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Age as a diagnostic of stratospheric transport

Estimates of stratospheric age from observations of long-lived trace gases with increasing tropospheric concentrations invoke the implicit assumption that an air parcel has been transported intact from the tropopical tropopause. However, because of rapid and irreversible mixing in the stratosphere, a particular air parcel cannot be identified with one that left the troposphere at some prior time. The parcel contains a mix of air with a range of transit times, and the mean value over this range is the most appropriate definition of age. The measured tracer concentration is also a mean over the parcel, but its value depends both on the transit time distribution and the past history of the tracer in the troposphere. In principle, only if the tropospheric concentration is increasing linearly can the age be directly inferred. We illustrate these points by employing both a one-dimensional diffusive analog of stratospheric transport, and the general circulation model (GCM) of the Goddard Institute for Space Studies (GISS). Within the limits of the GCM, we estimate the time over which tropospheric tracer concentrations must be approximately linear in order to determine stratospheric age unambiguously; the concentration of an exponentially increasing tracer is a function only of age if the growth time constant is greater than about 7 years, which is true for all the chlorofluorocarbons. More rapid source variations (for example, the annual cycle in CO2) have no such direct relationship with age.

Hall, Timothy M.↗

Trajectory modeling of emissions from lower stratospheric aircraft

A series of isentropic trajectory calculations has been performed for emissions by stratospheric aircraft moving across the northern midlatitude oceanic flight corridors. Emission of exhaust is simulated by the daily initialization of air parcels along a flight path on the 500 K isentropic surface. Parcels are tracked during the first three weeks of each January from 1980 to 1994 in order to determine the interannual variability in the spatial distribution of the exhaust and the likelihood of exposure to cold temperatures. Few parcels emitted along these flight paths at this time of year had experienced nitric acid trihydrate (NAT) formation temperatures, except for the particularly cold Januarys 1986, 1987, and 1992. Large zonal fluctuations in the distribution of the emissions are typical for this time year and are strongly dependent on flight path. An extended 6-month (January-June) run in which parcels were released daily along the New York-London route shows that emissions in the flight corridor increase at a time-averaged rate which is nearly twice the rate at which the zonal average increases. In addition, local fluctuations of pollutant density can be several times higher than the zonal average and can persist for several weeks. A rapid buildup of emissions occurred during the summer months. These elevated emission levels must be considered in the interpretation of environmental impact assessments based on two-dimensional transport models.

Sparling, Lynn C.↗

A Parameterization for the Triggering of Landscape Generated Moist Convection

A set of relatively high resolution three-dimensional (3D) simulations were produced to investigate the triggering of moist convection by landscape generated mesoscale circulations. The local accumulated rainfall varied monotonically (linearly) with the size of individual landscape patches, demonstrating the need to develop a trigger function that is sensitive to the size of individual patches. A new triggering function that includes the effect of landscapes generated mesoscale circulations over patches of different sizes consists of a parcel's perturbation in vertical velocity (nu(sub 0)), temperature (theta(sub 0)), and moisture (q(sub 0)). Each variable in the triggering function was also sensitive to soil moisture gradients, atmospheric initial conditions, and moist processes. The parcel's vertical velocity, temperature, and moisture perturbation were partitioned into mesoscale and turbulent components. Budget equations were derived for theta(sub 0) and q(sub 0). Of the many terms in this set of budget equations, the turbulent, vertical flux of the mesoscale temperature and moisture contributed most to the triggering of moist convection through the impact of these fluxes on the parcel's temperature and moisture profile. These fluxes needed to be parameterized to obtain theta(sub 0) and q(sub 0). The mesoscale vertical velocity also affected the profile of nu(sub 0). We used similarity theory to parameterize these fluxes as well as the parcel's mesoscale vertical velocity.

