Intercontinental Chemical Transport Experiment Phase B Research Articles

Simulation analysis of atmospheric SO2 contributions from different regions in China

Sulfur dioxide (SO2) is an atmospheric pollution source that poses a threat to the environment and human health. Investigating atmospheric SO2 contributions between different regions will help to reduce SO2 emissions and control pollution. Using the weather research and forecasting (WRF) model and the community multiscale air quality (CMAQ) modeling system, as well as the intercontinental chemical transport experiment phase B (INTEX-B) data, we analyzed the regional contributions of atmospheric SO2 in China. The results showed that SO2 contributions varied significantly between regions and seasons. The atmospheric SO2 levels in Central China (CTR) originated mostly from self-emissions, accounting for as much as 60% of the total emissions in January and April and up to 85% in July and October. The SO2 concentrations in Northeast China (NE) were mainly affected by emissions from CTR, especially in January (39.53%). SO2 concentrations in Northwest China (NW) were mainly affected by external emissions, which exceeded half of the SO2 in this region. SO2 concentrations in Southwest China (SW) were dominated by self-emissions, which accounted for more than 90% of the total SO2. In terms of seasons, SO2 concentrations were significantly affected by external emissions in January and April and were dominated by self-emissions in July and October. Coal use, population, area, and thermal power were found to have the greatest impacts on SO2 concentrations. Among these, coal consumption had the biggest impact on the national SO2 concentration.

WRF-Chem simulated surface ozone over south Asia during the pre-monsoon: effects of emission inventories and chemical mechanisms

Abstract. We evaluate numerical simulations of surface ozone mixing ratios over the south Asian region during the pre-monsoon season, employing three different emission inventories in the Weather Research and Forecasting model with Chemistry (WRF-Chem) with the second-generation Regional Acid Deposition Model (RADM2) chemical mechanism: the Emissions Database for Global Atmospheric Research – Hemispheric Transport of Air Pollution (EDGAR-HTAP), the Intercontinental Chemical Transport Experiment phase B (INTEX-B) and the Southeast Asia Composition, Cloud, Climate Coupling Regional Study (SEAC4RS). Evaluation of diurnal variability in modelled ozone compared to observational data from 15 monitoring stations across south Asia shows the model ability to reproduce the clean, rural and polluted urban conditions over this region. In contrast to the diurnal average, the modelled ozone mixing ratios during noontime, i.e. hours of intense photochemistry (11:30–16:30 IST – Indian Standard Time – UTC +5:30), are found to differ among the three inventories. This suggests that evaluations of the modelled ozone limited to 24 h average are insufficient to assess uncertainties associated with ozone buildup. HTAP generally shows 10–30 ppbv higher noontime ozone mixing ratios than SEAC4RS and INTEX-B, especially over the north-west Indo-Gangetic Plain (IGP), central India and southern India. The HTAP simulation repeated with the alternative Model for Ozone and Related Chemical Tracers (MOZART) chemical mechanism showed even more strongly enhanced surface ozone mixing ratios due to vertical mixing of enhanced ozone that has been produced aloft. Our study indicates the need to also evaluate the O3 precursors across a network of stations and the development of high-resolution regional inventories for the anthropogenic emissions over south Asia accounting for year-to-year changes to further reduce uncertainties in modelled ozone over this region.

Influence of Different Foreign Emissions Inventories on Simulated, Ground-Level Ozone in the Seoul Metropolitan Area during May 2014

