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Sensitivity of US air quality to mid-latitude cyclone frequency and implications of 1980–2006 climate change

We show that the frequency of summertime mid-latitude cyclones tracking across eastern North America at 40°–50° N (the southern climatological storm track) is a strong predictor of stagnation and ozone pollution days in the eastern US. The NCEP/NCAR Reanalysis, going back to 1948, shows a significant long-term decline in the number of summertime mid-latitude cyclones in that track starting in 1980 (−0.15 a−1). The more recent but shorter NCEP/DOE Reanalysis (1979–2006) shows similar interannual variability in cyclone frequency but no significant long-term trend. Analysis of NOAA daily weather maps for 1980–2006 supports the trend detected in the NCEP/NCAR Reanalysis 1. A GISS general circulation model (GCM) simulation including historical forcing by greenhouse gases reproduces this decreasing cyclone trend starting in 1980. Such a long-term decrease in mid-latitude cyclone frequency over the 1980–2006 period may have offset by half the ozone air quality gains in the northeastern US from reductions in anthropogenic emissions. We find that if mid-latitude cyclone frequency had not declined, the northeastern US would have been largely compliant with the ozone air quality standard by 2001. Mid-latitude cyclone frequency is expected to decrease further over the coming decades in response to greenhouse warming and this will necessitate deeper emission reductions to achieve a given air quality goal.
1-D Air-snowpack modeling of atmospheric nitrous acid at South Pole during ANTCI 2003

A 1-D air-snowpack model of HONO has been developed and constrained by observed chemistry and meteorology data. The 1-D model includes molecular diffusion and mechanical dispersion, windpumping in snow, gas phase to quasi-liquid layer phase HONO transfer and quasi-liquid layer nitrate and interstitial air HONO photolysis. Photolysis of nitrate is important as a dominant HONO source inside the snowpack, however, the observed HONO emission from the snowpack was triggered mainly by the equilibrium between quasi liquid layer nitrite and firn air HONO deep down the snow surface (i.e. 30 cm below snow surface). The high concentration of HONO in the firn air is subsequently transported above the snowpack by diffusion and windpumping. The model uncertainties come mainly from lack of measurements and the interpretation of the QLL properties based on the bulk snow measurements. One critical factor is the ionic strength of QLL nitrite, which is estimated here by the bulk snow pH, nitrite concentration, and QLL to bulk snow volume ratio.
Climate forcing and air quality change due to regional emissions reductions by economic sector

We examine the air quality (AQ) and radiative forcing (RF) response to emissions reductions by economic sector for North America and developing Asia in the CAM and GISS composition/climate models. Decreases in annual average surface particulate are relatively robust, with intermodel variations in magnitude typically <30% and very similar spatial structure. Surface ozone responses are small and highly model dependent. The largest net RF results from reductions in emissions from the North America industrial/power and developing Asia domestic fuel burning sectors. Sulfate reductions dominate the first case, for which intermodel variations in the sulfate (or total) aerosol optical depth (AOD) responses are ~30% and the modeled spatial patterns of the AOD reductions are highly correlated (R=0.9). Decreases in BC dominate the developing Asia domestic fuel burning case, and show substantially greater model-to-model differences. Intermodel variations in tropospheric ozone burden changes are also large, though aerosol changes dominate those cases with substantial net climate forcing. The results indicate that across-the-board emissions reductions in domestic fuel burning in developing Asia and in surface transportation in North America are likely to offer the greatest potential for substantial, simultaneous improvement in local air quality and near-term mitigation of global climate change via short-lived species. Conversely, reductions in industrial/power emissions have the potential to accelerate near-term warming, though they would improve AQ and have a long-term cooling effect on climate. These broad conclusions appear robust to intermodel differences.
Simulation of aerosol optical properties over Europe with a 3-D size-resolved aerosol model: comparisons with AERONET data

This paper aims at presenting a model-to-data comparison of the Aerosol Optical Thickness (AOT) and of a few sparse data for Single Scattering Albedo (SSA) over Europe for one year. The main contribution of this paper is the sensitivity study to a large number of parameters, including physical and numerical parameters of the aerosol model itself. The optical parameters are computed from a size-resolved aerosol model embedded in the Polyphemus system. The methodology is first described, showing that several hypothesis can be made for micro-physical aerosol properties. The simulation is made over one year (2001); statistics and monthly time series for the simulation and AERONET data are used to evaluate the ability of the model to reproduce AOT and vertically averaged SSA fields and their variability. The relation with the uncertainties of measurements is discussed. Then a sensitivity study with respect to the mixing state of the particle, the way to take into account water uptake, numerical parameters and physical parameterizations of the model is carried out. The results indicate that the mixing state of particles has an influence on optical parameters, as well as the computation of the wet diameter. But some physical and numerical parameters associated with the aerosol model itself have even more influence under certain conditions, through the uncertainties on the aerosol chemical composition, and their size distribution.
Effects of model resolution on entrainment (inversion heights), cloud-radiation interactions, and cloud radiative forcing