Lynn, Barry H.↗

Distribution of Halon-1211 in the Upper Troposphere and Lower Stratosphere and the 1994 Total Bromine Budget

We report here on the details of the first, in situ, real-time measurements of H-1211 (CBrClF2) and sulfur hexafluoride (SF6) mixing ratios in the stratosphere up to 20 km. Stratospheric air was analyzed for these gases and others with a new gas chromatograph, flown aboard a National Aeronautics and Space Administration ER-2 aircraft as part of the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft mission conducted in 1994. The mixing ratio of SF6, with its nearly linear increase in the troposphere, was used to estimate the mean age of stratospheric air parcels along the ER-2 flight path. Measurements of H-1211 and mean age estimates were then combined with simultaneous measurements of CFC-11 (CCl3F), measurements of brominated compounds in stratospheric whole air samples, and records of tropospheric organic bromine mixing ratios to calculate the dry mixing ratio of total bromine in the lower stratosphere and its partitioning between organic and inorganic forms. We estimate that the organic bromine-containing species were almost completely photolyzed to inorganic species in the oldest air parcels sampled. Our results for inorganic bromine are consistent with those obtained from a photochemical, steady state model for stratospheric air parcels with CFC- I I mixing ratios greater than 150 ppt. For stratospheric air parcels with CFC-11 mixing ratios less than 50 ppt (mean age greater than or equal to 5 years) we calculate inorganic bromine mixing ratios that are approximately 20% less than the photo-chemical, steady state model. There is a 20% reduction in calculated ozone loss resulting from bromine chemistry in old air relative to some previous estimates as a result of the lower bromine levels.

Wamsley, P. R.↗

Comet Shoemaker-Levy 9, Jupiter, and Impact Shock Chemistry

Four years ago this month, a hitherto unknown comet in loose orbit around Jupiter passed so near the giant planet that it was torn apart into 20 fragments by tides. One orbit later, two years ago this month, the fragments of doomed comet P/Shoemaker Levy (SL9) fell into Jupiter. The enormous energies of these impacts (the largest fragments were nearly 1 km across and, hitting at 60 km/s, released some 2-4 x 10(exp 27) ergs) produced enormous explosions. Several of the ejecta plumes were imaged towering 3000 km above Jupiter's limb. The heat released when the plumes fell was considerable and easily observed on Earth. The impacts produced strong shocks, both promptly at the impact site and again, later, and over thousands of kilometers, when the ejecta plume reentered the atmosphere. The focus of this talk will be to discuss what the SL9 impacts taught us about impact shock chemistry - the processes, the ingredients, the results - and what inferences we may draw for impacts on early Earth. Shock chemistry generates a suite of molecules not usually seen on Jupiter. The most surprising report was of a huge amount of diatomic sulfur S2 at the site of the G impact. Other unusual products include CS, CS2, OCS, H2S, SO2, HCN, CO, and H2O; although H2S and H2O are doubtless abundant below the visible clouds. Hot or enhanced CH4 and NH3 were also detected. A general rule of shock chemistry is that CO forms until either C or O is exhausted. If O greater than C, the other products are oxidized, and excess O goes to H2O. If C greater than O, the other products are reduced, and excess C goes to HCN, C2H2, and a wide variety of more complicated organics. Ultimately, given time, the carbon would react all the way to graphite, but in practice the reactions are incomplete. The dark ejecta debris were probably composed in part of carbonaceous particles generated by the shocks. In a sense, the SL9 impacts performed the famous Miller-Urey experiment on a grand scale, with one result being the production of a lot of complex brown organic solids (called "tholins"). We use, a straightforward chemical kinetics model for the H, N, C, O, S system to follow the nonequilibrium chemistry behind the shocks. The model traces the evolving chemical composition of a parcel of gas by directly integrating the web of chemical reactions. Pressure and temperature histories of the parcels are patterned after those calculated by numerical hydrodynamic simulations of the ejecta plume. A given plume parcel is generally shocked twice; t.e a parcel shocked near the impact site is ejected at high velocity and is shocked again when it reenters the atmosphere. The final state of the gas depends mostly on the second shock, provided that the latter is hot enough. The chemical evidence is ambiguous, but most indications are that C greater than O in the shocked, reacting gas. Telltale signatures of abundant oxygen - SO2, SO, CO2, O2 - were not seen, while signatures of abundant carbon - CS, CS2, and HCN - were. On the other hand, abundant H2O would appear to require O greater than C, and two other observed sulfur species, S2 and OCS, appear to form more easily in a somewhat oxidized gas, presumable vaporized from the comet itself. Since on general principles one expects the -comet to have had a more-or-less cosmic composition, i.e. O greater than C, the production of CS, CS2, and HCN probably requires C greater than O in the shocked jovian air. This in turn implies that even the largest fragments released the bulk of their energy above the jovian water table, in all likelihood above 5 bars . There is no evidence in favor of the proposition that a significant amount of wet jovian air was shocked strongly enough to coax water to react; i.e. wet jovian air saw only temperatures significantly below 2000 K.

