scholarly journals Tropospheric ozone variations at the Nepal climate observatory – pyramid (Himalayas, 5079 m a.s.l.) and influence of stratospheric intrusion events

2010 ◽  
Vol 10 (1) ◽  
pp. 1483-1516 ◽  
Author(s):  
P. Cristofanelli ◽  
A. Bracci ◽  
M. Sprenger ◽  
A. Marinoni ◽  
U. Bonafè ◽  
...  

Abstract. The paper presents the first 2-years of continuous surface ozone (O3) observations and systematic assessment of the influence of stratospheric intrusions (SI) at the Nepal Climate Observatory at Pyramid (NCO-P; 27°57' N, 86°48' E), located in the Southern Himalayas at 5079 m a.s.l. Continuous O3 monitoring has been carried out at this GAW-WMO station in the framework of the Ev-K2-CNR SHARE and UNEP ABC projects since March 2006. Over the period March 2006–February 2008, an average O3 value of 49±12 ppbv (±1δ) was recorded, with a large annual cycle characterized by a maximum during the pre-monsoon (61±9 ppbv) and a minimum during the monsoon (39±10 ppbv). In general, the average O3 diurnal cycles had different shapes in the different seasons, suggesting an important interaction between the synoptic-scale circulation and the local mountain wind regime. Short-term O3 behaviour in the middle/lower troposphere (e.g. at the altitude level of NCO-P) can be significantly affected by deep SI which, representing the most important natural input for tropospheric O3, can also influence the regional atmosphere radiative forcing. To identify days possibly influenced by SI at the NCO-P, analyses were performed on in-situ observations (O3 and meteorological parameters), total column O3 data from OMI satellite and air-mass potential vorticity provided by the LAGRANTO back-trajectory model. In particular, a specially designed statistical methodology was applied to the time series of the observed and modelled stratospheric tracers. On this basis, during the 2-year investigation, 14.1% of analysed days were found to be affected by SI. The SI frequency showed a clear seasonal cycle, with minimum during the summer monsoon (1.2%) and higher values during the rest of the year (21.5%). As suggested by the LAGRANTO analysis, the position of the subtropical jet stream could play an important role in determining the occurrence of deep SI transport on the Southern Himalayas. In order to estimate the fraction of O3 due to air-mass transport from the stratosphere at the NCO-P, the 30 min O3 concentrations recorded during the detected SI days were analysed. In particular, in-situ relative humidity and black carbon observations were used to exclude influence from wet and polluted air-masses transported by up-valley breezes. This analysis led to the conclusion that during SI O3 significantly increased by 27.1% (+13 ppbv) with respect to periods not affected by such events. Moreover, the integral contribution of SI (O3S) to O3 at the NCO-P was also calculated, showing that 13.7% of O3 recorded at the measurement site could be attributed to SI. On a seasonal basis, the lowest SI contributions were found during the summer monsoon (less than 0.1%), while the highest were found during the winter period (24.2%). These results indicated that, during non-monsoon periods, high O3 levels could affect NCO-P during SI, thus influencing the variability of tropospheric O3 over the Southern Himalayas. Being a powerful regional greenhouse gas, these results indicate that the evaluation of the current and future regional climate cannot be assessed without properly taking into account the influence of SI to tropospheric O3 in this important area.

2010 ◽  
Vol 10 (14) ◽  
pp. 6537-6549 ◽  
Author(s):  
P. Cristofanelli ◽  
A. Bracci ◽  
M. Sprenger ◽  
A. Marinoni ◽  
U. Bonafè ◽  
...  

