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Quasi-stationary planetary waves in late winter Antarctic stratosphere temperature as a possible indicator of spring total ozone

Stratospheric preconditions for the annual Antarctic ozone hole are analyzed using the amplitude of quasi-stationary planetary waves in temperature as a predictor of total ozone column behaviour. It is found that the quasi-stationary wave amplitude in August is highly correlated with September–November total ozone over Antarctica with correlation coefficient (r) as high as 0.83 indicating that quasi-stationary wave effects in late winter have a persisting influence on the evolution of the ozone hole during the following three months. Correlation maxima are found in both the lower and middle stratosphere. These likely result from the influence of wave activity on ozone depletion due to chemical processes, and ozone accumulation due to large-scale ozone transport, respectively. Both correlation maxima indicate that spring total ozone tends to increase in the case of amplified activity of quasi-stationary waves in late winter. Since the stationary wave number one dominates the planetary waves that propagate into the Antarctic stratosphere in late austral winter, it is largely responsible for the stationary zonal asymmetry of the ozone hole relative to the South Pole. Processes associated with zonally asymmetric ozone and temperature which possibly contribute to differences in the persistence and location of the correlation maxima are discussed.
A conceptual framework to quantify the influence of convective boundary layer development on carbon dioxide mixing ratios

Interpretation of observed diurnal carbon dioxide (CO2) mixing ratios near the surface requires knowledge of the local dynamics of the planetary boundary layer. In this paper, we study the relationship between the boundary layer dynamics and the CO2 budget in convective conditions through a newly derived set of analytical equations. From these equations, we are able to quantify how uncertainties in boundary layer dynamical variables or in the morning CO2 distribution in the mixed-layer or in the free atmosphere (FA) influence the bulk CO2 mixing ratio. We find that the largest uncertainty incurred on the mid-day CO2 mixing ratio comes from the prescribed early morning CO2 mixing ratios in the stable boundary layer, and in the free atmosphere. Errors in these values influence CO2 mixing ratios inversely proportional to the boundary layer depth (h), just like uncertainties in the assumed initial boundary layer depth and surface CO2 flux. The influence of uncertainties in the boundary layer depth itself is one order of magnitude smaller. If we "invert" the problem and calculate CO2 surface exchange from observed or simulated CO2 mixing ratios, the sensitivities to errors in boundary layer dynamics also invert: they become linearly proportional to the boundary layer depth. We demonstrate these relations for a typical well characterized situation at the Cabauw site in The Netherlands, and conclude that knowledge of the temperature and carbon dioxide profiles of the atmosphere in the early morning are of vital importance to correctly interpret observed CO2 mixing ratios during midday.
Direct N2O5 reactivity measurements at a polluted coastal site

Direct measurements of N2O5 reactivity on ambient aerosol particles were made during September 2009 at the Scripps Institution of Oceanography (SIO) Pier facility located in La Jolla, CA. N2O5 reactivity measurements were made using a custom flow reactor and the particle modulation technique alongside measurements of aerosol particle size distributions and non-refractory composition. The pseudo-first order rate coefficients derived from the particle modulation technique and the particle surface area concentrations were used to determine the population average N2O5 reaction probability, γ(N2O5), approximately every 50 min. Insufficient environmental controls within the instrumentation trailer led us to restrict our analysis primarily to nighttime measurements. Within this subset of data, γ(N2O5) ranged from <0.001 to 0.029 and showed significant day-to-day variations. We compare these data to a recent parameterization that utilizes aerosol composition measurements and an aerosol thermodynamics model. The parameterization captures several aspects of the measurements with similar general trends over the time series. However, the parameterization persistently overestimates the measurements by a factor of 1.5–3 and does not illustrate the same extent of variability. Assuming chloride is internally mixed across the particle population leads to the largest overestimates. Removing this assumption only partially reduces the discrepancies, suggesting that other particle characteristics that can suppress γ(N2O5) are important, such as organic coatings or non-aqueous particles. The largest apparent driver of day-to-day variability in the measured γ(N2O5) at this site was the particle nitrate loading, as inferred from both the measured particle composition and the parameterizations. The relative change in measured γ(N2O5) as a function of particle nitrate loading appears to be consistent with expectations based on laboratory data, providing direct support for the atmospheric importance of the so-called "nitrate effect".
Modelling the partitioning of ammonium nitrate in the convective boundary layer

