scholarly journals Sensitivity of free tropospheric carbon monoxide to atmospheric weather states and their persistency: an observational assessment over the Nordic countries

2014 ◽  
Vol 14 (21) ◽  
pp. 11545-11555 ◽  
Author(s):  
M. A. Thomas ◽  
A. Devasthale

Abstract. Among various factors that influence the long-range transport of pollutants in the free troposphere (FT), the prevailing atmospheric weather states probably play the most important role in governing characteristics and efficacy of such transport. The weather states, such as a particular wind pattern, cyclonic or anticyclonic conditions, and their degree of persistency determine the spatio-temporal distribution and the final fate of the pollutants. This is especially true in the case of Nordic countries, where baroclinic disturbances and associated weather fronts primarily regulate local meteorology, in contrast to the lower latitudes where a convective paradigm plays a similarly important role. Furthermore, the long-range transport of pollutants in the FT has significant contribution to the total column burden over the Nordic countries. However, there is insufficient knowledge on the large-scale co-variability of pollutants in the FT and atmospheric weather states based solely on observational data over this region. The present study attempts to quantify and understand this statistical co-variability while providing relevant meteorological background. To that end, we select eight weather states that predominantly occur over the Nordic countries and three periods of their persistency (3 days, 5 days, and 7 days), thus providing in total 24 cases to investigate sensitivity of free tropospheric carbon monoxide, an ideal tracer for studying pollutant transport, to these selected weather states. The eight states include four dominant wind directions (namely, NW, NE, SE and SW), cyclonic and anticyclonic conditions, and the enhanced positive and negative phases of the North Atlantic Oscillation (NAO). For our sensitivity analysis, we use recently released Version 6 retrievals of CO at 500 hPa from the Atmospheric Infrared Sounder (AIRS) onboard Aqua satellite covering the 11-year period from September 2002 through August 2013 and winds from the ECMWF's ERA-Interim project to classify weather states for the same 11-year period. We show that, among the various weather states studied here, southeasterly winds lead to highest observed CO anomalies (up to +8%) over the Nordic countries while transporting pollution from the central and eastern parts of Europe. The second (up to +4%) and third highest (up to +2.5%) CO anomalies are observed when winds are northwesterly (facilitating inter-continental transport from polluted North American regions) and during the enhanced positive phase of the NAO respectively. Higher than normal CO anomalies are observed during anticyclonic conditions (up to +1%) compared to cyclonic conditions. The cleanest conditions are observed when winds are northeasterly and during the enhanced negative phases of the NAO, when relatively clean Arctic air masses are transported over the Nordic regions in the both cases. In the case of nearly all weather states, the CO anomalies consistently continue to increase or decrease as the degree of persistency of a weather state is increased. The results of this sensitivity study further provide an observational basis for the process-oriented evaluation of chemistry transport models, especially with regard to the representation of large-scale coupling of chemistry and local weather states and its role in the long-range transport of pollutants in such models.

2014 ◽  
Vol 14 (7) ◽  
pp. 9249-9274
Author(s):  
M. A. Thomas ◽  
A. Devasthale