We undertook three-dimensional numerical studies of a marine stratus deck under a strong inversion using an interactive shortwave- and longwave-radiation module. A suite of sensitivity tests were conducted to address the effects of model resolution on entrainment (inversion heights), cloud-radiation interactions, and cloud radiative-forcings by varying model horizontal resolution only, varying vertical resolution only, and varying horizontal- and vertical-resolution simultaneously but with a fixed aspect ratio of 2.5. Our results showed that entrainment (inversion height) is more sensitive to vertical- than to horizontal-resolution. A vertical resolution finer than 40 m can simulate spatial- and temporal-variations in the inversion height well. The inversion height decreases with increasing vertical resolution, but tends to increase with increasing horizontal resolution. Cloud liquid water path doubles after refining both the vertical- and horizontal-resolution by a factor of four. This doubling is associated with a positive feedback between cloud water and cloud top radiative cooling, which amplifies small differences initiated by changes in the model resolution. The magnitude of the cloud radiative-forcing tends to increase with increasing model resolution, mainly attributable to the increase in the cloud liquid water path. Shortwave radiative forcing is dominant, and more sensitive to model resolution than the longwave counterpart.
Characteristics of the NO-NO2-O3 system in different chemical regimes during the MIRAGE-Mex field campaign

The NO-NO2 system was analyzed in different chemical regimes/air masses based on observations of reactive nitrogen species and peroxy radicals made during the intensive field campaign MIRAGE-Mex (4 to 29 March 2006). The air masses were categorized into 5 groups based on combinations of macroscopic observations, geographical location, meteorological parameters, models, and observations of trace gases: boundary layer (labeled as "BL"), biomass burning ("BB"), free troposphere (continental, "FTCO" and marine, "FTMA"), and Tula industrial complex ("TIC"). In general, NO2/NO ratios in different air masses are near photostationary state. Analysis of this ratio can be useful for testing current understanding of tropospheric chemistry. The ozone production efficiency (OPE) for the 5 air mass categories ranged from 4.5 (TIC) to 8.5 (FTMA), consistent with photochemical aging of air masses exiting the Mexico City Metropolitan Area.
Saharan dust levels in Greece and received inhalation doses

The desert of Sahara is one of the major sources of mineral dust on Earth, producing around 2×108 tons/yr. Under certain weather conditions, dust particles from Saharan desert get transported over the Mediterranean Sea and most of Europe. The limiting values set by the directive EC/30/1999 of European Union can easily be exceeded by the transport of desert dust particles in the south European Region and especially in urban areas, where there is also significant contribution from anthropogenic sources. In this study, the effects of dust transport on air quality in several Greek urban areas are quantified. PM10 concentration values from stationary monitoring stations are compared to dust concentrations for the 4-year period 2003–2006. The dust concentration values in the Greek areas were estimated by the SKIRON modelling system coupled with embedded algorithms describing the dust cycle. The mean annual dust contribution to daily-averaged PM10 concentration values was found to be around or even greater than 10% in the urban areas throughout the years examined. Natural dust transport may contribute by more than 20% to the annual number of exceedances – PM10 values greater than EU limits – depending on the specific monitoring location. In a second stage of the study, the inhaled lung dose received by the residents in various Greek locations is calculated. The particle deposition efficiency of mineral dust at the different parts of the human respiratory tract is determined by applying a lung dosimetry numerical model, which incorporates inhalation dynamics and aerosol physical processes. The inhalation dose from mineral dust particles was greater in the upper respiratory system (extrathoracic region) and less significant in the lungs, especially in the sensitive alveolar region. However, in cases of dust episodes, the amounts of mineral dust deposited along the human lung are comparable to those received during exposure in heavily polluted urban or smoking areas.
Characterization of the size-segregated water-soluble inorganic ions at eight Canadian rural sites

