scholarly journals Modelling the chemistry and transport of bromoform within a sea breeze driven convective system during the SHIVA Campaign

2013 ◽  
Vol 13 (8) ◽  
pp. 20611-20676 ◽  
Author(s):  
P. D. Hamer ◽  
V. Marécal ◽  
R. Hossaini ◽  
M. Pirre ◽  
N. Warwick ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Climate Models ◽  
Stratospheric Ozone ◽  
Sea Breeze ◽  
Convective System ◽  
North West ◽  
Mixing Ratios ◽  
The North ◽  
Relative Contribution ◽  
Convective Column

Abstract. We carry out a case study of the transport and chemistry of bromoform and its product gases (PGs) in a sea breeze driven convective episode on 19 November 2011 along the North West coast of Borneo during the "Stratospheric ozone: Halogen Impacts in a Varying Atmosphere" (SHIVA) campaign. We use ground based, ship, aircraft and balloon sonde observations made during the campaign, and a 3-D regional online transport and chemistry model capable of resolving clouds and convection explicitly that includes detailed bromine chemistry. The model simulates the temperature, wind speed, wind direction fairly well for the most part, and adequately captures the convection location, timing, and intensity. The simulated transport of bromoform from the boundary layer up to 12 km compares well to aircraft observations to support our conclusions. The model makes several predictions regarding bromine transport from the boundary layer to the level of convective detrainment (11 to 12 km). First, the majority of bromine undergoes this transport as bromoform. Second, insoluble organic bromine carbonyl species are transported to between 11 and 12 km, but only form a small proportion of the transported bromine. Third, soluble bromine species, which include bromine organic peroxides, hydrobromic acid (HBr), and hypobromous acid (HOBr), are washed out efficiently within the core of the convective column. Fourth, insoluble inorganic bromine species (principally Br2) are not washed out of the convective column, but are also not transported to the altitude of detrainment in large quantities. We expect that Br2 will make a larger relative contribution to the total vertical transport of bromine atoms in scenarios with higher CHBr3 mixing ratios in the boundary layer, which have been observed in other regions. Finally, given the highly detailed description of the chemistry, transport and washout of bromine compounds within our simulations, we make a series of recommendations about the physical and chemical processes that should be represented in 3-D chemical transport models (CTMs) and chemistry climate models (CCMs), which are the primary theoretical means of estimating the contribution made by CHBr3 and other very short-lived substances (VSLS) to the stratospheric bromine budget.

scholarly journals Ensemble models on palaeoclimate to predict India's groundwater challenge

2013 ◽  
Vol 2 (3) ◽  
Author(s):  
Partha Sarathi Datta
Keyword(s):  
Climate Change ◽  
Climate Models ◽  
Global Climate ◽  
Global Climate Models ◽  
Humid Climate ◽  
Ensemble Models ◽  
North West ◽  
The Past ◽  
The North ◽  
14C Age

In many parts of the world, freshwater crisis is largely due to increasing water consumption and pollution by rapidly growing population and aspirations for economic development, but, ascribed usually to the climate. However, limited understanding and knowledge gaps in the factors controlling climate and uncertainties in the climate models are unable to assess the probable impacts on water availability in tropical regions. In this context, review of ensemble models on δ18O and δD in rainfall and groundwater, 3H- and 14C- ages of groundwater and 14C- age of lakes sediments helped to reconstruct palaeoclimate and long-term recharge in the North-west India; and predict future groundwater challenge. The annual mean temperature trend indicates both warming/cooling in different parts of India in the past and during 1901–2010. Neither the GCMs (Global Climate Models) nor the observational record indicates any significant change/increase in temperature and rainfall over the last century, and climate change during the last 1200 yrs BP. In much of the North-West region, deep groundwater renewal occurred from past humid climate, and shallow groundwater renewal from limited modern recharge over the past decades. To make water management to be more responsive to climate change, the gaps in the science of climate change need to be bridged.

scholarly journals Atmospheric bromoform at Mace Head, Ireland: seasonality and evidence for a peatland source