Abstract. Among various factors that influence the long-range transport of pollutants in the free troposphere (FT), the prevailing atmospheric weather states probably play the most important role in governing characteristics and efficacy of such transport. The weather states, such as a particular wind pattern, cyclonic or anticyclonic conditions etc, and their degree of persistency determine the spatio-temporal distribution and the final fate of the pollutants. This is especially true in the case of Nordic countries, where baroclinic disturbances and associated weather fronts primarily regulate local meteorology, in contrast to the lower latitudes where convective paradigm plays similar important role. Furthermore, the long-range transport of pollutants in the FT has significant contribution to the total column burden over the Nordic countries. However, there is insufficient knowledge on the large-scale co-variability of pollutants in the FT and atmospheric weather states based solely on observational data over this region. The present study attempts to quantify and understand this statistical co-variability while providing relevant meteorological background. To that end, we select eight weather states that predominantly occur over the Nordic countries and three periods of their persistency (3 days, 5 days, and 7 days), thus providing in total 24 cases to investigate sensitivity of free tropospheric carbon monoxide, an ideal tracer for studying pollutant transport, to these selected weather states. The eight states include four dominant wind directions (namely, NW, NE, SE and SW), cyclonic and anticyclonic conditions, and the enhanced positive and negative phases of the North Atlantic Oscillation (NAO). For our sensitivity analysis, we use recently released Version 6 retrievals of CO at 500 hPa from the Atmospheric Infrared Sounder (AIRS) onboard Aqua satellite covering 11 yr period from September 2002 through August 2013 and winds from the ECMWF's ERA-Interim project to classify weather states for the same 11 yr period. We show that, among the various weather states studied here, southeasterly winds lead to highest observed CO anomalies (up to +8%) over the Nordic countries while transporting pollution from the central and eastern parts of Europe. The second (up to +4%) and third highest (up to +2.5%) CO anomalies are observed when winds are northwesterly (facilitating inter-continental transport from polluted North American regions) and during the enhanced positive phase of the NAO respectively. Higher than normal CO anomalies are observed during anticyclonic conditions (up to +1%) compared to cyclonic conditions. The cleanest conditions are observed when winds are northeasterly and during the enhanced negative phases of the NAO, when relatively clean Arctic air masses are transported over the Nordic regions in the both cases. In case of nearly all weather states, the CO anomalies consistently continue to increase or decrease as the degree of persistency of a weather state is increased. The results of this sensitivity study further provide an observational basis for the process-oriented evaluation of chemistry transport models, especially with regard to the representation of large-scale coupling of chemistry and local weather states and its role in the long-range transport of pollutants in such models.


2021 ◽  
Author(s):  
Leonie Villiger ◽  
Heini Wernli ◽  
Maxi Boettcher ◽  
Martin Hagen ◽  
Franziska Aemisegger

Abstract. Shallow clouds in the trade-wind region over the North Atlantic contribute substantially to the global radiative budget. In the vicinity of the Caribbean island Barbados, they appear in different mesoscale organisation patterns with distinct net cloud radiative effects (CRE). Cloud formation processes in this region are typically controlled by the prevailing large-scale subsidence. However, occasionally weather systems from remote origin cause significant disturbances. This study investigates the complex cloud-circulation interactions during the field campaign EUREC4A (Elucidate the Couplings Between Clouds, Convection and Circulation) from 16 January to 20 February 2020, using a combination of Eulerian and Lagrangian diagnostics. Based on observations and ERA5 reanalyses, we identify the relevant processes and characterise the formation pathways of two moist anomalies above the Barbados Cloud Observatory (BCO), one in the lower (~1000–650 hPa) and one in the middle troposphere (~650–300 hPa). These moist anomalies are associated with strongly negative CRE values and with contrasting long-range transport processes from the extratropics and the tropics, respectively. The low-level moist anomaly is characterised by an unusually thick cloud layer, high precipitation totals and a strongly negative CRE. Its formation is connected to an “extratropical dry intrusion” (EDI) that interacts with a trailing cold front. A quasi-climatological (2010–2020) analysis reveals that EDIs lead to different conditions at the BCO depending on how they interact with the associated cold front. Based on this climatology, we discuss the relevance of the strong large-scale forcing by EDIs for the low-cloud patterns near the BCO and the related CRE. The second case study about the mid-tropospheric moist anomaly is associated with an extended and persistent mixed-phase shelf cloud and the lowest daily CRE value observed during the campaign. Its formation is linked to “tropical mid-level detrainment” (TMD), which refers to detrainment from tropical deep convection near the melting layer. The quasi-climatological analysis shows that TMDs consistently lead to mid-tropospheric moist anomalies over the BCO and that the detrainment height controls the magnitude of the anomaly. However, no systematic relationship was found between the amplitude of this mid-tropospheric moist anomaly and the CRE at the BCO. Overall, this study reveals the important impact of the long-range transport, driven by dynamical processes either in the extratropics or the tropics, on the variability of the vertical structure of moisture and clouds, and on the resulting CRE in the North Atlantic winter trades.


