Chemistry and transport of pollution over the Gulf of Mexico and the  Pacific: Spring 2006 INTEX-B Campaign overview and first results

Abstract. Intercontinental Chemical Transport Experiment-B (INTEX-B) was a major NASA1 led multi-partner atmospheric field campaign completed in the spring of 2006 (http://cloud1.arc.nasa.gov/intex-b/). Its major objectives aimed at (i) investigating the extent and persistence of the outflow of pollution from Mexico; (ii) understanding transport and evolution of Asian pollution and implications for air quality and climate across western North America; and (iii) validating space-borne observations of tropospheric composition. INTEX-B was performed in two phases. In its first phase (1–21 March), INTEX-B operated as part of the MILAGRO campaign with a focus on observations over Mexico and the Gulf of Mexico. In the second phase (17 April–15 May), the main INTEX-B focus was on the trans-Pacific Asian pollution transport. Multiple airborne platforms carrying state of the art chemistry and radiation payloads were flown in concert with satellites and ground stations during the two phases of INTEX-B. Validation of Aura satellite instruments (TES, OMI, MLS, HIRDLS) was a key objective within INTEX-B. Satellite products along with meteorological and 3-D chemical transport model forecasts were integrated into the flight planning process to allow targeted sampling of air parcels. Inter-comparisons were performed among and between aircraft payloads to quantify the accuracy of data and to create a unified data set. Pollution plumes were sampled over the Gulf of Mexico and the Pacific several days after downwind transport from source regions. Signatures of Asian pollution were routinely detected by INTEX-B aircraft, providing a comprehensive data set on gas and aerosol composition to test models and evaluate pathways of pollution transport and their impact on air quality and climate. This overview provides details about campaign implementation and a context within which the present and future INTEX-B/MILAGRO publications can be understood. 1 Acronyms are provided in Appendix A.

Download Full-text

Chemistry and transport of pollution over the Gulf of Mexico and the Pacific: spring 2006 INTEX-B campaign overview and first results

Atmospheric Chemistry and Physics ◽

10.5194/acp-9-2301-2009 ◽

2009 ◽

Vol 9 (7) ◽

pp. 2301-2318 ◽

Cited By ~ 210

Author(s):

H. B. Singh ◽

W. H. Brune ◽

J. H. Crawford ◽

F. Flocke ◽

D. J. Jacob

Keyword(s):

Air Quality ◽

Gulf Of Mexico ◽

Transport Model ◽

Chemical Transport ◽

Second Phase ◽

Pollution Transport ◽

Aerosol Composition ◽

Data Set ◽

The Pacific ◽

Two Phases

Abstract. Intercontinental Chemical Transport Experiment-B (INTEX-B) was a major NASA (Acronyms are provided in Appendix A.) led multi-partner atmospheric field campaign completed in the spring of 2006 (http://cloud1.arc.nasa.gov/intex-b/). Its major objectives aimed at (i) investigating the extent and persistence of the outflow of pollution from Mexico; (ii) understanding transport and evolution of Asian pollution and implications for air quality and climate across western North America; and (iii) validating space-borne observations of tropospheric composition. INTEX-B was performed in two phases. In its first phase (1–21 March), INTEX-B operated as part of the MILAGRO campaign with a focus on observations over Mexico and the Gulf of Mexico. In the second phase (17 April–15 May), the main INTEX-B focus was on trans-Pacific Asian pollution transport. Multiple airborne platforms carrying state of the art chemistry and radiation payloads were flown in concert with satellites and ground stations during the two phases of INTEX-B. Validation of Aura satellite instruments (TES, OMI, MLS, HIRDLS) was a key objective within INTEX-B. Satellite products along with meteorological and 3-D chemical transport model forecasts were integrated into the flight planning process to allow targeted sampling of air parcels. Inter-comparisons were performed among and between aircraft payloads to quantify the accuracy of data and to create a unified data set. Pollution plumes were sampled over the Gulf of Mexico and the Pacific several days after downwind transport from source regions. Signatures of Asian pollution were routinely detected by INTEX-B aircraft, providing a valuable data set on gas and aerosol composition to test models and evaluate pathways of pollution transport and their impact on air quality and climate. This overview provides details about campaign implementation and a context within which the present and future INTEX-B/MILAGRO publications can be understood.

