T. P. Bui

Gravity waves generated by a tropical cyclone during the STEP tropical field program: A case study

Overflights of a tropical cyclone during the Australian winter monsoon field experiment of the Stratosphere-Troposphere Exchange Project (STEP) show the presence of two mesoscale phenomena: a vertically propagating gravity wave with a horizontal wavelength of about 110 km and a feature with a horizontal scale comparable to that of the cyclones entire cloud shield (wavelength of 250 km or greater). The larger feature is fairly steady, though its physical interpretation is ambiguous. The 110-km gravity wave is transient, having maximum amplitude early in the flight and decreasing in amplitude thereafter. Its scale is comparable to that of 100-to 150-km-diameter cells of low satellite brightness temperatures within the overall cyclone cloud shield; these cells have lifetimes of 4.5 to 6 hours. Aircraft flights through the anvil show that these cells correspond to regions of enhanced convection, higher cloud altitude, and upwardly displaced potential temperature surfaces. A three-dimensional transient linear gravity wave simulation shows that the temporal and spatial distribution of meteorological variables associated with the 110-km gravity wave can be simulated by a slowly moving transient forcing at the anvil top having an amplitude of 400–600 m, a lifetime of 4.5–6 hours and a size comparable to the cells of low brightness temperature. The forcing amplitudes indicate that the zonal drag due to breaking mesoscale transient convective gravity waves is definitely important to the westerly phase of the stratopause semiannual oscillation and possibly important to the easterly phase of the quasi-biennial oscillation. There is strong evidence that some of the mesoscale gravity waves break below 20 km as well. The effect of this wave breaking on the diabatic circulation below 20 km may be comparable to that of above-cloud diabatic cooling.

Comparison of MkIV balloon and ER‐2 aircraft measurements of atmospheric trace gases

On May 8, 1997, vertical profiles of over 30 different gases were measured remotely in solar occultation by the Jet Propulsion Laboratory MkIV Interferometer during a balloon flight launched from Fairbanks, Alaska. These gases included H 2 O, N 2 O, CH 4 , CO, NO x , NO y , HCI, ClNO 3 , CCl 2 F 2 , CCl 3 F, CCl 4 , CHClF 2 , CClF 2 CCl 2 F, SF 6 , CH 3 Cl, and C 2 H 6 , all of which were also measured in situ by instruments on board the NASA ER-2 aircraft, which was making flights from Fairbanks during this same early May time period as part of the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) experiment. A comparison of the gas volume mixing ratios in the upper troposphere and lower stratosphere reveals agreement better than 5% for most gases. The three significant exceptions to this are SF 6 and CCl 4 for which the remote measurements exceed the in situ observations by 15-20% at all altitudes, and H 2 O for which the remote measurements are up to 30% smaller than the in situ observations near the hygropause.

Prevalence of ice-supersaturated regions in the upper troposphere: Implications for optically thin ice cloud formation

In situ measurements of water vapor and temperature from recent aircraft campaigns have provided evidence that the upper troposphere is frequently supersaturated with respect to ice. The peak relative humidities with respect to ice (RHI) occasionally approached water saturation at temperatures ranging from −40°C to −70°C in each of the campaigns. The occurrence frequency of ice supersaturation ranged from about 20% to 45%. Even on flight segments when no ice crystals were detected, ice supersaturation was measured about 5–20% of the time. A numerical cloud model is used to simulate the formation of optically thin, low ice number density cirrus clouds in these supersaturated regions. The potential for scavenging of ice nuclei (IN) by these clouds is evaluated. The simulations suggest that if less than about 5 × 10-3 to 2 × 10-2 cm-3 ice nuclei are present when these supersaturations are generated, then the cirrus formed should be subvisible. These low ice number density clouds scavenge the IN from the supersaturated layer, but the crystals sediment out too rapidly to prevent buildup of high supersaturations. If higher numbers of ice nuclei are present, then the clouds that form are visible and deposition growth of the ice crystals reduces the RHI down to near 100%. Even if no ice clouds form, increasing the RHI from 100% to 150% between 10 and 10.5 km results in a decrease in outgoing longwave radiative flux at the top of the atmosphere of about 8 W m-2. If 0.02–0.1 cm-3 IN are present, the resulting cloud radiative forcing reduces the net radiative flux several watts per square meter further. Given the high frequency of supersaturated regions without optically thick clouds in the upper troposphere, there is a potential for a climatically important class of optically thin cirrus with relatively low ice crystal number densities. The optical properties of these clouds will depend very strongly on the abundance of ice nuclei in the upper troposphere.