2005 ◽  
Vol 5 (11) ◽  
pp. 2927-2934 ◽  
Author(s):  
L. J. Carpenter ◽  
D. J. Wevill ◽  
S. O'Doherty ◽  
G. Spain ◽  
P. G. Simmonds
Keyword(s):  
Boundary Layer ◽  
Wind Direction ◽  
Marine Boundary Layer ◽  
Land Breeze ◽  
Peat Bogs ◽  
Mixing Ratios ◽  
The North ◽  
Prevailing Wind Direction ◽  
Atmospheric Observations ◽  
Summer Minimum

Abstract. In situ atmospheric observations of bromoform (CHBr3) made over a 2.5 year period at Mace Head, Ireland from May 2001- Dec 2003, including during the NAMBLEX (North Atlantic Marine Boundary Layer Experiment) campaign, show broad maxima from spring until autumn and winter minima, with mixing ratios of 5.3+1.0 pptv (mid March - mid October) and 1.8+0.8 pptv (December-February). This indicates that, unlike CHCl3, which has a summer minimum and winter maximum at Mace Head, local biological sources of CHBr3 have a greater influence on the atmospheric data than photochemical decay during long-range transport. The emission sources are predominantly macroalgal, but we find evidence for a small terrestrial flux from peatland ecosystems, which so far has not been accounted for in the CHBr3 budget. Sharp increases in CHCl3 and CHBr3 concentrations and decreases in O3 concentrations occurred at night when the wind direction switched from an ocean- to a land-based sector (land breeze) and the wind speed dropped to below 5 ms-1. These observations infer a shallow atmospheric boundary layer with increased O3 deposition and concentration of local emissions of both CHCl3 and CHBr3. The ratio of ΔCHCl3/ΔCHBr3 varied strongly according to the prevailing wind direction; from 0.60+0.15 in south-easterly (100-170° and northerly (340-20°) air to 2.5+0.4 in north-easterly (40-70°) air. Of these land-sectors, the south-easterly air masses are likely to be strongly influenced by macroalgal beds along the coast and the emission ratios probably reflect those from seaweeds in addition to land sources. The north-easterly airmasses however had an immediate fetch inland, which locally is comprised of coastal peatland ecosystems (peat bogs and coastal conifer plantations), previously identified as being strong sources of atmospheric CHCl3 under these conditions. Although we cannot entirely rule out other local land or coastal sources, our observations also suggest peatland ecosystem emissions of CHBr3. We use correlations between CHCl3 and CHBr3 during the north-easterly land breeze events in conjunction with previous estimates of local wetland CHCl3 release to tentatively deduce a global wetland CHBr3 source of 20.4(0.4-948) Gg yr-1, which is approximately 7% of the total global source.

scholarly journals Verifying Operational Forecasts of Land–Sea-Breeze and Boundary Layer Mixing Processes

2020 ◽  
Vol 35 (4) ◽  
pp. 1427-1445
Author(s):  
Ewan Short
Keyword(s):  
Boundary Layer ◽  
Diurnal Cycle ◽  
Spatial Scales ◽  
Sea Breeze ◽  
Absolute Error ◽  
Wind Fields ◽  
Mixing Processes ◽  
Relative Contribution ◽  
The Mean ◽  
Diurnal Wind

AbstractForecasters working for Australia’s Bureau of Meteorology (BoM) produce a 7-day forecast in two key steps: first they choose a model guidance dataset to base the forecast on, and then they use graphical software to manually edit these data. Two types of edits are commonly made to the wind fields that aim to improve how the influences of boundary layer mixing and land–sea-breeze processes are represented in the forecast. In this study the diurnally varying component of the BoM’s official wind forecast is compared with that of station observations and unedited model guidance datasets. Coastal locations across Australia over June, July, and August 2018 are considered, with data aggregated over three spatial scales. The edited forecast produces a lower mean absolute error than model guidance at the coarsest spatial scale (over 50 000 km2), and achieves lower seasonal biases over all spatial scales. However, the edited forecast only reduces errors or biases at particular times and locations, and rarely produces lower errors or biases than all model guidance products simultaneously. To better understand physical reasons for biases in the mean diurnal wind cycles, modified ellipses are fitted to the seasonally averaged diurnal wind temporal hodographs. Biases in the official forecast diurnal cycle vary with location for multiple reasons, including biases in the directions that sea breezes approach coastlines, amplitude biases, and disagreement in the relative contribution of sea-breeze and boundary layer mixing processes to the mean diurnal cycle.

