L. M. Russell

New Mexico Institute of Mining and Technology, Socorro, New Mexico, United States

Are you L. M. Russell?

Claim your profile

Publications (219)664.04 Total impact

  • Lynn M. Russell
    [Show abstract] [Hide abstract]
    ABSTRACT: The Committee on “Geoengineering Climate: Technical Evaluation and Discussion of Impacts” was charged with the task of conducting a technical evaluation of a limited number of proposed geoengineering techniques, with this talk focusing on issues related to solar radiation management (SRM) or what is also termed albedo modification. The report comments generally on the potential impacts of deploying these technologies, including possible environmental, economic, and national security concerns. The study (1) evaluates what is currently known about the science of several selected example techniques, including potential risks and consequences (both intended and unintended), such as impacts, or lack thereof, on ocean acidification, (2) describes what is known about the viability for implementation of the proposed techniques including technological and cost considerations, (3) explains other geoengineering technologies that have been proposed (beyond the selected examples), and (4) identifies future research needed to provide a credible scientific underpinning for future discussions. The study also discusses historical examples of related technologies (e.g., cloud seeding and other weather modification) for lessons that might be learned about societal reactions, examines what international agreements exist which may be relevant to the experimental testing or deployment of geoengineering technologies, and briefly explores potential societal and ethical considerations related to geoengineering. This study is intended to provide a careful, clear scientific foundation that informs ethical, legal, and political discussions surrounding geoengineering. This study was sponsored by the U.S. intelligence community, the National Oceanic and Atmospheric Administration, the National Aeronautics and Space Administration, the Department of Energy, and the National Academies.
    American Association for the Advancement of Science 2014 Annual Meeting; 02/2015
  • [Show abstract] [Hide abstract]
    ABSTRACT: The sources and composition of atmospheric marine aerosol particles (aMA) have been investigated with a range of physical and chemical measurements from open-ocean research cruises. This study uses the characteristic functional group composition (from Fourier transform infrared, or FTIR, spectroscopy) of aMA from five ocean regions to show that: (i) The organic functional group composition of aMA that can be identified as mainly atmospheric primary marine (ocean-derived) aerosol particles (aPMA) is 65 ± 12% hydroxyl, 21 ± 9% alkane, 6 ± 6% amine, and 7 ± 8% carboxylic acid functional groups. Contributions from photochemical reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles from bubbled seawater (gPMA, which has 55 ± 14% hydroxyl, 32 ± 14% alkane, and 13 ± 3% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the gPMA remained nearly constant over a broad range of chlorophyll-a concentrations, the gPMA alkane group fraction appeared to increase with chlorophyll-a concentrations (r =0.66). gPMA from productive seawater had a larger fraction of alkane functional groups (42 ± 9%) compared to gPMA from non-productive seawater (22 ± 10%), perhaps due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group peak location is closer to that of polysaccharides. This may result from the larger saccharides preferentially remaining in the seawater during gPMA and aPMA production.
    Journal of Geophysical Research: Atmospheres. 10/2014;
  • [Show abstract] [Hide abstract]
    ABSTRACT: Although isocyanic acid (HNCO) may cause a variety of health issues via protein carbamylation and has been proposed as a key compound in smoke related health issues, our understanding of the atmospheric sources and fate of this toxic compound is currently incomplete. To address these issues, a field study was conducted at Mt. Soledad, La Jolla, CA to investigate partitioning of HNCO to clouds and fogs using an Acetate Chemical Ionization Mass Spectrometer (Acid-CIMS) coupled to a ground-based Counterflow Virtual Impactor (CVI). The first field evidence of cloud partitioning of HNCO is presented, demonstrating that HNCO is dissolved in cloudwater more efficiently than expected based on the effective Henry's law solubility. The measurements also indicate evidence for a secondary, photochemical source of HNCO in ambient air at this site.