Severe and extensive denitrification in the 1999–2000 Arctic winter stratosphere

Observations in the 1999-2000 Arctic winter stratosphere show the most severe and extensive denitrification ever observed in the northern hemisphere. Denitrification was inferred from in situ measurements conducted during high-altitude aircraft flights between January and March 2000. Average removal of more than 60% of the reactive nitrogen reservoir (NO y ) was observed in air masses throughout the core of the Arctic vortex. Denitrification was observed at altitudes between 16 and 21 km, with the most severe denitrification observed at 20 to 21 km. Nitrified air masses were also observed, primarily at lower altitudes. These results show that denitrification in the Arctic lower stratosphere can approach the severity and extent of that previously observed only in the Antarctic.

Empirical age spectra for the lower tropical stratosphere from in situ observations of CO2: Implications for stratospheric transport

Empirical age spectra for the lower tropical stratosphere (from the tropopause to ∼19.5 km) have been derived from in situ measurements of CO 2 , using information provided by the vertical propagation of the tropospheric seasonal cycle and long-term positive trend. Our method provides accurate and unambiguous mean ages for this region which are difficult to obtain by simple analysis of lag times from tracer measurements. We find that the air is 30-40% younger in northern spring than in autumn. For example, at 460 K the mean age (relative to the tropical tropopause) was 0.4 years in March and 0.6 years in September. The phase lag times and attenuation of CO 2 seasonal extrema in the stratosphere are shown to depend on seasonal variations in transport rates and on the presence of harmonics in the CO 2 boundary condition with frequencies higher than 2π/yr. Profiles of stratospheric water vapor, generated from the derived age spectra with a stratospheric boundary condition based on observed tropical tropopause temperatures, are consistent with in situ observations of H 2 O. Comparison of the predicted water vapor seasonal cycle with satellite observations suggests that satellite-borne instruments underestimate the amplitude near the tropical tropopause. We relate the empirical age spectra to the analytic solution for the 1-D advection-diffusion tracer continuity equation to obtain seasonally resolved estimates of the ascent rate and the vertical diffusion coefficient. The derived age spectra provide a unique observation-based diagnostic for evaluating the simulation of tracer transport in models.

Troposphere‐to‐stratosphere transport in the lowermost stratosphere from measurements of H2O, CO2, N2O and O3

The origin of air in the lowermost stratosphere is investigated with measurements from the NASA ER-2 aircraft. Air with high water vapor mixing ratios was observed in the stratosphere at θ∼330–380 K near 40 N in May 1995, indicating the influence of intrusions of tropospheric air. Assuming that observed tracer-tracer relationships reflect mixing lines between tropospheric and stratospheric air masses, we calculate mixing ratios of H2O (12–24 ppmv) and CO2 for the admixed tropospheric air at θ=352–364 K. Temperatures on the 355 K surface at 20–40 N were low enough to dehydrate air to these values. While most ER-2 CO2 data in both hemispheres are consistent with tropical or subtropical air entering the lowermost stratosphere, measurements from May 1995 for θ<362 K suggest that entry of air from the midlatitude upper troposphere can occur in conjunction with mixing processes near the tropopause.

Nitric Acid Uptake on Subtropical Cirrus Cloud Particles

The redistribution of HNO 3 via uptake and sedimentation by cirrus cloud particles is considered an important term in the upper tropospheric budget of reactive nitrogen. Numerous cirrus cloud encounters by the NASA WB-57F high-altitude research aircraft during the Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) were accompanied by the observation of condensed-phase HNO 3 with the NOAA chemical ionization mass spectrometer. The instrument measures HNO 3 with two independent channels of detection connected to separate forward and downward facing inlets that allow a determination of the amount of HNO 3 condensed on ice particles. Subtropical cirrus clouds, as indicated by the presence of ice particles, were observed coincident with condensed-phase HNO 3 at temperatures of 197-224 K and pressures of 122-224 hPa. Maximum levels of condensed-phase HNO 3 approached the gas-phase equivalent of 0.8 ppbv. Ice particle surface coverages as high as 1.4 x 10 14 molecules cm -2 were observed. A dissociative Langmuir adsorption model, when using an empirically derived HNO 3 adsorption enthalpy of -11.0 kcal mol -1 , electively describes the observed molecular coverages to within a factor of 5. The percentage of total HNO 3 in the condensed phase ranged from near zero to 100% in the observed cirrus clouds. With volume-weighted mean particle diameters up to 700 μm and particle fall velocities up to 10 m s -1 , some observed clouds have significant potential to redistribute HNO 3 in the upper troposphere.