An explanatory model study is presented on semi-volatile secondary inorganic aerosols on three clear days in May 2008 during the IMPACT campaign at the Cabauw tower in the Netherlands. A single column model in combination with the equilibrium aerosol model ISORROPIA is used. This model uses surface observations from IMPACT and calculates the gas-aerosol partitioning of ammonium nitrate. The calculated gas-aerosol equilibrium overestimates the gas phase fraction during daytime, and overestimates the aerosol phase fraction during night-time. This discrepancy can partly be solved when the approach of the gas-aerosol equilibrium is forced to proceed with a delay timescale of up to two hours. Although it is shown that the delay itself has a small effect, the most important effect is caused by the mixing of air from higher altitudes at which the equilibrium is shifted to the aerosol phase. Thus, vertical mixing is shown to have a significant influence on the calculated partitioning at the surface. On some occasions, the correspondence to the observed partitioning improves dramatically. Even though gas-aerosol partitioning of ammonium nitrate is not instantaneous, observations show that a different equilibrium in the upper boundary layer causes aerosol ammonium nitrate concentrations to increase with altitude. Our model calculates similar vertical gradients depending on the assumed speed of gas-aerosol equilibrium. The calculated optical properties of the aerosol show a similar behaviour. The aerosol optical properties depend on the aerosol size distribution both directly, because light scattering depends on particle size, and indirectly, because the equilibration timescale depends on the aerosol sizes. Future studies should therefore focus on a fully size-resolved treatment of the gas-aerosol partitioning. Finally, coarser-resolution models may treat the gas-aerosol equilibrium of ammonium nitrate by calculating the equilibrium with a temperature and humidity sampled at a different altitude. We found that the equilibrium at an altitude of 200 m (night) up to 600 m (day) is representative for the partitioning of ammonium nitrate at the surface in the beginning of May 2008.
The comparison of MODIS-Aqua (C5) and CALIOP (V2 & V3) aerosol optical depth

We assess the consistency between instantaneously collocated level-2 aerosol optical depth (AOD) retrievals from MODIS-Aqua (C5) and CALIOP (Version 2 & 3), comparing the standard MODIS AOD (MYD04_L2) data to the AOD calculated from CALIOP aerosol extinction profiles for both the previous release (V2) and the latest release (V3) of CALIOP data. Based on data collected in January 2007, we investigate the most useful criteria for screening the MODIS and CALIOP retrievals to achieve the best agreement between the two data sets. Applying these criteria to eight months of data (Jan, Apr, Jul, Oct 2007 and 2009), we find an order of magnitude increase for the CALIOP V3 data density (by comparison to V2), that is generally accompanied by equal or better agreement with MODIS AOD. Differences in global, monthly mean, over-ocean AOD (532 nm) between CALIOP and MODIS range between 0.03 and 0.04 for CALIOP V3, with CALIOP generally biased low, when all available data from both sensors are considered. Root-mean-squares (RMS) differences in instantaneously collocated AOD retrievals by the two instruments are reduced from values ranging between 0.14 and 0.19 using the unscreened V3 data to values ranging from 0.09 to 0.1 for the screened data. A restriction to scenes with cloud fractions less than 1% (as defined in the MODIS aerosol retrievals) generally results in improved correlation (R2>0.5), except for the month of July when correlations remain relatively lower. Regional assessments show hot spots in disagreement between the two sensors in Asian outflow during April and off the coast of South Africa in July.
Chemical characterization of particle emissions from controlled burns of biomass fuels using a high resolution time-of-flight aerosol mass spectrometer

