Upper-tropospheric Air Research Articles

The Venusian Insolation Atmospheric Topside Thermal Heating Pool

A 1 metre increment modelled pressure profile is used to study the troposphere of Venus from the surface to the lower stratosphere. Using a troposphere model lapse rate profile as the constraint on cooling by vertically convecting air, the modelled height of the tropopause convection limit is a close match to the level of the observed static atmosphere height for the 250 Kelvin freezing point level of 75% by weight of concentrated sulphuric acid, the primary condensing volatile in the Venusian atmosphere. This relationship suggests that the observed albedo of Venus is a response to and not a cause of planetary atmospheric solar radiant forcing.Using the thermal lapse rate for the troposphere of Venus in its top-down mode of application, the depth below the tropopause that solar irradiance is able to achieve effective heating of the Venusian atmosphere is established. This radiant quenching depth delineates a pool of upper tropospheric air that both captures and responds to solar radiant forcing. Consequently, this top of the troposphere insolation forcing induces a process of full troposphere adiabatic convective overturn and delivers solar heated air to the ground via the action of forced air descent in the twin polar vortices of Venus.

Circulation conservation in the outflow of warm conveyor belts and consequences for Rossby wave evolution

AbstractRossby waves on the jet stream are associated with meridional motions, displacing air and the strong potential vorticity (PV) gradient on isentropic surfaces. Poleward motion along sloping isentropic surfaces typically results in ascent and a ridge of air with low PV values. Latent heating in the ascending warm conveyor belt (WCB) enables air to cross isentropic surfaces so that the WCB outflow into a ridge occurs in a higher isentropic layer than the inflow. However, the PV impermeability theorem states that there can be no PV flux across isentropic surfaces, so how can heating alter the PV pattern of a Rossby wave? Here, the ways in which heating in WCBs can influence Rossby wave evolution at tropopause level are explained in the context of the PV impermeability theorem. First, a WCB outflow volume is defined by the upper tropospheric air in a ridge that has experienced net heating over the last few days, using a tracer within short global model forecasts. Second, the boundary of this outflow volume is tracked backwards using isentropic trajectories allowing quantification of the degree to which circulation is conserved, as predicted by theory, even though the WCB transports mass into the volume from lower isentropic layers. This diabatic flux of mass into the outflow volume results in an increase in density and expansion in the outflow area, the partition being determined approximately by PV inversion. The area expansion, combined with conservation of circulation, implies stronger anticyclonic vorticity. The relative vorticity change from divergent outflow can be as large as the decrease relative to the background planetary vorticity associated with poleward displacement of the circuit. The additional anticyclonic relative motion results in enhanced anticyclonic overturning of PV contours on the eastern flank of the ridge, altering qualitatively the nonlinear evolution of the Rossby wave.

Diagnostics of Convective Transport Over the Tropical Western Pacific From Trajectory Analyses

AbstractThis study characterizes the representation of convective transport by a Lagrangian trajectory model driven by kinematic (pressure tendency ω) vertical velocity. Four (re)analysis wind products are used in backward trajectory calculations with the TRAJ3D model, and their representations of convective transport are analyzed. Two observation‐based diagnostics are used for the evaluation: a database of observed convective cloud tops derived from satellite measurements and a set of transit time distributions (TTDs) derived from an airborne campaign during January–February 2014 in a domain over the Tropical Western Pacific (TWP). The analysis is designed to derive trajectory‐based TTDs that can be directly evaluated using the observation‐based TTDs. The results indicate a broad consistency between two independent TTD derivations characterizing vertical transport over the TWP, with a significant portion of convective transport processes represented in trajectory experiments driven by the selected (re)analysis wind products. The convective and boundary layer source regions of upper tropospheric air parcels are shown to be consistent with the climatological flow regime within the TWP. Furthermore, contributions of convection are identified in the ω fields of the (re)analysis wind data sets, as indicated by the spatiotemporal correlation of enhanced vertical velocity and observed convection. These results demonstrate the successful application of two observation‐based diagnostics and quantify the ability for kinematic trajectory models to represent convective transport processes.

