Uncertainties and assessments of chemistry-climate models of the stratosphere

In recent years a number of chemistry-climate models have been developed with an emphasis on the stratosphere. Such models cover a wide range of time scales of integration and vary considerably in complexity. The results of specific diagnostics are here analysed to examine the differences amongst individual models and observations, to assess the consistency of model predictions, with a particular focus on polar ozone. For example, many models indicate a significant cold bias in high latitudes, the “cold pole problem”, particularly in the southern hemisphere during winter and spring. This is related to wave propagation from the troposphere which can be improved by improving model horizontal resolution and with the use of non-orographic gravity wave drag. As a result of the widely differing modelled polar temperatures, different amounts of polar stratospheric clouds are simulated which in turn result in varying ozone values in the models. The results are also compared to determine the possible future behaviour of ozone, with an emphasis on the polar regions and mid-latitudes. All models predict eventual ozone recovery, but give a range of results concerning its timing and extent. Differences in the simulation of gravity waves and planetary waves as well as model resolution are likely major sources of uncertainty for this issue. In the Antarctic, the ozone hole has probably reached almost its deepest although the vertical and horizontal extent of depletion may increase slightly further over the next few years. According to the model results, Antarctic ozone recovery could begin any year within the range 2001 to 2008. The limited number of models which have been integrated sufficiently far indicate that full recovery of ozone to 1980 levels may not occur in the Antarctic until about the year 2050. For the Arctic, most models indicate that small ozone losses may continue for a few more years and that recovery could begin any year within the range 2004 to 2019. The start of ozone recovery in the Arctic is therefore expected to appear later than in the Antarctic.

Planetary-wave-induced transport in the stratosphere

In the stratosphere, chemical tracers are drawn systematically from the equator to the pole. This observed Brewer–Dobson circulation is driven by wave drag, which in the stratosphere arises mainly from the breaking and dissipation of planetary-scale Rossby waves. While the overall sense of the circulation follows from fundamental physical principles, a quantitative theoretical understanding of the connection between wave drag and Lagrangian transport is limited to linear, small-amplitude waves. However, planetary waves in the stratosphere generally grow to a large amplitude and break in a strongly nonlinear fashion. This paper addresses the connection between stratospheric wave drag and Lagrangian transport in the presence of strong nonlinearity, using a mechanistic three-dimensional primitive equations model together with offline particle advection. Attention is deliberately focused on a weak forcing regime, such that sudden warmings do not occur and a quasi-steady state is reached, in order to examine this question in the cleanest possible context. Wave drag is directly linked to the transformed Eulerian mean (TEM) circulation, which is often used as a surrogate for mean Lagrangian motion. The results show that the correspondence between the TEM and mean Lagrangian velocities is quantitatively excellent in regions of linear, nonbreaking waves (i.e., outside the surf zone), where streamlines are not closed. Within the surf zone, where streamlines are closed and meridional particle displacements are large, the agreement between the vertical components of the two velocity fields is still remarkably good, especially wherever particle paths are coherent so that diabatic dispersion is minimized. However, in this region the meridional mean Lagrangian velocity bears little relation to the meridional TEM velocity, and reflects more the kinematics of mixing within and across the edges of the surf zone. The results from the mechanistic model are compared with those from the Canadian Middle Atmosphere Model to test the robustness of the conclusions.

Issues in stratosphere-troposphere coupling

An overview is given of current issues concerning the coupling between the stratosphere and troposphere. The tropopause region, more generally the upper troposphere/lower stratosphere, is the region of direct contact where exchange of material takes place. Dynamical coupling through angular momentum transfer by waves occurs nonlocally, and provides a generally negative torque on the stratosphere which drives an equator-to-pole circulation (i.e., towards the Earth’s axis of rotation). This wave-driven circulation is the principal mechanism for intraseasonal and interannual variability in the extratropical stratosphere. Although such variability is generally dynamical in origin, there are important chemical and radiative feedbacks. The location of the tropopause has implications for radiative forcing of climate, through its effect on the distribution of relatively short-lived greenhouse gases (ozone and water vapour). Some outstanding puzzles in our current understanding are identified. Attention is focused on possible climate sensitivities, and how these may be tested and constrained. Results from the Canadian Middle Atmosphere Model (CMAM), a fully interactive radiative-chemical-dynamical general circulation model, are used to illustrate some of the points.