Zahnle, Kevin↗

Deep Convective Cloud Top Heights and Their Thermodynamic Control During CRYSTAL-FACE

Infrared (11 micron) radiances from GOES-8 and local radiosonde profiles, collected during the Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) in July 2002, are used to assess the vertical distribution of Florida-area deep convective cloud top height and test predictions as to its variation based on parcel theory. The highest infrared tops (Z(sub 11)) reached approximately to the cold point, though there is at least a 1-km uncertainty due to unknown cloud-environment temperature differences. Since lidar shows that visible 'tops' are 1 km or more above Z(sub 11), visible cloud tops frequently penetrated the lapse-rate tropopause (approx. 15 km). Further, since lofted ice content may be present up to approx. 1 km above the visible tops, lofting of moisture through the mean cold point (15.4 km) was probably common. Morning clouds, and those near Key West, rarely penetrated the tropopause. Non-entraining parcel theory (i.e., CAPE) does not successfully explain either of these results, but can explain some of the day-to-day variations in cloud top height over the peninsula. Further, moisture variations above the boundary layer account for most of the day-today variability not explained by CAPE, especially over the oceans. In all locations, a 20% increase in mean mixing ratio between 750 and 500 hPa was associated with about 1 km deeper maximum cloud penetration relative to the neutral level. These results suggest that parcel theory may be useful for predicting changes in cumulus cloud height over time, but that parcel entrainment must be taken into account even for the tallest clouds. Accordingly, relative humidity above the boundary layer may exert some control on the height of the tropical troposphere.

Sherwood, Steven C.↗

Isentropic Analysis of Convective Motions

This paper analyzes the convective mass transport by sorting air parcels in terms of their equivalent potential temperature to determine an isentropic streamfunction. By averaging the vertical mass flux at a constant value of the equivalent potential temperature, one can compute an isentropic mass transport that filters out reversible oscillatory motions such as gravity waves. This novel approach emphasizes the fact that the vertical energy and entropy transports by convection are due to the combination of ascending air parcels with high energy and entropy and subsiding air parcels with lower energy and entropy. Such conditional averaging can be extended to other dynamic and thermodynamic variables such as vertical velocity, temperature, or relative humidity to obtain a comprehensive description of convective motions. It is also shown how this approach can be used to determine the mean diabatic tendencies from the three-dimensional dynamic and thermodynamic fields. A two-stream approximation that partitions the isentropic circulation into a mean updraft and a mean downdraft is also introduced. This offers a straightforward way to identify the mean properties of rising and subsiding air parcels. The results from the two-stream approximation are compared with two other definitions of the cloud mass flux. It is argued that the isentropic analysis offers a robust definition of the convective mass transport that is not tainted by the need to arbitrarily distinguish between convection and its environment, and that separates the irreversible convective overturning fromoscillations associated with gravity waves.