    Geophysical Research Letters. 09/2014;
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: The performance of the Weather Research and Forecasting regional model with chemistry (WRF-Chem) in simulating the spatial and temporal variations in aerosol mass, composition, and size over California is quantified using the extensive meteorological, trace gas, and aerosol measurements collected during the California Nexus of Air Quality and Climate Experiment (CalNex) and the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted during May and June of 2010. The overall objective of the field campaigns was to obtain data needed to better understand processes that affect both climate and air quality, including emission assessments, transport and chemical aging of aerosols, aerosol radiative effects. Simulations were performed that examined the sensitivity of aerosol concentrations to anthropogenic emissions and to long-range transport of aerosols into the domain obtained from a global model. The configuration of WRF-Chem used in this study is shown to reproduce the overall synoptic conditions, thermally driven circulations, and boundary layer structure observed in region that controls the transport and mixing of trace gases and aerosols. Reducing the default emissions inventory by 50% led to an overall improvement in many simulated trace gases and black carbon aerosol at most sites and along most aircraft flight paths; however, simulated organic aerosol was closer to observed when there were no adjustments to the primary organic aerosol emissions. We found that sulfate was better simulated over northern California whereas nitrate was better simulated over southern California. While the overall spatial and temporal variability of aerosols and their precursors were simulated reasonably well, we show cases where the local transport of some aerosol plumes were either too slow or too fast, which adversely affects the statistics quantifying the differences between observed and simulated quantities. Comparisons with lidar and in situ measurements indicate that long-range transport of aerosols from the global model was likely too high in the free troposphere even though their concentrations were relatively low. This bias led to an over-prediction in aerosol optical depth by as much as a factor of 2 that offset the under-predictions of boundary-layer extinction resulting primarily from local emissions. Lowering the boundary conditions of aerosol concentrations by 50% greatly reduced the bias in simulated aerosol optical depth for all regions of California. This study shows that quantifying regional-scale variations in aerosol radiative forcing and determining the relative role of emissions from local and distant sources is challenging during `clean' conditions and that a wide array of measurements are needed to ensure model predictions are correct for the right reasons. In this regard, the combined CalNex and CARES data sets are an ideal test bed that can be used to evaluate aerosol models in great detail and develop improved treatments for aerosol processes.
    Atmospheric Chemistry and Physics 09/2014; 14(18):10013-10060. · 5.51 Impact Factor
  • Source
  • [Show abstract] [Hide abstract]
    ABSTRACT: Biogenic lipids and polymers are surveyed for their ability to adsorb at the water–air interfaces associated with bubbles, marine microlayers and particles in the overlying boundary layer. Representative ocean biogeochemical regimes are defined in order to estimate local concentrations for the major macromolecular classes. Surfactant equilibria and maximum excess are then derived based on a network of model compounds. Relative local coverage and upward mass transport follow directly, and specific chemical structures can be placed into regional rank order. Lipids and denatured protein-like polymers dominate at the selected locations. The assigned monolayer phase states are variable, whether assessed along bubbles or at the atmospheric spray droplet perimeter. Since oceanic film compositions prove to be irregular, effects on gas and organic transfer are expected to exhibit geographic dependence as well. Moreover, the core arguments extend across the sea–air interface into aerosol–cloud systems. Fundamental nascent chemical properties including mass to carbon ratio and density depend strongly on the geochemical state of source waters. High surface pressures may suppress the Kelvin effect, and marine organic hygroscopicities are almost entirely unconstrained. While bubble adsorption provides a well-known means for transporting lipidic or proteinaceous material into sea spray, the same cannot be said of polysaccharides. Carbohydrates tend to be strongly hydrophilic so that their excess carbon mass is low despite stacked polymeric geometries. Since sugars are abundant in the marine aerosol, gel-based mechanisms may be required to achieve uplift. Uncertainties distill to a global scale dearth of information regarding two dimensional kinetics and equilibria. Nonetheless simulations are recommended, to initiate the process of systems level quantification.
