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Impact of geographic variations of the convective and dehydration center on stratospheric water vapor over the Asian monsoon region

The Asian monsoon region is the most prominent moisture center of water vapor in the lower stratosphere (LS) during boreal summer. Previous studies have suggested that the transport of water vapor to the Asian monsoon LS is controlled by dehydration temperatures and convection mainly over the Bay of Bengal and Southeast Asia. However, there is a clear geographic variation of convection associated with the seasonal and intra-seasonal variations of the Asian monsoon circulation, and the relative influence of such a geographic variation of convection vs. the variation of local dehydration temperatures on water vapor transport is still not clear. Using satellite observations from the Aura Microwave Limb Sounder (MLS) and a domain-filling forward trajectory model, we show that almost half of the seasonal water vapor increase in the Asian monsoon LS are attributable to geographic variations of convection and resultant variations of the dehydration center, of which the influence is comparable to the influence of the local dehydration temperature increase. In particular, dehydration temperatures are coldest over the southeast and warmest over the northwest Asian monsoon region. Although the convective center is located over Southeast Asia, an anomalous increase of convection over the northwest Asia monsoon region increases local diabatic heating in the tropopause layer and air masses entering the LS are dehydrated at relatively warmer temperatures. Due to warmer dehydration temperatures, anomalously moist air enters the LS and moves eastward along the northern flank of the monsoon anticyclonic flow, leading to wet anomalies in the LS over the Asian monsoon region. Likewise, when convection increases over the Southeast Asia monsoon region, dry anomalies appear in the LS. On a seasonal scale, this feature is associated with the monsoon circulation, convection and diabatic heating marching towards the northwest Asia monsoon region from June to August. The march of convection leads to an increasing fraction of the air mass to be dehydrated at warmer temperatures over the northwest Asia monsoon region. Work presented here confirms the dominant role of temperatures on water vapor variations and emphasizes that further studies should take geographic variations of the dehydration center into consideration when studying water vapor variations in the LS as it is linked to changes of convection and large-scale circulation patterns.
Neutral atmosphere temperature trends and variability at 90 km, 70 °N, 19 °E, 2003–2014

Neutral temperatures at 90 km height above Tromsø, Norway, have been determined using ambipolar diffusion coefficients calculated from meteor echo fading times using the Nippon/Norway Tromsø Meteor Radar (NTMR). Daily temperature averages have been calculated from November 2003 to October 2014 and calibrated against temperature measurements from the Microwave Limb Sounder (MLS) on board Aura. Large-scale periodic oscillations ranging from ∼ 9 days to a year were found in the data using Lomb–Scargle periodogram analysis, and these components were used to seasonally detrend the daily temperature values before assessing trends. Harmonic oscillations found are associated with the large-scale circulation in the middle atmosphere together with planetary and gravity wave activity. The overall temperature change from 2003 to 2014 is −2.2 K ± 1.0 K decade−1, while in summer (May–June–July) and winter (November–December–January) the change is −0.3 K ± 3.1 K decade−1 and −11.6 K ± 4.1 K decade−1, respectively. The temperature record is at this point too short for incorporating a response to solar variability in the trend. How well suited a meteor radar is for estimating neutral temperatures at 90 km using meteor trail echoes is discussed, and physical explanations behind a cooling trend are proposed.
Rethinking the global secondary organic aerosol (SOA) budget: stronger production, faster removal, shorter lifetime

Recent laboratory studies suggest that secondary organic aerosol (SOA) formation rates are higher than assumed in current models. There is also evidence that SOA removal by dry and wet deposition occurs more efficiently than some current models suggest and that photolysis and heterogeneous oxidation may be important (but currently ignored) SOA sinks. Here, we have updated the global GEOS-Chem model to include this new information on formation (i.e., wall-corrected yields and emissions of semi-volatile and intermediate volatility organic compounds) and on removal processes (photolysis and heterogeneous oxidation). We compare simulated SOA from various model configurations against ground, aircraft and satellite measurements to assess the extent to which these improved representations of SOA formation and removal processes are consistent with observed characteristics of the SOA distribution. The updated model presents a more dynamic picture of the life cycle of atmospheric SOA, with production rates 3.9 times higher and sinks a factor of 3.6 more efficient than in the base model. In particular, the updated model predicts larger SOA concentrations in the boundary layer and lower concentrations in the upper troposphere, leading to better agreement with surface and aircraft measurements of organic aerosol compared to the base model. Our analysis thus suggests that the long-standing discrepancy in model predictions of the vertical SOA distribution can now be resolved, at least in part, by a stronger source and stronger sinks leading to a shorter lifetime. The predicted global SOA burden in the updated model is 0.88 Tg and the corresponding direct radiative effect at top of the atmosphere is −0.33 W m−2, which is comparable to recent model estimates constrained by observations. The updated model predicts a population-weighed global mean surface SOA concentration that is a factor of 2 higher than in the base model, suggesting the need for a reanalysis of the contribution of SOA to PM pollution-related human health effects. The potential importance of our estimates highlights the need for more extensive field and laboratory studies focused on characterizing organic aerosol removal mechanisms and rates.
Ship emissions measurement in the Arctic by plume intercepts of the Canadian Coast Guard icebreaker Amundsen from the Polar 6 aircraft platform