Lagrangian circulation↗

Lagrangian Decomposition of the Atlantic Ocean Heat Transport at 26.5°N

Abstract The Atlantic Meridional Overturning Circulation (AMOC) plays a critical role in the global climate system through the redistribution of heat, freshwater and carbon. At 26.5°N, the meridional heat transport has traditionally been partitioned geometrically into vertical and horizontal circulation cells; however, attributing these components to the AMOC and Subtropical Gyre (STG) flow structures remains widely debated. Using water parcel trajectories evaluated within an eddy‐rich ocean hindcast, we present the first Lagrangian decomposition of the meridional heat transport at 26.5°N. We find that water parcels recirculating within the STG account for 37% (0.36 PW) of the total heat transport across 26.5°N, more than twice that of the classical horizontal gyre component (15%). Our findings indicate that STG heat transport cannot be meaningfully distinguished from that of the basin‐scale overturning since water parcels cooled within the gyre subsequently feed the northward, subsurface limb of the AMOC.

Tooth, Oliver J.↗

Impact of Cloud-Base Turbulence on CCN Activation: Single-Size CCN

Abstract This paper examines the impact of cloud-base turbulence on activation of cloud condensation nuclei (CCN). Following our previous studies, we contrast activation within a nonturbulent adiabatic parcel and an adiabatic parcel filled with turbulence. The latter is simulated by applying a forced implicit large-eddy simulation within a triply periodic computational domain of 64 3 m 3 . We consider two monodisperse CCN. Small CCN have a dry radius of 0.01 μ m and a corresponding activation (critical) radius and critical supersaturation of 0.6 μ m and 1.3%, respectively. Large CCN have a dry radius of 0.2 μ m and feature activation radius of 5.4 μ m and critical supersaturation 0.15%. CCN are assumed in 200-cm −3 concentration in all cases. Mean cloud-base updraft velocities of 0.33, 1, and 3 m s −1 are considered. In the nonturbulent parcel, all CCN are activated and lead to a monodisperse droplet size distribution above the cloud base, with practically the same droplet size in all simulations. In contrast, turbulence can lead to activation of only a fraction of all CCN with a nonzero spectral width above the cloud base, of the order of 1 μ m, especially in the case of small CCN and weak mean cloud-base ascent. We compare our results to studies of the turbulent single-size CCN activation in the Pi chamber. Sensitivity simulations that apply a smaller turbulence intensity, smaller computational domain, and modified initial conditions document the impact of specific modeling assumptions. The simulations call for a more realistic high-resolution modeling of turbulent cloud-base activation.

54 ENVIRONMENTAL SCIENCES↗

Updraft Width Implications for Cumulonimbus Growth in a Moist Marine Environment

Abstract An idealized large-eddy simulation of a tropical marine cloud population was performed. At any time, it contained hundreds of clouds, and updraft width in shallow convection emerging from a subcloud layer appeared to be an important indicator of whether specific convective elements deepened. In an environment with 80%–90% relative humidity below the 0°C level, updrafts that penetrated the 0°C level were larger at and above cloud base, which occurred at the lifting condensation level near 600 m. Parcels rising in these updrafts appeared to emerge from boundary layer eddies that averaged ∼200 m wider than those in clouds that only reached 1.5–3 km height. The deeply ascending parcels (growers) possessed statistically similar values of effective buoyancy below the level of free convection (LFC) as parcels that began to ascend in a cloud but stopped before reaching 3000 m (nongrowers). The growers also experienced less dilution above the LFC. Nongrowers were characterized by negative effective buoyancy and rapid deceleration above the LFC, while growers continued to accelerate well above the LFC. Growers occurred in areas with a greater magnitude of background convergence (or weaker divergence) in the subcloud layer, especially between 300 m and cloud base, but whether the convergence actually led to eddy widening is unclear. Significance Statement Cumulonimbus clouds are responsible for many extreme weather phenomena and are important contributors to Earth’s energy balance. However, the processes leading to the growth of individual clouds are not completely understood nor well-represented in weather prediction models. We find that the clouds containing updrafts that start out wider at early stages of their life cycles grow taller, possibly because they are protected more from drier air outside the cloud than narrow clouds. In addition, this work shows how the initial width of clouds might be related to convergence in the lowest part of the atmosphere, at heights where clouds initially develop. However, meteorologists must be careful not to overinterpret these results because numerical simulations inherently include assumptions that may not reflect reality. This reinforces the need to also observe processes occurring at the scales of individual clouds.

