texture.

Since the pioneering experimental work of Bisiach et al. (1984) on deficits in sound localisation associated with unilateral brain lesions and visual neglect, a number of systematic investigations have examined auditory processing in visuospatial neglect patients. Evidence from a variety of experimental paradigms has revealed some auditory deficits in detection and identification tasks, during bilateral stimulation; plus localisation deficits for single sounds. These deficits emerge predominantly for contra-lesional sounds, although some auditory disturbances applying to both contra- and ipsilesional sounds have also been documented. Here we review evidence suggesting that some of these auditory deficits arise in relatively high-level stages of spatial processing. In addition, we present new analyses showing that auditory deficits in identification and localisation tasks often correlate with clinical measures of visual neglect, across a variety of different studies and tasks. This empirical relation suggests that a disturbance of multisensory spatial processing may often account for the joint auditory and visual spatial deficits in neglect patients, although rarer dissociations between the modalities should also be considered.

We investigated the changes in the size distribution, coating thickness, and mass absorption cross-section (MAC) of black carbon (BC) with aging and estimated the light absorption enhancement (Eabs) in the Asian outflow from airborne in-situ measurements during 2016 KORUS-AQ campaign. The BC number concentration decreased, but mass mean diameter increased with increasing altitude in the West Coast (WC) and Seoul Metropolitan Area (SMA), reflecting the contrast between freshly emitted BC-containing particles at the surface and more aged aerosol associated with aggregation during vertical mixing and transport. Contradistinctively, BC number and mass size distributions were relatively invariant with altitude over the Yellow Sea (YS) because sufficiently aged BC from eastern China were horizontally transported to all altitudes over the YS, and there are no significant sources at the surface. The averaged inferred MAC of refractory BC in three regions reflecting differences in their size distributions increased to 9.8 +/- 1.0 m(2) g(-1) (YS), 9.3 +/- 0.9 m(2) g(-1) (WC), and 8.2 +/- 0.9 m(2) g(-1) (SMA) as BC coating thickness increased from 20 nm to 120 nm. The absorption coefficient of BC calculated from the coating thickness and MAC were highly correlated with the filter-based absorption measurements with the slope of 1.16 and R-2 of 0.96 at 550 nm, revealing that the thickly coated BC had a large MAC and absorption coefficient. The Eabs due to the inferred coatings was estimated as 1.0-1.6, which was about 30% lower than those from climate models and laboratory experiments, suggesting that the increase in the BC absorption by the coatings in the Asian outflow is not as large as calculated in the previous studies. Organics contributed to the largest Eabs accounting for 69% (YS), 61% (WC), and 64% (SMA). This implies that organics are largely responsible for the lensing effect of BC rather than sulfates in the Asian outflow. (C) 2021 Elsevier B.V. All rights reserved.

We investigated the temporal and spatial variations of aerosol optical properties over the Korean peninsula during the KORUS-AQ (KORea–United States Air Quality) experiment with ground-based aerosol optical properties measured by remote and in-situ techniques. On the ground, AErosol RObotic NETwork (AERONET) and ground-level particulate matter (PM) concentration from air quality monitoring stations were used. From the NASA DC-8 research aircraft, the airborne Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research instrument (4STAR), an aerosol mass spectrometer (AMS), and a single particle soot photometer (SP2) provided aerosol information. Average hourly fine- and coarse-mode aerosol optical depth (AOD) and fine mode fraction (FMF), were divided into four clusters (background, Seoul Metropolitan Area (SMA), southwest, and east) representing different temporal/spatial variations; the results of those clusters were similar to the clustering results using PM from air quality monitoring stations. The downwind region of SMA was dominant by light-scattering fine-mode aerosols likely due to secondary aerosol formation with high fine-mode AOD and single scattering albedo compared to other regions, even Seoul. The fine-mode aerosols were more spatially homogeneous than coarse-mode aerosols, especially in the west-to-east direction, because fine-mode aerosols are usually transported on a regional scale by westerlies rather than emitted from local emission sources. However, the aerosol size distribution was spatially more homogeneous because of a consistent contribution of fine- and coarse-mode AOD to total AOD regardless of direction between the AERONET sites. During high-aerosol loading episodes, the temporal and spatial variations of aerosol optical properties were similar to those derived from 4STAR and ground-level PM concentrations, providing detailed information on aerosol behavior and characteristics. Using missed-approach flight segments (touchdown and take-off without a full-stop), investigation of diurnal variations over the SMA revealed a significant increase in AOD and Angstrom exponent (AE) in the afternoon compared to morning and noon, especially in the downwind region, because of more active secondary formation resulting from advected and/or emitted local pollutants and precursors. The diurnal variation of PM1 in the downwind region was similar to that of AOD; it was mainly increased during the day by secondary organic aerosols and ammonium nitrate due to large amounts of isoprene and meteorological conditions that supported secondary aerosol formation. Ammonium sulfate also partially led to increasing the PM1, but its behavior was unclear, because RH decreased during the day, which would imply the reduced aqueous-phase oxidation (the major pathway for sulfate production). Compared to the downwind region, ammonium nitrate and refractory black carbon decreased in Seoul because of a slightly decreased traffic volume, dissociation of ammonium nitrate, and increased boundary layer height according to meteorological conditions in the afternoon. The results of this study provide detailed information on aerosol behavior given the synergy of the various measurement platforms used. Along with the evidence of active photochemical reactions taking place in the downwind region, such data will be useful in formulating policies that improve air quality in Korea.