ABSTRACTThis study examines the effects of different foreign anthropogenic emissions inventories on predicted ozone concentrations in the Seoul Metropolitan Area (SMA), South Korea, and estimates changes in ozone due to emissions reductions. We ran the Community Multi-Scale Air Quality (CMAQ) model using the High-Order Decoupled Direct Method with three inventories of foreign anthropogenic emissions: (1) the Intercontinental Chemical Transport Experiment, Phase B (INTEX-B) 2006; (2) the Comprehensive Regional Emissions inventory for Atmospheric Transport Experiment (CREATE) 2010; and (3) the Model Inter-Comparison Study (MICS)-Asia 2010. All three inventories have different spatial distributions of emissions, yielding different modeled ozone concentrations. However, the ozone concentrations modeled for the SMA differ less than those modeled for large, foreign cities in the modeling domain. The simulations using INTEX-B 2006 and CREATE 2010 suggested greater reduction in ozone with NOx control than with VOCs control. All simulations show that (1) simultaneous reduction in NOx and VOCs leads to less ozone reduction than the sum of ozone reductions for individual NOx and VOCs controls and (2) ozone reductions are stronger for high ozone days than for low ozone days. Comparing the modeled reductions in the relative sense yields smaller differences between high and low ozone days than comparing the modeled reductions in the absolute sense. With a 20% reduction in only NOx emissions, the differences in MDA1O3 among the three inventories were between 0.3 and 0.7 ppb. Because air-quality planning often leads to defined tonnage reductions, we examined the model’s response to such a defined emissions reduction. Using the NOx reduction in China estimated by Zhao et al. (2013), we estimated that the differences in MDA1O3 among the three inventories were between 1.50 and 1.78 ppb. Based on these results, we recommend using different foreign anthropogenic emissions inventories to test future scenarios for air-quality control

Inter-comparison of different NOX emission inventories and associated variation in simulated surface ozone in Indian region

In this work, we compare for the first time different anthropogenic NOX emission inventories and examine the associate variation in simulated surface ozone (O3) in India. Six anthropogenic NOX emission inventories namely Emission Database for Global Atmospheric Research (EDGAR), Intercontinental Chemical Transport Experiment-Phase B (INTEX-B), Regional Emission Inventory in Asia (REAS), MACCity, Indian National Emission Inventory (India_NOx), and Top-Down NOX emission inventory for India (Top-Down) are included in the comparison. We include these emission inventories in regional chemical transport model WRF-Chem to simulate tropospheric column NO2 and surface O3 mixing ratios for the month of summer (15-March to 15-April) and winter (December) in 2005. Predicted tropospheric column NO2 using different NOX emission inventory are evaluated with the OMI satellite observations. All emission inventories show similar spatial features, however uncertainty in NOX emissions distribution is about 20–50% over rural regions and about 60–160% over the major point sources. Compared to OMI, the largest bias in simulated tropospheric NO2 columns is seen in the REAS (−243.0 ± 338.8 × 1013 molecules cm−2) emission inventory, followed by EDGAR (−199.1 ± 272.2 × 1013 molecules cm−2), MACCity (−150.5 ± 236.3 × 1013 molecules cm−2), INTEX-B (−96.8 ± 199.5 × 1013 molecules cm−2), India_NOx (−87.7 ± 159.9 × 1013 molecules cm−2) and Top-Down (−30.8 ± 69.6 × 1013 molecules cm−2) inventories during winter. Simulations using different NOX emission inventories produces maximum deviation in daytime 8-h averaged O3 of the order of 9–17 ppb (15–40%) in summer and 3–12 ppb (5–25%) in winter over most of the land area. The simulation suggests that choice of NOX emission inventories have significant effect on surface O3 concentration for air quality studies over India.

Uncertainties in anthropogenic aerosol concentrations and direct radiative forcing induced by emission inventories in eastern China

This study quantified the uncertainties in concentrations and direct radiative forcing of anthropogenic aerosols due to emissions in eastern China using a global chemistry–aerosol–climate model. The emission inventories included three global inventories, ACCMIP (Atmospheric Chemistry & Climate Model Intercomparison Project), EDGAR-HTAP (Emission Database for Global Atmospheric Research for Hemispheric Transport of Air Pollution), and EDGAR Version 4.2, and one regional INTEX-B (Intercontinental Chemical Transport Experiment—Phase B) inventory. The uncertainties (a percentage of the standard deviation divided by the mean value across the four inventories) in the regional surface-layer aerosol concentrations due to emissions were 3.9% in sulfate, 40.0% in nitrate, 18.4% in ammonium, 11.1% in POA, 16.7% in SOA and 15.4% in BC. Compared with the ACCMIP model results based on a uniform emission inventory, the impacts of emissions were smaller. One exception is the regional surface-layer nitrate concentration, which had comparable uncertainties due to the emissions (40.0%) and the models (43.8%) because of the complex nitrate chemistry and the highly uncertain NH3 emission. The mean regional aerosol direct forcing at the top of the atmosphere between 1850 and 2006 was −3.6Wm−2 under all-sky conditions and was enhanced up to −3.83Wm−2 after the model assimilated the MODIS find-mode aerosol optical depth (AOD). The impact of the assimilation of absorption AOD is discussed. The uncertainties in aerosol direct forcing were smaller than those of the ACCMIP inter-model results, but still significant. An accurate emission inventory is essential for quantifying the role of aerosols in regional climate.

