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Understanding Aitken Mode Aerosol Variability over the Southern Ocean and Antarctica: Insights from Cloud Condensation Nuclei Data
Aitken mode aerosol particles play an important role influencing cloud properties and sustenance, acting as a reservoir of potential cloud condensation nuclei against precipitation scavenging. However, there is limited data on Aitken mode aerosols. In this study, we develop a method to estimate Aitken mode aerosol concentrations and size distribution using cloud condensation nuclei measurements (CCN) and κ-Köhler theory. The performance of this method is evaluated using scanning mobility particle sizer (SMPS) data from recent field campaigns to demonstrate its skills and applicability. The method reasonably estimates Aitken- and accumulation-mode aerosol concentrations, achieving correlations of 0.7–0.9 with only modest biases (mean fractional bias within ±23% for Aitken mode and ±34% for accumulation-mode). This method is further applied to measurements collected over the Southern Ocean and Antarctica in recent years from multiple platforms, including ground sites, aircraft, and ships, to derive Aitken and accumulation-mode aerosol concentrations. Using the derived data, we examine the seasonal cycle, latitudinal variations, and vertical distribution of aerosols. Aitken mode aerosol concentrations are elevated over the Southern Ocean and Antarctica during the austral summer similar to the accumulation mode. In the austral summer, the free troposphere has more Aitken mode aerosols and fewer accumulation mode aerosols than the boundary layer, and thus likely serves as an important source of cloud-forming aerosol while also diluting the accumulation mode.
GoAmazon2014/15. Oxidation Flow Reactor Final Campaign Report
The primary goal of the Green Ocean Amazon (GoAmazon2014/5) field campaign was to measure and mechanistically understand the formation of particle number and mass in a region affected by large tropical rainforest biogenic emissions and sometimes anthropogenic influence from a large urban center. As part of the two intensive operational periods (IOPs) and in collaboration with Pacific Northwest National Laboratory (PNNL) and Harvard, the Jimenez Group proposed to deploy a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS), Thermal Denuder (TD), Scanning Mobility Particle Size (SMPS), two oxidation flow reactors (OFR; including supporting O 3 , CO/CO 2 /CH 4 , RH analyzers), and a high volume filter sampler (MCV) for the measurement of gas and aerosol chemical, physicochemical, and volatility properties. The two IOPs were conducted during the wet season (February to March, 2014) and dry season (August to October, 2014). This proposal was part of a collaborative proposal involving other university and government laboratories.
Correcting for filter-based aerosol light absorption biases at the Atmospheric Radiation Measurement program's Southern Great Plains site using photoacoustic measurements and machine learning
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.
Black Carbon at the Mt. Bachelor Observatory Field Campaign Report
This campaign was initiated to measure refractory black carbon (rBC, as defined in Schwarz et al. (2010)) at the Mt. Bachelor Observatory (MBO) using the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility single-particle soot photometer (SP2; unit 54). MBO is a high-elevation site located on the summit of Mt. Bachelor in central Oregon, USA (43.979°N, 121.687°W, 2,763 meters ASL). This site is operated by Professor Dan Jaffe’s group at the University of Washington Bothell and has been used continuously as an atmospheric observatory for the past 12 years (Jaffe et al., 2005; Gratz et al., 2014). The location of MBO allows frequent sampling of the free troposphere along with a wide array of plumes from regional and distant sources. MBO is currently supported with funding from the National Science Foundation (NSF) to the Principal Investigator (PI; D. Jaffe) via the project “Influence of Free Tropospheric Ozone and PM on Surface Air Quality in the Western U.S.” (#1447832) covering the period 03/15/2015 to 02/28/2018. The SP2 instrument from Droplet Measurement Technologies provides particle-resolved measurements of rBC mass loading, size and mass distributions, and mixing state. The SP2 was installed at MBO on 6/27/2016 and ran through 