Abstract. The paper presents the first 2 years of continuous surface ozone (O3) observations and systematic assessment of the influence of stratospheric intrusions (SI) at the Nepal Climate Observatory at Pyramid (NCO-P; 27°57' N, 86°48' E), located in the southern Himalayas at 5079 m a.s.l.. Continuous O3 monitoring has been carried out at this GAW-WMO station in the framework of the Ev-K2-CNR SHARE and UNEP ABC projects since March 2006. Over the period March 2006–February 2008, an average O3 value of 49±12 ppbv (±1δ) was recorded, with a large annual cycle characterized by a maximum during the pre-monsoon (61±9 ppbv) and a minimum during the monsoon (39±10 ppbv). In general, the average O3 diurnal cycles had different shapes in the different seasons, suggesting an important interaction between the synoptic-scale circulation and the local mountain wind regime. Short-term O3 behaviour in the middle/lower troposphere (e.g. at the altitude level of NCO-P) can be significantly affected by deep SI which, representing one of the most important natural input for tropospheric O3, can also influence the regional atmosphere radiative forcing. To identify days possibly influenced by SI at the NCO-P, a specially designed statistical methodology was applied to the time series of observed and modelled stratospheric tracers. On this basis, during the 2-year investigation, 14.1% of analysed days were found to be affected by SI. The SI frequency showed a clear seasonal cycle, with minimum during the summer monsoon (1.2%) and higher values during the rest of the year (21.5%). As suggested by back-trajectory analysis, the position of the subtropical jet stream could play an important role in determining the occurrence of deep SI transport on the southern Himalayas. We estimated the fraction of O3 due to SI at the NCO-P. This analysis led to the conclusion that during SI O3 significantly increased by 27.1% (+13 ppbv) with respect to periods not affected by such events. Moreover, the integral contribution of SI (O3S) to O3 at the NCO-P was also calculated, showing that up to 13.7% of O3 recorded at the measurement site could be possibly attributed to SI. On a seasonal basis, the lowest SI contributions were found during the summer monsoon (less than 0.1%), while the highest were found during the winter period (up to 24.2%). Even considering the rather large uncertainty associated with these estimates, the obtained results indicated that, during non-monsoon periods, high O3 levels could affect NCO-P during SI, thus influencing the variability of tropospheric O3 over the southern Himalayas.


2014 ◽  
Vol 14 (17) ◽  
pp. 9249-9258 ◽  
Author(s):  
S. O'Doherty ◽  
M. Rigby ◽  
J. Mühle ◽  
D. J. Ivy ◽  
B. R. Miller ◽  
...  

Abstract. High-frequency, in situ observations from the Advanced Global Atmospheric Gases Experiment (AGAGE), for the period 2003 to 2012, combined with archive flask measurements dating back to 1977, have been used to capture the rapid growth of HFC-143a (CH3CF3) and HFC-32 (CH2F2) mole fractions and emissions into the atmosphere. Here we report the first in situ global measurements of these two gases. HFC-143a and HFC-32 are the third and sixth most abundant hydrofluorocarbons (HFCs) respectively and they currently make an appreciable contribution to the HFCs in terms of atmospheric radiative forcing (1.7 ± 0.04 and 0.7 ± 0.02 mW m−2 in 2012 respectively). In 2012 the global average mole fraction of HFC-143a was 13.4 ± 0.3 ppt (1σ) in the lower troposphere and its growth rate was 1.4 ± 0.04 ppt yr−1; HFC-32 had a global mean mole fraction of 6.2 ± 0.2 ppt and a growth rate of 1.1 ± 0.04 ppt yr−1 in 2012. The extensive observations presented in this work have been combined with an atmospheric transport model to simulate global atmospheric abundances and derive global emission estimates. It is estimated that 23 ± 3 Gg yr−1 of HFC-143a and 21 ± 11 Gg yr−1 of HFC-32 were emitted globally in 2012, and the emission rates are estimated to be increasing by 7 ± 5% yr−1 for HFC-143a and 14 ± 11% yr−1 for HFC-32.


2014 ◽  
Vol 14 (5) ◽  
pp. 6471-6500 ◽  
Author(s):  
S. O'Doherty ◽  
M. Rigby ◽  
J. Mühle ◽  
D. J. Ivy ◽  
B. R. Miller ◽  
...  