Effect of different emission inventories on modeled ozone and carbon monoxide in Southeast Asia

Abstract. In order to improve our understanding of air quality in Southeast Asia, the anthropogenic emissions inventory must be well represented. In this work, we apply different anthropogenic emission inventories in the Weather Research and Forecasting Model with Chemistry (WRF-Chem) version 3.3 using Model for Ozone and Related Chemical Tracers (MOZART) gas-phase chemistry and Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) aerosols to examine the differences in predicted carbon monoxide (CO) and ozone (O3) surface mixing ratios for Southeast Asia in March and December 2008. The anthropogenic emission inventories include the Reanalysis of the TROpospheric chemical composition (RETRO), the Intercontinental Chemical Transport Experiment-Phase B (INTEX-B), the MACCity emissions (adapted from the Monitoring Atmospheric Composition and Climate and megacity Zoom for the Environment projects), the Southeast Asia Composition, Cloud, Climate Coupling Regional Study (SEAC4RS) emissions, and a combination of MACCity and SEAC4RS emissions. Biomass-burning emissions are from the Fire Inventory from the National Center for Atmospheric Research (NCAR) (FINNv1) model. WRF-Chem reasonably predicts the 2 m temperature, 10 m wind, and precipitation. In general, surface CO is underpredicted by WRF-Chem while surface O3 is overpredicted. The NO2 tropospheric column predicted by WRF-Chem has the same magnitude as observations, but tends to underpredict the NO2 column over the equatorial ocean and near Indonesia. Simulations using different anthropogenic emissions produce only a slight variability of O3 and CO mixing ratios, while biomass-burning emissions add more variability. The different anthropogenic emissions differ by up to 30% in CO emissions, but O3 and CO mixing ratios averaged over the land areas of the model domain differ by ~4.5% and ~8%, respectively, among the simulations. Biomass-burning emissions create a substantial increase for both O3 and CO by ~29% and ~16%, respectively, when comparing the March biomass-burning period to the December period with low biomass-burning emissions. The simulations show that none of the anthropogenic emission inventories are better than the others for predicting O3 surface mixing ratios. However, the simulations with different anthropogenic emission inventories do differ in their predictions of CO surface mixing ratios producing variations of ~30% for March and 10–20% for December at Thai surface monitoring sites.

First estimates of global free-tropospheric NO<sub>2</sub> abundances derived using a cloud-slicing technique applied to satellite observations from the Aura Ozone Monitoring Instrument (OMI)

Abstract. We derive free-tropospheric NO2 volume mixing ratios (VMRs) by applying a cloud-slicing technique to data from the Ozone Monitoring Instrument (OMI) on the Aura satellite. In the cloud-slicing approach, the slope of the above-cloud NO2 column versus the cloud scene pressure is proportional to the NO2 VMR. In this work, we use a sample of nearby OMI pixel data from a single orbit for the linear fit. The OMI data include cloud scene pressures from the rotational-Raman algorithm and above-cloud NO2 vertical column density (VCD) (defined as the NO2 column from the cloud scene pressure to the top of the atmosphere) from a differential optical absorption spectroscopy (DOAS) algorithm. We compare OMI-derived NO2 VMRs with in situ aircraft profiles measured during the NASA Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign in 2006. The agreement is generally within the estimated uncertainties when appropriate data screening is applied. We then derive a global seasonal climatology of free-tropospheric NO2 VMR in cloudy conditions. Enhanced NO2 in the free troposphere commonly appears near polluted urban locations where NO2 produced in the boundary layer may be transported vertically out of the boundary layer and then horizontally away from the source. Signatures of lightning NO2 are also shown throughout low and middle latitude regions in summer months. A profile analysis of our cloud-slicing data indicates signatures of lightning-generated NO2 in the upper troposphere. Comparison of the climatology with simulations from the global modeling initiative (GMI) for cloudy conditions (cloud optical depth > 10) shows similarities in the spatial patterns of continental pollution outflow. However, there are also some differences in the seasonal variation of free-tropospheric NO2 VMRs near highly populated regions and in areas affected by lightning-generated NOx.