Exploring the elevated water vapor signal associated with the free tropospheric biomass burning plume over the southeast Atlantic Ocean

Abstract. In southern Africa, widespread agricultural fires produce substantial biomass burning (BB) emissions over the region. The seasonal smoke plumes associated with these emissions are then advected westward over the persistent stratocumulus cloud deck in the southeast Atlantic (SEA) Ocean, resulting in aerosol effects which vary with time and location. Much work has focused on the effects of these aerosol plumes, but previous studies have also described an elevated free tropospheric water vapor signal over the SEA. Water vapor influences climate in its own right, and it is especially important to consider atmospheric water vapor when quantifying aerosol–cloud interactions and aerosol radiative effects. Here we present airborne observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign over the SEA Ocean. In observations collected from multiple independent instruments on the NASA P-3 aircraft (from near-surface to 6–7 km), we observe a strongly linear correlation between pollution indicators (carbon monoxide (CO) and aerosol loading) and atmospheric water vapor content, seen at all altitudes above the boundary layer. The focus of the current study is on the especially strong correlation observed during the ORACLES-2016 deployment (out of Walvis Bay, Namibia), but a similar relationship is also observed in the August 2017 and October 2018 ORACLES deployments. Using reanalyses from the European Centre for Medium-Range Weather Forecasts (ECMWF) and Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), and specialized WRF-Chem simulations, we trace the plume–vapor relationship to an initial humid, smoky continental source region, where it mixes with clean, dry upper tropospheric air and then is subjected to conditions of strong westward advection, namely the southern African easterly jet (AEJ-S). Our analysis indicates that air masses likely left the continent with the same relationship between water vapor and carbon monoxide as was observed by aircraft. This linear relationship developed over the continent due to daytime convection within a deep continental boundary layer (up to ∼5–6 km) and mixing with higher-altitude air, which resulted in fairly consistent vertical gradients in CO and water vapor, decreasing with altitude and varying in time, but this water vapor does not originate as a product of the BB combustion itself. Due to a combination of conditions and mixing between the smoky, moist continental boundary layer and the dry and fairly clean upper-troposphere air above (∼6 km), the smoky, humid air is transported by strong zonal winds and then advected over the SEA (to the ORACLES flight region) following largely isentropic trajectories. Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT) back trajectories support this interpretation. This work thus gives insights into the conditions and processes which cause water vapor to covary with plume strength. Better understanding of this relationship, including how it varies spatially and temporally, is important to accurately quantify direct, semi-direct, and indirect aerosol effects over this region.

On the Formation of Tropopause Folds and Constituent Gradient Enhancement Near Westerly Jets

AbstractThe role of differential advection in creating tropopause folds and strong constituent gradients near midlatitude westerly jets is investigated using the University of Wisconsin Non-hydrostatic Modeling System (UWNMS). Dynamical structures are compared with aircraft observations through a fold and subpolar jet (SPJ) during RF04 of the Stratosphere-Troposphere Analyses of Regional Transport (START08) campaign. The observed distribution of water vapor and ozone during RF04 provides evidence of rapid transport in the SPJ, enhancing constituent gradients above relative to below the intrusion. The creation of a tropopause fold by quasi-isentropic differential advection on the upstream side of the trough is described. This fold was created by a southward jet streak in the SPJ, where upper tropospheric air displaced the tropopause eastward in the 6-10 km layer, thereby overlying stratospheric air in the 3-6 km layer. The subsequent superposition of the subtropical and subpolar jets is also shown to result from quasi-isentropic differential advection.The occurrence of low values of ozone, water vapor, and potential vorticity on the equatorward side of the SPJ can be explained by convective transport of low-ozone air from the boundary layer, dehydration in the updraft, and detrainment of inertially-unstable air in the outflow layer. An example of rapid juxtaposition with stratospheric air in the jet core is shown for RF01. The net effect of upstream convective events is suggested as a fundamental cause of the strong constituent gradients observed in midlatitude jets. Idealized diagrams illustrate the role of differential advection in creating tropopause folds and constituent gradient enhancement.

Ice-supersaturated air masses in the northern mid-latitudes from regular in situ observations by passenger aircraft: vertical distribution, seasonality and tropospheric fingerprint