Abstract. High frequency, in situ observations from the Advanced Global Atmospheric Gases Experiment (AGAGE), for the period 2003 to 2012, combined with archive flask measurements dating back to 1977, have been used to capture the rapid growth of HFC-143a (CH3CF3) and HFC-32 (CH2F2) mole fractions and emissions into the atmosphere. Here we report the first in situ global measurements of these two gases. HFC-143a and HFC-32 are the third and sixth most abundant HFCs respectively and they currently make an appreciable contribution to the HFCs in terms of atmospheric radiative forcing (1.7 and 0.7 mW m2 in 2012, respectively). In 2012 the global average mole fraction of HFC-143a was 13.4 ± 0.3 ppt (1-sigma) in the lower troposphere and its growth rate was 1.4 ± 0.04 ppt yr−1; HFC-32 had a global mean mole fraction of 6.2 ± 0.2 ppt and a growth rate of 1.1 ± 0.04 ppt yr−1 in 2012. The extensive observations presented in this work have been combined with an atmospheric transport model to simulate global atmospheric abundances and derive global emission estimates. It is estimated that 23 ± 3 Gg yr−1 of HFC-143a and 21 ± 11 Gg yr−1 of HFC-32 were emitted globally in 2012, and the emission rates are estimated to be increasing 7 ± 5% yr−1 for HFC-143a and 14 ± 11% yr−1 for HFC-32.


2016 ◽  
Vol 16 (2) ◽  
pp. 455-504 ◽  
Author(s):  
M. Mallet ◽  
F. Dulac ◽  
P. Formenti ◽  
P. Nabat ◽  
J. Sciare ◽  
...  

Abstract. The Chemistry-Aerosol Mediterranean Experiment (ChArMEx; http://charmex.lsce.ipsl.fr) is a collaborative research program federating international activities to investigate Mediterranean regional chemistry-climate interactions. A special observing period (SOP-1a) including intensive airborne measurements was performed in the framework of the Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region (ADRIMED) project during the Mediterranean dry season over the western and central Mediterranean basins, with a focus on aerosol-radiation measurements and their modeling. The SOP-1a took place from 11 June to 5 July 2013. Airborne measurements were made by both the ATR-42 and F-20 French research aircraft operated from Sardinia (Italy) and instrumented for in situ and remote-sensing measurements, respectively, and by sounding and drifting balloons, launched in Minorca. The experimental setup also involved several ground-based measurement sites on islands including two ground-based reference stations in Corsica and Lampedusa and secondary monitoring sites in Minorca and Sicily. Additional measurements including lidar profiling were also performed on alert during aircraft operations at EARLINET/ACTRIS stations at Granada and Barcelona in Spain, and in southern Italy. Remote-sensing aerosol products from satellites (MSG/SEVIRI, MODIS) and from the AERONET/PHOTONS network were also used. Dedicated meso-scale and regional modeling experiments were performed in relation to this observational effort. We provide here an overview of the different surface and aircraft observations deployed during the ChArMEx/ADRIMED period and of associated modeling studies together with an analysis of the synoptic conditions that determined the aerosol emission and transport. Meteorological conditions observed during this campaign (moderate temperatures and southern flows) were not favorable to producing high levels of atmospheric pollutants or intense biomass burning events in the region. However, numerous mineral dust plumes were observed during the campaign, with the main sources located in Morocco, Algeria and Tunisia, leading to aerosol optical depth (AOD) values ranging between 0.2 and 0.6 (at 440 nm) over the western and central Mediterranean basins. One important point of this experiment concerns the direct observations of aerosol extinction onboard the ATR-42, using the CAPS system, showing local maxima reaching up to 150 M m−1 within the dust plume. Non-negligible aerosol extinction (about 50 M m−1) has also been observed within the marine boundary layer (MBL). By combining the ATR-42 extinction coefficient observations with absorption and scattering measurements, we performed a complete optical closure revealing excellent agreement with estimated optical properties. This additional information on extinction properties has allowed calculation of the dust single scattering albedo (SSA) with a high level of confidence over the western Mediterranean. Our results show a moderate variability from 0.90 to 1.00 (at 530 nm) for all flights studied compared to that reported in the literature on this optical parameter. Our results underline also a relatively low difference in SSA with values derived near dust sources. In parallel, active remote-sensing observations from the surface and onboard the F-20 aircraft suggest a complex vertical structure of particles and distinct aerosol layers with sea spray and pollution located within the MBL, and mineral dust and/or aged North American smoke particles located above (up to 6–7 km in altitude). Aircraft and balloon-borne observations allow one to investigate the vertical structure of the aerosol size distribution showing particles characterized by a large size (> 10 µm in diameter) within dust plumes. In most of cases, a coarse mode characterized by an effective diameter ranging between 5 and 10 µm, has been detected above the MBL. In terms of shortwave (SW) direct forcing, in situ surface and aircraft observations have been merged and used as inputs in 1-D radiative transfer codes for calculating the aerosol direct radiative forcing (DRF). Results show significant surface SW instantaneous forcing (up to −90 W m−2 at noon). Aircraft observations provide also original estimates of the vertical structure of SW and LW radiative heating revealing significant instantaneous values of about 5° K per day in the solar spectrum (for a solar angle of 30°) within the dust layer. Associated 3-D modeling studies from regional climate (RCM) and chemistry transport (CTM) models indicate a relatively good agreement for simulated AOD compared with observations from the AERONET/PHOTONS network and satellite data, especially for long-range dust transport. Calculations of the 3-D SW (clear-sky) surface DRF indicate an average of about −10 to −20 W m−2 (for the whole period) over the Mediterranean Sea together with maxima (−50 W m−2) over northern Africa. The top of the atmosphere (TOA) DRF is shown to be highly variable within the domain, due to moderate absorbing properties of dust and changes in the surface albedo. Indeed, 3-D simulations indicate negative forcing over the Mediterranean Sea and Europe and positive forcing over northern Africa. Finally, a multi-year simulation, performed for the 2003 to 2009 period and including an ocean–atmosphere (O–A) coupling, underlines the impact of the aerosol direct radiative forcing on the sea surface temperature, O–A fluxes and the hydrological cycle over the Mediterranean.