Download Full-text

Variability of springtime transpacific pollution transport during 2000–2006: the INTEX-B mission in the context of previous years

Atmospheric Chemistry and Physics ◽

10.5194/acp-10-1345-2010 ◽

2010 ◽

Vol 10 (3) ◽

pp. 1345-1359 ◽

Cited By ~ 16

Author(s):

G. G. Pfister ◽

L. K. Emmons ◽

D. P. Edwards ◽

A. Arellano ◽

T. Campos ◽

...

Keyword(s):

Transport Model ◽

Pollution Transport ◽

Chemistry Transport Model ◽

Pollution Levels ◽

Annual Variability ◽

Source Regions ◽

Time Period ◽

The Pacific ◽

The Us ◽

Transport Experiment

Abstract. We analyze the transport of pollution across the Pacific during the NASA INTEX-B (Intercontinental Chemical Transport Experiment Part B) campaign in spring 2006 and examine how this year compares to the time period for 2000 through 2006. In addition to aircraft measurements of carbon monoxide (CO) collected during INTEX-B, we include in this study multi-year satellite retrievals of CO from the Measurements of Pollution in the Troposphere (MOPITT) instrument and simulations from the chemistry transport model MOZART-4. Model tracers are used to examine the contributions of different source regions and source types to pollution levels over the Pacific. Additional modeling studies are performed to separate the impacts of inter-annual variability in meteorology and dynamics from changes in source strength. Interannual variability in the tropospheric CO burden over the Pacific and the US as estimated from the MOPITT data range up to 7% and a somewhat smaller estimate (5%) is derived from the model. When keeping the emissions in the model constant between years, the year-to-year changes are reduced (2%), but show that in addition to changes in emissions, variable meteorological conditions also impact transpacific pollution transport. We estimate that about 1/3 of the variability in the tropospheric CO loading over the contiguous US is explained by changes in emissions and about 2/3 by changes in meteorology and transport. Biomass burning sources are found to be a larger driver for inter-annual variability in the CO loading compared to fossil and biofuel sources or photochemical CO production even though their absolute contributions are smaller. Source contribution analysis shows that the aircraft sampling during INTEX-B was fairly representative of the larger scale region, but with a slight bias towards higher influence from Asian contributions.

Download Full-text

Pre-monsoon air quality over Lumbini, a world heritage site along the Himalayan foothills

10.5194/acp-2016-430 ◽

2016 ◽

Cited By ~ 2

Author(s):

Dipesh Rupakheti ◽

Bhupesh Adhikary ◽

Puppala S. Praveen ◽

Maheswar Rupakheti ◽

Shichang Kang ◽

...

Keyword(s):