    Environmental Research Letters 06/2014; 9(6):064012. · 3.58 Impact Factor
  • [Show abstract] [Hide abstract]
    ABSTRACT: An aerosol-enabled globally driven regional modeling system has been developed by coupling the National Center for Atmospheric Research's Community Atmosphere Model version 5 (CAM5) with the Weather Research and Forecasting model with chemistry (WRF-Chem). In this modeling system, aerosol-enabled CAM5, a state-of-the-art global climate model is downscaled to provide coherent meteorological and chemical boundary conditions for regional WRF-Chem simulations. Aerosol particle emissions originating outside the WRF-Chem domain can be a potentially important non-local aerosol source. As a test case, the potential impacts of non-local forest fire aerosols on regional precipitation and radiation were investigated over the Northeastern United States during the summer of 2004. During this period, forest fires in Alaska and Western Canada lofted aerosol particles into the mid-troposphere, which were advected across the United States. WRF-Chem simulations that included non-local biomass burning aerosols had domain-mean aerosol optical depths that were nearly three times higher than those without, which reduced peak downwelling domain-mean shortwave radiation at the surface by ~25 W m-2. In this classic twin experiment design, adding non-local fire plume led to near-surface cooling and changes in cloud vertical distribution, while variations in domain-mean cloud liquid water path were negligible. The higher aerosol concentrations in the simulation with the fire plume resulted in a ~10% reduction in domain-mean precipitation coincident with an ~8% decrease in domain-mean CAPE. A suite of simulations was also conducted to explore sensitivities of meteorological feedbacks to the ratio of black carbon to total plume aerosols, as well as to overall plume concentrations. Results from this ensemble revealed that plume-induced near-surface cooling and CAPE reduction occur in a wide range of conditions. The response of moist convection was very complex because of strong thermodynamic internal variability.
    Journal of Geophysical Research: Atmospheres. 06/2014;
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: This study uses a century length pre-industrial climate simulation by the Community Earth System Model (CESM 1.0) to explore statistical relationships between dust, clouds and atmospheric circulation, and to suggest a semi-direct dynamical mechanism linking subtropical North Atlantic lower tropospheric cloud cover with North African dust transport. The length of the run allows us to account for interannual variability of North African dust emissions and transport in the model. CESM's monthly climatology of both aerosol optical depth and surface dust concentration at Cape Verde and Barbados, respectively, agree well with available observations, as does the aerosol size distribution at Cape Verde. In addition, CESM shows strong seasonal cycles of dust burden and lower tropospheric cloud fraction, with maximum values occurring during boreal summer, when a strong correlation between these two variables exists over the subtropical North Atlantic. Calculations of Estimated Inversion Strength (EIS) and composites of EIS on high and low downstream North Africa dust months during boreal summer reveal that dust is likely increasing inversion strength over this region due to both solar absorption and reflection. We find no evidence for a microphysical link between dust and lower tropospheric clouds in this region. These results yield new insight over an extensive period of time into the complex relationship between North African dust and North Atlantic lower tropospheric clouds, which has previously been hindered by spatiotemporal constraints of observations. Our findings lay a framework for future analyses using different climate models and sub-monthly data over regions with different underlying dynamics.
    Journal of Geophysical Research: Atmospheres. 06/2014;
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: The refractive index is a fundamental property controlling aerosol optical properties. Secondary organic aerosols have variable refractive indices, presumably reflecting variations in their chemical composition. Here, we investigate the real refractive indices (mr) and chemical composition of secondary organic aerosols (SOA) generated from the oxidation of α-pinene and limonene with ozone and NOx/sunlight at different HC/NOx ratios. Refractive indices were retrieved from polar nephelometer measurements using parallel and perpendicular polarized 532-nm light. Particle chemical composition was monitored with a high-resolution time-of-flight aerosol mass spectrometer (HR-Tof-AMS). For photochemically generated SOA, the values of refractive indices are consistent with prior results, and ranged from about 1.34 to 1.55 for limonene and from 1.44 to 1.47 for α-pinene, generally increasing as the particles grew. While AMS fragments are strongly correlated to the refractive index for each type of SOA, the relationships are in most cases quite different for different SOA types. Consistent with its wide range of refractive index, limonene SOA shows larger variations compared to α-pinene SOA for most parameters measured with the AMS, including H:C, O:C, f43 (m/z 43/organic), fC4H7+, and others. Refractive indices for α-pinene ozonolysis SOA also fell in narrow ranges; 1.43–1.45 and 1.46–1.53 for particles generated at 19–22 and 23–29°C, respectively, with corresponding small changes of f43 and H:C ratio and other parameters. Overall, H:C ratio, m/z 43 and 55 (C2H3O+, C4H7+) were the best correlated with refractive index for all aerosol types investigated. The relationships between mr and most fragments support the notion that increasing condensation of less oxygenated semivolatile species (with a possible role for a concomitant decrease in low refractive index water) is responsible for the increasing mrs observed as the experiments progress. However, the possibility that oligomerization reactions play a role cannot be ruled out.