scholarly journals Continental outflow from the US to the upper troposphere over the North Atlantic during the NASA INTEX-NA Airborne Campaign

2008 ◽  
Vol 8 (7) ◽  
pp. 1989-2005 ◽  
Author(s):  
S. Y. Kim ◽  
R. Talbot ◽  
H. Mao ◽  
D. Blake ◽  
S. Vay ◽  
...  
Keyword(s):  
Boundary Layer ◽  
North Atlantic ◽  
The United States ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
The North ◽  
Southeastern Us ◽  
The Us ◽  
The North Atlantic ◽  
Continental Outflow

Abstract. A case of continental outflow from the United States (US) was examined using airborne measurements from NASA DC-8 flight 13 during the Intercontinental Chemical Transport Experiment – North America (INTEX-NA). Mixing ratios of methane (CH4) and carbon monoxide (CO) at 8–11 km altitude over the North Atlantic were elevated to 1843 ppbv and 134 ppbv respectively, while those of carbon dioxide (CO2) and carbonyl sulfide (COS) were reduced to 372.4 ppmv and 411 pptv respectively. In this region, urban and industrial influences were evidenced by elevated mixing ratios and good linear relationships between urban and industrial tracers compared to North Atlantic background air. Moreover, low mixing ratios and a good correlation between COS and CO2 showed a fingerprint of terrestrial uptake and minimal dilution during rapid transport over a 1–2 day time period. Analysis of synoptic conditions, backward trajectories, and photochemical aging estimates based on C3H8/C2H6 strongly suggested that elevated anthropogenic tracers in the upper troposphere of the flight region were the result of transport via convection and warm conveyor belt (WCB) uplifting of boundary layer air over the southeastern US. This mechanism is supported by the similar slope values of linear correlations between long-lived (months) anthropogenic tracers (e.g., C2Cl4 and CHCl3) from the flight region and the planetary boundary layer in the southeastern US. In addition, the aircraft measurements suggest that outflow from the US augmented the entire tropospheric column at mid-latitudes over the North Atlantic. Overall, the flight 13 data demonstrate a pervasive impact of US anthropogenic emissions on the troposphere over the North Atlantic.

scholarly journals Effects of halogens on European air-quality

2017 ◽  
Vol 200 ◽  
pp. 75-100 ◽  
Author(s):  
T. Sherwen ◽  
M. J. Evans ◽  
R. Sommariva ◽  
L. D. J. Hollis ◽  
S. M. Ball ◽  
...  
Keyword(s):  
Air Quality ◽  
Stratospheric Ozone ◽  
Mixing Ratios ◽  
The North ◽  
Halogen Chemistry ◽  
The North Sea ◽  
Regional Air Quality ◽  
The Uk ◽  
The Impact ◽  
Quality Policy

