• Energy Research

The Indian Ocean Experiment (INDOEX) was an international, multiplatform field campaign to measure long-range transport of air pollution from South and Southeast Asia toward the Indian Ocean during the dry monsoon season in January to March 1999. Surprisingly high pollution levels were observed over the entire northern Indian Ocean toward the Intertropical Convergence Zone at about 6°S. We show that agricultural burning and especially biofuel use enhance carbon monoxide concentrations. Fossil fuel combustion and biomass burning cause a high aerosol loading. The growing pollution in this region gives rise to extensive air quality degradation with local, regional, and global implications, including a reduction of the oxidizing power of the atmosphere.

AbstractAircraft‐based measurements of aerosol composition, either bulk or single‐particle, and both subsaturated and supersaturated hygroscopicity were made in the Los Angeles Basin and its outflows during May 2010 during the CalNex field study. Aerosol composition evolves from source‐rich areas in the western Basin to downwind sites in the eastern Basin, evidenced by transition from an external to internal mixture, as well as enhancements in organic O : C ratio, the amount of organics and nitrate internally mixed on almost all particle types, and coating thickness on refractory black carbon (rBC). Transport into hot, dilute outflow regions leads to significant volatilization of semivolatile material, resulting in a unimodal aerosol comprising primarily oxygenated, low‐volatility, water‐soluble organics and sulfate. The fraction of particles with rBC or soot cores is between 27 and 51% based on data from a Single Particle Soot Photometer (SP2) and Aerosol Time of Flight Mass Spectrometer (ATOFMS). Secondary organics appear to inhibit subsaturated water uptake in aged particles, while CCN activity is enhanced with photochemical age. A biomass‐burning event resulted in suppression of subsaturated hygroscopicity but enhancement in CCN activity, suggesting that BB particles may be nonhygroscopic at subsaturated RH but are important sources of CCN. Aerosol aging and biomass burning can lead to discrepancies between subsaturated and supersaturated hygroscopicity that may be related to mixing state. In the cases of biomass burning aerosol and aged particles coated with secondary material, more than a single parameter representation of subsaturated hygroscopicity and CCN activity is needed.

AbstractThe California Research at the Nexus of Air Quality and Climate Change (CalNex) field study was conducted throughout California in May, June, and July of 2010. The study was organized to address issues simultaneously relevant to atmospheric pollution and climate change, including (1) emission inventory assessment, (2) atmospheric transport and dispersion, (3) atmospheric chemical processing, and (4) cloud‐aerosol interactions and aerosol radiative effects. Measurements from networks of ground sites, a research ship, tall towers, balloon‐borne ozonesondes, multiple aircraft, and satellites provided in situ and remotely sensed data on trace pollutant and greenhouse gas concentrations, aerosol chemical composition and microphysical properties, cloud microphysics, and meteorological parameters. This overview report provides operational information for the variety of sites, platforms, and measurements, their joint deployment strategy, and summarizes findings that have resulted from the collaborative analyses of the CalNex field study. Climate‐relevant findings from CalNex include that leakage from natural gas infrastructure may account for the excess of observed methane over emission estimates in Los Angeles. Air‐quality relevant findings include the following: mobile fleet VOC significantly declines, and NOx emissions continue to have an impact on ozone in the Los Angeles basin; the relative contributions of diesel and gasoline emission to secondary organic aerosol are not fully understood; and nighttime NO3 chemistry contributes significantly to secondary organic aerosol mass in the San Joaquin Valley. Findings simultaneously relevant to climate and air quality include the following: marine vessel emissions changes due to fuel sulfur and speed controls result in a net warming effect but have substantial positive impacts on local air quality.

The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth’s clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol−cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol−cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol−cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.

Intense wildfires burning >360000 acres in San Diego during October, 2007 provided a unique opportunity to study the impact of wildfires on local air quality and biomass burning aerosol (BBA) aging. The size-resolved mixing state of individual particles was measured in real-time with an aerosol time-of-flight mass spectrometer (ATOFMS) for 10 days after the fires commenced. Particle concentrations were high county-wide due to the wildfires; 84% of 120-400 nm particles by number were identified as BBA, with particles <400 nm contributing to mass concentrations dangerous to public health, up to 148 μg/m(3). Evidence of potassium salts heterogeneously reacting with inorganic acids was observed with continuous high temporal resolution for the first time. Ten distinct chemical types shown as BBA factors were identified through positive matrix factorization coupled to single particle analysis, including particles comprised of potassium chloride and organic nitrogen during the beginning of the wildfires, ammonium nitrate and amines after an increase of relative humidity, and sulfate dominated when the air mass back trajectories passed through the Los Angeles port region. Understanding BBA aging processes and quantifying the size-resolved mass and number concentrations are important in determining the overall impact of wildfires on air quality, health, and climate.

Significance Wide adoption of algae cultivation to produce environmentally sustainable biofuels and fine chemicals is currently hampered by large losses (10 to 30%) incurred by grazer infections. We show the usage of real-time chemical ionization mass spectrometry to rapidly identify gaseous indicators of grazer infections in cyanobacteria cultures. Grazing was detected significantly faster (up to 3 d) using real-time mass spectrometry than the current methods of microscopy and qPCR. By employing this technology, cultivators may be empowered to treat grazer infestations sooner, thereby protecting the crop and enhancing profitability.