    Aerosol Science and Technology 05/2014; 48(5). · 2.78 Impact Factor
  • [Show abstract] [Hide abstract]
    ABSTRACT: Observations during CalNex and Cal-Mex field campaigns at Bakersfield, Pasadena, Tijuana, and on board the R/V Atlantis show a substantial contribution of fossil fuel emissions to the ambient particle organic mass (OM). At least two fossil fuel combustion (FFC) factors with a range of contributions of oxidized organic functional groups were identified at each site and accounted for 60─88% of the total OM. Additional marine, vegetative detritus, and biomass burning or biogenic sources contribute up to 40% of the OM. Comparison of the FTIR spectra of four different unburned fossil fuels (gasoline, diesel, motor oil, and ship diesel) with PMF factors from ambient samples shows absorbance peaks from the fuels are retained in organic aerosols, with the spectra of all of the FFC factors containing at least three of the four characteristic alkane peaks observed in fuel standards at 2954, 2923, 2869 and 2855 cm−1. Based on this spectral similarity, we estimate the primary OM from FFC sources for each site to be 16─20%, with secondary FFC OM accounting for an additional 42─62%. Two other methods for estimating primary OM that use carbon monoxide (CO) and elemental carbon (EC) as tracers of primary organic mass were investigated, but both approaches were problematic for the CalNex and Cal-Mex urban sites because they were influenced by multiple emission sources that had site-specific and variable initial ratios to OM. For example, using the ΔPOM/ΔCO ratio of 0.0094 μg ppb V−1 proposed by other studies produces unrealistically high estimates of primary FFC OM of 55─100%.
    04/2014;
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: The performance of the Weather Research and Forecasting regional model with chemistry (WRF-Chem) in simulating the spatial and temporal variations in aerosol mass, composition, and size over California is quantified using measurements collected during the California Nexus of Air Quality and Climate Experiment (CalNex) and the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted during May and June of 2010. The extensive meteorological, trace gas, and aerosol measurements collected at surface sites and along aircraft and ship transects during CalNex and CARES were combined with operational monitoring network measurements to create a single dataset that was used to evaluate the one configuration of the model. Simulations were performed that examined the sensitivity of regional variations in aerosol concentrations to anthropogenic emissions and to long-range transport of aerosols into the domain obtained from a global model. The configuration of WRF-Chem used in this study is shown to reproduce the overall synoptic conditions, thermally-driven circulations, and boundary layer structure observed in region that controls the transport and mixing of trace gases and aerosols. However, sub-grid scale variability in the meteorology and emissions as well as uncertainties in the treatment of secondary organic aerosol chemistry likely contribute to errors at a primary surface sampling site located at the edge of the Los Angeles basin. Differences among the sensitivity simulations demonstrate that the aerosol layers over the central valley detected by lidar measurements likely resulted from lofting and recirculation of local anthropogenic emissions along the Sierra Nevada. Reducing the default emissions inventory by 50% led to an overall improvement in many simulated trace gases and black carbon aerosol at most sites and along most aircraft flight paths; however, simulated organic aerosol was closer to observed when there were no adjustments to the primary organic aerosol emissions. The model performance for some aerosol species was not uniform over the region, and we found that sulfate was better simulated over northern California whereas nitrate was better simulated over southern California. While the overall spatial and temporal variability of aerosols and their precursors were simulated reasonably well, we show cases where the local transport of some aerosol plumes were either too slow or too fast, which adversely affects the statistics regarding the differences between observed and simulated quantities. Comparisons with lidar and in-situ measurements indicate that long-range transport of aerosols from the global model was likely too high in the free troposphere even though their concentrations were relatively low. This bias led to an over-prediction in aerosol optical depth by as much as a factor of two that offset the under-predictions of boundary-layer extinction resulting primarily from local emissions. Lowering the boundary conditions of aerosol concentrations by 50% greatly reduced the bias in simulated aerosol optical depth for all regions of California. This study shows that quantifying regional-scale variations in aerosol radiative forcing and determining the relative role of emissions from local and distant sources is challenging during "clean" conditions and that a wide array of measurements are needed to ensure model predictions are correct for the right reasons. In this regard, the combined CalNex and CARES datasets are an ideal testbed that can be used to evaluate aerosol models in great detail and develop improved treatments for aerosol processes.