The contribution of heterogeneous ice nucleation to the formation of cirrus cloud ice crystals is still not well quantified. This results in large uncertainties when predicting cirrus radiative effects and their role in Earth's climate system. The goal of this case study is to simulate the composition, and thus activation conditions, of ice nucleating particles (INPs) to evaluate their contribution to heterogeneous cirrus ice formation in relation to homogeneous ice nucleation. For this, the regional model COSMO-Aerosols and Reactive Trace Gases (COSMO-ART) was used to simulate a synoptic cirrus cloud over Texas on 13 April 2011. The simulated INP composition was then compared to measured ice residual particle (IRP) composition from the actual event obtained during the NASA Midlatitude Airborne Cirrus Properties Experiment (MACPEX) aircraft campaign. These IRP measurements indicated that the dominance of heterogeneous ice nucleation was mainly driven by mineral dust with contributions from a variety of other particle types. Applying realistic activation thresholds and concentrations of airborne transported mineral dust and biomass-burning particles, the model implementing the heterogeneous ice nucleation parameterization scheme of Ullrich et al. is able to reproduce the overall dominating ice formation mechanism in contrast to the model simulation with the scheme of Phillips et al. However, the model showed flaws in reproducing the IRP composition.

Recently, the aerosol microphysics submodel MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, third generation) was introduced as a successor to MADE and MADE-in. It includes nine aerosol species and nine lognormal modes to represent aerosol particles of three different mixing states throughout the aerosol size spectrum. Here, we describe the implementation of the most recent version of MADE3 into the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model, including a detailed evaluation of a 10-year aerosol simulation with MADE3 as part of EMAC.We compare simulation output to station network measurements of near-surface aerosol component mass concentrations, to airborne measurements of aerosol mass mixing ratio and number concentration vertical profiles, to ground-based and airborne measurements of particle size distributions, and to station network and satellite measurements of aerosol optical depth. Furthermore, we describe and apply a new evaluation method, which allows a comparison of model output to size-resolved electron microscopy measurements of particle composition. Although there are indications that fine-mode particle deposition may be underestimated by the model, we obtained satisfactory agreement with the observations. Remaining deviations are of similar size to those identified in other global aerosol model studies.Thus, MADE3 can be considered ready for application within EMAC. Due to its detailed representation of aerosol mixing state, it is especially useful for simulating wet and dry removal of aerosol particles, aerosol-induced formation of cloud droplets and ice crystals as well as aerosol–radiation interactions. Besides studies on these fundamental processes, we also plan to use MADE3 for a reassessment of the climate effects of anthropogenic aerosol perturbations.