Air Pollution ◽

Air Quality ◽

Forest Fires ◽

Air Pollutants ◽

Transport Model ◽

World Heritage ◽

World Heritage Site ◽

Pollution Level ◽

Pollution Transport ◽

Heritage Site

Abstract. Lumbini, in southern Nepal, is a UNESCO world heritage site of universal value as the birthplace of Buddha. Poor air quality in Lumbini and surrounding regions is a great concern for public health as well as for preservation, protection and promotion of Buddhist heritage and culture. We present here results from measurements of ambient concentrations of key air pollutants (PM, BC, CO, O3) in Lumbini, first of its kind for Lumbini, conducted during an intensive measurement period of three months (April–June 2013) in the pre-monsoon season. The measurements were carried out as a part of the international air pollution measurement campaign; SusKat-ABC (Sustainable Atmosphere for the Kathmandu Valley – Atmospheric Brown Clouds). The ranges of hourly average concentrations were: PM10: 10.5–604.0 µg m−3, PM2.5: 6.1–272.2 µg m−3; BC: 0.3–30.0 µg m−3; CO: 125.0–1430.0 ppbv; and O3: 1.0–118.1 ppbv. These levels are comparable to other very heavily polluted sites throughout South Asia. The 24-h average PM2.5 and PM10 concentrations exceeded the WHO guideline very frequently (94 % and 85 % of the sampled period, respectively), which implies significant health risks for the residents and visitors in the region. These air pollutants exhibited clear diurnal cycles with high values in the morning and evening. During the study period, the worst air pollution episodes were mainly due to agro-residue burning and regional forest fires combined with meteorological conditions conducive of pollution transport to Lumbini. Fossil fuel combustion also contributed significantly, accounting for more than half of the ambient BC concentration according to aerosol spectral light absorption coefficients obtained in Lumbini. WRF-STEM, a regional chemical transport model, was used to simulate the meteorology and the concentrations of pollutants. The model was able to reproduce the variation in the pollutant concentrations well; however, estimated values were 1.5 to 5 times lower than the observed concentrations for CO and PM10 respectively. Regionally tagged CO tracers showed the majority of CO came from the upwind region of Ganges valley. The model was also used to examine the chemical composition of the aerosol mixture, indicating that organic carbon was the main constituent of fine mode PM2.5, followed by mineral dust. Given the high pollution level, there is a clear and urgent need for setting up a network of long-term air quality monitoring stations in the greater Lumbini region.

Download Full-text

A new diagnostic for tropospheric ozone production

10.5194/acp-2017-378 ◽

2017 ◽

Author(s):

Peter M. Edwards ◽

Mathew J. Evans

Keyword(s):

Air Quality ◽

Tropospheric Ozone ◽

Transport Model ◽

Chemical Transport ◽

Ozone Production ◽

Chemical Transport Model ◽

Organic Species ◽

Earth’S Climate ◽

Oxidation Of Organics

Abstract. Tropospheric ozone is important for the Earth’s climate and air quality. It is produced during the oxidation of organics in the presence of nitrogen oxides. Due to the range of organic species emitted and the chain like nature of their oxidation, this chemistry is complex and understanding the role of different processes (emission, deposition, chemistry) is difficult. We demonstrate a new methodology for diagnosing ozone production based on the processing of bonds contained within emitted molecules, the fate of which is determined by the conservation of spin of the bonding electrons. Using this methodology to diagnose ozone production in the GEOS-Chem chemical transport model, we demonstrate its advantages over the standard diagnostic. We show that the number of bonds emitted, their chemistry and lifetime, and feedbacks on OH are all important in determining the ozone production within the model and its sensitivity to changes. This insight may allow future model-model comparisons to better identify the root causes of model differences.

Download Full-text

Skill-Testing Chemical Transport Models across Contrasting Atmospheric Mixing States Using Radon-222

10.20944/preprints201811.0607.v1 ◽

2018 ◽

Author(s):

Scott D. Chambers ◽

Elise-Andree Guérette ◽

Khalia Monk ◽

Alan D. Griffiths ◽

Yang Zhang ◽

...

Keyword(s):