9/23/2016. Additional measurements at MBO during this campaign included carbon monoxide (CO), fine particulate matter (PM1), aerosol light scattering coefficients (σscat) at three wavelengths using a TSI nephelometer, aerosol absorption coefficients (σabs) with the Brechtel tricolor absorption photometer (TAP), aerosol number size distributions with a scanning mobility particle sizer spectrometer (SMPS), and black carbon (eBC) with an aethalometer. BC data from this campaign have been submitted to the ARM Data Archive. Black carbon (BC) is the predominant light-absorbing aerosol constituent in the atmosphere, and is estimated to exert a positive radiative forcing second only to CO 2 (Ramanathan and Carmichael, 2008). One of the largest sources of BC globally is biomass burning (BB). (Akagi et al., 2011; Andreae and Merlet, 2001; Bond et al., 2013; Bond et al., 2004; Reid et al., 2005b): a source that is likely to increase in the Western U.S. due to climate change (Dennison et al., 2014; Abatzoglon and Williams, 2016; Westerling et al., 2006). Given the likely increased role of BB aerosol in atmospheric forcing, we need to improve our understanding of the physical and optical properties of aged BB aerosol. During the SP2 deployment period at MBO we observed seven BB events, all of which originated from the Gap Fire in Northern California, which burned 33,867 acres in the Klamath National Forest (https://inciweb.nwcg.gov/incident/4997/). Heavy smoke plumes from this fire were transported to MBO from 8/29/2016 to 8/31/2016. We calculated back-trajectories using the National Oceanic and Atmospheric Administration (NOAA) Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model, version 4 (Draxler, 1999; Draxler and Hess, 1997, 1998; Stein et al., 2015) to confirm transport from the fire locations to MBO. We identified the fire locations using moderate resolution imaging spectroradiometer (MODIS) satellite-derived active fire counts (Justice et al., 2002). Transport time for all of the BB events ranged from 8 to 32 hours.
Enhanced information content for three-dimensional localization and tracking using the double-helix point spread function with variable-angle illumination epifluorescence microscopy
The signal-to-noise ratio (SNR) and three-dimensional localization precision of a double helix point spread function (DH-PSF) can be significantly improved by applying variable-angle illumination epifluorescence microscopy (VAI, also commonly known as “pseudo-TIRF” or “quasi-TIRF”). In this paper, we performed a quantitative analysis of the dependence of SNR and localization precision on the number of measured photons and the incident angle for static particles under both low (at a planar index-matched interface) and high (within a porous silica matrix) fluorescent background conditions. We found that under noisier imaging conditions, the SNR and localization precision obtained using VAI are up to fivefold and threefold greater, respectively, than those obtained using epi-illumination. Finally and moreover, we demonstrate that the combination of DH-PSF and VAI can significantly improve the accuracy of the measured diffusion coefficient for mobile particles, even at a relatively large distance (50 μm) from the boundary of the optical cell.
Particle motion on Mars inferred from the Viking lander cameras
Data from Viking lander cameras indicate fine particle mobility on the surface of Mars such as: probable ventifacts, rock-associated raised streaks, and particulate drifts. Peak wind directions inferred from Chryse and Utopia are roughly equal, and are consistant with those inferred by orbiter photography. A 24 deg systematic offset between: (1) the direction of rock-associated streaks in the Viking I landing site, and (2) Mariner 9 and Viking observations of crater-associated streaks is consistant with a Coriolis acceleration of particles entrained by high-velocity winds during the production of crater-associated streaks. It is suggested that if a large fraction of collision impact energy goes into deformation, strain, and rupture, a preferential destruction of the most easily saltated grains and a depletion of 15-micron diameter grains will be observed. Investigations of particulates dumped on the landing grid suggest that major saltation events took place between sols 96 and 207, caused by winds of greater than 50 meters/sec normalized to the top of the boundary layer.
