scholarly journals Impacts of long-range transport of aerosols on marine-boundary-layer clouds in the eastern North Atlantic

2020 ◽  
Vol 20 (23) ◽  
pp. 14741-14755
Author(s):  
Yuan Wang ◽  
Xiaojian Zheng ◽  
Xiquan Dong ◽  
Baike Xi ◽  
Peng Wu ◽  
...  

Abstract. Vertical profiles of aerosols are inadequately observed and poorly represented in climate models, contributing to the current large uncertainty associated with aerosol–cloud interactions. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) aircraft field campaign near the Azores islands provided ample observations of vertical distributions of aerosol and cloud properties. Here we utilize the in situ aircraft measurements from the ACE-ENA and ground-based remote-sensing data along with an aerosol-aware Weather Research and Forecast (WRF) model to characterize the aerosols due to long-range transport over a remote region and to assess their possible influence on marine-boundary-layer (MBL) clouds. The vertical profiles of aerosol and cloud properties measured via aircraft during the ACE-ENA campaign provide detailed information revealing the physical contact between transported aerosols and MBL clouds. The European Centre for Medium-Range Weather Forecasts Copernicus Atmosphere Monitoring Service (ECMWF-CAMS) aerosol reanalysis data can reproduce the key features of aerosol vertical profiles in the remote region. The cloud-resolving WRF sensitivity experiments with distinctive aerosol profiles suggest that the transported aerosols and MBL cloud interactions (ACIs) require not only aerosol plumes to get close to the marine-boundary-layer top but also large cloud top height variations. Based on those criteria, the observations show that the occurrence of ACIs involving the transport of aerosol over the eastern North Atlantic (ENA) is about 62 % in summer. For the case with noticeable long-range-transport aerosol effects on MBL clouds, the susceptibilities of droplet effective radius and liquid water content are −0.11 and +0.14, respectively. When varying by a similar magnitude, aerosols originating from the boundary layer exert larger microphysical influence on MBL clouds than those entrained from the free troposphere.

2020 ◽  
Author(s):  
Yuan Wang ◽  
Xiaojian Zheng ◽  
Xiquan Dong ◽  
Baike Xi ◽  
Peng Wu ◽  
...  

Abstract. Vertical profiles of aerosols are inadequately observed and poorly represented in climate models, contributing to the current large uncertainty associated with aerosol-cloud interactions. The DOE ARM Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) aircraft field campaign near the Azores islands provided ample accurate observations of vertical distributions of aerosol and cloud properties. Here we utilize the in situ aircraft measurements from the ACE-ENA and ground-based remote sensing data along with an aerosol-aware Weather Research and Forecast (WRF) model to characterize the aerosols due to long-range transport over a remote region and to assess their possible influence on marine boundary-layer (MBL) clouds. The vertical profiles of aerosol and cloud properties measured via aircraft during the ACE-ENA campaign provide detailed information revealing the physical contact between transported aerosols and MBL clouds. The ECMWF-CAMS aerosol reanalysis data can reproduce the key features of aerosol vertical profiles in the remote region. The cloud-resolving WRF sensitivity experiments with distinctive aerosol profiles suggest that the transported aerosols and MBL cloud interactions (ACI) require not only low-altitude aerosol preferably getting close to the marine boundary layer top, but also large cloud top height variations. Based on those criteria, the observations show the occurrence of ACI involving the transport of aerosol over the Eastern North Atlantic is about 62 % in summer. For the case with noticeable long-range transport aerosol effect on MBL cloud, the susceptibilities of droplet effective radius and liquid water content are −0.11 and +0.14, respectively. When varying on the similar magnitude, aerosols originating from the boundary layer exert larger microphysical influence on MBL clouds than those entrained from free troposphere.


2004 ◽  
Vol 4 (4) ◽  
pp. 4407-4454 ◽  
Author(s):  
S. A. Penkett ◽  
M. J. Evans ◽  
C. E. Reeves ◽  
K. S. Law ◽  
P. S. Monks ◽  
...  