Size-segregated water-soluble inorganic ions, including particulate sulphate (SO42-), nitrate (NO3-), ammonium (NH4+), chloride (Cl-), and base cations (K+, Na+, Mg2+, Ca2+), were measured using a Micro-Orifice Uniform Deposit Impactor (MOUDI) during fourteen short-term field campaigns at eight locations in both polluted and remote regions of eastern and central Canada. The size distributions of SO42- and NH4+ were unimodal, peaking at 0.3–0.6 µm in diameter, during most of the campaigns, although a bimodal distribution was found during one campaign and a trimodal distribution was found during another campaign made at a coastal site. SO42- peaked at slightly larger sizes in the cold seasons (0.5–0.6 µm) compared to the hot seasons (0.3–0.4 µm) due to the higher relative humidity in the cold seasons. The size distributions of NO3- were unimodal, peaking at 4.0–7.0 µm during the warm-season campaigns, and bimodal, with one peak at 0.3–0.6 µm and another at 4–7 µm during the cold-season campaigns. A unimodal size distribution, peaking at 4–6 µm, was found for Cl-, Na+, Mg2+, and Ca2+ during approximately half of the campaigns and a bimodal distribution, with one peak at 2 µm and the other at 6 µm, was found during the rest of the campaigns. For K+, a bimodal distribution, with one peak at 0.3 µm and the other at 4 µm, was observed during most of the campaigns. Seasonal contrasts in the size-distribution profiles suggest that emission sources and air mass origins were the major factors controlling the size distributions of the primary aerosols while meteorological conditions were more important for the secondary aerosols. The dependence of the particle acidity on the particle size from the nucleation mode to the accumulation mode was not consistent from site to site or from season to season. Particles in the accumulation mode were more acidic than those in the nucleation mode when submicron particles were in the state of strong acidity; however, when submicron particles were neutral or weakly acidic, particles in the nucleation mode could sometimes be more acidic. The inconsistency of the dependence of the particle acidity on the particle size should have been caused by the different emission sources of all the related species and the different meteorological conditions during the different campaigns. The results presented here at least partially explain the controversial phenomenon found in previous studies on this topic.
Simulation of atmospheric mercury depletion events (AMDEs) during polar springtime using the MECCA box model

Atmospheric mercury depletion events (AMDEs) during polar springtime are closely correlated with bromine-catalyzed tropospheric ozone depletion events (ODEs). To study gas- and aqueous-phase reaction kinetics and speciation of mercury during AMDEs, we have included mercury chemistry into the box model MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere), which enables dynamic simulation of bromine activation and ODEs. We found that the reaction of Hg with Br atoms dominates the loss of gaseous elemental mercury (GEM). To explain the experimentally observed synchronous depletion of GEM and O3, the reaction rate of Hg+BrO has to be much lower than that of Hg+Br. The synchronicity is best reproduced with rate coefficients at the lower limit of the literature values for both reactions, i.e. kHg+Br≈3×10−13 and kHg+BrO≤1×10−15 cm3 molecule−1 s−1, respectively. Throughout the simulated AMDEs, BrHgOBr was the most abundant reactive mercury species, both in the gas phase and in the aqueous phase. The aqueous-phase concentrations of BrHgOBr, HgBr2, and HgCl2 were several orders of magnitude larger than that of Hg(SO3)22−. Considering chlorine chemistry outside depletion events (i.e. without bromine activation), the concentration of total divalent mercury in sea-salt aerosol particles (mostly HgCl42−) was much higher than in dilute aqueous droplets (mostly Hg(SO3)22−), and did not exhibit a diurnal cycle (no correlation with HO2 radicals).
Investigation of the hygroscopic properties of Ca(NO3)2 and internally mixed Ca(NO3)2/CaCO3 particles by micro-Raman spectrometry

To understand and predict the role of mineral aerosol particles processed by reactive nitrogen species in the atmosphere, the hygroscopic properties of both Ca(NO3)2 and Ca(NO3)2-containing mineral particles must be well understood. Using a micro-Raman system, the hygroscopic behaviors of micro-sized individual Ca(NO3)2 and internally mixed Ca(NO3)2/CaCO3 particles in both dehumidifying and humidifying processes were investigated systematically. In addition to accurate quantification of the dependence of water content on relative humidity (RH), significant new spectroscopic evidence related to chemical structure was also obtained to confirm the occurrence of amorphous solid state and to better understand the phase transition process. The Ca(NO3)2 particles exhibit reversible behavior in the dehumidifying and humidifying processes; they are in the state of solution droplets above 10% RH and amorphous hydrates below 7% RH, and phase transition occurs at 7–10% RH. The hygroscopic behavior of Ca(NO3)2/CaCO3 particles is identical to that of pure Ca(NO3)2 particles, suggesting a negligible effect of the slightly soluble CaCO3 inclusion on the hygroscopic behavior of a(NO3)2/CaCO3 particles.