2017 ◽  
Vol 17 (21) ◽  
pp. 13233-13263 ◽  
Author(s):  
Uri Dayan ◽  
Philippe Ricaud ◽  
Régina Zbinden ◽  
François Dulac

Abstract. The eastern Mediterranean (EM) is one of the regions in the world where elevated concentrations of primary and secondary gaseous air pollutants have been reported frequently, mainly in summer. This review discusses published studies of the atmospheric dispersion and transport conditions characterizing this region during the summer, followed by a description of some essential studies dealing with the corresponding concentrations of air pollutants such as ozone, carbon monoxide, total reactive nitrogen, methane, and sulfate aerosols observed there. The interlaced relationship between the downward motion of the subsiding air aloft induced by global circulation systems affecting the EM and the depth of the Persian Trough, a low-pressure trough that extends from the Asian monsoon at the surface controlling the spatiotemporal distribution of the mixed boundary layer during summer, is discussed. The strength of the wind flow within the mixed layer and its depth affect much the amount of pollutants transported and determine the potential of the atmosphere to disperse contaminants off their origins in the EM. The reduced mixed layer and the accompanying weak westerlies, characterizing the summer in this region, led to reduced ventilation rates, preventing an effective dilution of the contaminants. Several studies pointing at specific local (e.g., ventilation rates) and regional peculiarities (long-range transport) enhancing the build-up of air pollutant concentrations are presented. Tropospheric ozone (O3) concentrations observed in the summer over the EM are among the highest over the Northern Hemisphere. The three essential processes controlling its formation (i.e., long-range transport of polluted air masses, dynamic subsidence at mid-tropospheric levels, and stratosphere-to-troposphere exchange) are reviewed. Airborne campaigns and satellite-borne initiatives have indicated that the concentration values of reactive nitrogen identified as precursors in the formation of O3 over the EM were found to be 2 to 10 times higher than in the hemispheric background troposphere. Several factors favor sulfate particulate abundance over the EM. Models, aircraft measurements, and satellite-derived data have clearly shown that sulfate has a maximum during spring and summer over the EM. The carbon monoxide (CO) seasonal cycle, as obtained from global background monitoring sites in the EM, is mostly controlled by the tropospheric concentration of the hydroxyl radical (OH) and therefore demonstrates high concentrations over winter months and the lowest concentrations during summer when photochemistry is active. Modeling studies have shown that the diurnal variations in CO concentration during the summer result from long-range CO transport from European anthropogenic sources, contributing 60 to 80 % of the boundary-layer CO over the EM. The values retrieved from satellite data enable us to derive the spatial distribution of methane (CH4), identifying August as the month with the highest levels over the EM. The outcomes of a recent extensive examination of the distribution of methane over the tropospheric Mediterranean Basin, as part of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx) program, using model simulations and satellite measurements, are coherent with other previous studies. Moreover, this methane study provides some insight into the role of the Asian monsoon anticyclone in controlling the variability of CH4 pollutant within mid-to-upper tropospheric levels above the EM in summer.


2011 ◽  
Vol 8 (3) ◽  
pp. 5537-5562 ◽  
Author(s):  
Z. Xie ◽  
B. P. Koch ◽  
A. Möller ◽  
R. Sturm ◽  
R. Ebinghaus

Abstract. Hexachlorocyclohexanes (HCHs) are ubiquitous organic pollutants derived from pesticide application. They are subject to long-range transport, persistent in the environment, and capable of accumulation in biota. Shipboard measurements of HCH isomers (α-, γ- and β-HCH) in surface seawater and boundary layer atmospheric samples were conducted in the Atlantic and the Southern Ocean in October to December of 2008. ΣHCHs concentrations (the sum of α-, γ- and β-HCH) in the lower atmosphere ranged from 11.8 to 36.9 pg m−3 (mean: 26.6 ± 11.0 pg m−3) in the Northern Hemisphere (NH), and from 1.5 to 4.0 pg m−3 (mean: 2.8 ± 1.1 pg m−3) in the Southern Hemisphere (SH), respectively. Water concentrations were: α-HCH 0.33–46.8 pg l−1, γ-HCH 0.02–33.2 pg l−1 and β-HCH 0.11–2 pg l−1. HCH concentrations decreased from the North Atlantic to the Southern Ocean, indicating historical use of HCHs in the NH. Spatial distribution showed increasing concentrations from the equator towards North and South latitudes illustrating the concept of cold condensation and less interhemispheric mixing process. In comparison to concentrations measured in 1987–1999/2000, gaseous HCHs were slightly lower, while dissolved HCHs decreased by factor of 2–3 orders of magnitude. Air-water exchange gradients suggested net deposition for α-HCH (mean: 3759 pg m−2 day−1) and γ-HCH (mean: 1987 pg m−2 day−1), whereas β-HCH varied between equilibrium (volatilization: <0–12 pg m−2 day−1) and net deposition (range: 6–687 pg m−2 day−1), indicating a multi-hopper transport behavior. Climate change may significantly accelerate the releasing process of "old" HCHs from continental storage (e.g. soil, vegetation and high mountains) and drive long-range transport from sources to deposition in the open oceans. Biological productivities may interfere with the air-water exchange process as well. Consequently, further investigation is necessary to elucidate the long term trends and the biogeochemical turnover of HCHs in the oceanic environment.