Decreasing sea ice and increasing marine navigability in northern latitudes have changed Arctic ship traffic patterns in recent years and are predicted to increase annual ship traffic in the Arctic in the future. Development of effective regulations to manage environmental impacts of shipping requires an understanding of ship emissions and atmospheric processing in the Arctic environment. As part of the summer 2014 NETCARE (Network on Climate and Aerosols) campaign, the plume dispersion and gas and particle emission factors of effluents originating from the Canadian Coast Guard icebreaker Amundsen operating near Resolute Bay, NU, Canada, were investigated. The Amundsen burned distillate fuel with 1.5 wt % sulfur. Emissions were studied via plume intercepts using the Polar 6 aircraft measurements, an analytical plume dispersion model, and using the FLEXPART-WRF Lagrangian particle dispersion model. The first plume intercept by the research aircraft was carried out on 19 July 2014 during the operation of the Amundsen in the open water. The second and third plume intercepts were carried out on 20 and 21 July 2014 when the Amundsen had reached the ice edge and operated under ice-breaking conditions. Typical of Arctic marine navigation, the engine load was low compared to cruising conditions for all of the plume intercepts. The measured species included mixing ratios of CO2, NOx, CO, SO2, particle number concentration (CN), refractory black carbon (rBC), and cloud condensation nuclei (CCN). The results were compared to similar experimental studies in mid-latitudes. Plume expansion rates (γ) were calculated using the analytical model and found to be γ  =  0.75 ± 0.81, 0.93 ± 0.37, and 1.19 ± 0.39 for plumes 1, 2, and 3, respectively. These rates were smaller than prior studies conducted at mid-latitudes, likely due to polar boundary layer dynamics, including reduced turbulent mixing compared to mid-latitudes. All emission factors were in agreement with prior observations at low engine loads in mid-latitudes. Ice-breaking increased the NOx emission factor from EFNOx  =  43.1 ± 15.2 to 71.6 ± 9.68 and 71.4 ± 4.14 g kg-diesel−1 for plumes 1, 2, and 3, likely due to changes in combustion temperatures. The CO emission factor was EFCO  =  137 ± 120, 12.5 ± 3.70 and 8.13 ± 1.34 g kg-diesel−1 for plumes 1, 2, and 3. The rBC emission factor was EFrBC  =  0.202 ± 0.052 and 0.202 ± 0.125 g kg-diesel−1 for plumes 1 and 2. The CN emission factor was reduced while ice-breaking from EFCN  =  2.41 ± 0.47 to 0.45 ± 0.082 and 0.507 ± 0.037  ×  1016 kg-diesel−1 for plumes 1, 2, and 3. At 0.6 % supersaturation, the CCN emission factor was comparable to observations in mid-latitudes at low engine loads with EFCCN  =  3.03 ± 0.933, 1.39 ± 0.319, and 0.650 ± 0.136  ×  1014 kg-diesel−1 for plumes 1, 2, and 3.
A DNS study of aerosol and small-scale cloud turbulence interaction

The purpose of this study is to investigate the interaction between small-scale turbulence and aerosol and cloud microphysical properties using direct numerical simulations (DNS). We consider the domain located at the height of about 2000 m from the sea level, experiencing transient high supersaturation due to atmospheric fluctuations of temperature and humidity. To study the effect of total number of particles (Ntot) on air temperature, activation and supersaturation, we vary Ntot. To investigate the effect of aerosol dynamics on small-scale turbulence and vertical air motion, we vary the intensity of turbulent fluctuations and the buoyant force. We find that even a small number of aerosol particles (55.5 cm−3), and therefore a small droplet number concentration, strongly affects the air temperature due to release of latent heat. The system comes to an equilibrium faster and the relative number of activated particles appears to be smaller for larger Ntot. We conclude that aerosol particles strongly affect the air motion. In a case of updraught coursed by buoyant force, the presence of aerosol particles results in acceleration of air motion in vertical direction and increase of turbulent fluctuations.
The Nonequilbrium Thermodynamics of Atmospheric Blocking