Simulation and validation of the aerosol optical thickness over China in 2006

The Model of Atmospheric Transport and Chemistry (MATCH) developed by the US National Center for Atmospheric Research (NCAR) was used to calculate the aerosol optical thickness (AOT) over China in 2006, with emission source data of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) and NCEP/NCAR reanalysis data as inputs. The simulation results of AOT were then validated with observational data from the Moderate Resolution Imaging Spectroradiometer (MODIS), Chinese Sun Hazemeter Network (CSHNET), Aerosol Robotics Network (AERONET), and China Aerosol Remote Sensing Network (CARSNET) at more than 30 stations over China. The comparison results indicated that the high values of AOT in the areas such as the Sichuan basin and East and South China and the low values of AOT over the Tibetan Plateau and Northwest and Northeast China were reasonably simulated by the MATCH. This model tended to underestimate the AOT values in high-aerosol-loading areas but overestimate the AOT values in less polluted areas because there are still large uncertainties in the expression of emission sources, the description of the optical properties of aerosols, the treatment of cloud and precipitation, and the selection of grid resolution. The modeling results were consistent with the CSHNET, CARSNET, AERONET, and MODIS data in most parts of China, and the correlation coefficient of the monthly mean AOT between the model and the observation was 0.79 with CSHNET data at 23 stations, 0.51 with MODIS data, and 0.88 with data at 3 CARSNET stations and 2 other stations. All of them passed the significance test with α < 0.0001. The results demonstrated that the MATCH has the ability to simulate the characteristics of the AOT distribution and its seasonal variation over China.

Source contributions to carbonaceous aerosol concentrations in Korea

We estimated the source contributions to carbonaceous aerosol concentration in Korea on the basis of Intercontinental Chemical Transport Experiment Phase B (INTEX-B) anthropogenic emissions and satellite-derived biomass burning emissions by using a nested version of GEOS-Chem with a spatial resolution of 0.5 � � 0.667 � for the period March 2006eFebruary 2007. First, we evaluated the model by comparing the simulated and observed aerosol concentrations at East Asia Network (EANET) sites and at a site in Korea. The results indicate that the model reproduces the variability and magnitudes of the observed SO4 2� ,N O 3 � , and NH 4 þ concentrations in Korea and those of the observed PM 10 concentrations in East Asia. However, the organic carbon (OC) and black carbon (BC) aerosol concentrations estimated by the model are lower than those observed in Korea by a factor of 2, especially in winter. This underestimation is likely due to extremely low domestic anthropogenic emissions and lack in seasonal variation. Source adjustments using a simple fitting and the Emission Database for Global Atmospheric Research (EDGAR) monthly allocation factors for seasonal variation yield significantly improved model results (R 2

A comparison study between model-predicted and OMI-retrieved tropospheric NO2 columns over the Korean peninsula