2016 ◽  
Author(s):  
Leonardo A. Mingari ◽  
Estela A. Collini ◽  
Arnau Folch ◽  
Walter Báez ◽  
Emilce Bustos ◽  
...  

Abstract. On the 13 June 2015, the London Volcanic Ash Advisory Centre (VAAC) warned the Buenos Aires VAAC about a possible volcanic eruption from the Nevados Ojos del Salado volcano (6879 m), located in the Andes mountain range on the border between Chile and Argentina. A volcanic ash cloud was detected by the SEVIRI instrument on board the Meteosat Second Generation (MSG) satellites from 14:00 UTC on 13 June. Further studies concluded that the phenomenon was caused by remobilization of ancient pyroclastic deposits (circa 4.5 Ka Cerro Blanco eruption) from the Bolsón de Fiambalá (Fiambalá Basin) in northwestern Argentina. In this paper, we provide the first comprehensive description of the dust episode through observations and numerical simulations. We have investigated the spatio-temporal distribution of aerosols and the emission process over complex terrain to gain insight into the key role played by the orography and the condition that triggered the long-range transport episode. Numerical simulations of windblown dust were performed using the WRF-ARW/FALL3D modeling system with meteorological fields downscaled to a spatial resolution of 2 km in order to resolve the complex orography of the area. Results indicated that favourable conditions to generate dust uplifting occurred in northern Fiambalá Basin, where orographic effects caused strong surface winds. According to short-range numerical simulations, dust particles were confined to near-ground layers around the emission areas. On the other hand, dust aerosols were injected up to 5–6 km high in central and southern regions of the Fiambalá Basin, where intense ascending airflows are driven by horizontal convergence. Long-range transport numerical simulations were also performed to model dust cloud spreading over northern Argentina. Results of simulated vertical particle column mass were compared with the MSG-SEVIRI retrieval product. We tested two numerical schemes: with the default configuration of the FALL3D model, we found difficulties to simulate transport through orographic barriers, whereas an alternative configuration, using a numerical scheme to more accurately compute the horizontal advection in abrupt terrains, substantially improved the model performance.


2017 ◽  
Author(s):  
Uri Dayan ◽  
Philippe Ricaud ◽  
Regina Zbinden ◽  
Francois Dulac