Halogens (Cl, Br) have a profound influence on stratospheric ozone (O3). They (Cl, Br and I) have recently also been shown to impact the troposphere, notably by reducing the mixing ratios of O3 and OH. Their potential for impacting regional air-quality is less well understood. We explore the impact of halogens on regional pollutants (focussing on O3) with the European grid of the GEOS-Chem model (0.25° × 0.3125°). It has recently been updated to include a representation of halogen chemistry. We focus on the summer of 2015 during the ICOZA campaign at the Weybourne Atmospheric Observatory on the North Sea coast of the UK. Comparisons between these observations together with those from the UK air-quality network show that the model has some skill in representing the mixing ratios/concentration of pollutants during this period. Although the model has some success in simulating the Weybourne ClNO2 observations, it significantly underestimates ClNO2 observations reported at inland locations. It also underestimates mixing ratios of IO, OIO, I2 and BrO, but this may reflect the coastal nature of these observations. Model simulations, with and without halogens, highlight the processes by which halogens can impact O3. Throughout the domain O3 mixing ratios are reduced by halogens. In northern Europe this is due to a change in the background O3 advected into the region, whereas in southern Europe this is due to local chemistry driven by Mediterranean emissions. The proportion of hourly O3 above 50 nmol mol−1 in Europe is reduced from 46% to 18% by halogens. ClNO2 from N2O5 uptake onto sea-salt leads to increases in O3 mixing ratio, but these are smaller than the decreases caused by the bromine and iodine. 12% of ethane and 16% of acetone within the boundary layer is oxidised by Cl. Aerosol response to halogens is complex with small (∼10%) reductions in PM2.5 in most locations. A lack of observational constraints coupled to large uncertainties in emissions and chemical processing of halogens make these conclusions tentative at best. However, the results here point to the potential for halogen chemistry to influence air quality policy in Europe and other parts of the world.

scholarly journals Nitrogen oxides in the boundary layer and free troposphere at the Mt. Bachelor Observatory

2010 ◽  
Vol 10 (13) ◽  
pp. 6043-6062 ◽  
Author(s):  
D. R. Reidmiller ◽  
D. A. Jaffe ◽  
E. V. Fischer ◽  
B. Finley
Keyword(s):  
Boundary Layer ◽  
North America ◽  
Gulf Of Alaska ◽  
Aleutian Islands ◽  
Transport Pathways ◽  
North American Continent ◽  
Mixing Ratios ◽  
The North ◽  
Synoptic Conditions ◽  
The Difference

Abstract. Nitrogen oxide (NOx=NO+NO2) observations were made at the Mt. Bachelor Observatory in central Oregon, USA (MBO; 2.73 km above sea level) during one autumn and three springtime (15 April–20 May) periods. This is the first study to discuss interannual variability in NOx for this region. NOx concentrations (mean±1σ) for spring 2007, 2008 and 2009 were 119±65, 117±65, and 91±54 pptv, respectively. The difference in mean mixing ratios between 2007 and 2008 is not statistically significant, whereas the difference between these years and 2009 is significant (p<0.01). We attribute the decline in NOx from 2007–2008 to 2009 to changes in free tropospheric synoptic conditions over the Northeast Pacific and trans-Pacific transport pathways during spring 2009. In 2009, there were: (1) higher geopotential heights over the Gulf of Alaska, (2) warmer temperatures over the Aleutian Islands/Gulf of Alaska and (3) much weaker winds throughout the North Pacific. During the autumn 2008 campaign, NOx concentrations (mean±1σ) were 175±548 pptv. The highly non-normal distribution of data (skewness coefficient of 19.1 vs. 2.5, 2.8 and 2.4 in spring 2007, 2008 and 2009, respectively) resulted from periods of very high NOx levels. Using MODIS Rapid Response (Aqua and Terra) results, we show that during autumn our site can be heavily influenced by wildfires in western North America. This is in contrast to springtime, when the smaller positive (i.e., right) tail of the NOx distribution is driven largely by Asian long-range transport (ALRT) events. We developed a novel means of segregating boundary layer (BL)-influenced vs. free tropospheric (FT) air. During spring 2008 we collected "chairlift soundings" of temperature, relative humidity and pressure in an effort to better understand the diurnal pattern of a BL influence at our summit station. Results from this experiment revealed that, on average, a BL influence begins around 10:00 PDT (UTC – 07:00 h) in spring. Using this information to isolate FT air, we characterize probable pollution sources and synoptic conditions for the top 20 FT NOx events over three spring campaigns. Half (n=10) of these 20 events were determined to be "Imported" events characterized by anomalously: (1) high geopotential heights off the west coast of North America, (2) warm temperatures stretching from the Aleutian Islands to Baja California, and (3) strong southwesterly winds in the Asian outflow region. Five events exhibited an influence from the North American continent. These events are characterized by very strong cyclonic behavior off the northwestern USA coast.