A total of forty-nine burns were conducted at the Missoula Fire Sciences Lab consisting of nine fuel types; i.e., chamise scrub oak, ceanothus, maritime chaparral, coastal sage scrub, California sage brush, Manzanita, oak savanna, oak woodland and masticated mesquite. This paper focuses on the chemical characterization of fine particle emissions collected for flaming, mixed and smoldering phases using a HR ToF-AMS. The evolution of OM/OC, H/C, O/C and N/C from fire ignition to extinction was measured to capture the transient and integrated chemical composition of the non-refractory portion of bulk particles. Real time elemental ratios and empirical formulas derived with respect to modified combustion efficiency (MCE) are reported. For each fuel, the hydrogen fragment ions dominate the unit mass resolution (UMR) mass spectra with no specific fragment ions attributable to an individual ecological combination. An interference ion in the UMR m/z 73, a fragment normally attributed to levoglucosan, is noted. Therefore, the results imply that C2H4O2+ (m/z 60.021) plus C3H5O2+ (m/z 73.029) are more sufficient to estimate the contribution of levoglucosan. The results did not show significant variations of levoglucosan content in the organic particle with the overall average contribution fraction ranging from 0.74% for coastal sage to 1.93% for chamise.
Monitoring of the Eyjafjallajökull volcanic aerosol plume over the Iberian Peninsula by means of four EARLINET lidar stations

Lidar and sun-photometer measurements were performed intensively over the Iberian Peninsula (IP) during the eruption of the Eyjafjallajökull volcano (Iceland) in April–May 2010. The volcanic plume reached all the IP stations for the first time on 5 May 2010. A thorough study of the event was conducted for the period 5–8 May. Firstly, the spatial and temporal evolution of the plume was described by means of lidar and sun-photometer measurements supported with backtrajectories. The volcanic aerosol layers observed over the IP were rather thin (<1000 m) with a top height up to 11–12 km. However, in some cases at the beginning of the period the thickness of those layers reached several kilometers in Évora and Madrid. The optical thicknesses associated to those layers were rather low (between 0.013 and 0.020 in average over the whole period), with peak values near 0.10 detected on 7 May. Secondly, the volcanic aerosols were characterized in terms of extinction and backscatter coefficients, lidar ratios, Ångström exponents and linear particle depolarization ratio. Lidar ratios at different sites varied between 30 and 50 sr without a marked spectral dependency. Similar extinction-related Ångström exponents varying between 0.6 and 0.8 were observed at different sites. The temporal evolution of the backscatter-related Ångström exponents points out a possible decrease of the volcanic particle size as the plume moved from west to east. Particle depolarization ratios on the order of 0.06–0.08 confirmed the coexistence of both ash and non-ash particles. Additionally, profiles of mass concentration were obtained with a method using the opposite depolarizing effects of ash particles (strongly depolarizing), non-ash particles (very weakly depolarizing), and sun-photometer observations. In Granada the ash mass concentration was found to be approximately 1.5 times higher than that of non-ash particles, and probably did not exceed the value of 200 μg m−3 during the whole event.
Meteorological modes of variability for fine particulate matter (PM2.5) air quality in the United States: implications for PM2.5 sensitivity to climate change