Abstract. The Eastern Mediterranean (EM) is one of the regions in the world where elevated concentrations of primary and secondary gaseous air pollutants have been reported frequently, mainly in summer. This review discusses published studies of the atmospheric dispersion and transport conditions characterizing this region during the summer, followed by a description of some essential studies dealing with the corresponding concentrations of air pollutants such as ozone, carbon monoxide, total reactive nitrogen, methane and sulfate aerosols observed there. The interlaced relationship between the downward motion of the subsiding air aloft induced by global circulation systems affecting the EM and the depth of the Persian Trough, a low-pressure trough that extends from the Asian monsoon at the surface controlling the spatio-temporal distribution of the mixed boundary layer during summer is discussed. The strength of the wind flow within the mixed layer and its depth affect much the amount of pollutants transported and determine the potential of the atmosphere to disperse contaminants off their origins in the EM. The reduced mixed layer and the accompanying weak westerlies, characterizing the summer in this region, lead to reduced ventilation rates, preventing an effective dilution of the contaminants. Several studies pointing at specific local (e.g. ventilation rates) and regional peculiarities (long-range transport) enhancing the building up of pollutant concentrations are presented. Tropospheric ozone concentrations observed in the summer over the EM are among the highest over the Northern Hemisphere. The three essential processes controlling its formation (i.e., long- range transport of polluted air masses, dynamic subsidence at mid-tropospheric levels, and stratosphere-to-troposphere exchange) are reviewed. Airborne campaigns and satellite-borne initiatives have indicated that the concentration values of reactive nitrogen identified as precursors in the formation of ozone over the EM were found to be 2 to 10 times higher than in the hemispheric background troposphere. Several factors favor sulfate particulate abundance over the EM. Models, aircraft measurements, and satellite derived data, have clearly shown that sulfate has a maximum during spring and summer over the EM. The carbon monoxide (CO) seasonal cycle, as obtained from global background monitoring sites in the EM is mostly controlled by the tropospheric concentration of the hydroxyl radical (OH), and therefore demonstrates high concentrations over winter months and the lowest during summer when photochemistry is active. Modeling studies have shown that the diurnal variations in CO concentration during the summer result from long-range CO transport from European anthropogenic sources, contributing 60 to 80 % of the boundary-layer CO over the EM. The values retrieved from satellite data enable us to derive the spatial distribution of methane (CH4), identifying August as the month with the highest levels over the EM. The outcomes of a recent extensive examination of the distribution of methane over the tropospheric Mediterranean Basin, as part of the Chemical and Aerosol Mediterranean Experiment (ChArMEx) program, using model simulations and satellite measurements is coherent with other previous studies. Moreover, this methane study provides some insights on the role of the Asian monsoon anticyclone in controlling the variability of CH4 pollutant within mid-to-upper tropospheric levels above the EM in summer.


2012 ◽  
Vol 12 (15) ◽  
pp. 7015-7039 ◽  
Author(s):  
M. Cain ◽  
J. Methven ◽  
E. J. Highwood

Abstract. During long-range transport, many distinct processes – including photochemistry, deposition, emissions and mixing – contribute to the transformation of air mass composition. Partitioning the effects of different processes can be useful when considering the sensitivity of chemical transformation to, for example, a changing environment or anthropogenic influence. However, transformation is not observed directly, since mixing ratios are measured, and models must be used to relate changes to processes. Here, four cases from the ITCT-Lagrangian 2004 experiment are studied. In each case, aircraft intercepted a distinct air mass several times during transport over the North Atlantic, providing a unique dataset and quantifying the net changes in composition from all processes. A new framework is presented to deconstruct the change in O3 mixing ratio (Δ O3) into its component processes, which were not measured directly, taking into account the uncertainty in measurements, initial air mass variability and its time evolution. The results show that the net chemical processing (Δ O3chem) over the whole simulation is greater than net physical processing (Δ O3phys) in all cases. This is in part explained by cancellation effects associated with mixing. In contrast, each case is in a regime of either net photochemical destruction (lower tropospheric transport) or production (an upper tropospheric biomass burning case). However, physical processes influence O3 indirectly through addition or removal of precursor gases, so that changes to physical parameters in a model can have a larger effect on Δ O3chem than Δ O3phys. Despite its smaller magnitude, the physical processing distinguishes the lower tropospheric export cases, since the net photochemical O3 change is −5 ppbv per day in all three cases. Processing is quantified using a Lagrangian photochemical model with a novel method for simulating mixing through an ensemble of trajectories and a background profile that evolves with them. The model is able to simulate the magnitude and variability of the observations (of O3, CO, NOy and some hydrocarbons) and is consistent with the time-average OH following air-masses inferred from hydrocarbon measurements alone (by Arnold et al., 2007). Therefore, it is a useful new method to simulate air mass evolution and variability, and its sensitivity to process parameters.


1997 ◽  
Vol 102 (D23) ◽  
pp. 28637-28649 ◽  
Author(s):  
Yoshizumi Kajii ◽  
Hajime Akimoto ◽  
Yuichi Komazaki ◽  
Shigeru Tanaka ◽  
Hitoshi Mukai ◽  
...  

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