scholarly journals Wet scavenging of SO<sub>2</sub> emissions around India's largest lignite based power plant

2010 ◽  
Vol 25 ◽  
pp. 65-70 ◽  
Author(s):  
A. Rai ◽  
S. Ghosh ◽  
S. Chakraborty
Keyword(s):  
Boundary Layer ◽  
Power Plant ◽  
Sulphur Dioxide ◽  
Power Plants ◽  
Climate Models ◽  
South East Asia ◽  
The North ◽  
Large Eddy ◽  
North Eastern ◽  
Wet Scavenging

Abstract. The Neyveli Lignite Corporation (NLC) is among the largest lignite based power plants in South East Asia. The four elevated stacks from this power plant emanate a substantial amount of sulphur dioxide into a tropical boundary layer. Sulphur dioxide being a soluble pollutant gas is absorbed by falling raindrops. This is a first study that quantifies the scavenging action of the North Eastern monsoonal rains from a lignite based power plant. We find that although the North Eastern monsoonal rains have a preponderance of very large droplets, the contribution of the small droplets cannot be neglected. We expect that the estimated scavenging coefficients can be used by large eddy and climate models.

scholarly journals Nitrogen oxides in the boundary layer and free troposphere at the Mt. Bachelor Observatory

2010 ◽  
Vol 10 (2) ◽  
pp. 5751-5801 ◽  
Author(s):  
D. R. Reidmiller ◽  
D. A. Jaffe ◽  
E. V. Fischer ◽  
B. Finley
Keyword(s):  
Boundary Layer ◽  
North America ◽  
Gulf Of Alaska ◽  
Aleutian Islands ◽  
Transport Pathways ◽  
North American Continent ◽  
Mixing Ratios ◽  
The North ◽  
Synoptic Conditions ◽  
The Difference

Abstract. Nitrogen oxide (NOx = NO + NO2) observations were made at the Mt. Bachelor Observatory in central Oregon, USA (MBO; 2.73 km above sea level) during one autumn and three springtime (15 April–20 May) periods. This is the first study to discuss interannual variability in NOx for this region. NOx concentrations (mean ±1σ) for spring 2007, 2008 and 2009 were 119±65, 117±65, and 91±54 pptv, respectively. The difference in mean mixing ratios between 2007 and 2008 is not statistically significant, whereas the difference between these years and 2009 is significant (p<0.01). We attribute the decline in NOx from 2007–2008 to 2009 to changes in free tropospheric synoptic conditions over the Northeast Pacific and trans-Pacific transport pathways during spring 2009. In 2009, there were: (1) higher geopotential heights over the Gulf of Alaska, (2) warmer temperatures over the Aleutian Islands/Gulf of Alaska and (3) much weaker winds throughout the North Pacific. During the autumn 2008 campaign, NOx concentrations (mean ±1σ) were 175±548 pptv. The highly non-normal distribution of data (skewness coefficient of 19.1 vs. 2.5, 2.8 and 2.4 in spring 2007, 2008 and 2009, respectively) resulted from periods of very high NOx levels. Using MODIS Rapid Response (Aqua and Terra) results, we show that during autumn our site can be heavily influenced by wildfires in western North America. This is in contrast to springtime, when the smaller positive (i.e., right) tail of the NOx distribution is driven largely by Asian long-range transport (ALRT) events. We developed a novel means of segregating boundary layer (BL)-influenced vs. free tropospheric (FT) air. During spring 2008 we collected "chairlift soundings" of temperature, relative humidity and pressure in an effort to better understand the diurnal pattern of a BL influence at our summit station. Results from this experiment revealed that, on average, a BL influence begins around 10:00 PDT (UTC – 7 h) in spring. Using this information to isolate FT air, we characterize probable pollution sources and synoptic conditions for the top 20 FT NOx events over three spring campaigns. Half (n = 10) of these 20 events were determined to be "Imported" events characterized by anomalously: (1) high geopotential heights off the west coast of North America, (2) warm temperatures stretching from the Aleutian Islands to Baja California, and (3) strong southwesterly winds in the Asian outflow region. Five events exhibited an influence from the North American continent. These events are characterized by very strong cyclonic behavior off the northwestern USA coast.