In this study, Community Multi-scale Air Quality (CMAQ) model simulations, using the INTEX-B (Intercontinental Chemical Transport Experiment-Phase B) emission inventory for North Korea and China, CAPSS (Clean Air Policy Support System) emission inventory for South Korea, and REAS (Regional Emission Inventory in Asia) emission inventory for Japan, were carried out over four seasonal episodes from 2006, with a fine grid resolution of 30 km × 30 km, in order to evaluate the accuracy of the NO x emissions over the Korean peninsula. The tropospheric NO 2 columns from the CMAQ model simulations were then compared with those retrieved from a satellite sensor, Ozone Monitoring Instrument (OMI), over the Korean peninsula as well as briefly over East Asia. The results showed that the CMAQ modeling, using the NO x emissions from the CAPSS inventory over South Korea, produced tropospheric NO 2 columns that were over-predicted by factors between 1.38 and 1.87 compared to the OMI-retrieved tropospheric NO 2 columns. This appears to be in line with the findings from a previous study, i.e. when the ACE-ASIA emission inventory was used for the episodes from 2001 to 2003, the CMAQ modeling tended to produce NO 2 columns that were ∼1.46 times larger than the GOME-derived NO 2 columns over South Korea. On the other hand, over North Korea, the NO x emissions of the INTEX-B emission inventory appear to be overestimated by factors between 1.55 and 7.46 (3.18 over the four seasonal episodes), based on the comparison study between the CMAQ-simulated and OMI-retrieved tropospheric NO 2 columns. This may be caused by the large uncertainty in the NO x emission fluxes from North Korea due to insufficient information on the economic activity and energy consumption related to the political instability in North Korea. ► There is a clear contrast between the NO 2 columns over South and North Korea. ► NO x emission of the 2006-CAPSS inventory was overestimated over South Korea. ► NO x emission of the INTEX-B inventory was overestimated over North Korea.

Trans-Pacific transport of reactive nitrogen and ozone to Canada during spring

Abstract. We interpret observations from the Intercontinental Chemical Transport Experiment, Phase B (INTEX-B) in spring 2006 using a global chemical transport model (GEOS-Chem) to evaluate sensitivities of the free troposphere above the North Pacific Ocean and North America to Asian anthropogenic emissions. We develop a method to use satellite observations of tropospheric NO2 columns to provide timely estimates of trends in NOx emissions. NOx emissions increased by 33% for China and 29% for East Asia from 2003 to 2006. We examine measurements from three aircraft platforms from the INTEX-B campaign, including a Canadian Cessna taking vertical profiles of ozone near Whistler Peak. The contribution to the mean simulated ozone profiles over Whistler below 5.5 km is at least 7.2 ppbv for Asian anthropogenic emissions and at least 3.5 ppbv for global lightning NOx emissions. Tropospheric ozone columns from OMI exhibit a broad Asian outflow plume across the Pacific, which is reproduced by simulation. Mean modelled sensitivities of Pacific (30° N–60° N) tropospheric ozone columns are at least 4.6 DU for Asian anthropogenic emissions and at least 3.3 DU for lightning, as determined by simulations excluding either source. Enhancements of ozone over Canada from Asian anthropogenic emissions reflect a combination of trans-Pacific transport of ozone produced over Asia, and ozone produced in the eastern Pacific through decomposition of peroxyacetyl nitrates (PANs). A sensitivity study decoupling PANs globally from the model's chemical mechanism establishes that PANs increase ozone production by removing NOx from regions of low ozone production efficiency (OPE) and injecting it into regions with higher OPE, resulting in a global increase in ozone production by 2% in spring 2006. PANs contribute up to 4 ppbv to surface springtime ozone concentrations in western Canada. Ozone production due to PAN transport is greatest in the eastern Pacific; commonly occurring transport patterns advect this ozone northeastward into Canada. Transport events observed by the aircraft confirm that polluted airmasses were advected in this way.

Characterization of particle cloud droplet activity and composition in the free troposphere and the boundary layer during INTEX-B

Abstract. Measurements of cloud condensation nuclei (CCN), aerosol size distributions, and submicron aerosol composition were made as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign during spring 2006. Measurements were conducted from an aircraft platform over the northeastern Pacific and western North America with a focus on how the transport and evolution of Asian pollution across the Pacific Ocean affected CCN properties. A broad range of air masses were sampled and here we focus on three distinct air mass types defined geographically: the Pacific free troposphere (FT), the marine boundary layer (MBL), and the polluted continental boundary layer in the California Central Valley (CCV). These observations add to the few observations of CCN in the FT. CCN concentrations showed a large range of concentrations between air masses, however CCN activity was similar for the MBL and CCV (κ~0.2–0.25). FT air masses showed evidence of long-range transport from Asia and CCN activity was consistently higher than for the boundary layer air masses. Bulk chemical measurements predicted CCN activity reasonably well for the CCV and FT air masses. Decreasing trends in κ with organic mass fraction were observed for the combination of the FT and CCV air masses and can be explained by the measured soluble inorganic chemical components. Changes in hygroscopicity associated with differences in the non-refractory organic composition were too small to be distinguished from the simultaneous changes in inorganic ion composition in the FT and MBL, although measurements for the large organic fractions (0.6–0.8) found in the CCV showed values of the organic fraction hygroscopicity consistent with other polluted regions (κorg~0.1–0.2). A comparison of CCN-derived κ (for particles at the critical diameter) to H-TDMA-derived κ (for particles at 100 nm diameter) showed similar trends, however the CCN-derived κ values were significantly higher.