Abstract. This paper presents strong experimental evidence for a major perturbation in ozone concentrations over large parts of the North Atlantic Ocean from the surface to 8 km associated with continental pollutants. The evidence was gathered in the course of 7 flights by the UK Meteorological Office C-130 aircraft based on the Azores, and 4 ferry flights between the UK to the Azores in spring and summer 1997 as a component of the NERC-funded ACSOE project. The total latitude range covered was approximately 55°N–25°N, and the longitude range was approximately 0° to 40°W. Many profiles were made between the sea surface and altitudes up to 9 km to survey the composition of the marine atmosphere. The C-130 aircraft was comprehensively equipped to measure many chemical and physical parameters along with standard meteorological instrumentation. Thus it was able to measure ozone and speciated NOy, along with tracers including water vapour, carbon monoxide and condensation nuclei, in near real time. The overall "picture" of the troposphere over large parts of the North Atlantic is of layers of pollution from the continents of different ages interspersed with layers of air uplifted from the marine boundary layer. The lowest ozone concentrations were recorded in the marine boundary layer where there is evidence for extensive ozone destruction in summer. Flights were made to penetrate the outflow of hurricane Erica, to determine the southerly extent of polluted air in summer, to examine the impact of frontal systems on the composition of remote marine air, and to trace long-range pollution from the west coast of the USA interspersed with air with a stratospheric origin. In one of the spring flights it is possible that a plume of polluted air with high ozone and NOy, and with an origin in southeast Asia, was intercepted off the coast of Portugal. The concentrations of NOx, in this plume were sufficient for ozone formation to be continuing along its track from west to east. The instrument to measure NOy almost certainly was only measuring the sum of organic nitrates (mostly in the form of PAN) plus NOx. The high correlation between NOy and ozone under these conditions strongly suggests a non-stratospheric source for most of the ozone encountered over large parts of the atmosphere upwind of Europe. There was a marked seasonal variation in the NOy with about twice as much present in the spring flights than in the summer flights. The overall ozone levels in both spring and summer were somewhat similar although the highest ozone concentration encountered (~100 ppbv) was observed in summer in some polluted layers in mid Atlantic with an origin in the boundary layer over the southeastern USA. The bulk of the pollutants, ozone, CO, and NOy, were in the free troposphere at altitudes between 3 and 8 km. The only instances of pollution at lower levels were in the form of ship plumes, which were encountered several times. The data therefore strongly support the need for more in-situ aircraft experiments to quantify and understand the phenomenon of long-range transport of pollution from continent to continent. Observations at ground-based stations are inadequate for this purpose and satellite data is incomplete both in terms of its altitude detail and in the extent of chemical speciation, particularly for ascertaining whether chemical production and destruction processes for ozone are occurring.


2020 ◽  
Vol 139 ◽  
pp. 105680 ◽  
Author(s):  
Guangjie Zheng ◽  
Arthur J. Sedlacek ◽  
Allison C. Aiken ◽  
Yan Feng ◽  
Thomas B. Watson ◽  
...  

2014 ◽  
Vol 119 (14) ◽  
pp. 9142-9167 ◽  
Author(s):  
Rebecca M. C. Simpson ◽  
Steven G. Howell ◽  
Byron W. Blomquist ◽  
Antony D. Clarke ◽  
Barry J. Huebert

2021 ◽  
Author(s):  
Yang Wang ◽  
Guangjie Zheng ◽  
Michael Jensen ◽  
Daniel Knopf ◽  
Alexander Laskin ◽  
...  

Abstract. Because of their extensive coverage, marine low clouds greatly impact the global climate. Presently, the response of marine low clouds to the changes in atmospheric aerosols remains a major source of uncertainty in climate simulations. One key contribution to this large uncertainty derives from the poor understanding of the properties and processes of marine aerosols under natural conditions, and the perturbation by anthropogenic emissions. The Eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer (MBL) clouds, where cloud albedo and precipitation are highly susceptible to perturbations in aerosol properties. Here we examine the key processes that drive the cloud condensation nuclei (CCN) population in the MBL using comprehensive characterizations of aerosol and trace gas vertical profiles during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. During ACE-ENA, a total of 39 research flights were conducted in the Azores, 20 during summer 2017, and 19 during winter 2018. During summer, long-range transported aerosol layers were periodically observed in the lower free troposphere (FT), leading to elevated FT CCN concentrations (NCCN). Both biomass burning and pollution from North America contribute to submicron aerosol mass in these layers, with pollution likely the dominant contributor. In contrast, long-range transported continental emissions have a much weaker influence on the aerosol properties in the ENA during the winter season. While the entrainment of FT air is a major source of particle number in the MBL for both seasons, on average, it does not serve as a direct source of CCN in the MBL because the average FT NCCN is the same or even lower than that in the MBL. The particle number flux due to FT entrainment is dominated by pre-CCN (particles that are too small to form cloud droplets under typical conditions, i.e., particles with sizes below the Hoppel minimum) due to the elevated Npre-CCN in the lower FT. Once these pre-CCN are entrained into the MBL, they can grow and reach CCN size range through condensational growth, representing an indirect and major source of MBL CCN at ENA. The impact of synoptic condition on the aerosol properties is examined. Under pre-front and post-front conditions, shallow convective activity often leads to a deep and decoupled boundary layer. Coalescence scavenging and evaporation of drizzle below clouds leads to much reduced NCCN and larger accumulation-mode particle sizes in the upper, cloud-containing decoupled layer, indicating that surface measurements overestimate the NCCN relevant to the formation of MBL clouds under decoupled conditions.


2021 ◽  
Vol 21 (14) ◽  
pp. 11079-11098
Author(s):  
Yang Wang ◽  
Guangjie Zheng ◽  
Michael P. Jensen ◽  
Daniel A. Knopf ◽  
Alexander Laskin ◽  
...  