Due to low concentrations and chemical complexity, in situ observations of bioaerosol are geographically and temporally sparse, and this limits the accuracy of current emissions inventories. In this study, we apply a new methodology, including corrections for misidentification of mineral dust, to measurements of single particles over four airborne sampling campaigns to derive vertical profiles of bioaerosol over the continental United States. The new methodology is based on single-particle mass spectrometry (SPMS); it can extend historic datasets to include measurements of bioaerosol, it allows comparisons to other techniques, and it generally agrees with a global aerosol model. In the locations sampled, bioaerosols were at least a factor of 10 less abundant than mineral dust. Below 2 km, bioaerosol concentrations were measured between 6×103 and 2×104 m−3. Between 2 and 8 km, bioaerosol concentrations were between 0 and 2×104 m−3, and above 8 km, bioaerosol concentrations were between 0 and 1×103 m−3. Between 30 % and 80 % of single bioaerosol particles detected were internally mixed with dust. A direct comparison of the SPMS methodology with a co-located wideband integrated bioaerosol sensor (WIB) fluorescence sensor on a mountaintop site showed agreement to within a factor of 3 over the common size range.

The Forests gAses aeRosols Clouds Exploratory (FARCE) campaign was conducted in March–April 2015 on the tropical island of La Réunion. For the first time, several scientific teams from different disciplines collaborated to provide reference measurements and characterization of La Réunion vegetation, volatile organic compounds (VOCs), biogenic VOCs (BVOCs), (bio)aerosols and composition of clouds, with a strong focus on the Maïdo mountain slope area. The main observations obtained during this 2-month intensive field campaign are summarized. They include characterizations of forest structure, concentrations of VOCs and precursors emitted by forests, aerosol loading and optical properties in the planetary boundary layer (PBL), formation of new particles by nucleation of gas-phase precursors, ice-nucleating particles concentrations, and biological loading in both cloud-free and cloudy conditions. Simulations and measurements confirm that the Maïdo Observatory lies within the PBL from late morning to late evening and that, when in the PBL, the main primary sources impacting the Maïdo Observatory are of marine origin via the Indian Ocean and of biogenic origin through the dense forest cover. They also show that (i) the marine source prevails less and less while reaching the observatory; (ii) when in the PBL, depending on the localization of a horizontal wind shear, the Maïdo Observatory can be affected by air masses coming directly from the ocean and passing over the Maïdo mountain slope, or coming from inland; (iii) bio-aerosols can be observed in both cloud-free and cloudy conditions at the Maïdo Observatory; (iv) BVOC emissions by the forest covering the Maïdo mountain slope can be transported upslope within clouds and are a potential cause of secondary organic aerosol formation in the aqueous phase at the Maïdo Observatory; and (v) the simulation of dynamics parameters, emitted BVOCs and cloud life cycle in the Meso-NH model are realistic, and more advanced Meso-NH simulations should use an increased horizontal resolution (100 m) to better take into account the orography and improve the simulation of the wind shear front zone within which lies the Maïdo Observatory. Using various observations and simulations, this work draws up an inventory of the in situ studies that could be performed in La Réunion and at the Maïdo Observatory. It also aims to develop scientific collaborations and to support future scientific projects in order to better understand the forest–gas–aerosol–cloud system in an insular tropical environment.

Organic aerosols (OA) that strongly absorb solar radiation in the near-UV are referred to as brown carbon (BrC). The sources, evolution, and optical properties of BrC remain highly uncertain and contribute significantly to uncertainty in the estimate of the global direct radiative effect (DRE) of aerosols. Previous modeling studies of BrC optical properties and DRE have been unable to fully evaluate model performance due to the lack of direct measurements of BrC absorption. In this study, we develop a global model simulation (GEOS-Chem) of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental US (SEAC4RS and DC3). To the best of our knowledge, this is the first study to compare simulated BrC absorption with direct aircraft measurements. We show that BrC absorption properties estimated based on previous laboratory measurements agree with the aircraft measurements of freshly emitted BrC absorption but overestimate aged BrC absorption. In addition, applying a photochemical scheme to simulate bleaching/degradation of BrC improves model skill. The airborne observations are therefore consistent with a mass absorption coefficient (MAC) of freshly emitted biomass burning OA of 1.33 m2 g−1 at 365 nm coupled with a 1-day whitening e-folding time. Using the GEOS-Chem chemical transport model integrated with the RRTMG radiative transfer model, we estimate that the top-of-the-atmosphere all-sky direct radiative effect (DRE) of OA is −0.344 Wm−2, 10 % higher than that without consideration of BrC absorption. Therefore, our best estimate of the absorption DRE of BrC is +0.048 Wm−2. We suggest that the DRE of BrC has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.