Mechanisms for tropical upwelling in the stratosphere

The dynamics of the tropical upwelling branch of the stratospheric Brewer–Dobson circulation are examined, with a particular focus on the role of the middle-atmosphere Hadley circulation. Upwelling is examined in terms of both the diabatic circulation and Lagrangian trajectories using a zonally symmetric balance model. The behavior of the wave-driven circulation in the presence of angular momentum redistribution by the Hadley circulation is also considered. The results of the zonally symmetric model are compared with fields from a middle-atmosphere GCM. It is found that the Hadley circulation makes a significant contribution to annual mean tropical upwelling at the upwelling maximum in the vicinity of the stratopause, and can account for most of the annual mean upwelling seen in the GCM. In the mid- to lower stratosphere, the role of the Hadley circulation is much weaker and wave drag appears to be required to explain the observed upwelling, although the Hadley circulation makes a nonnegligible contribution to the annual cycle of the upwelling. Subtropical wave drag can produce annual mean upwelling through a nonlinear mechanism; viscosity is not required. However, the magnitude of the observed upwelling suggests that wave drag must penetrate quite close to the equator.

On the nature of large-scale mixing in the stratosphere and mesosphere

Studies of tracer transport in the stratosphere have shown that adiabatic quasi-horizontal tracer evolution is controlled primarily by the large-scale low-frequency component of the flow. This behavior is consistent with the concept of chaotic advection, wherein the Eulerian velocity field is spatially coherent and temporally quasi-regular on timescales over which the Lagrangian evolution is chaotic. In this study, winds from a middle atmosphere general circulation model (the Canadian Middle Atmosphere Model) are used to compare and contrast the nature of tracer evolution in the stratosphere and mesosphere. It is found that the concept of chaotic advection is relevant in the stratosphere but not in the mesosphere. The explanation for this behavior is the increased strength of gravity wave activity in the mesosphere as compared with the stratosphere, which leads to shallower kinetic energy spectra on synoptic scales and a much shorter Eulerian correlation time. The shallower kinetic energy spectra imply that tracer evolution in the mesosphere is spectrally local, in contrast with the spectrally nonlocal regime that prevails in the stratosphere. This means that tracer advection calculations in the mesosphere are controlled primarily by the gravity wave spectrum and are intrinsically resolution dependent.

A closer look at chaotic advection in the stratosphere: part I: geometric structure

The relevance of chaotic advection to stratospheric mixing and transport is addressed in the context of (i) a numerical model of forced shallow-water flow on the sphere, and (ii) a middle-atmosphere general circulation model. It is argued that chaotic advection applies to both these models if there is suitable large-scale spatial structure in the velocity field and if the velocity field is temporally quasi-regular. This spatial structure is manifested in the form of “cat’s eyes” in the surf zone, such as are commonly seen in numerical simulations of Rossby wave critical layers; by analogy with the heteroclinic structure of a temporally aperiodic chaotic system the cat’s eyes may be thought of as an “organizing structure” for mixing and transport in the surf zone. When this organizing structure exists, Eulerian and Lagrangian autocorrelations of the velocity derivatives indicate that velocity derivatives decorrelate more rapidly along particle trajectories than at fixed spatial locations (i.e., the velocity field is temporally quasi-regular). This phenomenon is referred to as Lagrangian random strain.

