Influence of trans-Pacific pollution transport on acyl peroxy nitrate abundances and speciation at Mount Bachelor Observatory during INTEX-B

International audienceWe present month-long observations of speciated acyl peroxy nitrates (APNs), including PAN, PPN, MPAN, APAN, and the sum of PiBN and PnBN, measured at the Mount Bachelor Observatory (MBO) as part of the INTEX-B collaborative field campaign during spring 2006. APN abundances, measured by thermal dissociation-chemical ionization mass spectrometry (TD-CIMS), are discussed in terms of differing contributions from the boundary layer and the free troposphere and in the context of previous APN measurements in the NE Pacific region. PAN mixing ratios range from 11 to 3955 pptv, with a mean value of 334 pptv for the full measurement period. PPN is linearly correlated with PAN (r2=0.96), with an average abundance of 6.5% relative to PAN; other APNs are generally <1% of PAN. Diurnal cycles and relationships of APNs with ozone reveal a gradient in hydrocarbon chemistry between the boundary layer and the free troposphere. On average, the highest levels of APNs, ozone and PPN/PAN are found in free tropospheric air masses, suggesting that this site is strongly influenced by distant pollution sources. To estimate the impact of long-range transport of Asian pollution on atmospheric composition at MBO, we perform a detailed analysis utilizing HYSPLIT back trajectories. This analysis suggests that trans-Pacific transport of Asian pollution leads to substantial increases in APN and ozone mixing ratios at MBO, especially when transport occurs via the free troposphere. The ensemble of trajectories indicate that Asian-influenced free tropospheric air was sampled in ~16% of our data and contained a median PAN mixing ratio double that of the full dataset

Observations of TeV gamma-rays from Mrk 421 during Dec. 2005 to Apr. 2006 with the TACTIC telescope

The TACTIC $\gamma$-ray telescope has observed Mrk 421 on 66 clear nights from Dec. 07, 2005 to Apr. 30, 2006, totalling $\sim$ 202 hours of on-source observations. Here, we report the detection of flaring activity from the source at $\geq$ 1 TeV energy and the time-averaged differential $\gamma$-ray spectrum in the energy range 1-11 TeV for the data taken between Dec. 27, 2005 to Feb. 07, 2006 when the source was in a relatively higher state as compared to the rest of the observation period. Analysis of this data spell, comprising about $\sim$97h reveals the presence of a $\sim 12.0 \sigma$ $\gamma$-ray signal with daily flux of $>$ 1 Crab unit on several days. A pure power law spectrum with exponent $-3.11\pm0.11$ as well as a power law spectrum with an exponential cutoff $(\Gamma = -2.51\pm0.26$ and $E_0=(4.7\pm2.1) TeV)$ are found to provide reasonable fits to the inferred differential spectrum within statistical uncertainties. We believe that the TeV light curve presented here, for nearly 5 months of extensive coverage, as well as the spectral information at $\gamma$-ray energies of $>$ 5 TeV provide a useful input for other groups working in the field of $\gamma$-ray astronomy.Comment: 13pages,4figures; Accepted for publication in Astroparticle Physic

A regional scale modeling analysis of aerosol and trace gas distributions over the eastern Pacific during the INTEX-B field campaign