During the SEAC(4)RS campaign in 2013, inflight measurements of light-absorption by aerosol in biomass burning and agriculture fire plumes were collected along with concomitant measurements of aerosol extinction, scattering, and black carbon mass concentration. Here, we compare three measurements of aerosol absorption coefficients: from a photoacoustic spectrometer (PAS), a particle soot absorption photometer (PSAP), and a continuous light absorption photometer (CLAP). Each of these absorption measurements was collected in three visible spectral regions: red, green, and blue (although the precise wavelength and bandwidth vary with each instrument). The absorption measurements were compared during the plumes, in the boundary layer, and in the free troposphere. The slopes from the comparison ranged from 0.6 to 1.24. For biomass burning plumes, the uncertainty in the absorption measurements translates into a range in single scattering albedos of 0.93-0.94 at a wavelength of 660 nm, 0.94-0.95 at 532 nm and 0.92-0.95 at 405 nm. Overall, the aerosol absorption instruments agreed within their stated accuracies. Comparisons with simultaneous measurements of refractive black carbon mass concentration (collected by a single particle soot photometer), were used to derive the mass absorption coefficients (MAC). For all wavelengths, the MAC was high by greater than a factor of three compared to the expected MAC for black carbon.

The aging of refractory black carbon (rBC) aerosol by sulfate-driven chemistry has been constrained in coal-fired power-plant plumes using the NOAA WP-3D research aircraft during the Southern Nexus (SENEX) study, which took place in the Southeastern US in June and July of 2013. A Single Particle Soot Photometer (SP2) determined the microphysical properties of rBC-containing particles including single-particle rBC mass and the presence and amount of internally-mixed non-rBC material, hereafter referred to as “coatings”. Most power-plant influenced air was associated with very slightly increased amounts of non-refractory material, likely sulfate internally mixed with the rBC, however this increase was statistically insignificant even after semi-Lagrangian exposure for up to 5 h. On average, the increase in coating thickness was 2 ± 4 nm for particles containing 3–5 fg rBC. Similarly, the number fraction of rBC-containing particles that could be identified as internally mixed was increased by plume chemistry by only 1.3 ± 1.3%. These direct measurements of microphysical aging of rBC-containing aerosol by power plant emissions constrain the enhancement of sulfate chemistry on both rBC’s column-integrated absorption optical depth, and rBC-containing aerosol’s ability to act as cloud condensation nuclei. Appling Mie and k-Köhler theories to the SP2 observations, permits the resulting effect on rBC ambient light-absorption to be capped at the 2–6% level.

Operational parameters for a single particle soot photometer (SP2) and a CETAC Marin-5 nebulizer were optimized for detection of particulates aerosolized from liquid samples. The sensitivity of nebulization efficiency on nebulizer input gas pressure, liquid sample flow rate, and alcohol doping of the sample were explored. The nebulization efficiency of the Marin-5 was found to be roughly independent of applied gas pressure once above a minimum pressure. The nebulization efficiency changed by approximate to 50% for an order of magnitude change in liquid sample flow. Doping the sample with isopropyl alcohol at a 1:1 ratio results in a approximate to 50% relative increase in nebulization efficiency over a broad range of liquid flows. These results should apply to all particulate materials in the size range studied. SP2 operational parameters including sheath and sample flow were explored to optimize detection of refractory black carbon (rBC) specifically via coupling to the nebulizer. The SP2 tested samples up to 5 cc s-1 with 100% detection of rBC in its size range of detection, with increased sample jet spread and corresponding lack of detected rBC in the air at higher flows, leading to a total undetected rBC mass fraction of approximate to 15% at 16 cc s-1. Varying sheath flow does not improve this result, which is significant because under reasonable Marin-5 operating conditions, the SP2 only samples a fraction of the total air flow out of the nebulizer. Recommended operational parameters for cases of sample with low rBC loadings are presented: first, when very little liquid sample is available; second, when considerable sample is available.(c) 2017 American Association for Aerosol Research