In the past, studies of stratosphere-tropo-sphere exchange of mass and chemical species have mainly emphasized the synoptic-and small-scale mechanisms of exchange. This review, however, includes also the global-scale aspects of exchange, such as the transport across an isentropic surface (potential temperature about 380 K) that in the tropics lies just above the tropopause, near the 100-hPa pressure level. Such a surface divides the stratosphere into an "over-world" and an extratropical "lowermost strato-sphere" that for transport purposes need to be sharply distinguished. This approach places stratosphere-tro-posphere exchange in the framework of the general circulation and helps to clarify the roles of the different mechanisms involved and the interplay between large and small scales. The role of waves and eddies in the extratropical overworld is emphasized. There, wave-induced forces drive a kind of global-scale extratropi-cal "fluid-dynamical suction pump," which withdraws air upward and poleward from the tropical lower stratosphere and pushes it poleward and downward into the extratropical troposphere. The resulting global scale circulation drives the stratosphere away from radiative equilibrium conditions. Wave-induced forces may be considered to exert a nonlocal control, mainly downward in the extratropics but reaching laterally into the tropics, over the transport of mass across lower stratospheric isentropic surfaces. This mass transport is for many purposes a useful measure of global-scale stratosphere-troposphere exchange, especially on seasonal or longer timescales. Because the strongest wave-induced forces occur in the northern hemisphere winter season, the exchange rate is also a maximum at that season. The global exchange rate is not determined by details of near-tropopause phenomena such as penetrative cumulus convection or small-scale mixing associated with upper level fronts and cyclones. These smaller-scale processes must be considered , however, in order to understand the finer details of exchange. Moist convection appears to play an important role in the tropics in accounting for the extreme dehydration of air entering the stratosphere. Stratospheric air finds its way back into the tropo-sphere through a vast variety of irreversible eddy exchange phenomena, including tropopause folding and the formation of so-called tropical upper tropo-spheric troughs and consequent irreversible exchange. General circulation models are able to simulate the mean global-scale mass exchange and its seasonal cycle but are not able to properly resolve the tropical dehydration process. Two-dimensional (height-latitude) models commonly used for assessment of human impact on the ozone layer include representation of stratosphere-troposphere exchange that is adequate to allow reasonable simulation of photochemical processes occurring in the overworld. However, for assessing changes in the lowermost stratosphere, the strong longitudinal asymmetries in stratosphere-troposphere exchange render current two-dimensional m...

We observed a plume of air highly enriched in carbon monoxide and particles in the stratosphere at altitudes up to 15.8 km. It can be unambiguously attributed to North American forest fires. This plume demonstrates an extra‐tropical direct transport path from the planetary boundary layer several kilometers deep into the stratosphere, which is not fully captured by large‐scale atmospheric transport models. This process indicates that the stratospheric ozone layer could be sensitive to changes in forest burning associated with climatic warming.

Optically thin cirrus near the tropical tropopause regulate the humidity of air entering the stratosphere, which in turn has a strong influence on the Earth's radiation budget and climate. Recent highaltitude, unmanned aircraft measurements provide evidence for two distinct classes of cirrus formed in the tropical tropopause region: (i) vertically extensive cirrus with low ice number concentrations, low extinctions, and large supersaturations (up to ∼70%) with respect to ice; and (ii) vertically thin cirrus layers with much higher ice concentrations that effectively deplete the vapor in excess of saturation. The persistent supersaturation in the former class of cirrus is consistent with the long time-scales (several hours or longer) for quenching of vapor in excess of saturation given the low ice concentrations and cold tropical tropopause temperatures. The low-concentration clouds are likely formed on a background population of insoluble particles with concentrations less than 100 L −1 (often less than 20 L −1 ), whereas the high ice concentration layers (with concentrations up to 10,000 L −1 ) can only be produced by homogeneous freezing of an abundant population of aqueous aerosols. These measurements, along with past high-altitude aircraft measurements, indicate that the low-concentration cirrus occur frequently in the tropical tropopause region, whereas the high-concentration cirrus occur infrequently. The predominance of the low-concentration clouds means cirrus near the tropical tropopause may typically allow entry of air into the stratosphere with as much as ∼1.7 times the ice saturation mixing ratio. ATTREX | ice nucleiA lthough the stratosphere is extremely dry compared with the troposphere, stratospheric humidity plays crucial roles in both atmospheric chemistry and climate. As the primary source of hydroxyl (OH) radicals, H 2 O plays an important role in the regulation of stratospheric ozone. Small changes in stratospheric humidity can have significant influence on the Earth's radiation budget and climate (1, 2). Model simulations show that increases in stratospheric humidity enhance the rate of ozone destruction, cool the lower stratosphere, and warm the surface (3, 4).Air enters the stratospheric overworld (above 380 K potential temperature) almost exclusively via ascent across the tropical tropopause. This fact has motivated interest in understanding processes occurring in the transition layer between the tropical troposphere and stratosphere, a region of the atmosphere referred to as the Tropical Tropopause Layer (TTL). Physical processes occurring in this layer set the boundary condition for the composition and humidity of the stratosphere. It is well established that the aridity of the stratosphere is associated with "freeze-drying" of air as it passes through the cold TTL (5, 6). Deposition growth of ice crystals in optically thin, laminar TTL cirrus depletes vapor in excess of saturation, and the ice crystals sediment relative to the slowly ascending air. The common occurrence of these thin, ...

Abstract. Aerosol composition was measured by the NOAA single-particle mass spectrometer (PALMS) aboard the NASA WB-57 high altitude aircraft platform during two Aura Validation Experiment (AVE) campaigns based in Costa Rica in 2004 and 2006. These studies yielded the most complete set of aerosol composition measurements to date throughout the tropical tropopause layer (TTL) and tropical lower stratosphere. We describe the aerosol properties of the tropical atmosphere and use composition tracers to examine particle sources, the role of recent convection, and cirrus-forming potential in the TTL. Tropical dynamics and regional air sources played principal roles in dictating tropospheric aerosol properties. There was a sharp change in aerosol chemical composition at about 12 km altitude coincident with a change in convective influence. Below this level, maritime convection lofted condensable material that generated acidic, sulfate-rich aerosol. These particles contained significant amounts of methanesulfonic acid (MSA) and showed evidence of cloud processes. In contrast, continental convection injected particles and precursors directly into the TTL, yielding a population of neutralized, organic-rich aerosol. The organics were often highly oxidized and particles with oxidized organics also contained nitrate. Above the tropopause, chemical composition gradually changed toward sulfuric acid particles but neutralized particles were still abundant 2 km above the tropopause. Deep continental convection, though sporadic and geographically localized, may strongly influence TTL aerosol properties on a global scale. The abundance of organic-rich aerosol may inhibit ice nucleation and formation of tropopause level cirrus.