A study of Asian dust plumes using satellite, surface, and aircraft measurements during the INTEX‐B field experiment

Asian dust events occur frequently during the boreal spring season. Their optical properties have been analyzed by using a combination of source region (ground‐based and satellite) and remote Pacific Ocean (aircraft) measurements during the Intercontinental Chemical Transport Experiment‐Phase B (INTEX‐B) field campaign which lasted from 7 April to 15 May 2006. A strong dust event originating from the Gobi Desert and passing over the Xianghe surface site on 17 April 2006 has been extensively analyzed. The surface averaged aerosol optical depth (AOD) values increased from 0.17 (clear sky) to 4.0 (strong dust), and the Angström exponent (α) dropped from 1.26 (clear sky) to below 0.1. Its total downwelling SW flux over the Xianghe site (thousands of kilometers away from the dust source region) is only 46% of the clear‐sky value with almost no direct transmission and nearly double the diffuse SW clear‐sky value. This event was also captured 6 days later by satellite observations as well as the UND/NASA DC‐8 aircraft over the eastern Pacific Ocean. The DC‐8 measurements in the remote Pacific region further classified the plumes into dust dominant, pollution dominant, and a mixture of dust and pollution events. HYSPLIT backward trajectories not only verified the origins of each case we selected but also showed (1) two possible origins for the dust: the Gobi and Taklimakan deserts; and (2) pollution: urban areas in eastern China, Japan, and other industrialized cities east of the two deserts. Based on the averaged satellite retrieved AOD data (0.5° × 0.5° grid box), declining AOD values with respect to longitude demonstrated the evolution of the transpacific transport pathway of Asian dust and pollution over the period of the field campaign.

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

Abstract. 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 ~20° N and 50° 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%).

Evolution of Asian aerosols during transpacific transport in INTEX-B

Abstract. Measurements of aerosol composition were made with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) on board the NSF/NCAR C-130 aircraft as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) field campaign over the Eastern Pacific Ocean. The HR-ToF-AMS measurements of non-refractory submicron aerosol mass are shown to compare well with other aerosol instrumentation in the INTEX-B field study. Two case studies are described for pollution layers transported across the Pacific from the Asian continent, intercepted 3–4 days and 7–10 days downwind of Asia, respectively. Aerosol chemistry is shown to be a robust tracer for air masses originating in Asia, specifically the presence of sulfate dominated aerosol is a distinguishing feature of Asian pollution layers that have been transported to the Eastern Pacific. We examine the time scales of processing for sulfate and organic aerosol in the atmosphere and show that our observations confirm a conceptual model for transpacific transport from Asia proposed by Brock et al. (2004). Our observations of both sulfate and organic aerosol in aged Asian pollution layers are consistent with fast formation near the Asian continent, followed by washout during lofting and subsequent transformation during transport across the Pacific. Our observations are the first atmospheric measurements to indicate that although secondary organic aerosol (SOA) formation from pollution happens on the timescale of one day, the oxidation of organic aerosol continues at longer timescales in the atmosphere. Comparisons with chemical transport models of data from the entire campaign reveal an under-prediction of organic aerosol mass in the MOZART model, but much smaller discrepancies with the GEOS-Chem model than found in previous studies over the Western Pacific. No evidence is found to support a previous hypothesis for significant secondary organic aerosol formation in the free troposphere.