2010 ◽  
Vol 10 (22) ◽  
pp. 10753-10770 ◽  
Author(s):  
K. S. Law ◽  
F. Fierli ◽  
F. Cairo ◽  
H. Schlager ◽  
S. Borrmann ◽  
...  

Abstract. Trace gas and aerosol data collected in the tropical tropopause layer (TTL) between 12–18.5 km by the M55 Geophysica aircraft as part of the SCOUT-AMMA campaign over West Africa during the summer monsoon in August 2006 have been analysed in terms of their air mass origins. Analysis of domain filling back trajectories arriving over West Africa, and in the specific region of the flights, showed that the M55 flights were generally representative of air masses arriving over West Africa during the first 2 weeks of August, 2006. Air originating from the mid-latitude lower stratosphere was under-sampled (in the mid-upper TTL) whilst air masses uplifted from central Africa (into the lower TTL) were over-sampled in the latter part of the campaign. Signatures of recent (previous 10 days) origins were superimposed on the large-scale westward flow over West Africa. In the lower TTL, air masses were impacted by recent local deep convection over Africa at the level of main convective outflow (350 K, 200 hPa) and on certain days up to 370 K (100 hPa). Estimates of the fraction of air masses influenced by local convection vary from 10 to 50% depending on the method applied and from day to day during the campaign. The analysis shows that flights on 7, 8 and 11 August were more influenced by local convection than on 4 and 13 August allowing separation of trace gas and aerosol measurements into "convective" and "non-convective" flights. Strong signatures, particularly in species with short lifetimes (relative to CO2) like CO, NO and fine-mode aerosols were seen during flights most influenced by convection up to 350–365 K. Observed profiles were also constantly perturbed by uplift (as high as 39%) of air masses from the mid to lower troposphere over Asia, India, and oceanic regions resulting in import of clean oceanic (e.g. O3-poor) or polluted air masses from Asia (high O3, CO, CO2) into West Africa. Thus, recent uplift of CO2 over Asia may contribute to the observed positive CO2 gradients in the TTL over West Africa. This suggests a more significant fraction of younger air masses in the TTL and needs to taken into consideration in derivations of mean age of air. Transport of air masses from the mid-latitude lower stratosphere had an impact from the mid-TTL upwards (20–40% above 370 K) during the campaign period importing air masses with high O3 and NOy. Ozone profiles show a less pronounced lower TTL minimum than observed previously by regular ozonesondes at other tropical locations. Concentrations are less than 100 ppbv in the lower TTL and vertical gradients less steep than in the upper TTL. The air mass origin analysis and simulations of in-situ net photochemical O3 production, initialised with observations, suggest that the lower TTL is significantly impacted by uplift of O3 precursors (over Africa and Asia) leading to positive production rates (up to 2 ppbv per day) in the lower and mid TTL even at moderate NOx levels. Photochemical O3 production increases with higher NOx and H2O in air masses with O3 less than 150 ppbv.