Two strong NE Pacific blocking events that occurred nearly one year apart and in the same region are examined here by methods from nonequilbrium thermodynamics. In a nonequilibrium setting, the time variation of entropy is a sum of two parts: the external entropy supply and the internal entropy production. The internal entropy production and external entropy supply (the surface entropy supply) are calculated and compared to recent trends in the region that encompassed both blocking events. The entropy production and entropy surface supply were found to be high during both blocking events. However, the surface conditions during the events were markedly different. The surface conditions during the first event were dominated by the NE Pacific sea surface temperature anomaly known as the Blob, while the other event was less influenced. In particular, the surface entropy supply increased from January to February for the first event. The entropy production decreased slightly but any negative entropy flows from extratropical cyclones were offset by the increasing surface entropy supply, maintaining the blocking event. On the other hand, the second event had no large changes in the surface entropy supply or entropy production during its lifetime even though it was similar to the first event in many respects. The use of entropy as a convenient variable to examine the mechanisms that maintain blocking events is considered.
A long term study of polar ozone loss derived from data assimilation of Odin/SMR observations

Odin, a Swedish-led satellite project in collaboration with Canada, France and Finland, was launched on 20 February 2001 and continues to produce profiles of chemical species relevant to understanding the middle and upper atmosphere. Long-term observations of stratospheric ozone are useful for trend analysis of chemical ozone loss. This study concerns ozone loss over both poles utilizing 12 years of ozone data from Odin/Sub-Millimetre Radiometer (SMR). We have applied the data assimilation technique described by Rösevall et al. (2007) with a number of improvements to study the inter-annual variability during the entire Odin period. The chemical ozone losses at potential temperature levels between 425 K and 950 K, (corresponding to an altitude range of 15 to 40 km approximately 90 hPa and 7 hPa in pressure), are derived. Two SMR ozone products retrieved from the emission lines centred at 501 GHz and 544 GHz were used. An internal comparison of the two analyses using 501 GHz and 544 GHz ozone has been carried out by inspecting the vortex mean ozone in March and October during 2002–2013 and 2003–2012 in the Northern and Southern Hemisphere, respectively. Ozone derived from data assimilation using the two data sets match within 10 % at the levels studied, while below 550 K in the Southern Hemispheremore than 50 % of the difference is found. Here, 544 GHz ozone is 0.5 parts per million volume (ppmv) lower than 501 GHz ozone because of better sensitivity in 544 GHz ozone in the lower stratosphere. Comparisons with other studies have been mainly performed against Sonkaew et al. (2013) since Sonkaew et al. (2013) is one of the few studies having consistent estimations of ozone depletion using a SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY (SCIAMACHY) from 2002 to 2009. 544 GHz ozone loss in the Arctic winter 2004/2005 is in good agreement with SCIAMACHY loss below 450 K to within 0.2 ppmv, while showing no loss around 550 K where SCIAMACHY detected 0.5 ppmv loss. The comparison of Antarctic ozone depletions with Kuttippurath et al. (2015) shows agreement with MLS ozone loss within 0.1 ppmv, while our results were constantly 0.3 ppmv lower than Mimosa-Chim model calculations. In the Northern Hemisphere, our assimilation analyses show large inter-annual variability. Three classes of chemical ozone losses are found to occur in cold, warm and intermediate winters between cold and warm. The cold type loss maximises in March below 500 K as in the Southern Hemisphere. The maximum loss in the Northern Hemisphere between 2001/2002 and 2012/2013 was during the cold winter, which happened in 2010/2011 with a loss in volume mixing ratio of 2.1 ppmv at 450 K. Losses of 1.5 ppmv took place at 700 K in the warm winters related to the occurrence of mid-winter major sudden stratospheric warming (SSW) events. In the Southern Hemisphere between 2002 and 2012, chemical ozone losses began in mid-August and generally grew to 2.5 ppmv by the end of October. The vertical extent of this loss was 425–550 K. All Antarctic winters except 2002 had approximately 80 DU loss in the stratospheric column. In both hemispheres partial columns in the stratosphere show a small increase over the time period from 2002 to 2013, however the statistical confidence is not high enough to identify ozone recovery.
Persistence of upper stratospheric wintertime tracer variability into the Arctic spring and summer