Relative humidity effect on the formation of highly oxidized molecules and new particles during monoterpene oxidation
It has been widely observed around the world that the frequency and intensity of new particle formation (NPF) events are reduced during periods of high relative humidity (RH). The current study focuses on how RH affects the formation of highly oxidized molecules (HOMs), which are key components of NPF and initial growth caused by oxidized organics. The ozonolysis of α -pinene, limonene, and Δ 3 -carene, with and without OH scavengers, were carried out under low NO x conditions under a range of RH (from ~3 % to ~92 %) in a temperature-controlled flow tube to generate secondary organic aerosol (SOA). A Scanning Mobility Particle Sizer (SMPS) was used to measure the size distribution of generated particles, and a novel transverse ionization chemical ionization inlet with a high-resolution time-of-fight mass spectrometer detected HOMs. A major finding from this work is that neither the detected HOMs nor their abundance changed significantly with RH, which indicates that the detected HOMs must be formed from water-independent pathways. In fact, the distinguished OH - and O 3 -derived peroxy radicals ( RO 2 ), HOM monomers, and HOM dimers could mostly be explained by the autoxidation of RO 2 followed by bimolecular reactions with other RO 2 or hydroperoxy radicals ( HO 2 ), rather than from a water-influenced pathway like through the formation of a stabilized Criegee intermediate (sCI). However, as RH increased from ~3 % to ~92 %, the total SOA number concentrations decreased by a factor of 2–3 while SOA mass concentrations remained relatively constant. These observations show that, while high RH appears to inhibit NPF as evident by the decreasing number concentration, this reduction is not caused by a decrease in RO 2 -derived HOM formation. Possible explanations for these phenomena were discussed.
Chemical changes in thirdhand smoke associated with remediation using an ozone generator
Ozonation is a common remediation approach to eliminate odors from mold, tobacco and fire damage in buildings. Little information exists to: 1) assess its effectiveness; 2) provide guidance on operation conditions; and 3) identify potential risks associated with the presence of indoor ozone and ozonation byproducts. The goal of this study is to evaluate chemical changes in thirdhand smoke (THS) aerosols induced by high levels of ozone, in comparison with THS aerosols aged under similar conditions in the absence of ozone. Samples representing different stages of smoke aging in the absence of ozone, including freshly emitted secondhand smoke (SHS) and THS, were collected inside an 18-m 3 room-sized chamber over a period of 42 h after six cigarettes were consumed. The experiments involved collection and analysis of gas phase species including volatile organic compounds (VOCs), volatile carbonyls, semivolatile organic compounds (SVOCs), and particulate matter. VOC analysis was carried out by gas chromatography/mass spectrometry with a thermal desorption inlet (TD-GC/MS), and volatile carbonyls were analyzed by on-line derivatization with dinitrophenylhydrazine (DNPH), followed by liquid chromatography with UV/VIS detection. SVOCs were extracted from XAD-coated denuders and Teflon-coated fiberglass filters in the absence of ozone. In those extracts, tobacco-specific nitrosamines (TSNAs) and other SVOCs were analyzed by gas chromatography with positive chemical ionization-triple quadrupole mass spectrometric detection (GC/PCI-QQQ-MS), and polycyclic aromatic hydrocarbons (PAHs) were quantified by gas chromatography with ion trap mass spectrometric detection (GC/IT-MS) in selected ion monitoring mode. Particulate matter concentration was determined gravimetrically. In a second experiment, a 300 mg h -1 commercial ozone generator was operated during 1 h, one day after smoke was generated, to evaluate the remediation of THS by ozonation. VOCs and volatile carbonyls were analyzed before and after ozonation. Extracts from fabrics that were exposed in the chamber before and after ozonation as surrogates for indoor furnishings were analyzed by GC/IT-MS, and aerosol size distribution was studied with a scanning mobility particle sizer. Ozone concentration was measured with a photometric detector. An estimated 175 mg ozone reacted with THS after 1 h of treatment, corresponding to 58% of the total O 3 released during that period. Fabric-bound nicotine was depleted after ozonation, and the surface concentration of PAHs adsorbed to fabric specimens decreased by an order of magnitude due to reaction with ozone, reaching pre-smoking levels. These results suggest that ozonation has the potential to remove harmful THS chemicals from indoor surfaces. However, gas phase concentrations of volatile carbonyls, including formaldehyde, acetaldehyde and acetone were higher immediately after ozonation. Ultrafine particles (UFP, in most cases with size <60 nm) were a major ozonation byproduct. UFP number concentrations peaked shortly after ozonation ended, and remained at higher-than background levels for several hours. Based on these results, minimum re-entry times after ozone treatment were predicted for different indoor scenarios. Clearly defining re-entry times can serve as a practical measure to prevent acute exposures to ozone and harmful ozonation byproducts after treatment. This study evaluated potential benefits and risks associated with THS remediation using ozone, providing insights into this technology.
