Mijeong Park

Asian Monsoon Transport of Pollution to the Stratosphere

Riding the Monsoon Most air transport from the troposphere to the stratosphere occurs in the tropics, but additional transport may occur in areas of strong upward convection. Randel et al. (p. 611, published online 25 March) report satellite measurements of atmospheric hydrogen cyanide over the region where the Asian summer monsoon occurs, which indicate that air is transported from the surface to deep within the stratosphere. This mechanism represents a pathway for pollutants to enter the global stratosphere, where they might affect ozone chemistry, aerosol characteristics, and radiative properties. Satellite observations of atmospheric hydrogen cyanide reveal that the Asian monsoon transports air deep into the stratosphere. Transport of air from the troposphere to the stratosphere occurs primarily in the tropics, associated with the ascending branch of the Brewer-Dobson circulation. Here, we identify the transport of air masses from the surface, through the Asian monsoon, and deep into the stratosphere, using satellite observations of hydrogen cyanide (HCN), a tropospheric pollutant produced in biomass burning. A key factor in this identification is that HCN has a strong sink from contact with the ocean; much of the air in the tropical upper troposphere is relatively depleted in HCN, and hence, broad tropical upwelling cannot be the main source for the stratosphere. The monsoon circulation provides an effective pathway for pollution from Asia, India, and Indonesia to enter the global stratosphere.

Transport above the Asian summer monsoon anticyclone inferred from Aura Microwave Limb Sounder tracers

[1] Tracer variability above the Asian summer monsoon anticyclone is investigated using Aura Microwave Limb Sounder (MLS) measurements of carbon monoxide, ozone, water vapor, and temperature during Northern Hemisphere summer (June to August) of 2005. Observations show persistent maxima in carbon monoxide and minima in ozone within the anticyclone in the upper troposphere–lower stratosphere (UTLS) throughout summer, and variations in these tracers are closely related to the intensity of underlying deep convection. Temperatures in the UTLS are also closely coupled to deep convection (cold anomalies are linked with enhanced convection), and the three-dimensional temperature patterns are consistent with a dynamical response to near- equatorial convection. Upper tropospheric water vapor in the monsoon region is strongly coherent with deep convection, both spatially and temporally. However, at the altitude of the tropopause, maximum water vapor is centered within the anticyclone, distant from the deepest convection, and is also less temporally correlated with convective intensity. Because the main outflow of deep convection occurs near 12 km, well below the tropopause level (16 km), we investigate the large-scale vertical transport within the anticyclone. The mean vertical circulation obtained from the ERA40 reanalysis data set and a free-running general circulation model is upward across the tropopause on the eastern end of the anticyclone, as part of the balanced threedimensional monsoon circulation. In addition to deep transport from the most intense convection, this large-scale circulation may help explain the transport of constituents to tropopause level.

Transport pathways of carbon monoxide in the Asian summer monsoon diagnosed from Model of Ozone and Related Tracers (MOZART)

[1] Satellite observations of tropospheric chemical constituents (such as carbon monoxide, CO) reveal a persistent maximum in the upper troposphere―lower stratosphere (UTLS) associated with the Asian summer monsoon anticyclone. Diagnostic studies suggest that the strong anticyclonic circulation acts to confine air masses, but the sources of pollution and transport pathways to altitudes near the tropopause are the subject of debate. Here we use the Model for Ozone and Related Tracers 4 (MOZART-4) global chemistry transport model, driven by analyzed meteorological fields, to study the source and transport of CO in the Asian monsoon circulation. A MOZART-4 simulation for one summer is performed, and results are compared with satellite observations of CO from the Aura Microwave Limb Sounder and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer. Overall, good agreement is found between the modeled and observed CO in the UTLS, promoting confidence in the model simulation. The model results are then analyzed to understand the sources and transport pathways of CO in the Asian monsoon region, and within the anticyclone in particular. The results show that CO is transported upward by monsoon deep convection, with the main surface sources from India and Southeast Asia. The uppermost altitude of the convective transport is ∼12 km, near the level of main deep convective outflow, and much of the CO is then advected in the upper troposphere northeastward across the Pacific Ocean and southwestward with the cross-equatorial Hadley flow. However, some of the CO is also advected vertically to altitudes near the tropopause (∼16 km) by the large-scale upward circulation on the eastern side of the anticyclone, and this air then becomes trapped within the anticyclone (to the west of the convection, extending to the Middle East). Within the anticyclone, the modeled CO shows a relative maximum near 15 km, in good agreement with observations.

