New Insights for Tracking Global and Local Trends in Exposure to Air Pollutants.

Over six million people die prematurely each year from exposure to air pollution. Current air quality metrics insufficiently monitor exposure to air pollutants. This gap hinders the ability of decisionmakers to address the public health impacts of air pollution. To spur new emissions control policies and ensure implemented solutions realize meaningful gains in environmental health, we develop a framework of public-health-focused air quality indicators that quantifies over 200 countries' trends in exposure to particulate matter, ozone, nitrogen oxides, sulfur dioxide, carbon monoxide, and volatile organic compounds. We couple population density to ground-level pollutant concentrations to derive population-weighted exposure metrics that quantify the pollutant levels experienced by the average resident in each country. Our analyses demonstrate that most residents in 171 countries experience pollutant levels exceeding international health guidelines. In addition, we find a negative correlation between temporal trends in ozone and nitrogen oxide concentrations, which─when qualitatively interpreted with a simple atmospheric chemistry box model─can help describe the apparent tradeoff between the mitigation of these two pollutants on local scales. These novel indicators and their applications enable regulators to identify their most critical pollutant exposure trends and allow countries to track the performance of their emission control policies over time.

Bottom-Up Synthesized All-Thermal-Catalyst Aerogels for Heat-Regenerative Air Filtration.

Airborne particular matter (PM) pollution is an increasing global issue and alternative sources of filter fibers are now an area of significant focus. Compared with relatively mature hazardous gas treatments, state of the art high-efficiency PM filters still lack thermal decomposition ability for organic PM pollutants, such as soot from coal-fired power plants and waste-combustion incinerators, resulting in frequent replacement, high cost, and second-hand pollution. In this manuscript, we propose a bottom-up synthesis method to make the first all-thermal-catalyst air filter (ATCAF). Self-assembled from ∼50 nm diameter TiO2 fibers, ATCAF could not only capture the combustion-generated PM pollutants with >99.999% efficiency but also catalyze the complete decomposition of the as-captured hydrocarbon pollutants at high temperature. It has the potential of in situ eliminating the PM pollutants from burning of hydrocarbon materials leveraging the burning heat.

Investigating the Heterogeneous Ice Nucleation of Sea Spray Aerosols Using Prochlorococcus as a Model Source of Marine Organic Matter.

Sea spray is the largest aerosol source on Earth. Bubble bursting mechanisms at the ocean surface create smaller film burst and larger jet drop particles. This study quantified the effects of particle chemistry on the depositional ice nucleation efficiency of laboratory-generated sea spray aerosols under the cirrus-relevant conditions. Cultures of Prochlorococcus, the most abundant phytoplankton species in the global ocean, were used as a model source of organic sea spray aerosols. We showed that smaller particles generated from lysed Prochlorococcus cultures are organically enriched and nucleate more effectively than larger particles generated from the same cultures. We then quantified the ice nucleation efficiency of single component organic molecules that mimic Prochlorococcus proteins, lipids, and saccharides. Amylopectin, agarose, and aspartic acid exhibited similar critical ice saturations, fractional activations, and ice nucleation active site number densities to particles generated from Prochlorococcus cultures. These findings indicate that saccharides and proteins with numerous and well-ordered hydrophilic functional groups may determine the ice nucleation abilities of organic sea spray aerosols.

A biogenic secondary organic aerosol source of cirrus ice nucleating particles.

Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments. Ambient INPs were measured in a remote mountaintop location at -46 °C and an ice supersaturation of 30% with concentrations ranging from 0.1 to 70 L-1. Concentrations of depositional INPs were positively correlated with the mass fractions and loadings of isoprene-derived secondary organic aerosols. Compositional analysis of ice residuals showed that ambient particles with isoprene-derived SOA material can act as depositional ice nuclei. Laboratory experiments further demonstrated the ability of isoprene-derived SOA to nucleate ice under a range of atmospheric conditions. We further show that ambient concentrations of isoprene-derived SOA can be competitive with other INP sources. This demonstrates that isoprene and potentially other biogenically-derived SOA materials could influence cirrus formation and properties.

Unanticipated Side Effects of Stratospheric Albedo Modification Proposals Due to Aerosol Composition and Phase.

The Earth has now warmed ~1.0 °C since the period 1850-1900, due in large part to the anthropogenic addition of greenhouse gases to the atmosphere. Most strategies to address this warming have called for a reduction of emissions and, often, accompanying removal of greenhouse gases. Other proposals suggest masking the increased radiative forcing by an increase in particles and/or clouds to increase scattering of incoming solar radiation. Two related recent proposals have suggested addition of calcite particles to the stratosphere, which one model suggests may enhance ozone. Here we show that the interaction of calcite with acidic materials in the stratosphere results in a more complex aerosol than has been previously considered, including aqueous and hydrate phases that can lead to ozone loss. Our study suggests particle addition to the stratosphere could also perturb global radiative balance by affecting high altitude cloud formation and properties. Experimental and modeling results suggest particles will act as the nucleation sites for polar stratospheric cloud ice and, after sedimentation into the troposphere, impact cirrus clouds in the absence of other efficient ice nucleating particles. These results show that an overly simplistic set of assumptions regarding intentional particle emissions to the atmosphere can lead to incorrect estimates of the radiative effect and fail to identify unintended consequences.

A new in vivo Raman probe for enhanced applicability to the body.

This paper describes a new in vivo Raman probe that allows investigation of areas of the body that are otherwise difficult to access. It is coupled to a previously described commercially available in vivo Raman spectrometer that samples the skin through an optical flat. In the work presented here, the laser light emerges from a smaller pen-shaped probe. It thus works on the same principles as the original spectrometer, while its relative performance in terms of signal-to-noise ratio of the spectra and obtained spatial resolution is only slightly diminished. It allows the window to be placed against the subject in more curved and recessed areas of subject's body and also for them to be more comfortable while the measurements take place. Results from three areas of the body that have previously been very difficult to study are described, the mouth, axilla, and scalp. Results from the scalp and axilla strata cornea (SC) show significant differences from the "normal" SC of the volar forearm. For instance, the scalp is observed to have lower amounts of natural moisturizing factors (NMF) compared to the volar forearm within the same subjects. Also for both the axilla and scalp the lipids show a change in order as compared to the lipids in the volar forearm and also differences from each other. The potential significance of these observations is discussed. Further, we show how we can probe the mouth, in this case observing the presence of the astringent tea polyphenol epigallocatechin gallate within the oral mucosa.