54 ENVIRONMENTAL SCIENCES↗

An Improved Convection Parameterization with Detailed Aerosol–Cloud Microphysics for a Global Model

Abstract A new microphysical treatment that includes aerosol–cloud interactions and secondary ice production (SIP) mechanisms is implemented in the convection scheme of the Community Atmosphere Model, version 6 (CAM6). The approach is to embed a 1D Lagrangian parcel model in the bulk convective plume of the existing deep convection parameterization. Aerosol activation, growth processes including collision/coalescence, and three processes of SIP mechanisms, two of which are normally overlooked in atmospheric models, are represented in this embedded parcel model. These microphysical processes are treated with a hybrid bin/bulk scheme and a high spatial and temporal resolution for the integration of the embedded parcel in 1D, allowing vertical velocity to determine the microphysical evolution following the in-cloud motion during ascent. Simulations of an observed case (Midlatitude Continental Convective Clouds Experiment) of a mesoscale convective system in Oklahoma, United States, with a single-column model (SCAM) version of CAM, are compared with aircraft in situ and ground-based observations of microphysical properties from the convection and precipitation. Results from the validation show the new microphysical scheme has a good representation of the ice initiation in the bulk convective plume, including the known and empirically quantified pathways of primary and secondary initiation, with benefits for the accuracy of properties of its supercooled cloud liquid. The sensitivity simulations and use of tagging tracers for the validated simulation confirm that the newly included SIP mechanisms are of paramount importance for convective microphysics and can be successfully treated in the global model.

54 ENVIRONMENTAL SCIENCES↗

The Moist Available Energy of a Conditionally Unstable Atmosphere

Two simple methods for computing the moist available energy for cases in which the total number of parcels is fairly small are discussed. The first is a swapping routine that finds the reference state by exchanging parcels whenever the swap reduces the total enthalpy. However, it can be proved by contrived example that the swapping algorithm does not always find the true reference state. A second brute force routine actually examines all possible arrangements of the parcels and chooses the one with the smallest moist enthalpy. At present, both routines allow only horizontally homogeneous reference states. In an exploratory study, the swapping routine was used to find MAE and reference state for a time sequence of GATE soundings, all of which are conditionally unstable. In spot checks, the brute force routine always agreed with the swapper. Results show that in passing from the given state of the reference state the lowest three hundred mb of the atmosphere typically exchanges places with the 300 mb above it. The reference state then contains a dry warm layer near the surface, but a supersaturated but cool layer in the middle troposphere. The upper portion of the sounding is not modified in passing from the given state to the reference state.

Randall, D.↗

Lagrangian mean circulations in the stratosphere

The mean Lagrangian motion in the winter stratosphere is computed on the basis of three-dimensional winds derived from the 1978/1979 winter LIMS satellite observations, initializing material tubes of air parcels every 4 days and following them for periods of 10 days each. When the wave amplitudes are large, the tubes break and the parcels disperse; during the major sudden warming, every material tube in the stratosphere was broken, leading to extensive mixing between low and high amplitude parcels. The Lagrangian mean vertical motion tended to be smaller than the motion in the transformed Eulerian coordinate system.