Abstract. The vertical distribution and seasonal variation of water vapour volume mixing ratio (H2O VMR), of relative humidity with respect to ice (RHice) and particularly of regions with ice-supersaturated air masses (ISSRs) in the extratropical upper troposphere and lowermost stratosphere are investigated at northern mid-latitudes over the eastern North American, North Atlantic and European regions for the period 1995 to 2010. Observation data originate from regular and continuous long-term measurements on board instrumented passenger aircraft in the framework of the European research programme MOZAIC (1994–2010), which continues as the European research infrastructure IAGOS (from 2011). Data used in our study result from collocated observations of O3 VMR, RHice and temperature, as well as H2O VMR deduced from RHice and temperature data. The in situ observations of H2O VMR and RHice with a vertical resolution of 30 hPa (< 750 m at the extratropical tropopause level) and a horizontal resolution of 1 km resolve detailed features of the distribution of water vapour and ice-supersaturated air relative to the thermal tropopause, including their seasonal and regional variability and chemical signatures at various distances from the tropopause layer. Annual cycles of the investigated properties document the highest H2O VMR and temperatures above the thermal tropopause in the summer months, whereas RHice above the thermal tropopause remains almost constant in the course of the year. Over all investigated regions, upper tropospheric air masses close to the tropopause level are nearly saturated with respect to ice and contain a significant fraction of ISSRs with a distinct seasonal cycle of minimum values in summer (30 % over the ocean, 20 %–25 % over land) and maximum values in late winter (35 %–40 % over both land and ocean). Above the thermal tropopause, ISSRs are occasionally observed with an occurrence probability of 1.5 ± 1.1 %, whereas above the dynamical tropopause at 2 PVU (PVU: potential vorticity unit), the occurrence probability increases 4-fold to 8.4 ± 4.4 %. In both coordinate systems related to tropopause height (TPH), the ISSR occurrence probabilities drop to values below 1 % for the next higher air mass layer with pressure levels p < pTPH−15 hPa. For both tropopause definitions, the tropospheric nature or fingerprint, based on O3 VMR, indicates the continuing tropospheric influence on ISSRs inside and above the respective tropopause layer. For the non-ISSRs, however, the stratospheric nature is clearly visible above the thermal tropopause, whereas above the dynamical tropopause the air masses show a still substantial tropospheric influence. For all three regions, seasonal deviations from the long-term annual cycle of ISSR occurrence show no significant trends over the observation period of 15 years, whereas a statistically significant correlation between the North Atlantic Oscillation (NAO) index and the deviation of ISSR occurrence from the long-term average is observed for the North Atlantic region but not for the eastern North American and European regions.

Strengthened linkage between midlatitudes and Arctic in boreal winter

Early studies have suggested a linkage between the surface warming over the Barents-Kara Seas and the strength of the Siberian high in boreal winter. Here, we show that the linkage is not stable, and with an apparent interdecadal change in the late-1990s. Coinciding with Arctic surface warm anomalies in recent decades (1997–2017), the Siberian high has been significantly intensified, the East Asian jet stream has expanded westward, and an apparent Rossby wave has propagated from the Arctic to East Asia, suggesting an atmospheric teleconnection between midlatitudes and Arctic. In contrast, midlatitude atmospheric circulation anomalies coinciding with Arctic surface warm anomalies were barely statistically significant during 1979–1996. The associated strong anomalous ascending/descending motions and divergent/convergent upper troposphere air masses over the Arctic-Eurasian sector seem to have favored the midlatitude-Arctic linkage during 1997–2017. We further hypothesize that Arctic mid-tropospheric warming plays a crucial role for the linkage between midlatitudes and Arctic in boreal winter. Multi-model simulations support this, and also point to internal atmospheric variability as the cause for the interdecadal shift in the strength of the midlatitude-Arctic linkage.

Spring Ozone's Connection to South Africa's Temperature and Rainfall

The Brewer–Dobson circulation (BDC), whose dynamic activity is enhanced from winter to spring, transports stratospheric ozone from the tropical source regions to higher latitudes. But it is the BDC’s shallow branch which transfers lower stratospheric ozone (LSO) from the tropics to the subtropics. Hence the accumulation of ozone in the subtropics is at its maximum at the end of spring (October) in the Southern Hemisphere (SH). Here we use observation and observation constrained reanalysis data to investigate the extent to which the interannual variability of this end of spring accumulated LSO is able to impact on the maximum surface air temperature (SATmax) and precipitation of South Africa. This is achieved through contrasting years of high positive and negative October ozone anomalies for the extreme BDC activity, referred to as weak (wBDC) and strong (sBDC) respectively. It is found that the w(s)BDC event composites coincide with significant negative (positive) SATmax anomalies and positive (negative) rainfall over South Africa. We suggest that the wBDC’s related lower stratospheric ozone (LSO) surpluses trap the UVB meant to heat the troposphere and surface. This induces the observed negative middle to upper tropospheric air temperatures and geopotential heights resulting in cyclonic circulation anomalies that enhances rainfall and suppresses SATmax. The opposite is true for the sBDC composites where ultimately the elevated geopotential heights result in middle to upper anticyclonic tropospheric anomalies that are accompanied by rainfall deficits and increased SATmax.