A closer look at chaotic advection in the stratosphere: part II: statistical diagnostics

Statistical diagnostics of mixing and transport are computed for a numerical model of forced shallow-water flow on the sphere and a middle-atmosphere general circulation model. In particular, particle dispersion statistics, transport fluxes, Liapunov exponents (probability density functions and ensemble averages), and tracer concentration statistics are considered. It is shown that the behavior of the diagnostics is in accord with that of kinematic chaotic advection models so long as stochasticity is sufficiently weak. Comparisons with random-strain theory are made.

Tracing troposphere-to-stratosphere transport above a mid-latitude deep convective system

Within the project SPURT (trace gas measurements in the tropopause region) a variety of trace gases have been measured in situ in order to investigate the role of dynamical and chemical processes in the extra-tropical tropopause region. In this paper we report on a flight on 10 November 2001 leading from Hohn, Germany (52�N) to Faro, Portugal (37�N) through a strongly developed deep stratospheric intrusion. This streamer was associated with a large convective system over the western Mediterranean with potentially significant troposphere-to-stratosphere transport. Along major parts of the flight we measured unexpectedly high NOy mixing ratios. Also H2O mixing ratios were significantly higher than stratospheric background levels confirming the extraordinary chemical signature of the probed air masses in the interior of the streamer. Backward trajectories encompassing the streamer enable to analyze the origin and physical characteristics of the air masses and to trace troposphere-to-stratosphere transport. Near the western flank of the streamer features caused by long range transport, such as tropospheric filaments characterized by sudden drops in the O3 and NOy mixing ratios and enhanced CO and H2O can be reconstructed in great detail using the reverse domain filling technique. These filaments indicate a high potential for subsequent mixing with the stratospheric air. At the south-western edge of the streamer a strong gradient in the NOy and the O3 mixing ratios coincides very well with a sharp gradient in potential vorticity in the ECMWF fields. In contrast, in the interior of the streamer the observed highly elevated NOy and H2O mixing ratios up to a potential temperature level of 365K and potential vorticity values of maximum 10 PVU cannot be explained in terms of resolved troposphere-to-stratosphere transport along the backward trajectories. Also mesoscale simulations with a High Resolution Model reveal no direct evidence for convective H2O injection up to this level. Elevated H2O mixing ratios in the ECMWF and HRM are seen only up to about tropopause height at 340 hPa and 270 hPa, respectively, well below flight altitude of about 200 hPa. However, forward tracing of the convective influence as identified by satellite brightness temperature measurements and counts of lightning strokes shows that during this part of the flight the aircraft was closely following the border of an air mass which was heavily impacted by convective activity over Spain and Algeria. This is evidence that deep convection at mid-latitudes may have a large impact on the tracer distribution of the lowermost stratosphere reaching well above the thunderstorms anvils as claimed by recent studies using cloud-resolving models.

Jet characterization in the upper troposphere/lower stratosphere (UTLS): applications to climatology and transport studies

A method of classifying the upper tropospheric/lower stratospheric (UTLS) jets has been developed that allows satellite and aircraft trace gas data and meteorological fields to be efficiently mapped in a jet coordinate view. A detailed characterization of multiple tropopauses accompanies the jet characterization. Jet climatologies show the well-known high altitude subtropical and lower altitude polar jets in the upper troposphere, as well as a pattern of concentric polar and subtropical jets in the Southern Hemisphere, and shifts of the primary jet to high latitudes associated with blocking ridges in Northern Hemisphere winter. The jet-coordinate view segregates air masses differently than the commonly-used equivalent latitude (EqL) coordinate throughout the lowermost stratosphere and in the upper troposphere. Mapping O3 data from the Aura Microwave Limb Sounder (MLS) satellite and the Winter Storms aircraft datasets in jet coordinates thus emphasizes different aspects of the circulation compared to an EqL-coordinate framework: the jet coordinate reorders the data geometrically, thus highlighting the strong PV, tropopause height and trace gas gradients across the subtropical jet, whereas EqL is a dynamical coordinate that may blur these spatial relationships but provides information on irreversible transport. The jet coordinate view identifies the concentration of stratospheric ozone well below the tropopause in the region poleward of and below the jet core, as well as other transport features associated with the upper tropospheric jets. Using the jet information in EqL coordinates allows us to study trace gas distributions in regions of weak versus strong jets, and demonstrates weaker transport barriers in regions with less jet influence. MLS and Atmospheric Chemistry Experiment-Fourier Transform Spectrometer trace gas fields for spring 2008 in jet coordinates show very strong, closely correlated, PV, tropopause height and trace gas gradients across the jet, and evidence of intrusions of stratospheric air below the tropopause below and poleward of the subtropical jet; these features are consistent between instruments and among multiple trace gases. Our characterization of the jets is facilitating studies that will improve our understanding of upper tropospheric trace gas evolution.

