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Atmospheric Cluster Dynamics Code: a flexible method for solution of the birth-death equations

The Atmospheric Cluster Dynamics Code (ACDC) is presented and explored. This program was created to study the first steps of atmospheric new particle formation by examining the formation of molecular clusters from atmospherically relevant molecules. The program models the cluster kinetics by explicit solution of the birth–death equations, using an efficient computer script for their generation and the MATLAB <tt>ode15s</tt> routine for their solution. Through the use of evaporation rate coefficients derived from formation free energies calculated by quantum chemical methods for clusters containing dimethylamine or ammonia and sulphuric acid, we have explored the effect of changing various parameters at atmospherically relevant monomer concentrations. We have included in our model clusters with 0–4 base molecules and 0–4 sulfuric acid molecules for which we have commensurable quantum chemical data. The tests demonstrate that large effects can be seen for even small changes in different parameters, due to the non-linearity of the system. In particular, changing the temperature had a significant impact on the steady-state concentrations of all clusters, while the boundary effects (allowing clusters to grow to sizes beyond the largest cluster that the code keeps track of, or forbidding such processes), coagulation sink terms, non-monomer collisions, sticking probabilities and monomer concentrations did not show as large effects under the conditions studied. Removal of coagulation sink terms prevented the system from reaching the steady state when all the initial cluster concentrations were set to the default value of 1 m−3, which is probably an effect caused by studying only relatively small cluster sizes.
Five blind men and the elephant: what can the NASA Aura ozone measurements tell us about stratosphere-troposphere exchange?

We examine whether the individual ozone (O3) measurements from the four Aura instruments can quantify the stratosphere-troposphere exchange (STE) flux of O3, an important term of the tropospheric O3 budget. The level 2 (L2) Aura swath data and the nearly coincident ozone sondes for the years 2005–2006 are compared with the 4-D, high-resolution (1° × 1° × 40-layer × 0.5 h) model simulation of atmospheric ozone for the same period from the University of California, Irvine chemistry transport model (CTM). The CTM becomes a transfer standard for comparing individual profiles from these five, not-quite-coincident measurements of atmospheric ozone. Even with obvious model discrepancies identified here, the CTM can readily quantify instrument-instrument biases in the tropical upper troposphere and mid-latitude lower stratosphere. In terms of STE processes, all four Aura datasets have some skill in identifying stratosphere-troposphere folds, and we find several cases where both model and measurements see evidence of high-O3 stratospheric air entering the troposphere. In many cases identified in the model, however, the individual Aura profile retrievals in the upper troposphere and lower stratosphere show too much noise, as expected from their low sensitivity and coarse vertical resolution at and below the tropopause. These model-measurement comparisons of individual profiles do provide some level of confidence in the model-derived STE O3 flux, but it will be difficult to integrate this flux from the satellite data alone.
Relationship between particulate matter and childhood asthma – basis of a future warning system for central Phoenix

Statistically significant correlations between increase of asthma attacks in children and elevated concentrations of particulate matter of diameter 10 microns and less (PM10) were determined for metropolitan Phoenix, Arizona. Interpolated concentrations from a five-site network provided spatial distribution of PM10 that was mapped onto census tracts with population health records. The case-crossover statistical method was applied to determine the relationship between PM10 concentration and asthma attacks. For children ages 5–17, a significant relationship was discovered between the two, while children ages 0–4 exhibited virtually no relationship. The risk of adverse health effects was expressed as a function of the change from the 25th to 75th percentiles of mean level PM10 (36 μg m−3). This increase in concentration was associated with a 12.6% (95% CI: 5.8%, 19.4%) increase in the log odds of asthma attacks among children ages 5–17. Neither gender nor other demographic variables were significant. The results are being used to develop an asthma early warning system for the study area.
Error characterization of CO2 vertical mixing in the atmospheric transport model WRF-VPRM

One of the dominant uncertainties in inverse estimates of regional CO2 surface-atmosphere fluxes is related to model errors in vertical transport within the planetary boundary layer (PBL). In this study we present the results from a synthetic experiment using the atmospheric model WRF-VPRM to realistically simulate transport of CO2 for large parts of the European continent at 10 km spatial resolution. To elucidate the impact of vertical mixing error on modeled CO2 mixing ratios we simulated a month during the growing season (August 2006) with different commonly used parameterizations of the PBL (Mellor-Yamada-Janjić (MYJ) and Yonsei-University (YSU) scheme). To isolate the effect of transport errors we prescribed the same CO2 surface fluxes for both simulations. Differences in simulated CO2 mixing ratios (model bias) were on the order of 3 ppm during daytime with larger values at night. We present a simple method to reduce this bias by 70–80% when the true height of the mixed layer is known.
Some issues in uncertainty quantification and parameter tuning: a case study of convective parameterization scheme in the WRF regional climate model