Use of Airborne In Situ VOC Measurements to Estimate Transit Time Spectrum: An Observation‐Based Diagnostic of Convective Transport

AbstractConvective transport from the marine boundary layer to the upper troposphere (UT) is investigated using airborne in situ measurements of chemical species over the tropical western Pacific. Using 42 volatile organic compounds with photochemical lifetimes ranging from shorter than a day to multiple decades, we derive a transit time spectrum G(t) and the associated modal and mean transit times for the UT air mass over the convectively dominant tropical western Pacific region. G(t) describes relative contributions of air masses transported from the marine boundary layer to the UT via all transport paths with different transit times. We further demonstrate that the volatile organic compound‐derived transit time scale is broadly comparable to that estimated from convective mass flux. The observation‐based transit time spectrum not only provides insights into convective transport pathways, but also has the potential to serve as an effective diagnostic for evaluating the representation of convective transport in global models.

Springtime Beryllium-7, meteorology, and ozone variability in the southeastern United States

Ground level 24 h average observations of 7Be activity, combined with continuous ozone (O3), carbon monoxide (CO) and minimum relative humidity (minRH) measurements, were conducted at two non-urban sites in the Deep South of the United States. One site is inland at Yorkville, Georgia, YRK (33°55′27″N; 84°59′44″W); the other is near the coast of the Gulf of Mexico outside Pensacola, Florida, OLF (30°25′N:87°13′W). The objective of the measurements was to explore the potential for estimating a contribution to surface O3 from stratospheric and upper tropospheric air for during the springtime months from April 2 to June 13, 2015 using 7Be as a tracer. The observed 24 h average 7Be activities were 1.88 ± 0.66 mBq/m3 at YRK and 1.99 ± 0.68 mBq/m3 at OLF. Corresponding means of 24 h average O3 mixing ratios were 38.3 ± 10.1 ppbv for YRK and 28.7 ± 8.9 ppbv at OLF. A weak statistically significant O37Be regression based estimate of O3 from the stratosphere and upper troposphere was constrained to a conservative upper bound of 14 ± 4 (1σ) ppbv. From daily inspection of meteorological features, a lower bound of 3–7 ppbv was estimated. A multiple regression of O3 versus 7Be and daily minimum relative humidity (minRH) improved the statistical fit and indicated stratosphere-upper troposphere contributions of 8.6 ± 4.0 ppbv for YRK and 6.6 ± 3.3 ppbv for OLF. Daily variability of 7Be and O3 was explored with respect to meteorological variability. 7BeO3 relationships in this experiment were examined using (a) ozonesonde and vertical dew point temperature profiles, inferring very dry air as an upper atmosphere tracer descending into the boundary layer, (b) backward air trajectories, identifying 7Be spatial and temporal variation, and (c) precipitation, indicating 7Be scavenging and lowered O3 with suppression of photochemistry. The average 7Be measurements at the ground during the study are useful for helping estimate the long-term O3 contributions from the upper atmosphere. However, the day-to-day 7Be observations had limited value for determining the contributions of upper air O3 to daily O3 mixing ratios. Conventional surface and upper-air meteorological data could be used effectively as an alternative.

Vertical profile variations of ozone in lower stratosphere in Indonesia and influence to upper troposphere ozone based on satellite

This study examined the vertical profile and ozone variation in the lower stratosphere in Indonesia using AQUA/AIRS and AURA/MLS satellite data. Ozone in the stratosphere as an important component in atmospheric chemistry as well as radiation and climate becomes important to learn. Seasonal vertical profiles, time-varying vertical profiles, ozone seasonal variations at pressures of 100 hPa and 70 hPa, ozone time series at pressures of 100 hPa and 70 hPa from 2002 to 2016, average zonal variation (influence latitude) ozone concentrations in Indonesia, and the comparison of the vertical profiles of ozone, HCl, and N2O in the lower stratosphere layer in Indonesia from MLS/AURA satellite data have been done to understand the variation of ozone in the lower stratosphere in Indonesia. The results show that the vertical ozone profile increased from the tropopause then the lower stratosphere to the middle stratosphere with the highest concentration of up to 9 ppmv. The monthly variation of ozone climatology at 70 hPa shows a pattern with a maximum peak in August while at a pressure of 100 hPa it indicates the presence of two maximum peaks in June and September. Time series of ozone at 100 hPa and 70 hPa from 2002 to 2016 show that ozone concentration tended to be constant with very small concentration increase occurring at 70 hPa and 100 hPa. Zonal variation shows the lowest ozone concentration at zero degrees latitude compared to other latitudes, and the vertical profile of ozone has the same pattern as HCl while it is different from N2O. Vertical-time series cross section of ozone and Potential Vorticity (PV) in upper troposphere show influenced of stratospheric air into upper tropospheric air which showed by higher ozone and PV value and can reach until pressure 150 hPa occurred in the same season.