    Atmospheric Chemistry and Physics Discussions. 03/2014; 14(6):7187-7303.
  • [Show abstract] [Hide abstract]
    ABSTRACT: Physical and biogeochemical processes in seawater controlling primary marine aerosol (PMA) production and composition are poorly understood and associated with large uncertainties in estimated fluxes into the atmosphere. PMA production was investigated in the biologically-productive NE Pacific Ocean and in biologically-productive and oligotrophic regions of the NW Atlantic Ocean. Physicochemical properties of model PMA, produced by aeration of fresh seawater under controlled conditions, were quantified. Diel variability in model PMA mass and number fluxes was observed in biologically productive waters, increasing following sunrise and decreasing to pre-dawn levels overnight. Such variability was not seen in oligotrophic waters. Surfactant scavenging by aeration in the aerosol generator without replenishing the seawater in the reservoir during daytime reduced model PMA production in productive waters to nighttime levels but had no influence on production from oligotrophic waters. Results suggest bubble-plume interactions with sunlight-mediated biogenic surfactants in productive seawater significantly enhanced model PMA production.
    Geophysical Research Letters. 03/2014;
  • [Show abstract] [Hide abstract]
    ABSTRACT: The presence of a large fraction of organic matter in primary sea spray aerosol (SSA) can strongly affect its cloud condensation nuclei activity and interactions with marine clouds. Global climate models require new parameterizations of the SSA composition in order to improve the representation of these processes. Existing proposals for such a parameterization use remotely-sensed chlorophyll a concentrations as a proxy for the biogenic contribution to the aerosol. However, both observations and theoretical considerations suggest that existing relationships with chlorophyll a, derived from observations at only a few locations, may not be representative for all ocean regions. We introduce a novel framework for parameterizing the fractionation of marine organic matter into SSA based on a competitive Langmuir adsorption equilibrium at bubble surfaces. Marine organic matter is partitioned into classes with differing molecular weights, surface excesses, and Langmuir adsorption parameters. The classes include a lipid-like mixture associated with labile dissolved organic carbon (DOC), a polysaccharide-like mixture associated primarily with semi-labile DOC, a protein-like mixture with concentrations intermediate between lipids and polysaccharides, a processed mixture associated with recalcitrant surface DOC, and a deep abyssal humic-like mixture. Box model calculations have been performed for several cases of organic adsorption to illustrate the underlying concepts. We then apply the framework to output from a global marine biogeochemistry model, by partitioning total dissolved organic carbon into several classes of macromolecules. Each class is represented by model compounds with physical and chemical properties based on existing laboratory data. This allows us to globally map the predicted organic mass fraction of the nascent submicron sea spray aerosol. Predicted relationships between chlorophyll a and organic fraction are similar to existing empirical parameterizations, but can vary between biologically productive and non-productive regions, and seasonally within a given region. Major uncertainties include the bubble film thickness at bursting and the variability of organic surfactant activity in the ocean, which is poorly constrained. In addition, polysaccharides may enter the aerosol more efficiently than Langmuir adsorption would suggest. Potential mechanisms for include the formation of marine colloidal particles that may be more efficiently swept up by rising particles, and cooperative adsorption of polysaccharides with proteins or lipids. These processes may make important contributions to the aerosol, but are not included here. This organic fractionation framework is an initial step towards a closer linking of ocean biogeochemistry and aerosol chemical composition in Earth system models. Future work should focus on improving constraints on model parameters through new laboratory experiments or through empirical fitting to observed relationships in the real ocean and atmosphere, as well as on atmospheric implications of the variable composition of organic matter in sea spray.