Air Quality ◽

Diurnal Cycle ◽

Transport Model ◽

Chemical Transport ◽

Chemical Transport Model ◽

Transport Models ◽

Potential Health ◽

Meteorological Model ◽

Model Skill ◽

Chemical Transport Models

We propose a new technique to prepare statistically-robust benchmarking data for evaluating chemical transport model meteorology and air quality parameters within the urban boundary layer. The approach employs atmospheric class-typing, using nocturnal radon measurements to assign atmospheric mixing classes, and can be applied temporally (across the diurnal cycle), or spatially (to create angular distributions of pollutants as a top-down constraint on emissions inventories). In this study only a short (<1-month) campaign is used, but grouping of the relative mixing classes based on nocturnal mean radon concentrations can be adjusted according to dataset length (i.e., number of days per category), or desired range of within-class variability. Calculating hourly distributions of observed and simulated values across diurnal composites of each class-type helps to: (i) bridge the gap between scales of simulation and observation, (ii) represent the variability associated with spatial and temporal heterogeneity of sources and meteorology without being confused by it, and (iii) provide an objective way to group results over whole diurnal cycles that separates ‘natural complicating factors’ (synoptic non-stationarity, rainfall, mesoscale motions, extreme stability, etc.) from problems related to parameterizations, or between-model differences. We demonstrate the utility of this technique using output from a suite of seven contemporary regional forecast and chemical transport models. Meteorological model skill varied across the diurnal cycle for all models, with an additional dependence on the atmospheric mixing class that varied between models. From an air quality perspective, model skill regarding the duration and magnitude of morning and evening “rush hour” pollution events varied strongly as a function of mixing class. Model skill was typically the lowest when public exposure would have been the highest, which has important implications for assessing potential health risks in new and rapidly evolving urban regions, and also for prioritizing the areas of model improvement for future applications.

Download Full-text

Ozone and carbon monoxide observations over open oceans on R/V <i>Mirai</i> from 67° S to 75° N during 2012 to 2017: Testing global chemical reanalysis in terms of Arctic processes, low ozone levels at low latitudes, and pollution transport

10.5194/acp-2018-1354 ◽

2019 ◽

Cited By ~ 1

Author(s):

Yugo Kanaya ◽

Kazuyuki Miyazaki ◽

Fumikazu Taketani ◽

Takuma Miyakawa ◽

Hisahiro Takashima ◽

...

Keyword(s):

Carbon Monoxide ◽

Atmospheric Chemistry ◽

Critical Evaluation ◽

Chemical Transport ◽

Tropospheric Chemistry ◽

Set Covering ◽

The Arctic ◽

Pollution Transport ◽

Data Set ◽

Air Masses

Abstract. Constraints from ozone (O3) observations over oceans are needed in addition to those from terrestrial regions to fully understand global tropospheric chemistry and its impact on the climate. Here, we provide a large data set of ozone and carbon monoxide (CO) levels observed (for 11 666 and 10 681 h, respectively) over oceans. The data set is derived from observations made during 24 research cruise legs of R/V Mirai during 2012 to 2017, in the Southern, Indian, Pacific, and Arctic Oceans, covering the region from 67° S to 75° N. The data are suitable for critical evaluation of the over-ocean distribution of ozone derived from chemical transport models. We first give an overview of the statistics in the data set and highlight key features in terms of geographical distribution and air mass type. We then use the data set to evaluate ozone concentration fields from Tropospheric Chemistry Reanalysis version 2 (TCR-2), produced by assimilating a suite of satellite observations of multiple species into a chemical transport model, namely CHASER. For long-range transport of polluted air masses from continents to the oceans, during which the effects of forest fires and fossil fuel combustion were recognized, TCR-2 gave an excellent performance in reproducing the observed temporal variations and photochemical buildup of O3 when assessed from ΔO3 / ΔCO ratios. For clean marine conditions with low and stable CO concentrations, two focused analyses were performed. The first was in the Arctic (> 70° N) in September every year from 2013 to 2016; TCR-2 underpredicted O3 levels by 6.7 ppb (21 %) on average. The observed vertical profiles from O3 soundings from R/V Mirai during September 2014 had less steep vertical gradients at low altitudes (> 850 hPa) than those obtained TCR-2. This suggests the possibilities of more efficient descent of the O3-rich air from above or less efficient dry deposition on the surface than were assumed in the model. In the second analysis, over the western Pacific equatorial region (125–165° E, 10° S to 25° N), the observed O3 level frequently decreased to less than 10 ppb in comparison to that obtained with TCR-2, and also those obtained in most of the Atmospheric Chemistry Climate Model Intercomparison Project (ACCMIP) model runs for the decade from 2000. These results imply loss processes that are unaccounted for in the models. We found that the model’s positive bias positively correlated with the daytime residence times of air masses over a particular grid, namely 165–180° E and 15–30° N; an additional loss rate of 0.25 ppb h−1 in the grid best explained the gap. Halogen chemistry, which is commonly omitted from currently used models, might be active in this region and could have contributed to additional losses. Our open data set covering wide ocean regions is complementary to the Tropospheric Ozone Assessment Report data set, which basically comprises ground-based observations, and enables a fully global study of the behavior of O3.