scholarly journals In situ observations of CH<sub>2</sub>Cl<sub>2</sub> and CHCl<sub>3</sub> show efficient transport pathways for very short-lived species into the lower stratosphere via the Asian and North American summer monsoons

2021 ◽  
Author(s):  
Valentin Lauther ◽  
Bärbel Vogel ◽  
Johannes Wintel ◽  
Andrea Rau ◽  
Peter Hoor ◽  
...  
Keyword(s):  
North American ◽  
Lower Stratosphere ◽  
Stratospheric Ozone ◽  
Late Summer ◽  
Anthropogenic Sources ◽  
North American Monsoon ◽  
Transport Pathway ◽  
Transport Pathways ◽  
Mixing Ratios ◽  
The North

Abstract. Efficient transport pathways for ozone depleting very short-lived substances (VSLS) from their source regions into the stratosphere are a matter of current scientific debate, however they have yet to be fully identified on an observational basis. Understanding the increasing impact of chlorine containing VSLS (Cl-VSLS) on stratospheric ozone depletion is important in order to validate and improve model simulations and future predictions. We report on the first transport study using airborne in situ measurements of the Cl-VSLS dichloromethane (CH2Cl2) and trichloromethane (chloroform, CHCl3) to derive a detailed description of the two most efficient and fast transport pathways from (sub-)tropical source regions into the extratropical lower stratosphere (Ex-LS) in northern hemisphere (NH) late summer. The Cl-VSLS measurements were obtained in the upper troposphere and lower stratosphere (UTLS) above Western Europe and the mid latitude Atlantic Ocean in the frame of the WISE (Wave-driven ISentropic Exchange) aircraft campaign in autumn 2017 and are combined with the results from a three-dimensional simulation of a Lagrangian transport model as well as back-trajectory calculations. Compared to background measurements of similar age we find up to 150 % enhanced CH2Cl2 and up to 100 % enhanced CHCl3 mixing ratios in the Ex-LS. We link the measurements of enhanced mixing ratios to emissions in the region of southern and eastern Asia. Transport from this area to the Ex-LS at potential temperatures in the range of 370–400 K takes about 5–10 weeks via the Asian summer monsoon anticyclone (ASMA). Our measurements suggest anthropogenic sources to be the cause of these strongly elevated Cl-VSLS concentrations observed at the top of the lowermost stratosphere (LMS). A faster transport pathway into the Ex-LS is derived from particularly low CH2Cl2 and CHCl3 mixing ratios in the UTLS. These low mixing ratios reflect weak emission sources and a local seasonal minimum of both species in the boundary layer of Central America and the tropical Atlantic. We show that air masses uplifted by hurricanes, the North American monsoon, and general convection above Central America into the tropical tropopause layer to potential temperatures of about 360–370 K are transported isentropically within 1–5 weeks into the Ex-LS. This transport pathway linked to the North American monsoon mainly impacts the middle and lower part of the LMS with particularly low CH2Cl2 and CHCl3 mixing ratios. In a case study, we specifically analyze air samples directly linked to the uplift by the category 5 hurricane Maria that occurred during October 2017 above the Atlantic Ocean. Regionally differing CHCl3 : CH2Cl2 emission ratios derived from our UTLS measurements suggest a clear similarity between CHCl3 and CH2Cl2 when emitted by anthropogenic sources and differences between the two species mainly caused by additional, likely biogenic, CHCl3 sources. Overall, the transport of strongly enhanced CH2Cl2 and CHCl3 mixing ratios from southern and eastern Asia via the ASMA is the main factor for increasing the chlorine loading from the analyzed VSLS in the Ex-LS during NH late summer. Thus, further increases in Asian CH2Cl2 and CHCl3 emissions, as frequently reported in recent years, will further increase the impact of Cl-VSLS on stratospheric ozone depletion.

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