    02/2014; 14(5).
  • [Show abstract] [Hide abstract]
    ABSTRACT: Breaking waves on the ocean surface generate air bubbles that scavenge organic matter from the surrounding sea water. When injected into the atmosphere, these bubbles burst, yielding sea spray aerosols enriched in organic matter, relative to the sea water. Downwind of plankton blooms, the organic carbon content of sea spray aerosol is weakly correlated with satellite-derived measurements of chlorophyll a levels, a measure of phytoplankton biomass. This correlation has been used in large-scale models to calculate the organic enrichment in sea spray aerosol. Here, we assess the relationship between the organic carbon content of sea water and freshly emitted sea spray aerosol in the presence and absence of plankton blooms in the North Atlantic Ocean and the coastal waters of California. The organic carbon content of freshly emitted sea spray aerosol was similar in all regions sampled, despite significant differences in seawater chlorophyll a levels. The proportion of freshly emitted aerosols that served as cloud condensation nuclei at a given supersaturation was also similar across sampling sites. The large reservoir of organic carbon in surface sea water remained relatively constant across the regions sampled, and independent of variations in chlorophyll a concentrations. We suggest that this reservoir is responsible for the organic carbon enrichment of freshly emitted sea spray aerosol, overwhelming any influence of local biological activity as measured by chlorophyll a levels.
    02/2014; 7(3).
  • [Show abstract] [Hide abstract]
    ABSTRACT: Atmospheric aerosols affect the Earth's energy balance by interacting directly with incoming solar radiation or indirectly by altering cloud properties by acting as cloud condensation nuclei (CCN). The interaction between aerosols and clouds remains the largest uncertainty in model predictions of future climate change in response to anthropogenic activity. The concentration of available CCN depends on aerosol size and chemical composition as well as ambient water vapor supersaturation. Therefore, supersaturation serves as the link between aerosol and cloud droplet number. The Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) included a targeted aircraft campaign off the coast of Monterey, California, in July and August 2011. The Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft made measurements of aerosol and cloud properties targeting three types of emissions in the stratocumulus-rich northeastern Pacific: smoke emissions from the R/V Point Sur, salt aerosol released by the Twin Otter, and emissions from cargo ships. In-cloud measurements sampled cloud residuals from behind a counterflow virtual impactor (CVI.) A cloud condensation nuclei (CCN) spectrometer (a Droplet Measurement Technologies Continuous Flow Streamwise Thermal Gradient Chamber operating in Scanning Flow CCN Analysis mode) aboard the Twin Otter provided CCN spectra once every forty seconds and are used to derive ambient supersaturation. We present the effects of aerosol perturbations on cloud droplet properties and in-cloud supersaturation for a variety of environments sampled during E-PEACE.