Organic composition of single and submicron particles in different regions of western North America and the eastern Pacific during INTEX-B 2006

Abstract. Single particles were collected from an aircraft platform as part of the Intercontinental Chemical Transport Experiment – Phase B (INTEX-B) conducted over the eastern Pacific and western North America. Single particle spectra were obtained using scanning transmission X-ray microscopy-near edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). Bulk submicron particles were also collected and organic functional group and elemental concentrations were quantified with Fourier transform infrared (FTIR) spectroscopy and X-ray fluorescence (XRF). Single particle spectra were classified into metaclasses associated with different sources and atmospheric processing. Particles with spectra indicative of secondary organic aerosol production and combustion sources were found at several locations and a range of altitudes. At lower altitudes, particles with spectra resembling soil dust and biomass burning fingerprints were commonly observed. The types of particle spectra most commonly observed aloft were similar to those observed during a previous study over the northwestern Pacific, indicating that long-range transport may have been an important particle source. Single particle spectra provided evidence that condensation and surface-limited oxidation contributed to particle growth. Organic mass (OM) concentrations ranged from 1 to 7 μg m−3 and averaged 2.4–4.1 μg m−3. Alkane functional groups were the largest fraction of OM, averaging 1.9–2.1 μg m−3 or 50–76% of OM, followed by alcohol functional groups (0.35–0.39 μg m−3, 9–14%). Organic and elemental concentrations are compared within and among geographical air mass regions: "Pacific" free troposphere, "Continental" free troposphere, "Seattle" metropolitan region, and the California "Central Valley". OM concentrations were highest and most variable in the Central Valley (3.5±2 μg m−3). Oxygen-to-carbon ratios were relatively constant in the Central Valley but variable for the Continental air masses. Overall, the OM concentrations showed greater variability within air mass categories as compared to averages among them, suggesting sampled air mass regions included a variety of sources and processing of organic aerosol.

Characterization of volatile organic compounds (VOCs) in Asian and north American pollution plumes during INTEX-B: identification of specific Chinese air mass tracers

Abstract. We present results from the Intercontinental Chemical Transport Experiment – Phase B (INTEX-B) aircraft mission conducted in spring 2006. By analyzing the mixing ratios of volatile organic compounds (VOCs) measured during the second part of the field campaign, together with kinematic back trajectories, we were able to identify five plumes originating from China, four plumes from other Asian regions, and three plumes from the United States. To identify specific tracers for the different air masses we characterized their VOC composition and we compared their background levels with those obtained during the 2004 INTEX-A mission. The Chinese and other Asian air masses were significantly enhanced in carbonyl sulfide (OCS) and methyl chloride (CH3Cl), while all CFC replacement compounds were elevated in US plumes, particularly HFC-134a. Although elevated mixing ratios of Halon-1211 were measured in some Chinese plume samples, several measurements at background levels were also observed. After analyzing the VOC distribution and correlations within the Chinese pollution plumes and applying principal component analysis (PCA), we suggest the use of a suite of species, rather than a single gas, as specific tracers of Chinese air masses (namely OCS, CH3Cl, 1,2-dichloroethane, ethyl chloride, and Halon-1211). In an era of constantly changing halocarbon usage patterns, this suite of gases best reflects new emission characteristics from China.

Asian emissions in 2006 for the NASA INTEX-B mission

Abstract. A new inventory of air pollutant emissions in Asia in the year 2006 is developed to support the Intercontinental Chemical Transport Experiment-Phase B (INTEX-B) funded by the National Aeronautics and Space Administration (NASA). Emissions are estimated for all major anthropogenic sources, excluding biomass burning. We estimate total Asian anthropogenic emissions in the year 2006 as follows: 47.1 Tg SO2, 36.7 Tg NOx, 298.2 Tg CO, 54.6 Tg NMVOC, 29.2 Tg PM10, 22.2 Tg PM2.5, 2.97 Tg BC, and 6.57 Tg OC. We emphasize emissions from China because they dominate the Asia pollutant outflow to the Pacific and the increase of emissions from China since 2000 is of great concern. We have implemented a series of improved methodologies to gain a better understanding of emissions from China, including a detailed technology-based approach, a dynamic methodology representing rapid technology renewal, critical examination of energy statistics, and a new scheme of NMVOC speciation for model-ready emissions. We estimate China's anthropogenic emissions in the year 2006 to be as follows: 31.0 Tg SO2, 20.8 Tg NOx, 166.9 Tg CO, 23.2 Tg NMVOC, 18.2 Tg PM10, 13.3 Tg PM2.5, 1.8 Tg BC, and 3.2 Tg OC. We have also estimated 2001 emissions for China using the same methodology and found that all species show an increasing trend during 2001–2006: 36% increase for SO2, 55% for NOx, 18% for CO, 29% for VOC, 13% for PM10, and 14% for PM2.5, BC, and OC. Emissions are gridded at a resolution of 30 min×30 min and can be accessed at our web site (http://mic.greenresource.cn/intex-b2006).