Aerosol emissions from water-lean solvents for post-combustion CO 2 capture
Advanced water-lean solvents (WLS) for post-combustion CO 2 capture have been gaining interest due to their ability to reduce the parasitic penalty from energy needed for solvent regeneration. Commercial implementation of these novel CO 2 capture technologies hinges on successful control of amine emissions. RTI conducted a parametric study of fundamental and operational variables influence on overall amine aerosol and vapor emissions from our water-lean solvent eCO 2 Sol™ using our 6-kW equivalent bench-scale gas absorption system. The parametric testing used a simulated flue gas with 15 % CO 2 , 2.3–4.2 % H 2 O, and 0–6 ppm sulfite (SO 3 ) to examine the impact of the presence of aerosols to the capture performance and amine emissions from the system. The SO 3 reacts with water in the flue gas to create H 2 SO 4 , which forms liquid aerosol droplets and provide nucleation sites for growth of aerosols. Scanning Mobility Particle Sizer and Aerodynamic Particle Sizer instruments monitored the aerosol particle size distribution. Parametric testing results suggested that the presence of the aerosols in the flue gas could increase the overall amine emissions by 10X compared to the baseline emissions from WLS’s vapor pressure. Principal component analysis (PCA) and projection to latent squares (PLS) developed models to predict the aerosol-based amine emissions from process data. The predictive PLS model had a correlation coefficient (Q 2 ) of 0.92 and could predict the aerosol-based emissions from the NAS process with ±15 % accuracy (average absolute deviation, AAD). The PLS regression model also identified key variables affecting aerosol-based emissions from WLS.
The Transport of Asian Dust and Combustion Aerosols and Associated Ozone to North America as Observed From a Mountaintop Monitoring Site in the California Coast Range
Aerosol and tropospheric ozone transport to North America has important implications for regional air quality and climate. We present data from Chews Ridge, a remote mountaintop site in California, in February–September 2012, which identifies separate Asian dust and Asian combustion aerosol signals and quantifies exogenous ozone. We use positive matrix factorization of size-fractionated aerosol X-ray fluorescence data and 206 Pb/ 207 Pb and 208 Pb/ 207 Pb isotope measurements to isolate aerosol signals of Asian origins and find good agreement between both types source attribution techniques. Power spectra of Asian dust and Asian combustion signals reveal two distinct peaks, one seasonal (~90 days) and one monthly (~25–30 days). Overall, 89% of the Asian dust signal occurs in March–May, compared with June–September, whereas only 51% of the Asian combustion signal occurs in March–May. Nearly half the Pb observed at Chews Ridge was derived from Asia (46%; 8.3% from Asian dust, 23% from Asian combustion, and 15% of the Asian Pb signal was not explained by the positive matrix factorization). A positive correlation between deseasonalized ozone concentrations and the Asian factors suggests that ozone is elevated by 6.3 ± 0.8 ppb due to transpacific transport. Scanning mobility particle size spectra were also measured from May to September and indicate that new particles are often produced and grow throughout the afternoon during onshore flow. We hypothesize that particle nucleation on the windward edge of the continent is an important source of new particles.
Quantitative probing of the fast particle motion during the solidification of battery electrodes
Synchrotron x-ray tomography represents one of the most powerful imaging techniques that can visualize the three-dimensional microstructural complexity with a high spatial resolution. To date, however, the temporal resolution of this technique has been handicapped by the intrinsic limitations in the data acquisition speed and the lack of a suitable data processing method. The present study aims to fundamentally resolve this challenge by implementing a data analysis method that is based on differentiating discrete tomography reconstruction from a continuous scan reconstruction. With this methodological development, we capture and quantify the particle motion during the solidification of battery electrodes and reveal the statistics of the dynamically evolving motion in the drying process, which has been challenging to resolve. We discover that the particle motion exhibits a strong dependence on its geometric location within a drying electrode. Our results also imply that the final electrode quality can be controlled by balancing the solvent evaporation rate and the particle mobility in the region close to the drying surface.