The Sulfur Transport and dEposition Model (STEM) is applied to the analysis of observations obtained during the Intercontinental Chemical Transport Experiment-Phase B (INTEX-B), conducted over the eastern Pacific Ocean during spring 2006. Predicted trace gas and aerosol distributions over the Pacific are presented and discussed in terms of transport and source region contributions. Trace species distributions show a strong west (high) to east (low) gradient, with the bulk of the pollutant transport over the central Pacific occurring between similar to 20 degrees N and 50 degrees N in the 2-6 km altitude range. These distributions are evaluated in the eastern Pacific by comparison with the NASA DC-8 and NSF/NCAR C-130 airborne measurements along with observations from the Mt. Bachelor (MBO) surface site. Thirty different meteorological, trace gas and aerosol parameters are compared. In general the meteorological fields are better predicted than gas phase species, which in turn are better predicted than aerosol quantities. PAN is found to be significantly overpredicted over the eastern Pacific, which is attributed to uncertainties in the chemical reaction mechanisms used in current atmospheric chemistry models in general and to the specifically high PAN production in the SAPRC-99 mechanism used in the regional model. A systematic underprediction of the elevated sulfate layer in the eastern Pacific observed by the C-130 is another issue that is identified and discussed. Results from source region tagged CO simulations are used to estimate how the different source regions around the Pacific contribute to the trace gas species distributions. During this period the largest contributions were from China and from fires in South/Southeast and North Asia. For the C-130 flights, which operated off the coast of the Northwest US, the regional CO contributions range as follows: China (35%), South/Southeast Asia fires (35%), North America anthropogenic (20%), and North Asia fires (10%). The transport of pollution into the western US is studied at MBO and a variety of events with elevated Asian dust, and periods with contributions from China and fires from both Asia and North America are discussed. The role of heterogeneous chemistry on the composition over the eastern Pacific is also studied. The impacts of heterogeneous reactions at specific times can be significant, increasing sulfate and nitrate aerosol production and reducing gas phase nitric acid levels appreciably (~50%)

The Influence of Foreign vs North American Emissions on Surface Ozone in the US

As part of the Hemispheric Transport of Air Pollution (HTAP; www.htap.org) project, we analyze results from 16 global and hemispheric chemical transport models and compare these to Clean Air Status and Trends Network (CASTNet) observations in the United States (US) for 2001. Using the policy-relevant maximum daily 8-h ozone (MDA8 O3) statistic, the multi-model ensemble represents the observations well (mean r2=0.57, ensemble bias=+4.1 ppbv for all regions and all seasons) despite a wide range in the individual model results. Correlations are strongest in the NorthEastern US during spring and fall (r2=0.68); and weakest in the Midwestern US in summer (r2=0.46). However, large positive mean biases exist during summer for all Eastern US regions, ranging from 10¿20 ppbv, and a smaller negative bias is present in the Western US during spring (3 ppbv). In most all other regions and seasons, the biases of the model ensemble simulations are 5 ppbv. Sensitivity simulations in which anthropogenic O3-precursor emissions (NOx+NMVOC+CO+aerosols) were decreased by 20% in each of four source regions: East Asia (EA), South Asia (SA), Europe (EU) and North America (NA) show that the greatest response of MDA8 O3 to the summed foreign emissions reductions occurs during spring in the West (0.9 ppbv reduction due to 20% reductions from EA+SA+EU). East Asia is the largest contributor to MDA8 O3 at all ranges of the O3 distribution for most regions (typically 0.45 ppbv). The exception is in the NorthEastern US where European emissions reductions had the greatest impact on MDA8 O3, particularly in the middle of the MDA8 O3 distribution (response of 0.35 ppbv between 35¿55 ppbv). In all regions and seasons, however, O3-precursor emissions reductions of 20% in the NA source region decrease MDA8 O3 the most by a factor of 2 to nearly 10 relative to foreign emissions reductions. The O3 response to anthropogenic NA emissions is greatest in the Eastern US during summer at the high end of the O3 distribution (5-6 ppbv for 20% reductions). While the impact of foreign emissions on surface O3 in the US is not negligible and is of increasing concern given the growth in emissions upwind of the US - domestic emissions reductions remain a farmore effective means of decreasing MDA8 O3 values, particularly those above 75 ppb(the current US standard).JRC.H.2-Air and Climat