Modulation of Winter Precipitation Dynamics Over the Arabian Gulf by ENSO

AbstractThe Arabian Gulf (Gulf) and the surrounding regions are centers of intense economic activity. The precipitating weather systems that form over the Gulf are important for this predominantly arid region. It is suggested that El Niño–Southern Oscillation (ENSO) influences the Middle East precipitation variability through an equatorward shift of the subtropical jet. Here we present compelling evidence to illustrate the role of ENSO in modulating the local dynamics and moisture transport in initiating precipitation during different ENSO phases using satellite and reanalysis data. It is found that the moisture transport from the Red and Arabian Seas toward the Gulf is stronger during El Niño years. The pattern and strength of moisture transport toward the Gulf is weakened during La Niña and neutral years, with most of the transport directed toward the northern Gulf. Using a 120 h back trajectory analysis, it is found that while the air parcels coming toward the Gulf from the Arabian and Red Seas side originate at lower tropospheric levels, the air parcels from the Mediterranean originate at middle and upper tropospheric levels during El Niño years. In contrast, upper tropospheric air parcels originating over the southern Arabian Sea plays a dominant role on Gulf precipitation during La Niña and neutral years. The seasonal mean transients of zonal winds show a robust ENSO signature over the Gulf, indicating a favorable (less favorable) condition for the penetration of midlatitude eddies over the region during El Niño (La Niña) winters.

A growing threat to the ozone layer from short-lived anthropogenic chlorocarbons

Abstract. Large and effective reductions in emissions of long-lived ozone-depleting substance (ODS) are being achieved through the Montreal Protocol, the effectiveness of which can be seen in the declining atmospheric abundances of many ODSs. An important remaining uncertainty concerns the role of very short-lived substances (VSLSs) which, owing to their relatively short atmospheric lifetimes (less than 6 months), are not regulated under the Montreal Protocol. Recent studies have found an unexplained increase in the global tropospheric abundance of one VSLS, dichloromethane (CH2Cl2), which has increased by around 60 % over the past decade. Here we report dramatic enhancements of several chlorine-containing VSLSs (Cl-VSLSs), including CH2Cl2 and CH2ClCH2Cl (1,2-dichloroethane), observed in surface and upper-tropospheric air in East and South East Asia. Surface observations were, on occasion, an order of magnitude higher than previously reported in the marine boundary layer, whilst upper-tropospheric data were up to 3 times higher than expected. In addition, we provide further evidence of an atmospheric transport mechanism whereby substantial amounts of industrial pollution from East Asia, including these chlorinated VSLSs, can rapidly, and regularly, be transported to tropical regions of the western Pacific and subsequently uplifted to the tropical upper troposphere. This latter region is a major provider of air entering the stratosphere, and so this mechanism, in conjunction with increasing emissions of Cl-VSLSs from East Asia, could potentially slow the expected recovery of stratospheric ozone.

Stratospheric entry point for upper-tropospheric air within the Asian summer monsoon anticyclone

The Asian summer monsoon (ASM) anticyclone isolates upper-tropospheric air within the interior of the anticyclone from the outside. Forward trajectory simulations in previous studies have shown that much of the air within the ASM anticyclone can be trapped for up to two or three weeks, not only laterally but also vertically. Here, we investigate the locations of exit points for upper-tropospheric air trapped within the ASM anticyclone, especially the preferred tropopause-crossing locations, using a 3-dimensional trajectory model. Forward trajectory calculations show two-thirds of the air crosses the tropopause at the southern part of the anticyclone via upward diabatic transport. Furthermore, some air crosses at northern and eastern parts via isentropic shedding, but air crosses rarely through the center of the anticyclone. However, calculations also show that many stratospheric parcels within the anticyclone are traceable from the upper-tropospheric anticyclone. This implies they cannot break through the tropopause directly overhead but instead enter the stratosphere via other entry points.