    94th American Meteorological Society Annual Meeting 2014; 02/2014
  • [Show abstract] [Hide abstract]
    ABSTRACT: The interaction of aerosol with atmospheric water affects the processing and wet removal of atmospheric particles. Understanding such interaction is mandatory to improve model description of aerosol lifetime and ageing. We analyzed the aerosol-water interaction at high relative humidity during fog events in the Po Valley, in the framework of the ARPA-ER Supersite project. For the first time in this area, the changes in particle chemical composition caused by fog are discussed along with changes in particle microphysics. During the experiment, 14 fog events were observed. The average mass scavenging efficiency was 70% for nitrate, 68% for ammonium, 61% for sulfate, 50% for organics, and 39% for black carbon. After fog formation, the interstitial aerosol was dominated by particles smaller than 200 nm Dva (vacuum aerodynamic diameter) and enriched in carbonaceous aerosol, mainly black carbon and water insoluble organic aerosol (WIOA). For each fog event, the size segregated scavenging efficiency of nitrate and organic aerosol (OA) was calculated by comparing chemical species size distribution before and after fog formation. For both nitrate and OA, the size segregated scavenging efficiency followed a sigmoidal curve, with values close to zero below 100 nm Dva and close to 1 above 700 nm Dva. OA was able to affect scavenging efficiency of nitrate in particles smaller than 300 nm Dva. A linear correlation between nitrate scavenging and particle hygroscopicity (κ) was observed, indicating that 44-51% of the variability of nitrate scavenging in smaller particles (below 300 nm Dva) was explained by changes in particle chemical composition. The size segregated scavenging curves of OA followed those of nitrate, suggesting that organic scavenging was controlled by mixing with water-soluble species. In particular, functional group composition and OA elemental analysis indicated that more oxidized OA was scavenged more efficiently than less oxidized OA. Nevertheless, the small variability of organic functional group composition during the experiment did not allow us to discriminate the effect of different organic functionalities on OA scavenging.
    Atmospheric Chemistry and Physics 01/2014; 14(4). · 5.51 Impact Factor
  • [Show abstract] [Hide abstract]
    ABSTRACT: Copyright 2014 American Association for Aerosol Research
    Aerosol Science and Technology 01/2014; 48(3). · 2.78 Impact Factor
  • [Show abstract] [Hide abstract]
    ABSTRACT: [1] Frost flowers are clusters of highly saline ice crystals growing on newly formed sea ice or frozen lakes. Based on observations of particles derived from frost flowers in the Arctic, we formulate an observation-based parameterization of salt aerosol source function from frost flowers. The particle flux from frost flowers in winter has the order of 106 m−2 s−1 at the wind speed of 10 m s−1, but the source flux is highly localized to new sea ice regions and strongly dependent on wind speed. We have implemented this parameterization into the regional Weather Research and Forecasting model with Chemistry initialized for two wintertime scenarios. The addition of sea salt aerosol emissions from frost flowers increases averaged sea salt aerosol mass and number concentration and subsequent cloud droplet number. This change of cloud droplet number concentration increases downward longwave cloud radiative forcing through enhanced cloud optical depth and emissivity. The magnitude of this forcing of sea salt aerosols from frost flowers on clouds and radiation, however, contributes negligibly to surface warming in Barrow, Alaska, in the wintertime scenarios studied here.
    Journal of Geophysical Research: Atmospheres. 12/2013; 118(23).
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: The chemical composition of submicron aerosol during the comprehensive field campaign HUMPPA-COPEC 2010 at Hyytiälä, Finland, is presented. The focus lies on online measurements of organic acids, which were achieved by using atmospheric pressure chemical ionization (APCI) ion trap mass spectrometry (IT-MS). These measurements were accompanied by aerosol mass spectrometry (AMS) measurements and Fourier transform infrared spectroscopy (FTIR) of filter samples, all showing a high degree of correlation. The soft ionization mass spectrometer alternated between gas-phase measurements solely and measuring the sum of gas and particle phase. The AMS measurements of C, H and O elemental composition show that the aerosol during the campaign was highly oxidized, which appears reasonable due to high and prolonged radiation during the boreal summer measurement period as well as the long transport times of some of the aerosol. In order to contrast ambient and laboratory aerosol, an average organic acid pattern, measured by APCI-IT-MS during the campaign, was compared to terpene ozonolysis products in a laboratory reaction chamber. Identification of single organic acid species remains a major challenge due to the complexity of the boreal forest aerosol. Unambiguous online species identification was attempted by the combinatorial approach of identifying unique fragments in the MS2 mode of standards, and then comparing these results with MS2 field spectra. During the campaign, unique fragments of limonene-derived organic acids (limonic acid and ketolimononic acid) and of the biomass burning tracer vanillic acid were detected. Other specific fragments (neutral loss of 28 Da) in the MS2 suggest the occurrence of semialdehydes. Furthermore, an approach to determine the average molecular weight of the aerosol is presented. The campaign average organic molecular weight was determined to be 300 g mol-1. However, a plume of aged biomass burning aerosol, arriving at Hyytiälä from Russia, contained organic compounds up to 800 Da ( MW om≈450 g mol-1), showing that the average molecular weight can vary significantly. The high measurement frequency of both AMS and APCI-IT-MS enabled the partitioning of selected organic acids between gas and particle phase as a function of the total particulate mass to be quantified. Surprisingly high fractions of the higher molecular weight organic acids were observed to reside in the gas phase. These observations might be a consequence of large equilibration timescales for semi-solid boreal forest aerosol, as has been recently hypothesized by Shiraiwa and Seinfeld (2012).