2014 ◽  
Vol 7 (1) ◽  
pp. 107-128 ◽  
Author(s):  
S. Freitag ◽  
A. D. Clarke ◽  
S. G. Howell ◽  
V. N. Kapustin ◽  
T. Campos ◽  
...  

Abstract. The history of air masses is often investigated using backward trajectories to gain knowledge about processes along the air parcel path as well as possible source regions. Here, we describe a refined approach that incorporates airborne gas, aerosol, and environmental data into back trajectories and show how this technique allows for simultaneous evaluation of air mass history and back trajectory reliability without the need to calculate trajectory errors. We use the HYbrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model and add a simple semi-automated computing routine to facilitate high-frequency coverage of back trajectories initiated along free tropospheric (FT) flight tracks and profiles every 10 s. We integrate our in situ physiochemical data by color-coding each of these trajectories with its corresponding in situ tracer values measured at the back trajectory start points along the flight path. The unique color for each trajectory aids assessment of trajectory reliability through the visual clustering of air mass pathways of similar coloration. Moreover, marked changes in trajectories associated with marked changes evident in measured physiochemical or thermodynamic properties of an air mass add credence to trajectories. This is particularly true when these air mass properties are linked to trajectory features characteristic of recognized sources or processes. This visual clustering of air mass pathways is of particular value for large-scale 3-D flight tracks common to aircraft experiments where air mass features of interest are often spatially distributed and temporally separated. The cluster-visualization tool used here reveals that most FT back trajectories with pollution signatures measured in the central equatorial Pacific reach back to sources on the South American continent over 10 000 km away and 12 days back in time, e.g., the Amazonian basin. We also demonstrate the distinctions in air mass properties between these and trajectories that penetrate deep convection in the Inter-Tropical Convergence Zone. Additionally, for the first time we show consistency of modeled precipitation along back trajectories with scavenging signatures in the aerosol measured for these trajectories.


2006 ◽  
Vol 6 (6) ◽  
pp. 11465-11520 ◽  
Author(s):  
B. Sauvage ◽  
R. V. Martin ◽  
A. van Donkelaar ◽  
X. Liu ◽  
K. Chance ◽  
...  

Abstract. We use a global chemical transport model (GEOS-Chem) to evaluate the consistency of satellite measurements of lightning flashes and ozone precursors with in situ measurements of tropical tropospheric ozone. The measurements are tropospheric O3, NO2, and HCHO columns from the GOME satellite instrument, lightning flashes from the OTD and LIS instruments, profiles of O3, CO, and relative humidity from the MOZAIC aircraft program, and profiles of O3 from the SHADOZ ozonesonde network. We interpret these multiple data sources with our model to better understand what controls tropical tropospheric ozone. Tropical tropospheric ozone is mainly affected by lightning and convection in the upper troposphere and by surface emissions in the lower troposphere. Scaling the spatial distribution of lightning in the model to the observed flash counts improves the simulation of O3 in the upper troposphere by 5–20 ppbv versus in situ observations and by 1–4 Dobson Units versus GOME retrievals of tropospheric O3 columns. A lightning source strength of 5±2 Tg N/yr best represents in situ observations from aircraft and ozonesonde. Tropospheric NO2 and HCHO columns from GOME are applied to provide top-down constraints on emission inventories of NOx (biomass burning and soils) and VOCs (biomass burning). The top-down biomass burning inventory is larger by a factor of 2 for HCHO and alkenes, and by 2.6 for NOx over northern equatorial Africa. These emissions increase lower tropospheric O3 by 5–20 ppbv, improving the simulation versus aircraft observations, and by 4 Dobson Units versus GOME observations of tropospheric O3 columns. Emission factors in the a posteriori inventory are more consistent with a recent compilation from in situ measurements. The ozone simulation using two different dynamical schemes (GEOS-3 and GEOS-4) is evaluated versus observations; GEOS-4 better represents O3 observations by 5–15 ppbv due to enhanced convective detrainment in the upper troposphere. Heterogeneous uptake of HNO3 on aerosols reduces simulated O3 by 5–7 ppbv, reducing a model bias versus in situ observations over and downwind of deserts. Exclusion of HO2 uptake on aerosols improves O3 by 5 ppbv in biomass burning regions.