We applied a multiple linear regression model to understand the relationships of PM2.5 with meteorological variables in the contiguous US and from there to infer the sensitivity of PM2.5 to climate change. We used 2004–2008 PM2.5 observations from ~1000 sites (~200 sites for PM2.5 components) and compared to results from the GEOS-Chem chemical transport model (CTM). All data were deseasonalized to focus on synoptic-scale correlations. We find strong positive correlations of PM2.5 components with temperature in most of the US, except for nitrate in the Southeast where the correlation is negative. Relative humidity (RH) is generally positively correlated with sulfate and nitrate but negatively correlated with organic carbon. GEOS-Chem results indicate that most of the correlations of PM2.5 with temperature and RH do not arise from direct dependence but from covariation with synoptic transport. We applied principal component analysis and regression to identify the dominant meteorological modes controlling PM2.5 variability, and show that 20–40% of the observed PM2.5 day-to-day variability can be explained by a single dominant meteorological mode: cold frontal passages in the eastern US and maritime inflow in the West. These and other synoptic transport modes drive most of the overall correlations of PM2.5 with temperature and RH except in the Southeast. We show that interannual variability of PM2.5 in the US Midwest is strongly correlated with cyclone frequency as diagnosed from a spectral-autoregressive analysis of the dominant meteorological mode. An ensemble of five realizations of 1996–2050 climate change with the GISS general circulation model (GCM) using the same climate forcings shows inconsistent trends in cyclone frequency over the Midwest (including in sign), with a likely decrease in cyclone frequency implying an increase in PM2.5. Our results demonstrate the need for multiple GCM realizations (because of climate chaos) when diagnosing the effect of climate change on PM2.5, and suggest that analysis of meteorological modes of variability provides a computationally more affordable approach for this purpose than coupled GCM-CTM studies.
Nucleation and condensational growth to CCN sizes during a sustained pristine biogenic SOA event in a forested mountain valley

The Whistler Aerosol and Cloud Study (WACS 2010), included intensive measurements of trace gases and particles at two sites on Whistler Mountain. Between 6–11 July 2010 there was a sustained high-pressure system over the region with cloud-free conditions and the highest temperatures of the study. During this period, the organic aerosol concentrations rose from <1 μg m−3 to &sim;6 μg m−3. Precursor gas and aerosol composition measurements show that these organics were almost entirely of secondary biogenic nature. Throughout 6–11 July, the anthropogenic influence was minimal with sulfate concentrations <0.2 μg m−3 and SO2 mixing ratios ≈ 0.05–0.1 ppbv. Thus, this case provides excellent conditions to probe the role of biogenic secondary organic aerosol in aerosol microphysics. Although SO2 mixing ratios were relatively low, box-model simulations show that nucleation and growth may be modeled accurately if Jnuc = 3 × 10−7[H2SO4] and the organics are treated as effectively non-volatile. Due to the low condensation sink and the fast condensation rate of organics, the nucleated particles grew rapidly (2–5 nm h−1) with a 10–25% probability of growing to CCN sizes (100 nm) in the first two days as opposed to being scavenged by coagulation with larger particles. The nucleated particles were observed to grow to &sim;200 nm after three days. Comparisons of size-distribution with CCN data show that particle hygroscopicity (κ) was &sim;0.1 for particles larger 150 nm, but for smaller particles near 100 nm the κ value decreased near midway through the period from 0.17 to less than 0.06. In this environment of little anthropogenic influence and low SO2, the rapid growth rates of the regionally nucleated particles – due to condensation of biogenic SOA – results in an unusually high efficiency of conversion of the nucleated particles to CCN. Consequently, despite the low SO2, nucleation/growth appear to be the dominant source of particle number.
Signature of the 27-day solar rotation cycle in mesospheric OH and H2O observed by the Aura Microwave Limb Sounder

The mesospheric hydroxyl radical (OH) is mainly produced by the water vapor (H2O) photolysis and could be considered as a proxy for the influence of the solar irradiance variability on the mesosphere. We analyze the tropical mean response of the mesospheric OH and H2O data as observed by the Aura Microwave Limb Sounder (MLS) to 27-day solar variability. The analysis is performed for two time periods corresponding to the different phases of the 11-yr cycle: from December 2004 to December 2005 (the period of "high activity" with a pronounced 27-day solar cycle) and from August 2008 to August 2009 ("solar minimum" period with a vague 27-day solar cycle). We demonstrate, for the first time, that in the mesosphere the daily time series of OH concentrations correlate well with the solar irradiance (correlation coefficients up to 0.79) at zero time-lag. At the same time H2O anticorrelates (correlation coefficients up to −0.74) with the solar irradiance at non-zero time-lag. We found that the response of OH and H2O to the 27-day variability of the solar irradiance is strong for the period of the high solar activity and negligible for the solar minimum conditions. It allows us to suggest that the 27-day cycle in the solar irradiance and in OH and H2O are physically connected.