Measurements of NO, NOy, N2O, and O3 during SPURT: implications for transport and chemistry in the lowermost stratosphere

We present measurements of NO, NOy, O3, and N2O within the lowermost stratosphere (LMS) over Europe obtained during the SPURT project. The measurements cover all seasons between November 2001 and July 2003. They span a broad band of latitudes from 30° N to 75° N and a potential temperature range from 290 to 380 K. The measurements represent a comprehensive data set of these tracers and reveal atmospheric transport processes that influence tracer distributions in the LMS. Median mixing ratios of stratospheric tracers in equivalent latitude-potential temperature coordinates show a clear seasonal cycle related to the Brewer-Dobson circulation, with highest values in spring and lowest values in autumn. Vertical tracer profiles show strong gradients at the extratropical tropopause, suggesting that vertical (cross-isentropic) mixing is reduced above the tropopause. Pronounced meridional gradients in the tracer mixing ratios are found on potential temperature surfaces in the LMS. This suggests strongly reduced mixing along isentropes. Concurrent large gradients in static stability in the vertical direction, and of PV in the meridional direction, suggest the presence of a mixing barrier. Seasonal cycles were found in the correlation slopes ΔO3/ΔN2O and ΔNOy/ΔN2O well above the tropopause. Absolute slope values are smallest in spring indicating chemically aged stratospheric air originating from high altitudes and latitudes. Larger values were measured in summer and autumn suggesting that a substantial fraction of air takes a "short-cut" from the tropical tropopause region into the extratropical LMS. The seasonal change in the composition of the LMS has direct implications for the ozone chemistry in this region. Comparisons of measured NO with the critical NO value at which net ozone production changes from negative to positive, imply ozone production up to 20 K above the local tropopause in spring, up to 30 K in summer, and up to 40 K in autumn. Above these heights, and in winter, net ozone production is negative.

Highly resolved observations of trace gases in the lowermost stratosphere and upper troposphere from the SPURT project: an overview

During SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) we performed measurements of a wide range of trace gases with different lifetimes and sink/source characteristics in the northern hemispheric upper troposphere (UT) and lowermost stratosphere (LMS). A large number of in-situ instruments were deployed on board a Learjet 35A, flying at altitudes up to 13.7 km, at times reaching to nearly 380 K potential temperature. Eight measurement campaigns (consisting of a total of 36 flights), distributed over all seasons and typically covering latitudes between 35° N and 75° N in the European longitude sector (10° W–20° E), were performed. Here we present an overview of the project, describing the instrumentation, the encountered meteorological situations during the campaigns and the data set available from SPURT. Measurements were obtained for N2O, CH4, CO, CO2, CFC12, H2, SF6, NO, NOy, O3 and H2O. We illustrate the strength of this new data set by showing mean distributions of the mixing ratios of selected trace gases, using a potential temperature-equivalent latitude coordinate system. The observations reveal that the LMS is most stratospheric in character during spring, with the highest mixing ratios of O3 and NOy and the lowest mixing ratios of N2O and SF6. The lowest mixing ratios of NOy and O3 are observed during autumn, together with the highest mixing ratios of N2O and SF6 indicating a strong tropospheric influence. For H2O, however, the maximum concentrations in the LMS are found during summer, suggesting unique (temperature- and convection-controlled) conditions for this molecule during transport across the tropopause. The SPURT data set is presently the most accurate and complete data set for many trace species in the LMS, and its main value is the simultaneous measurement of a suite of trace gases having different lifetimes and physical-chemical histories. It is thus very well suited for studies of atmospheric transport, for model validation, and for investigations of seasonal changes in the UT/LMS, as demonstrated in accompanying and elsewhere published studies.