Atmospheric boundary layer sources for upper tropospheric air over the Asian summer monsoon region

AbstractPrevious satellite measurements and model simulations have shown that the Asian summer monsoon (ASM) anticyclone is co-located with higher concentrations of pollutants, which are emitted in the continental atmospheric boundary layer (ABL). Backward trajectory calculations show that the air at the 150-hPa level has the maximum frequency of ABL sources within 30 days over the most intensive convection regions and their downwind areas, which are not located within the ASM anticyclone, but rather at the southern flank or periphery of the ASM anticyclone. The upper tropospheric airs originated from the ABL sources include two parts: one from the ocean, which has the dominant impact to the south of 20°N, particularly over the South China Sea (SCS) and the west tropical Pacific Ocean; and another from the continent, which is dominant between 10°N and 30°N, particularly over the Bay of Bengal (BoB), continental India, the Arabian Sea, and the Arabian Peninsula. It is the latter part that forms the higher ...

Trace gas composition in the Asian summer monsoon anticyclone: a case study based on aircraft observations and model simulations

Abstract. We present in situ measurements of the trace gas composition of the upper tropospheric (UT) Asian summer monsoon anticyclone (ASMA) performed with the High Altitude and Long Range Research Aircraft (HALO) in the frame of the Earth System Model Validation (ESMVal) campaign. Air masses with enhanced O3 mixing ratios were encountered after entering the ASMA at its southern edge at about 150 hPa on 18 September 2012. This is in contrast to the presumption that the anticyclone's interior is dominated by recently uplifted air with low O3 in the monsoon season. We also observed enhanced CO and HCl in the ASMA, which are tracers for boundary layer pollution and tropopause layer (TL) air or stratospheric in-mixing respectively. In addition, reactive nitrogen was enhanced in the ASMA. Along the HALO flight track across the ASMA boundary, strong gradients of these tracers separate anticyclonic from outside air. Lagrangian trajectory calculations using HYSPLIT show that HALO sampled a filament of UT air three times, which included air masses uplifted from the lower or mid-troposphere north of the Bay of Bengal. The trace gas gradients between UT and uplifted air masses were preserved during transport within a belt of streamlines fringing the central part of the anticyclone (fringe), but are smaller than the gradients across the ASMA boundary. Our data represent the first in situ observations across the southern part and downstream of the eastern ASMA flank. Back-trajectories starting at the flight track furthermore indicate that HALO transected the ASMA where it was just splitting into a Tibetan and an Iranian part. The O3-rich filament is diverted from the fringe towards the interior of the original anticyclone, and is at least partially bound to become part of the new Iranian eddy. A simulation with the ECHAM/MESSy Atmospheric Chemistry (EMAC) model is found to reproduce the observations reasonably well. It shows that O3-rich air is entrained by the outer streamlines of the anticyclone at its eastern flank. Back-trajectories and increased HCl mixing ratios indicate that the entrained air originates in the stratospherically influenced TL. Photochemical ageing of air masses in the ASMA additionally increases O3 in originally O3-poor, but CO-rich air. Simulated monthly mean trace gas distributions show decreased O3 in the ASMA centre only at the 100 hPa level in July and August, but at lower altitudes and in September the ASMA is dominated by increased O3. The combination of entrainment from the tropopause region, photochemistry and dynamical instabilities can explain the in situ observations, and might have a larger impact on the highly variable trace gas composition of the anticyclone than previously thought.

Two types of summertime heating over the Asian large-scale orography and excitation of potential-vorticity forcing I. Over Tibetan Plateau

Based on numerical simulation, this study explored the characteristics and interactions of surface sensible heating and atmospheric latent heating over the main part of the Tibetan Plateau, i.e., terrain at elevations >2 km in summer. The impacts of these two types of heating on local vertical motion and monsoonal meridional circulation were compared. Theoretical analysis and numerical experimentation demonstrated that by changing the configuration of the upper-tropospheric air temperature and circulation, the two types of heating could generate both minimum absolute vorticity and abnormal potential vorticity forcing near the tropopause, enhance the meridional circulation of the Asian summer monsoon, and produce an eastward- propagating Rossby wave train within the mid-latitude westerly flow. Consequently, the manifestations of these features were shown to influence the circulation of the Northern Hemisphere.