The current tuning process of parameters in global climate models is often performed subjectively or treated as an optimization procedure to minimize model biases based on observations. While the latter approach may provide more plausible values for a set of tunable parameters to approximate the observed climate, the system could be forced to an unrealistic physical state or improper balance of budgets through compensating errors over different regions of the globe. In this study, the Weather Research and Forecasting (WRF) model was used to provide a more flexible framework to investigate a number of issues related uncertainty quantification (UQ) and parameter tuning. The WRF model was constrained by reanalysis of data over the Southern Great Plains (SGP), where abundant observational data from various sources was available for calibration of the input parameters and validation of the model results. Focusing on five key input parameters in the new Kain-Fritsch (KF) convective parameterization scheme used in WRF as an example, the purpose of this study was to explore the utility of high-resolution observations for improving simulations of regional patterns and evaluate the transferability of UQ and parameter tuning across physical processes, spatial scales, and climatic regimes, which have important implications to UQ and parameter tuning in global and regional models. A stochastic importance sampling algorithm, Multiple Very Fast Simulated Annealing (MVFSA) was employed to efficiently sample the input parameters in the KF scheme based on a skill score so that the algorithm progressively moved toward regions of the parameter space that minimize model errors. The results based on the WRF simulations with 25-km grid spacing over the SGP showed that the precipitation bias in the model could be significantly reduced when five optimal parameters identified by the MVFSA algorithm were used. The model performance was found to be sensitive to downdraft- and entrainment-related parameters and consumption time of Convective Available Potential Energy (CAPE). Simulated convective precipitation decreased as the ratio of downdraft to updraft flux increased. Larger CAPE consumption time resulted in less convective but more stratiform precipitation. The simulation using optimal parameters obtained by constraining only precipitation generated positive impact on the other output variables, such as temperature and wind. By using the optimal parameters obtained at 25-km simulation, both the magnitude and spatial pattern of simulated precipitation were improved at 12-km spatial resolution. The optimal parameters identified from the SGP region also improved the simulation of precipitation when the model domain was moved to another region with a different climate regime (i.e. the North America monsoon region). These results suggest that benefits of optimal parameters determined through vigorous mathematical procedures such as the MVFSA process are transferable across processes, spatial scales, and climatic regimes to some extent. This motivates future studies to further assess the strategies for UQ and parameter optimization at both global and regional scales.
Measurement-based modelling of bromine-induced oxidation of mercury above the Dead Sea

Atmospheric mercury depletion events (AMDEs) outside the polar region – driven by high levels of gaseous Br and BrO (i.e., BrOx) – were observed recently in the warm Dead Sea boundary layer. The efficient oxidation of gaseous elemental mercury (GEM) under temperate conditions by BrOx was unexpected considering that the thermal back dissociation reaction of HgBr is about 2.5 orders of magnitude higher under Dead Sea temperatures compared to polar temperatures, and hence was expected to significantly slow down GEM oxidation under warm temperatures. The goal of this modelling study was to improve understanding of the interaction of reactive bromine and mercury during Dead Sea AMDEs using numerical simulations based on a comprehensive measurement campaign in summer 2009. Our analysis is focused on daytime AMDE when chemical processes dominate concentration changes. Best agreements between simulations and observations were achieved using rate constants for kHg+Br and kHg+BrO of 2.7 × 10−13 cm3 molecule−1 s−1 and 1.5 × 10−13 cm3 molecule−1 s−1, respectively. Our model also predicted that a rate constant kHg+BrO of 5.0 × 10−14 cm3 molecule−1 s−1 may be considered as a minimum, which is higher than most reported values. These rate constants suggest that BrO could be a more efficient oxidant than Br in the troposphere as long as [Br]/[BrO] ratios are smaller than ~0.2 to 0.5. Under Dead Sea conditions, these kinetics demonstrate a high efficiency and central role of BrOx for AMDEs, with relative contributions to GEM depletion of more than ~90%. Unexpectedly, BrO was found to be the dominant oxidant with relative contributions above 80%. The strong contribution of BrO could explain why the efficiency of GEM oxidation at the Dead Sea does not critically depend on Br and, therefore, is comparable to that in cold polar regions. In order to confirm the suggested kinetics, additional studies, particularly for temperature-dependence of rate constants, are required.
Evidence of a possible turning point in solar UV-B over Canada, Europe and Japan

This study examines the long-term variability of UV solar irradiances at 305 nm and 325 nm over selected sites in Canada, Europe and Japan. Site selection was restricted to the availability of the most complete UV spectroradiometric datasets during the period 1990–2011. The analysis includes the long-term variability of total ozone, aerosol optical depth and cloud fraction at the sites studied. The results, based on observations and modeling, suggest that over Canada, Europe and Japan the period under study can be divided into three sub-periods of scientific merit: the first period (1991–1994) is the period perturbed by the Pinatubo volcanic eruption, during which excess volcanic aerosol has enhanced the "conventional" amplification factor of UV-B at ground level by an additional factor that depends on solar elevation. The increase of the UV-B amplification factor is the result of enhanced scattering processes caused by the injection of huge amounts of volcanic aerosols during the perturbed period. The second period (1995–2006) is characterized by a 0.14% yr−1 increase in total ozone and an increasing trend in spectral irradiance by 0.94% yr−1 at 305 nm and 0.88% yr−1 at 325 nm. That paradox was caused by the significant decline of the aerosol optical depth by more than 1% yr−1 (the "brightening" effect) and the absence of any statistically significant trend in the cloud fraction. The third period (2007–2011) shows statistically significant evidence of a slowdown or even a turning point in the previously reported upward UV-B trends over Canada, Europe and Japan.
Complex refractive indices of Saharan dust samples at visible and near UV wavelengths: a laboratory study