A Large Annual Cycle in Ozone above the Tropical Tropopause Linked to the Brewer–Dobson Circulation

Near-equatorial ozone observations from balloon and satellite measurements reveal a large annual cycle in ozone above the tropical tropopause. The relative amplitude of the annual cycle is large in a narrow vertical layer between 16 and 19 km, with approximately a factor of 2 change in ozone between the minimum (during NH winter) and maximum (during NH summer). The annual cycle in ozone occurs over the same altitude region, and is approximately in phase with the well-known annual variation in tropical temperature. This study shows that the large annual variation in ozone occurs primarily because of variations in vertical transport associated with mean upwelling in the lower stratosphere (the Brewer–Dobson circulation); the maximum relative amplitude peak in the lower stratosphere is collocated with the strongest background vertical gradients in ozone. A similar large seasonal cycle is observed in carbon monoxide (CO) above the tropical tropopause, which is approximately out of phase with ozone (associated with an oppositely signed vertical gradient). The observed ozone and CO variations can be used to constrain estimates of the seasonal cycle in tropical upwelling.

Global variations of HDO and HDO/H2O ratios in the upper troposphere and lower stratosphere derived from ACE-FTS satellite measurements

[1] High-quality satellite observations of water and deuterated water in the upper troposphere and lower stratosphere (UTLS) from the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) are used to map global climatological behavior. Spatial and temporal variability in these data suggest that convection plays a significant role in setting water vapor isotopic composition in these regions. In many instances, enhancements in HDO/H2O (i.e., dD) are closely tied to patterns of climatological deep convection and uncorrelated with water vapor, although convection appears to have different isotopic effects in different locations. The ACE-FTS data reveal seasonal variations in the tropics and allow mapping of climatological regional structure. These data reveal strong regional isotopic enhancement associated with the North American summer monsoon but not the Asian monsoon or the western Pacific warm pool. We suggest that the isotopic effects of deep convection near the tropopause are moderated by the ambient relative humidity, which controls the amount of convective ice that evaporates. Local convective signals can in turn affect global behavior: the North America monsoon influence introduces a Northern Hemisphere–Southern Hemisphere asymmetry in water isotopic composition in the lower stratosphere that extends into the tropics and influences the apparent seasonal cycle in averaged tropical UTLS data. Seasonal variation in tropical lower stratospheric water isotopic composition extends up to � 20 km in ACE retrievals, but in contrast to previous reports, there is no clear evidence of propagation beyond the lowermost stratosphere. The reliability of these observations is supported by the broad consistency of ACE-FTS averaged tropical profiles with previous remote and in situ dD measurements.

Processes regulating short-lived species in the tropical tropopause layer

[1] A one-dimensional model of vertical transport in the tropical tropopause layer (TTL) is developed. The model uses vertical advection, a convective source, and a chemical sink to simulate the profiles of very short lived substances in the TTL. The model simulates evanescent profiles of short-lived hydrocarbon species observed by satellite and is also used to simulate short-lived bromine species. Tracers with chemical lifetimes of 25 days or longer have significant concentrations in the stratosphere, and vertical advection is critical. Convection is important up to its peak altitude, nearly 19 km. Convection dominates the distribution of species with lifetimes less than 25 days. The annual cycle of species with lifetimes longer than 25 days is governed primarily by the variations of vertical velocity, not convection. This is particularly true for carbon monoxide, where a seasonal cycle in the lower stratosphere of the right phase is produced without variations in tropospheric emissions. An analysis of critical short-lived bromine species (CH 2 Br 2 and CHBr 3 ) indicates that substantial amounts of these tracers may get advected into the lower stratosphere as source gases at 18 km, and are estimated to contribute 2.8 pptv (1.1-4.1) to stratospheric bromine.

Comparison of upper tropospheric carbon monoxide from MOPITT, ACE-FTS, and HIPPO-QCLS

Products from the Measurements Of Pollution In The Troposphere (MOPITT) instrument are regularly validated using in situ airborne measurements. However, few of these measurements reach into the upper troposphere, thus hindering MOPITT validation in that region. Here we evaluate upper tropospheric (~500 hPa to the tropopause) MOPITT CO profiles by comparing them to satellite Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) retrievals and to measurements from the High-performance Instrumented Airborne Platform for Environmental Research Pole to Pole Observations (HIPPO) Quantum Cascade Laser Spectrometer (QCLS). Direct comparison of colocated v5 MOPITT thermal infrared-only retrievals, v3.0 ACE-FTS retrievals, and HIPPO-QCLS measurements shows a slight positive MOPITT CO bias within its 10% accuracy requirement with respect to the other two data sets. Direct comparison of colocated ACE-FTS and HIPPO-QCLS measurements results in a small number of samples due to the large disparity in sampling pattern and density of these data sets. Thus, two additional indirect techniques for comparison of noncoincident data sets have been applied: tracer-tracer (CO-O3) correlation analysis and analysis of profiles in tropopause coordinates. These techniques suggest a negative bias of ACE-FTS with respect to HIPPO-QCLS; this could be caused by differences in resolution (horizontal, vertical) or by deficiencies in the ACE-FTS CO retrievals below ~20 km of altitude, among others. We also investigate the temporal stability of MOPITT and ACE-FTS data, which provide unique global CO records and are thus important in climate analysis. Our results indicate that the relative bias between the two data sets has remained generally stable during the 2004–2010 period.