Lyjak, Lawrence V.↗

Polar cap diurnal temperature variations - Observations and modeling

High-spectral-resolution measurements of the O(1D) emission line, performed with the Fabry-Perot interferometer (Thule, Greenland), were used to observe the diurnal variation of the thermospheric temperature in the geomagnetic polarcap at solar minimum (January 1987). By tracing the trajectory of a parcel backward in time and space from the Thule location, it is shown that the observed diurnal temperature variation is due to the degree of solar heat input that a parcel experiences en route to the polar cap, and the route a parcel takes through the polar cusp. It is also shown that the hydrodynamic variations in the winter high-latitude regions from solar maximum to solar minimum are insufficient to mask the thermodynamical effects associated with the offset of the geographic and geomagnetic poles.

Mccormac, F. G.↗

Chemical consequences of the initial diffusional growth of cloud droplets - A clean marine case

A simple microphysical cloud parcel model and a simple representation of the background marine aerosol are used to predict the concentrations and compositions of droplets of various sizes near cloud base. The aerosol consists of an externally-mixed ammonium bisulfate accumulation mode and a sea-salt coarse particle mode. The difference in diffusional growth rates between the small and large droplets as well as the differences in composition between the two aerosol modes result in substantial differences in solute concentration and composition with size of droplets in the parcel. The chemistry of individual droplets is not, in general, representative of the bulk (volume-weighted mean) cloud water sample. These differences, calculated to occur early in the parcel's lifetime, should have important consequences for chemical reactions such as aqueous phase sulfate production.

Twohy, C. H.↗

Lagrangian photochemical modeling studies of the 1987 Antarctic spring vortex. II - Seasonal trends in ozone

A photochemical model consisting of 40 species and 107 reactions is integrated along 80-day air parcel trajectories calculated in the lower stratosphere for the springtime Antarctic. For the trajectory starting at 58 deg S, which may be regarded as outside the circumpolar vortex, only a small change in O3 occurs in the model. In contrast, for the air parcel starting in the vortex at 74 deg S, the O3 concentration is reduced by 93 percent during the 80 days from the beginning of August to late October. The model results for several species are compared with measurements from the Airborne Antarctic Ozone Experiment and, in general, good agreement is obtained. In the model, the dentrification of the air parcels in polar stratospheric clouds increases the amount of chlorine present in active form. Heterogeneous reactions maintain high active chlorine which destroys O3 via the formation of the ClO dimer. Results of calculations with reduced concentrations of inorganic chlorine show considerably reduced O3 destruction rates and compare favorably with the behavior of total O3 since the late 1970s. The remaining major uncertainties in the photochemical aspects of the Antarctic ozone hole are highlighted.

Austin, J.↗

Saturation point representation of cloud-top entrainment instability

Cloud-top entrainment instability was investigated using a mixing line analysis. Mixing time scales are closely related to the actual size of the parcel, so that local instabilities are largely dependent on the scales of mixing near the cloud top. Given a fixed transport velocity, variation over a small range of parcel length scales (parcel mixing velocities) turns an energy-producing mixing process into an energy-consuming mixing process. It is suggested that a single criterion for cloud-top entrainment instability will not be found due to the role of at least three factors operating more or less independently; the stability of the mixing line, the entrainment speed, and the strength of the internal boundary-layer circulation.

Boers, Reinout↗

Springtime stratospheric water vapour in the Southern Hemisphere as measured by MLS

The effects of the break-up of the Antarctic vortex on the water vapor distribution are studied using MLS measurements of water vapor made during September 1991 and November 1991. In early November at 22 hPa a moist area is found within the polar vortex, consistent with an observed descent of order 10 km and strong radiative cooling. As the vortex erodes (beginning of November 1991), parcels of moist air become detached from the edge of the vortex and mix rapidly (within 2-3 days) with drier mid-latitude air. When the vortex breaks up (mid-November), larger parcels of moist air from both the edge and the inner vortex migrate to mid-latitudes. These parcels have a longer lifetime than those produced by vortex erosion, probably because they are correlated with higher potential vorticity gradients. The break-up of the vortex is accompanied by a mean adiabatic equatorward transport resulting in a significant increase in midstratospheric water vapor values at mid-latitudes in late spring.

Harwood, R. S.↗