2010 ◽  
Vol 10 (6) ◽  
pp. 15485-15536 ◽  
Author(s):  
K. S. Law ◽  
F. Fierli ◽  
F. Cairo ◽  
H. Schlager ◽  
S. Borrmann ◽  
...  

Abstract. Trace gas and aerosol data collected in the tropical tropopause layer (TTL) between 12–18.5 km by the M55 Geophysica aircraft as part of the SCOUT-AMMA campaign over West Africa during the summer monsoon in August 2006 have been analysed in terms of their air mass origins. Analysis of domain filling back trajectories arriving over West Africa, and in the specific region of the flights, showed that the M55 flights were generally representative of air masses arriving over West Africa during the first 2 weeks of August, 2006. Air originating from the mid-latitude lower stratosphere was under-sampled (in the mid-upper TTL) whilst air masses uplifted from central Africa (into the lower TTL) were over-sampled in the latter part of the campaign. Signatures of recent (previous 10 days) origins were superimposed on the large-scale westerly flow over West Africa. In the lower TTL, air masses were impacted by recent local deep convection over Africa at the level of main convective outflow (350 K, 200 hPa) and on certain days up to 370 K (100 hPa). Estimates of the fraction of air masses influenced by local convection vary from 10 to 50% depending on the method applied and from day to day during the campaign. The analysis shows that flights on 7, 8 and 11 August were more influenced by local convection than on 4 and 13 August allowing separation of trace gas and aerosol measurements into ''convective'' and ''non-convective'' flights. Strong signatures, particularly in short-lived species like CO, NO and fine-mode aerosols were seen during flights most influenced by convection up to 350–365 K. Observed profiles were also constantly perturbed by uplift (as high as 39%) of air masses from the mid to lower troposphere over Asia, India, and oceanic regions resulting in import of clean oceanic (e.g., O3-poor) or polluted air masses from Asia (high O3, CO, CO2) into West Africa. Thus, recent uplift of CO2 over Asia may contribute to the observed positive CO2 gradients in the TTL over West Africa. This suggests a more significant fraction of younger air masses in the TTL making it difficult to derive mean age of air from average gradients. Transport of air masses from the mid-latitude lower stratosphere had an impact from the mid-TTL upwards (20–40% above 370 K) during the campaign period importing air masses with high O3 and NOy. Ozone profiles show a less pronounced lower TTL minimum than observed previously by regular ozonesondes at other tropical locations. Concentrations are less than 100 ppbv in the lower TTL and vertical gradients less steep than in the upper TTL. The air mass origin analysis and simulations of in-situ net photochemical O3 production, initialised with observations, suggest that the lower TTL is significantly impacted by uplift of O3 precursors (over Africa and Asia) leading to positive production rates (up to 2 ppbv per day) in the lower and mid TTL even at moderate NOx levels. Photochemical O3 production increases with higher NOx and H2O in air masses with O3 less than 150 ppbv.