Optimizing protic ionic liquid electrolyte for pre-intercalated Ti 3 C 2 T x MXene supercapacitor electrodes
Electrical double-layer capacitors (EDLCs) are of increasing importance in energy storage from renewable sources. The properties of the electrode and electrolyte materials influence the energy and power densities of EDLCs. We examined the specific capacitance and ion dynamics of a protic ionic liquid confined in pre-intercalated Ti 3 C 2 T x MXene. Our electrochemical measurements demonstrated that the creation of a protic ionic liquid, 1-butyl-3-H-imidazolium bis(trifluoromethanesulfonyl)imide (BuIMH-NTf2), using a mixture of ionic liquid, 1-butyl imidazole (BuIM), and salt, bis(trifluoromethanesulfonyl)imide (HNTf2), in a ratio of 0.8:0.2 led to the optimal capacitance. Remarkably, quasi-elastic neutron scattering measurements revealed increased particle mobility at this composition, attributed to the more efficient accumulation of BuIMH + on the electrode surface. This deposit of additional ions results in fewer BuIM molecules away from the surface, enhancing their mobility due to reduced crowding. This composition-dependent electrochemical behavior will guide the formulation of more efficient protic ionic liquid systems, enabling faster ion transport in energy storage devices.
Heterogeneous Dynamics in Shear Thickening Colloids Revealed by Intrinsic Heterodyne Correlation Spectroscopy
Shear induced frictional networks have been proposed to be responsible for the emergence of discontinuous shear thickening (DST) in complex fluids. However, little experimental evidence exists to support this model directly. Here, in this study, using x-ray photon correlation spectroscopy (XPCS), we show the existence of an intrinsic heterodyne feature during shear cessation, which originates from the relative motion of mobile particles against an aggregated or jammed network induced by shear thickening. Upon removing the shear, the shear stress dissipates rather quickly in a two-step fashion, whereas the heterogeneous particle dynamics persist much longer with the relative velocity decaying slowly with time as 𝑡 −1 . More importantly, both continuous shear thickening (CST) and DST show similar heterodyne features, indicating the intrinsic mechanisms causing shear thickening are similar in nature
Intercomparison of Aerosol Instrumental Responses Using AEROTRAK, SMPS, and APS in a Simulated Building
In this work, three aerosol instruments were intercompared by using data collected from field campaigns in a simulated building environment during the last quarter of 2020 from October to December at Oak Ridge National Laboratory. The three aerosol instruments—AeroTrak Model 9110, Scanning Mobility Particle Spectrometer (SMPS) 3080L + 3025A, and Aerodynamic Particle Sizer (APS) 3320—were manufactured by TSI Inc. to perform in situ measurements of particle number concentration in the air. These instruments were co-located in one room in which an aerosol generator was used to produce a defined aerosol population for the instruments to sample and detect in each campaign. The SMPS measured aerosol particles with diameters from 0.01 to 0.7 µm, APS measured aerosol particles with diameters from 0.5 to 20 µm, and AeroTrak measured aerosol particles with diameters from 0.1 to 10 µm. The results suggest that although AeroTrak is fast and easy to use, it does not provide measurements comparable with those obtained by SMPS and APS. The differences in particle counts were orders of magnitude in size (i.e., the AeroTrak data were unreasonably small in the tested scenarios). The results clearly indicate that AeroTrak should not be used in ambient applications in which the level of particle concentration is expected to be high. This would cause difficulty to a campaign in which the dilution factor is unknow a priori. The high particle concentration could also lead to an erroneous aerosol size distribution (e.g., a bimodal size distribution was measured as opposed to a single-mode one). The number concentration limit that AeroTrak is expected to run reliably (i.e., with a counting coincidence error less than ±10%) is approximately three to four per cubic centimeter. This suggests that the instrument is best used in a clean room environment, not in an ambient or indoor application, such as the Flexible Research Platform campaigns.
Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area
Field studies in polluted areas over the last decade have observed large formation of secondary organic aerosol (SOA) that is often poorly captured by models. The study of SOA formation using ambient data is often confounded by the effects of advection, vertical mixing, emissions, and variable degrees of photochemical aging. An oxidation flow reactor (OFR) was deployed to study SOA formation in real-time during the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign in Pasadena, CA, in 2010. A high-resolution aerosol mass spectrometer (AMS) and a scanning mobility particle sizer (SMPS) alternated sampling ambient and reactor-aged air. The reactor produced OH concentrations up to 4 orders of magnitude higher than in ambient air. OH radical concentration was continuously stepped, achieving equivalent atmospheric aging of 0.8 days–6.4 weeks in 3 min of processing every 2 h. Enhancement of organic aerosol (OA) from aging showed a maximum net SOA production between 0.8–6 days of aging with net OA mass loss beyond 2 weeks. Reactor SOA mass peaked at night, in the absence of ambient photochemistry and correlated with trimethylbenzene concentrations. Reactor SOA formation was inversely correlated with ambient SOA and O x , which along with the short-lived volatile organic compound correlation, indicates the importance of very reactive ( τ OH ~ 0.3 day) SOA precursors (most likely semivolatile and intermediate volatility species, S/IVOCs) in the Greater Los Angeles Area. Evolution of the elemental composition in the reactor was similar to trends observed in the atmosphere (O : C vs. H : C slope ~ –0.65). Oxidation state of carbon (OSc) in reactor SOA increased steeply with age and remained elevated (OS C ~ 2) at the highest photochemical ages probed. The ratio of OA in the reactor output to excess CO (ΔCO, ambient CO above regional background) vs. photochemical age is similar to previous studies at low to moderate ages and also extends to higher ages where OA loss dominates. The mass added at low-to-intermediate ages is due primarily to condensation of oxidized species, not heterogeneous oxidation. The OA decrease at high photochemical ages is dominated by heterogeneous oxidation followed by fragmentation/evaporation. A comparison of urban SOA formation in this study with a similar study of vehicle SOA in a tunnel suggests the importance of vehicle emissions for urban SOA. Pre-2007 SOA models underpredict SOA formation by an order of magnitude, while a more recent model performs better but overpredicts at higher ages. Furthermore, these results demonstrate the value of the reactor as a tool for in situ evaluation of the SOA formation potential and OA evolution from ambient air.
Fast and sensitive measurements of sub-3 nm particles using Condensation Particle Counters For Atmospheric Rapid Measurements (CPC FARM)
New particle formation (NPF) is the atmospheric process whereby gas molecules react and nucleate to form detectable particles. NPF has a strong impact on Earth's radiative balance as it produces roughly half of global cloud condensation nuclei. However, the time resolution and sensitivity of current instrumentation are inadequate in measuring the size distribution of sub-3 nm particles, the particles critical for understanding NPF. Here we present the Condensation Particle Counters For Atmospheric Rapid Measurements (CPC FARM), a method to measure the concentrations of freshly nucleated particles. The CPC FARM consists of five CPCs operating in parallel, each configured to operate at different detectable particle sizes between 1–3 nm. This study explores two methods to calculate the size distribution from the differential measurements across the CPC channels. The performance of both inversion methods was tested against the size distribution measured by a pair of stepping particle mobility sizers (SMPSs) during an ambient air sampling study in Pittsburgh, PA. Observational results indicate that the CPC FARM is more accurate with higher time resolution and sensitivity in the sub-3 nm range compared to the SMPS.
CACTI: Best Estimate Aerosol Size Distribution by airborne measurements
These data were collected during the Cloud, Aerosol, and Complex Terrain Interactions (CACTI; https://www.arm.gov/research/campaigns/amf2018cacti ) field campaign in the Sierras de Córdoba mountain range of north-central Argentina as part of ARM Aerial Facility (AAF) deployment. The ARM Aerial Facility Gulfstream-1 was operated from Las Higueras Airport (IATA: RCU, ICAO: SAOC), Río Cuarto, Córdoba, Argentina, for the Intensive Observation Period (IOP) from Nov. 1 through Dec. 15, 2018. The G-1 aircraft performed 22 research flights over the first ARM Mobile Facility (AMF1) location in the Sierras de Córdoba mountain range to measure atmospheric state and turbulence, cloud water content and droplet size distributions, aerosol precursor gases, aerosol chemical composition and size distributions. The current data set presents Best Estimate Aerosol Size Distribution: a merged aerosol size distribution composed of the data from 5 sensors; three aerosol spectrometers: Scanning Mobility Particle Sizer (SMPS), Ultra-High Sensitivity Aerosol Spectrometer (UHSAS), and Passive Cavity Aerosol Spectrometer (PCASP); and two cloud probes: Cloud Aerosol Spectrometer (CAS) and Fast Cloud Droplet Probe (FCDP). The SMPS data were interpolated to 1 second from “native” time resolution of about 64 second to match all other probes.