Using data from the Aeronomy of Ice in the Mesosphere (AIM) and Aura satellites, we have categorized the interannual variability of winter- and springtime upper stratospheric methane (CH4). We further show the effects of this variability on the chemistry of the upper stratosphere throughout the following summer. Years with strong wintertime mesospheric descent followed by dynamically quiet springs, such as 2009, lead to the lowest summertime CH4. Years with relatively weak wintertime descent, but strong springtime planetary wave activity, such as 2011, have the highest summertime CH4. By sampling the Aura Microwave Limb Sounder (MLS) according to the occultation pattern of the AIM Solar Occultation for Ice Experiment (SOFIE), we show that summertime upper stratospheric chlorine monoxide (ClO) almost perfectly anticorrelates with the CH4. This is consistent with the reaction of atomic chlorine with CH4 to form the reservoir species, hydrochloric acid (HCl). The summertime ClO for years with strong, uninterrupted mesospheric descent is about 50 % greater than in years with strong horizontal transport and mixing of high CH4 air from lower latitudes. Small, but persistent effects on ozone are also seen such that between 1 and 2 hPa, ozone is about 4–5 % higher in summer for the years with the highest CH4 relative to the lowest. This is consistent with the role of the chlorine catalytic cycle on ozone. These dependencies may offer a means to monitor dynamical effects on the high-latitude upper stratosphere using summertime ClO measurements as a proxy. Additionally, these chlorine-controlled ozone decreases, which are seen to maximize after years with strong uninterrupted wintertime descent, represent a new mechanism by which mesospheric descent can affect polar ozone. Finally, given that the effects on ozone appear to persist much of the rest of the year, the consideration of winter/spring dynamical variability may also be relevant in studies of ozone trends.
Gravity-wave effects on tracer gases and stratospheric aerosol concentrations during the 2013 ChArMEx campaign

Coupled balloon-borne observations of Light Optical Aerosol Counter (LOAC), M10 meteorological global positioning system (GPS) sondes, ozonesondes, and GPS radio occultation data, are examined to identify gravity-wave (GW)-induced fluctuations on tracer gases and on the vertical distribution of stratospheric aerosol concentrations during the 2013 ChArMEx (Chemistry-Aerosol Mediterranean Experiment) campaign. Observations reveal signatures of GWs with short vertical wavelengths less than 4 km in dynamical parameters and tracer constituents, which are also correlated with the presence of thin layers of strong local enhancements of aerosol concentrations in the upper troposphere and the lower stratosphere. In particular, this is evident from a case study above Ile du Levant (43.02° N, 6.46° E) on 26–29 July 2013. Observations show a strong activity of dominant mesoscale inertia GWs with horizontal and vertical wavelengths of 370–510 km and 2–3 km respectively, and periods of 10–13 h propagating southward at altitudes of 13–20 km during 27–28 July. The European Centre for Medium-Range Weather Forecasts (ECMWF) analyses also show evidence of mesoscale inertia GWs with similar horizontal characteristics above the eastern part of France. Ray-tracing experiments indicate the jet-front system as the main source of observed GWs. Using a simplified linear GW theory, synthetic vertical profiles of dynamical parameters with large stratospheric vertical wind maximum oscillations of ±40 mms−1 are produced for the dominant mesoscale GW observed at heights of 13–20 km. Parcel advection method reveals signatures of GWs in the ozone mixing ratio and the tropospheric-specific humidity. Simulated vertical wind perturbations of the dominant GWs and small-scale perturbations of aerosol concentration (aerosol size of 0.2–0.7 µm) are revealed to be in phase in the lower stratosphere. Present results support the importance of vertical wind perturbations in the GW–aerosol relationship. Observed mesoscale GWs induce a strong modulation of the amplitude of tracer gases and the stratospheric aerosol background.
Anthropogenic and biogenic influence on VOC fluxes at an urban background site in Helsinki, Finland

We measured volatile organic compounds (VOCs), carbon dioxide (CO2) and carbon monoxide (CO) at an urban background site near the city centre of Helsinki, Finland, northern Europe. The VOC and CO2 measurements were obtained between January 2013 and September 2014 whereas for CO a shorter measurement campaign in April–May 2014 was conducted. Both anthropogenic and biogenic sources were identified for VOCs in the study. Strong correlations between VOC fluxes and CO fluxes and traffic rates indicated anthropogenic source of many VOCs. The VOC with the highest emission rate to the atmosphere was methanol, which originated mostly from traffic and other anthropogenic sources. The traffic was also a major source for aromatic compounds in all seasons whereas isoprene was mostly emitted from biogenic sources during summer. Some amount of traffic-related isoprene emissions were detected during other seasons but this might have also been an instrumental contamination from cycloalkane products. Generally, the observed VOC fluxes were found to be small in comparison with previous urban VOC flux studies. However, the differences were probably caused by lower anthropogenic activities as the CO2 fluxes were also relatively small at the site.