We have retrieved the wavelength-dependent imaginary parts of the complex refractive index for five different Saharan dust aerosol particles of variable mineralogical composition at wavelengths between 305 and 955 nm. The dust particles were generated by dispersing soil samples into a laboratory aerosol chamber, typically yielding particle sizes with mean diameters ranging from 0.3 to 0.4 μm and maximum diameters from 2 to 4 μm. The extinction and absorption coefficients as well as the number size distribution of the dust particles were simultaneously measured by various established techniques. An inversion scheme based on a spheroidal dust model was employed to deduce the refractive indices. The retrieved imaginary parts of the complex refractive index were in the range from 0.003 to 0.005, 0.005 to 0.011, and 0.016 to 0.050 at the wavelengths 955, 505, and 305 nm. The hematite content of the dust particles was determined by electron-microscopical single particle analysis. Hematite volume fractions in the range from 1.1 to 2.7% were found for the different dusts, a range typical for atmospheric mineral dust. We have performed a sensitivity study to assess how accurately the retrieved imaginary refractive indices could be reproduced by calculations with mixing rule approximations using the experimentally determined hematite contents as input.
Comment on "Tropospheric temperature response to stratospheric ozone recovery in the 21st century" by Hu et al. (2011)

In a recent paper Hu et al. (2011) suggest that the recovery of stratospheric ozone during the first half of this century will significantly enhance free tropospheric and surface warming caused by the anthropogenic increase of greenhouse gases, with the effects being most pronounced in Northern Hemisphere middle and high latitudes. These surprising results are based on a multi-model analysis of CMIP3 model simulations with and without prescribed stratospheric ozone recovery. Hu et al. suggest that in order to properly quantify the tropospheric and surface temperature response to stratospheric ozone recovery, it is necessary to run coupled atmosphere-ocean climate models with stratospheric ozone chemistry. The results of such an experiment are presented here, using a state-of-the-art chemistry-climate model coupled to a three-dimensional ocean model. In contrast to Hu et al., we find a much smaller Northern Hemisphere tropospheric temperature response to ozone recovery, which is of opposite sign. We suggest that their result is an artifact of the incomplete removal of the large effect of greenhouse gas warming between the two different sets of models.
Assimilation of IASI partial tropospheric columns with an Ensemble Kalman Filter over Europe

Partial lower tropospheric ozone columns provided by the IASI (Infrared Atmospheric Sounding Interferometer) instrument have been assimilated into a chemistry-transport model at continental scale (CHIMERE) using an Ensemble Square Root Kalman Filter (EnSRF). Analyses are made for the month of July 2007 over the European domain. Launched in 2006, aboard the MetOp-A satellite, IASI shows high sensitivity for ozone in the free troposphere and low sensitivity at the ground; therefore it is important to evaluate if assimilation of these observations can improve free tropospheric ozone, and possibly surface ozone. The analyses are validated against independent ozone observations from sondes, MOZAIC1 aircraft and ground based stations (AIRBASE – the European Air quality dataBase) and compared with respect to the free run of CHIMERE. These comparisons show a decrease in error of 6 parts-per-billion (ppb) in the free troposphere over the Frankfurt area, and also a reduction of the root mean square error (respectively bias) at the surface of 19% (33%) for more than 90% of existing ground stations. This provides evidence of the potential of data assimilation of tropospheric IASI columns to better describe the tropospheric ozone distribution, including surface ozone, despite the lower sensitivity. The changes in concentration resulting from the observational constraints were quantified and several geophysical explanations for the findings of this study were drawn. The corrections were most pronounced over Italy and the Mediterranean region, we noted an average reduction of 8–9 ppb in the free troposphere with respect to the free run, and still a reduction of 5.5 ppb at ground, likely due to a longer residence time of air masses in this part associated to the general circulation pattern (i.e. dominant western circulation) and to persistent anticyclonic conditions over the Mediterranean basin. This is an important geophysical result, since the ozone burden is large over this area, with impact on the radiative balance and air quality. 1 Measurements of OZone, water vapour, carbon monoxide and nitrogen oxides by in-service AIrbus airCraft (<a href="http://mozaic.aero.obs-mip.fr/web/"target="_blank">http://mozaic.aero.obs-mip.fr/web/</a>).