Download Full-text

Coupling between surface ozone and leaf area index in a chemical transport model: strength of feedback and implications for ozone air quality and vegetation health

Atmospheric Chemistry and Physics ◽

10.5194/acp-18-14133-2018 ◽

2018 ◽

Vol 18 (19) ◽

pp. 14133-14148 ◽

Cited By ~ 10

Author(s):

Shan S. Zhou ◽

Amos P. K. Tai ◽

Shihan Sun ◽

Mehliyar Sadiq ◽

Colette L. Heald ◽

...

Keyword(s):

Air Quality ◽

Leaf Area Index ◽

Leaf Area ◽

Dry Deposition ◽

Transport Model ◽

Surface Ozone ◽

Chemical Transport ◽

Chemical Transport Model ◽

Area Index ◽

Ozone Levels

Abstract. Tropospheric ozone is an air pollutant that substantially harms vegetation and is also strongly dependent on various vegetation-mediated processes. The interdependence between ozone and vegetation may constitute feedback mechanisms that can alter ozone concentration itself but have not been considered in most studies to date. In this study we examine the importance of dynamic coupling between surface ozone and leaf area index (LAI) in shaping ozone air quality and vegetation. We first implement an empirical scheme for ozone damage on vegetation in the Community Land Model (CLM) and simulate the steady-state responses of LAI to long-term exposure to a range of prescribed ozone levels (from 0 to 100 ppb). We find that most plant functional types suffer a substantial decline in LAI as ozone level increases. Based on the CLM-simulated results, we develop and implement in the GEOS-Chem chemical transport model a parameterization that computes fractional changes in monthly LAI as a function of local mean ozone levels. By forcing LAI to respond to ozone concentrations on a monthly timescale, the model simulates ozone–LAI coupling dynamically via biogeochemical processes including biogenic volatile organic compound (VOC) emissions and dry deposition, without the complication from meteorological changes. We find that ozone-induced damage on LAI can lead to changes in ozone concentrations by −1.8 to +3 ppb in boreal summer, with a corresponding ozone feedback factor of −0.1 to +0.6 that represents an overall self-amplifying effect from ozone–LAI coupling. Substantially higher simulated ozone due to strong positive feedbacks is found in most tropical forests, mainly due to the ozone-induced reductions in LAI and dry deposition velocity, whereas reduced isoprene emission plays a lesser role in these low-NOx environments. In high-NOx regions such as the eastern US, Europe, and China, however, the feedback effect is much weaker and even negative in some regions, reflecting the compensating effects of reduced dry deposition and reduced isoprene emission (which reduces ozone in high-NOx environments). In remote, low-LAI regions, including most of the Southern Hemisphere, the ozone feedback is generally slightly negative due to the reduced transport of NOx–VOC reaction products that serve as NOx reservoirs. This study represents the first step to accounting for dynamic ozone–vegetation coupling in a chemical transport model with ramifications for a more realistic joint assessment of ozone air quality and ecosystem health.

Download Full-text

Model Performance Differences in Sulfate Aerosol in Winter over Japan Based on Regional Chemical Transport Models of CMAQ and CAMx

Atmosphere ◽

10.3390/atmos9120488 ◽

2018 ◽

Vol 9 (12) ◽

pp. 488 ◽

Cited By ~ 5

Author(s):

Syuichi Itahashi ◽

Kazuyo Yamaji ◽

Satoru Chatani ◽

Kunihiro Hisatsune ◽

Shinji Saito ◽

...