2020 ◽  
Vol 20 (21) ◽  
pp. 13191-13216
Author(s):  
Marc Mallet ◽  
Fabien Solmon ◽  
Pierre Nabat ◽  
Nellie Elguindi ◽  
Fabien Waquet ◽  
...  

Abstract. Simulations are performed for the period 2000–2015 by two different regional climate models, ALADIN and RegCM, to quantify the direct and semi-direct radiative effects of biomass-burning aerosols (BBAs) in the southeast Atlantic (SEA) region. Different simulations have been performed using strongly absorbing BBAs in accordance with recent in situ observations over the SEA. For the July–August–September (JAS) season, the single scattering albedo (SSA) and total aerosol optical depth (AOD) simulated by the ALADIN and RegCM models are consistent with the MACv2 climatology and MERRA-2 and CAMS-RA reanalyses near the biomass-burning emission sources. However, the above-cloud AOD is slightly underestimated compared to satellite (MODIS and POLDER) data during the transport over the SEA. The direct radiative effect exerted at the continental and oceanic surfaces by BBAs is significant in both models and the radiative effects at the top of the atmosphere indicate a remarkable regional contrast over SEA (in all-sky conditions), with a cooling (warming) north (south) of 10 ∘S, which is in agreement with the recent MACv2 climatology. In addition, the two models indicate that BBAs are responsible for an important shortwave radiative heating of ∼0.5–1 K per day over SEA during JAS with maxima between 2 and 4 km a.m.s.l. (above mean sea level). At these altitudes, BBAs increase air temperature by ∼0.2–0.5 K, with the highest values being co-located with low stratocumulus clouds. Vertical changes in air temperature limit the subsidence of air mass over SEA, creating a cyclonic anomaly. The opposite effect is simulated over the continent due to the increase in lower troposphere stability. The BBA semi-direct effect on the lower troposphere circulation is found to be consistent between the two models. Changes in the cloud fraction are moderate in response to the presence of smoke, and the models differ over the Gulf of Guinea. Finally, the results indicate an important sensitivity of the direct and semi-direct effects to the absorbing properties of BBAs. Over the stratocumulus (Sc) region, DRE varies from +0.94 W m−2 (scattering BBAs) to +3.93 W m−2 (most absorbing BBAs).


2019 ◽  
Vol 100 (11) ◽  
pp. 2260-2283 ◽  
Author(s):  
Julia Schmale ◽  
Andrea Baccarini ◽  
Iris Thurnherr ◽  
Silvia Henning ◽  
Avichay Efraim ◽  
...  

AbstractUncertainty in radiative forcing caused by aerosol–cloud interactions is about twice as large as for CO2 and remains the least well understood anthropogenic contribution to climate change. A major cause of uncertainty is the poorly quantified state of aerosols in the pristine preindustrial atmosphere, which defines the baseline against which anthropogenic effects are calculated. The Southern Ocean is one of the few remaining near-pristine aerosol environments on Earth, but there are very few measurements to help evaluate models. The Antarctic Circumnavigation Expedition: Study of Preindustrial-like Aerosols and their Climate Effects (ACE-SPACE) took place between December 2016 and March 2017 and covered the entire Southern Ocean region (Indian, Pacific, and Atlantic Oceans; length of ship track >33,000 km) including previously unexplored areas. In situ measurements covered aerosol characteristics [e.g., chemical composition, size distributions, and cloud condensation nuclei (CCN) number concentrations], trace gases, and meteorological variables. Remote sensing observations of cloud properties, the physical and microbial ocean state, and back trajectory analyses are used to interpret the in situ data. The contribution of sea spray to CCN in the westerly wind belt can be larger than 50%. The abundance of methanesulfonic acid indicates local and regional microbial influence on CCN abundance in Antarctic coastal waters and in the open ocean. We use the in situ data to evaluate simulated CCN concentrations from a global aerosol model. The extensive, available ACE-SPACE dataset (https://zenodo.org/communities/spi-ace?page=1&size=20) provides an unprecedented opportunity to evaluate models and to reduce the uncertainty in radiative forcing associated with the natural processes of aerosol emission, formation, transport, and processing occurring over the pristine Southern Ocean.


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