Determination of eddy-diffusivity in the lowermost stratosphere

We present a 2D-advection-diffusion model that simulates the main transport pathways influencing tracer distributions in the lowermost stratosphere (LMS). The model describes slow diabatic descent of aged stratospheric air, vertical (cross-isentropic) and horizontal (along isentropes) diffusion within the LMS and across the tropopause using equivalent latitude and potential temperature coordinates. Eddy diffusion coefficients parameterize the integral effect of dynamical processes leading to small scale turbulence and mixing. They were specified by matching model simulations to observed CO distributions. Interestingly, the model suggests mixing across isentropes to be more important than horizontal mixing across surfaces of constant equivalent latitude, shining new light on the interplay between various transport mechanisms in the LMS. The model achieves a good description of the small scale tracer features at the tropopause with squared correlation coefficients R2 = 0.72…0.94.

18 Nov 2013 In situ detection of electrified aerosols in the upper troposphere and stratosphere

Electrified aerosols have been observed in the lower troposphere and in the mesosphere, but have never been detected in the stratosphere and upper troposphere. We present measurements of aerosols obtained during a balloon flight to an altitude of 24 km. The measurements were per- formed with an improved version of the Stratospheric and Tropospheric Aerosol Counter (STAC) aerosol counter dedi- cated to the search for charged aerosols. It is found that most of the aerosols are charged in the upper troposphere for altitudes below 10 km and in the stratosphere for altitudes above 20 km. Conversely, the aerosols seem to be uncharged between 10 km and 20 km. Model calculations are used to quantify the electrification of the aerosols with a stratospheric aerosol–ion model. The percentages of charged aerosols obtained with model calculations are in excellent agreement with the observations below 10 km and above 20 km. However, the model cannot reproduce the absence of electrification found in the lower stratosphere, as the processes leading to neutralisation in this altitude range are unknown. The presence of sporadic transient layers of electrified aerosol in the upper troposphere and in the stratosphere could have significant implications for sprite formation

The SPARC Data Initiative: Comparison of upper troposphere/lower stratosphere ozone climatologies from limb-viewing instruments and the nadir-viewing Tropospheric Emission Spectrometer

We present the first comprehensive intercomparison of currently available satellite ozone climatologies in the upper troposphere/lower stratosphere (UTLS) (300–70 hPa) as part of the Stratosphere-troposphere Processes and their Role in Climate (SPARC) Data Initiative. The Tropospheric Emission Spectrometer (TES) instrument is the only nadir-viewing instrument in this initiative, as well as the only instrument with a focus on tropospheric composition. We apply the TES observational operator to ozone climatologies from the more highly vertically resolved limb-viewing instruments. This minimizes the impact of differences in vertical resolution among the instruments and allows identification of systematic differences in the large-scale structure and variability of UTLS ozone. We find that the climatologies from most of the limb-viewing instruments show positive differences (ranging from 5 to 75%) with respect to TES in the tropical UTLS, and comparison to a “zonal mean” ozonesonde climatology indicates that these differences likely represent a positive bias for p ≤ 100 hPa. In the extratropics, there is good agreement among the climatologies regarding the timing and magnitude of the ozone seasonal cycle (differences in the peak-to-peak amplitude of <15%) when the TES observational operator is applied, as well as very consistent midlatitude interannual variability. The discrepancies in ozone temporal variability are larger in the tropics, with differences between the data sets of up to 55% in the seasonal cycle amplitude. However, the differences among the climatologies are everywhere much smaller than the range produced by current chemistry-climate models, indicating that the multiple-instrument ensemble is useful for quantitatively evaluating these models.