Oxidation of mercury by bromine in the subtropical Pacific free troposphere

AbstractMercury is a global toxin that can be introduced to ecosystems through atmospheric deposition. Mercury oxidation is thought to occur in the free troposphere by bromine radicals, but direct observational evidence for this process is currently unavailable. During the 2013 Nitrogen, Oxidants, Mercury and Aerosol Distributions, Sources and Sinks campaign, we measured enhanced oxidized mercury and bromine monoxide in a free tropospheric air mass over Texas. We use trace gas measurements, air mass back trajectories, and a chemical box model to confirm the origin and chemical history of the sampled air mass. We find the presence of elevated oxidized mercury to be consistent with oxidation of elemental mercury by bromine atoms in this subsiding upper tropospheric air mass within the subtropical Pacific High, where dry atmospheric conditions are conducive to oxidized mercury accumulation. Our results support the role of bromine as the dominant oxidant of mercury in the upper troposphere.

Methyl chloride as a tracer of tropical tropospheric air in the lowermost stratosphere inferred from IAGOS‐CARIBIC passenger aircraft measurements

AbstractWe present variations of methyl chloride (CH3Cl) and nitrous oxide (N2O) in the lowermost stratosphere (LMS) obtained from air samples collected by the In‐service Aircraft for a Global Observing System‐Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container (IAGOS‐CARIBIC) passenger aircraft observatory for the period 2008–2012. To correct for the temporal increase of atmospheric N2O, the CARIBIC N2O data are expressed as deviations from the long‐term trend at the northern hemispheric baseline station Mauna Loa, Hawaii (ΔN2O). ΔN2O undergoes a pronounced seasonal variation in the LMS with a minimum in spring. The amplitude increases going deeper in the LMS (up to potential temperature of 40 K above the thermal tropopause), as a result of the seasonally varying subsidence of air from the stratospheric overworld. Seasonal variation of CH3Cl above the tropopause is similar in phase to that of ΔN2O. Significant correlations are found between CH3Cl and ΔN2O in the LMS from winter to early summer, both being affected by mixing between stratospheric air and upper tropospheric air. This correlation, however, disappears in late summer to autumn. The slope of the CH3Cl‐ΔN2O correlation observed in the LMS allows us to determine the stratospheric lifetime of CH3Cl to be 35 ± 7 years. Finally, we examine the partitioning of stratospheric air and tropical/extratropical tropospheric air in the LMS based on a mass balance approach using ΔN2O and CH3Cl. This analysis clearly indicates efficient inflow of tropical tropospheric air into the LMS in summer and demonstrates the usefulness of CH3Cl as a tracer of tropical tropospheric air.

Aerosol transport and wet scavenging in deep convective clouds: A case study and model evaluation using a multiple passive tracer analysis approach

AbstractWet scavenging of aerosols by continental deep convective clouds is studied for a supercell storm complex observed over Oklahoma during the Deep Convective Clouds and Chemistry campaign. A new passive‐tracer‐based transport analysis framework is developed to characterize convective transport using vertical profiles of several passive trace gases. For this case, the analysis estimates that observed passive gas mixing ratios in the upper troposphere convective outflow consist of 47% low level (<3 km) inflow air, 32% entrained midtroposphere air, and 21% upper troposphere air. The new analysis framework is used to estimate aerosol wet scavenging efficiencies. Observations yield high overall scavenging efficiencies of 81% for submicron aerosol mass. Organic, sulfate, and ammonium aerosols have similar wet scavenging efficiencies (80%–84%). The apparent scavenging efficiency for nitrate aerosol is much lower (57%), but the scavenging efficiency for nitrate aerosol plus nitric acid combined (84%) is close to the other species. Scavenging efficiencies for aerosol number are high for larger particles (84% for 0.15–2.5 µm diameter) but are lower for smaller particles (64% for 0.03–0.15 µm). The storm is simulated using the chemistry version of the Weather Research and Forecasting model. Compared to the observation‐based analysis, the standard model strongly underestimates aerosol scavenging efficiencies by 32% and 41% in absolute differences for submicron mass and number. Adding a new treatment of secondary activation significantly improves simulated aerosol scavenging, producing wet scavenging efficiencies that are only 7% and 8% lower than observed efficiencies. This finding emphasizes the importance of secondary activation for aerosol wet removal in deep convective storms.