    ATMOSPHERIC CHEMISTRY AND PHYSICS 11/2013; 13(21):10933-10950. · 5.51 Impact Factor
  • [Show abstract] [Hide abstract]
    ABSTRACT: Atmospheric photooxidation of isoprene is an important source of secondary organic aerosol (SOA) and there is increasing evidence that anthropogenic oxidant emissions can enhance this SOA formation. In this work, we use ambient observations of organosulfates formed from isoprene epoxydiols (IEPOX) and methacrylic acid epoxide (MAE) and a broad suite of chemical measurements to investigate the relative importance of nitrogen oxide (NO/NO2) and hydroperoxyl (HO2) SOA formation pathways from isoprene at a forested site in California. In contrast to IEPOX, the calculated production rate of MAE was observed to be independent of temperature. This is the result of the very fast thermolysis of MPAN at high temperatures that affects the distribution of the MPAN reservoir (MPAN / MPA radical) reducing the fraction that can react with OH to form MAE and subsequently SOA (FMAE formation). The strong temperature dependence of FMAE formation helps to explain our observations of similar concentrations of IEPOX-derived organosulfates (IEPOX-OS; 1 ng m–3) and MAE-derived organosulfates (MAE-OS; 1 ng m–3) under cooler conditions (lower isoprene concentrations) and much higher IEPOX-OS (20 ng m–3) relative to MAE-OS (<0.0005 ng m–3) at higher temperatures (higher isoprene concentrations). A kinetic model of IEPOX and MAE loss showed that MAE forms 10−100 times more ring-opening products than IEPOX and that both are strongly dependent on aerosol water content when aerosol pH is constant. However, the higher fraction of MAE ring opening products does not compensate for the lower MAE production under warmer conditions (higher isoprene concentrations) resulting in lower formation of MAE-derived products relative to IEPOX at the surface. In regions of high NOx, high isoprene emissions and strong vertical mixing the slower MPAN thermolysis rate aloft could increase the fraction of MPAN that forms MAE resulting in a vertically varying isoprene SOA source.
    Environmental Science & Technology 09/2013; 47:11403-11413. · 5.48 Impact Factor

Publication Stats

3k Citations
664.04 Total Impact Points

Institutions

  • 2014
    • New Mexico Institute of Mining and Technology
      • Department of Chemistry
      Socorro, New Mexico, United States
  • 2006–2014
    • National University (California)
      San Diego, California, United States
  • 2005–2014
    • The Scripps Research Institute
      La Jolla, California, United States
  • 2004–2014
    • University of California, San Diego
      San Diego, California, United States
  • 2012
    • University of California, Berkeley
      • Department of Chemistry
      Berkeley, CA, United States
  • 2009
    • Universidad Nacional Autónoma de México
      • Centre of Atmospheric Sciences
      Ciudad de México, The Federal District, Mexico
    • University of the Pacific (California - USA)
      Stockton, California, United States
  • 2007
    • Harvard University
      • School of Engineering and Applied Sciences
      Cambridge, MA, United States
  • 2000–2004
    • Princeton University
      • Department of Chemical and Biological Engineering
      Princeton, New Jersey, United States
  • 2003
    • Rutgers, The State University of New Jersey
      • Department of Environmental Sciences
      New Brunswick, NJ, United States
  • 1995
    • California Institute of Technology
      • Division of Chemistry and Chemical Engineering
      Pasadena, CA, United States