The influence of foreign vs. North American emissions on surface ozone in the US

As part of the Hemispheric Transport of Air Pollution (HTAP; http:// www.htap.org) project, we analyze results from 15 global and 1 hemispheric chemical transport models and compare these to Clean Air Status and Trends Network (CASTNet) observations in the United States (US) for 2001. Using the policy-relevant maximum daily 8-h average ozone (MDA8 O3) statistic, the multi-model ensemble represents the observations well (mean r2=0.57, ensemble bias = +4.1 ppbv for all US regions and all seasons) despite a wide range in the individual model results. Correlations are strongest in the northeastern US during spring and fall (r2=0.68); and weakest in the midwestern US in summer (r2=0.46). However, large positive mean biases exist during summer for all eastern US regions, ranging from 10–20 ppbv, and a smaller negative bias is present in the western US during spring (~3 ppbv). In nearly all other regions and seasons, the biases of the model ensemble simulations are ≤5 ppbv. Sensitivity simulations in which anthropogenic O3-precursor emissions (NOx + NMVOC + CO + aerosols) were decreased by 20% in four source regions: East Asia (EA), South Asia (SA), Europe (EU) and North America (NA) show that the greatest response of MDA8 O3 to the summed foreign emissions reductions occurs during spring in the West (0.9 ppbv reduction due to 20% emissions reductions from EA + SA + EU). East Asia is the largest contributor to MDA8 O3 at all ranges of the O3 distribution for most regions (typically ~0.45 ppbv) followed closely by Europe. The exception is in the northeastern US where emissions reductions in EU had a slightly greater influence than EA emissions, particularly in the middle of the MDA8 O3 distribution (response of ~0.35 ppbv between 35–55 ppbv). EA and EU influences are both far greater (about 4x) than that from SA in all regions and seasons. In all regions and seasons O3-precursor emissions reductions of 20% in the NA source region decrease MDA8 O3 the most – by a factor of 2 to nearly 10 relative to foreign emissions reductions. The O3 response to anthropogenic NA emissions is greatest in the eastern US during summer at the high end of the O3 distribution (5–6 ppbv for 20% reductions). While the impact of foreign emissions on surface O3 in the US is not negligible – and is of increasing concern given the recent growth in Asian emissions – domestic emissions reductions remain a far more effective means of decreasing MDA8 O3 values, particularly those above 75 ppb (the current US standard)

Twenty-first century reversal of the surface ozone seasonal cycle over the northeastern United States

Changing emissions can alter the surface O3 seasonal cycle, as detected from northeastern U.S. (NE) observations during recent decades. Under continued regional precursor emission controls (>80% decreases in NE NOx by 2100), the NE surface O3 seasonal cycle reverses (to a winter maximum) in 21st century transient chemistry-climate simulations. Over polluted regions, regional NOx largely controls the shape of surface O3 seasonal cycles. In the absence of regional NOx controls, climate warming contributes to a higher surface O3 summertime peak over the NE. A doubling of the global CH4 abundance by 2100 partially offsets summertime surface O3 decreases attained via NOx reductions and contributes to raising surface O3 during December–March when the O3 lifetime is longer. The similarity between surface O3 seasonal cycles over the NE and the Intermountain West by 2100 indicates a NE transition to a region representative of baseline surface O3 conditions

Protein-Protein Interaction Site Predictions with Three-Dimensional Probability Distributions of Interacting Atoms on Protein Surfaces

Protein-protein interactions are key to many biological processes. Computational methodologies devised to predict protein-protein interaction (PPI) sites on protein surfaces are important tools in providing insights into the biological functions of proteins and in developing therapeutics targeting the protein-protein interaction sites. One of the general features of PPI sites is that the core regions from the two interacting protein surfaces are complementary to each other, similar to the interior of proteins in packing density and in the physicochemical nature of the amino acid composition. In this work, we simulated the physicochemical complementarities by constructing three-dimensional probability density maps of non-covalent interacting atoms on the protein surfaces. The interacting probabilities were derived from the interior of known structures. Machine learning algorithms were applied to learn the characteristic patterns of the probability density maps specific to the PPI sites. The trained predictors for PPI sites were cross-validated with the training cases (consisting of 432 proteins) and were tested on an independent dataset (consisting of 142 proteins). The residue-based Matthews correlation coefficient for the independent test set was 0.423; the accuracy, precision, sensitivity, specificity were 0.753, 0.519, 0.677, and 0.779 respectively. The benchmark results indicate that the optimized machine learning models are among the best predictors in identifying PPI sites on protein surfaces. In particular, the PPI site prediction accuracy increases with increasing size of the PPI site and with increasing hydrophobicity in amino acid composition of the PPI interface; the core interface regions are more likely to be recognized with high prediction confidence. The results indicate that the physicochemical complementarity patterns on protein surfaces are important determinants in PPIs, and a substantial portion of the PPI sites can be predicted correctly with the physicochemical complementarity features based on the non-covalent interaction data derived from protein interiors