Abstract. Because of their extensive coverage, marine low clouds greatly impact the global climate. Presently, the response of marine low clouds to the changes in atmospheric aerosols remains a major source of uncertainty in climate simulations. One key contribution to this large uncertainty derives from the poor understanding of the properties and processes of marine aerosols under natural conditions and the perturbation by anthropogenic emissions. The eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer (MBL) clouds, where cloud albedo and precipitation are highly susceptible to perturbations in aerosol properties. Here we examine the key processes that drive the cloud condensation nuclei (CCN) population in the MBL using comprehensive characterizations of aerosol and trace gas vertical profiles during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. During ACE-ENA, a total of 39 research flights were conducted in the Azores: 20 during summer 2017 and 19 during winter 2018. During summer, long-range-transported aerosol layers were periodically observed in the lower free troposphere (FT), leading to elevated FT CCN concentrations (NCCN). Both biomass burning and pollution from North America contribute to submicron aerosol mass in these layers, with pollution likely the dominant contributor. In contrast, long-range transported continental emissions have a much weaker influence on the aerosol properties in the ENA during the winter season. While the entrainment of FT air is a major source of particle number in the MBL for both seasons, on average it does not serve as a direct source of CCN in the MBL because the average FT NCCN is the same or even lower than that in the MBL. The particle number flux due to FT entrainment is dominated by pre-CCN (particles that are too small to form cloud droplets under typical conditions, i.e., particles with sizes below the Hoppel minimum) due to the elevated Npre-CCN in the lower FT. Once these pre-CCN are entrained into the MBL, they can grow and reach CCN size range through condensational growth, representing an indirect and major source of MBL CCN in the ENA. The impact of synoptic conditions on the aerosol properties is examined. Under pre-front and post-front conditions, shallow convective activity often leads to a deep and decoupled boundary layer. Coalescence scavenging and evaporation of drizzle below clouds lead to reduced NCCN and larger accumulation-mode particle sizes in the upper cloud-containing decoupled layer, indicating that surface measurements overestimate the NCCN relevant to the formation of MBL clouds under decoupled conditions.


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.


Author(s):  
Hervé Petetin ◽  
Bastien Sauvage ◽  
Mark Parrington ◽  
Hannah Clark ◽  
Alain Fontaine ◽  
...  

<p><strong>Abstract.</strong> This study investigates the role of biomass burning and long-range transport in the anomalies of carbon monoxide (CO) regularly observed along the tropospheric vertical profiles measured in the framework of IAGOS. Considering the high interannual variability of biomass burning emissions and the episodic nature of pollution long-range transport, one strength of this study is the amount of data taken into account, namely 30,000 vertical profiles at 9 clusters of airports in Europe, North America, Asia, India and southern Africa over the period 2002&amp;ndash;2017. </p> <p> As a preliminary, a brief overview of the spatio-temporal variability, latitudinal distribution, interannual variability and trends of biomass burning CO emissions from 14 regions is provided. The distribution of CO mixing ratios at different levels of the troposphere is also provided based on the entire IAGOS database (125 million CO observations). </p> <p> This study focuses on the free troposphere (altitudes above 2<span class="thinspace"></span>km) where the long-range transport of pollution is favoured. Anomalies at a given airport cluster are here defined as departures from the local seasonally-averaged climatological vertical profile. The intensity of these anomalies varies significantly depending on the airport, with maximum (minimum) CO anomalies of 110&amp;ndash;150 (48)<span class="thinspace"></span>ppbv in Asia (Europe). Looking at the seasonal variation of the frequency of occurrence, the 25<span class="thinspace"></span>% strongest CO anomalies appears reasonably well distributed along the year, in contrast to the 5<span class="thinspace"></span>% or 1<span class="thinspace"></span>% strongest anomalies that exhibit a strong seasonality with for instance more frequent anomalies during summertime in northern United-States, during winter/spring in Japan, during spring in South-east China, during the non-monsoon seasons in south-east Asia and south India, and during summer/fall at Windhoek, Namibia. Depending on the location, these strong anomalies are observed in different parts of the free troposphere. </p> <p> In order to investigate the role of biomass burning emissions in these anomalies, we used the SOFT-IO v1.0 IAGOS added-value products that consist of FLEXPART 20-days backward simulations along all IAGOS aircraft trajectories, coupled with anthropogenic (MACCity) and biomass burning (GFAS) CO emission inventories and vertical injections. SOFT-IO estimates the contribution (in ppbv) of the recent (less than 20 days) primary worldwide CO emissions, tagged per source region. Biomass burning emissions are found to play an important role in the strongest CO anomalies observed at most airport clusters. The regional tags indicate a large contribution from boreal regions at airport clusters in Europe and North America during summer season. In both Japan and south India, the anthropogenic emissions dominate all along the year, except for the strongest summertime anomalies observed in Japan that are due to Siberian fires. The strongest CO anomalies at airport clusters located in south-east Asia are induced by fires burning during spring in south-east Asia and during fall in equatorial Asia. In southern Africa, the Windhoek airport was mainly impacted by fires in southern hemisphere Africa and South America. </p> <p> To our knowledge, no other studies have used such a large dataset of in situ vertical profiles for deriving a climatology of the impact of biomass burning versus anthropogenic emissions on the strongest CO anomalies observed in the troposphere, in combination with information on the source regions. This study therefore provides both qualitative and quantitative information for interpreting the highly variable CO vertical distribution in several regions of interest.</p>


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