Size-resolved aerosol chemistry on Whistler Mountain, Canada with a high-resolution aerosol mass spectrometer during INTEX-B

Abstract. An Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed at the peak of Whistler Mountain (2182 m above sea level), British Columbia, from 19 April to 16 May 2006, as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign. The mass concentrations and size distributions of non-refractory submicron particle (NR-PM1) species (i.e., sulfate, nitrate, ammonium, chloride, and organics) were measured in situ at 10-min time resolution. The HR-ToF-AMS results agreed well with collocated measurements. The average concentration of non-refractory submicron particulate matter (NR-PM1; 1.9 μg m−3) is similar to those observed at other remote, high elevation sites in North America. Episodes of enhanced aerosol loadings were observed, due to influences of regional and trans-Pacific transport of air pollution. Organics and sulfate were the dominant species, on average accounting for 55% and 30%, respectively, of the NR-PM1 mass. The average size distributions of sulfate and ammonium both showed an accumulation mode peaking at ~500 nm in vacuum aerodynamic diameter (Dva) while those of organic aerosol (OA) and nitrate peaked at ~300 nm. The size differences suggested that sulfate and OA were mostly present in external mixtures from different source origins. We also quantitatively determined the elemental composition of OA using the high resolution mass spectra. Overall, OA at Whistler Peak was highly oxygenated, with an average organic-mass-to-organic-carbon ratio (OM/OC) of 2.28±0.23 and an atomic ratio of oxygen-to-carbon (O/C) of 0.83±0.17. The nominal formula for OA was C1H1.66N0.03O0.83 for the entire study. Two significant trans-Pacific dust events originated from Asia were observed at Whistler Peak during this study. While both events were characterized with significant enhancements of coarse mode particles and mineral contents, the composition and characteristics of NR-PM1 were significantly different between them. One trans-Pacific event occurred on 15 May 2006, during which ammonium sulfate contributed &gt;90% of the total NR-PM1 mass. This event was followed by a high OA episode likely associated with regional emissions. In total, three enhanced regional OA events, each of which lasted 2–3 days, were observed during this study. In contrast to the two dust events, the regional OA events were generally characterized with higher OA/sulfate ratio, less oxidized OA, and lower OM/OC ratio.

Airborne High Spectral Resolution Lidar for profiling aerosol optical properties

A compact, highly robust airborne High Spectral Resolution Lidar (HSRL) that provides measurements of aerosol backscatter and extinction coefficients and aerosol depolarization at two wavelengths has been developed, tested, and deployed on nine field experiments (over 650 flight hours). A unique and advantageous design element of the HSRL system is the ability to radiometrically calibrate the instrument internally, eliminating any reliance on vicarious calibration from atmospheric targets for which aerosol loading must be estimated. This paper discusses the design of the airborne HSRL, the internal calibration and accuracy of the instrument, data products produced, and observations and calibration data from the first two field missions: the Joint Intercontinental Chemical Transport Experiment--Phase B (INTEX-B)/Megacity Aerosol Experiment--Mexico City (MAX-Mex)/Megacities Impacts on Regional and Global Environment (MILAGRO) field mission (hereafter MILAGRO) and the Gulf of Mexico Atmospheric Composition and Climate Study/Texas Air Quality Study II (hereafter GoMACCS/TexAQS II).