Keyword(s):

Air Quality ◽

Deposition Velocity ◽

Model Performance ◽

Chemical Transport ◽

Sulfate Aerosol ◽

Performance Criteria ◽

Second Phase ◽

Transport Models ◽

Chemical Transport Models ◽

So2 Concentration

Sulfate aerosol (SO42−) is a major component of particulate matter in Japan. The Japanese model intercomparison study, J-STREAM, found that although SO42− is well captured by models, it is underestimated during winter. In the first phase of J-STREAM, we refined the Fe- and Mn-catalyzed oxidation and partly improved the underestimation. The winter haze in December 2016 was a target period in the second phase. The results from the Community Multiscale Air Quality (CMAQ) and Comprehensive Air quality Model with eXtentions (CAMx) regional chemical transport models were compared with observations from the network over Japan and intensive observations at Nagoya and Tokyo. Statistical analysis showed both models satisfied the suggested model performance criteria. CMAQ sensitivity simulations explained the improvements in model performance. CMAQ modeled lower SO42− concentrations than CAMx, despite increased aqueous oxidation via the metal catalysis pathway and NO2 reaction in CMAQ. Deposition explained this difference. A scatter plot demonstrated that the lower SO42− concentration in CMAQ than in CAMx arose from the lower SO2 concentration and higher SO42− wet deposition in CMAQ. The dry deposition velocity caused the difference in SO2 concentration. These results suggest the importance of deposition in improving our understanding of ambient concentration behavior.

Download Full-text

Applying the delta tool to support the Air Quality Directive: evaluation of the TCAM chemical transport model

Air Quality Atmosphere & Health ◽

10.1007/s11869-014-0240-4 ◽

2014 ◽

Vol 7 (3) ◽

pp. 335-346 ◽

Cited By ~ 10

Author(s):

C. Carnevale ◽

G. Finzi ◽

A. Pederzoli ◽

E. Pisoni ◽

P. Thunis ◽

...

Keyword(s):

Air Quality ◽

Transport Model ◽

Chemical Transport ◽

Chemical Transport Model

Download Full-text

Statistical diagnostic and correction of a chemistry-transport model for the prediction of total column ozone

Atmospheric Chemistry and Physics ◽

10.5194/acp-6-525-2006 ◽

2006 ◽

Vol 6 (2) ◽

pp. 525-537 ◽

Cited By ~ 10

Author(s):

S. Guillas ◽

G. C. Tiao ◽

D. J. Wuebbles ◽

A. Zubrow

Keyword(s):

Transport Model ◽

Chemical Transport ◽

Satellite System ◽

Chemical Transport Model ◽

Quasi Biennial Oscillation ◽

Data Set ◽

Total Column Ozone ◽

Noise Component ◽

Column Ozone ◽

Total Column

Abstract. In this paper, we introduce a statistical method for examining and adjusting chemical-transport models. We illustrate the findings with total column ozone predictions, based on the University of Illinois at Urbana-Champaign 2-D (UIUC 2-D) chemical-transport model of the global atmosphere. We propose a general diagnostic procedure for the model outputs in total ozone over the latitudes ranging from 60° South to 60° North to see if the model captures some typical patterns in the data. The method proceeds in two steps to avoid possible collinearity issues. First, we regress the measurements given by a cohesive data set from the SBUV(/2) satellite system on the model outputs with an autoregressive noise component. Second, we regress the residuals of this first regression on the solar flux, the annual cycle, the Antarctic or Arctic Oscillation, and the Quasi Biennial Oscillation. If the coefficients from this second regression are statistically significant, then they mean that the model did not simulate properly the pattern associated with these factors. Systematic anomalies of the model are identified using data from 1979 to 1995, and statistically corrected afterwards. The 1996–2003 validation sample confirms that the combined approach yields better predictions than the direct UIUC 2-D outputs.

Download Full-text