A comparison of observations and model simulations of NOx/NOy in the lower stratosphere

Extensive airborne measurements of the reactive nitrogen reservoir (NO_(y)) and its component nitric oxide (NO) have been made in the lower stratosphere. Box model simulations that are constrained by observations of radical and long-lived species and which include heterogeneous chemistry systematically underpredict the NO_x (= NO + NO_2) to NO_y ratio. The model agreement is substantially improved if newly measured rate coefficients for the OH + NO_2 and OH + HNO_3 reactions are used. When included in 2-D models, the new rate coefficients significantly increase the calculated ozone loss due to NO_x and modestly change the calculated ozone abundances in the lower stratosphere. Ozone changes associated with the emissions of a fleet of supersonic aircraft are also altered.

Subsidence, mixing, and denitrification of Arctic polar vortex air measured during POLARIS

We determine the degree of denitrification that occurred during the 1996-1997 Arctic winter using a technique that is based on balloon and aircraft borne measurements of NO y , N 2 O, and CH 4 . The NO 3 /N 2 O relation can undergo significant change due to isentropic mixing of subsided vortex air masses with extravortex air due to the high nonlinearity of the relation. These transport related reductions in NO y can be difficult to distinguish from the effects of denitrification caused by sedimentation of condensed HNO 3 . In this study, high-altitude balloon measurements are used to define the properties of air masses that later descend in the polar vortex to altitudes sampled by the ER-2 aircraft (i.e., ∼20 km) and mix isentropically with extravortex air. Observed correlations of CH 4 and N 2 O are used to quantify the degree of subsidence and mixing for individual air masses. On the basis of these results the expected mixing ratio of NO y resulting from subsidence and mixing, defined here as NO y ** , is calculated and compared with the measured mixing ratio of NO y . Values of NO y and NO y ** agree well during most parts of the flights. A slight deficit of NO y versus NO y ** is found only for a limited region during the ER-2 flight on April 26, 1997. This deficit is interpreted as indication for weak denitrification (∼2-3 ppbv) in that air mass. The small degree of denitrification is consistent with the general synoptic-scale temperature history of the sampled air masses, which did not encounter temperatures below the frostpoint and had relatively brief encounters with temperatures below the nitric acid trihydrate equilibrium temperature. Much larger degrees of denitrification would have been inferred if mixing effects had been ignored, which is the traditional approach to diagnose denitrification. Our analysis emphasizes the importance of using other correlations of conserved species to be able to accurately interpret changes in the NO y /N 2 O relation with respect to denitrification.

An examination of chemistry and transport processes in the tropical lower stratosphere using observations of long‐lived and short‐lived compounds obtained during STRAT and POLARIS

A suite of compounds with a wide range of photochemical lifetimes (3 months to several decades) was measured in the tropical and midlatitude upper troposphere and lower stratosphere during the Stratospheric Tracers of Atmospheric Transport (STRAT) experiment (fall 1995 and winter, summer, and fall 1996) and the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) deployment in late summer 1997. These species include various chlorofluorocarbons, hydrocarbons, halocarbons, and halons measured in whole air samples and CO measured in situ by tunable diode laser spectroscopy. Mixing ratio profiles of long-lived species in the tropical lower stratosphere are examined using a one-dimensional (1-D) photochemical model that includes entrainment from the extratropical stratosphere and is constrained by measured concentrations of OH. Profiles of tracers found using the 1-D model agree well with all the observed tropical profiles for an entrainment time scale of 8.5 -4 +6 months, independent of altitude between potential temperatures of 370 and 500 K. The tropical profile of CO is used to show that the annually averaged ascent rate profile, on the basis of a set of radiative heating calculations, is accurate to approximately ±44%, a smaller uncertainty than found by considering the uncertainties in the radiative model and its inputs. Tropical profiles of ethane and C 2 Cl 4 reveal that the concentration of Cl is higher than expected on the basis of photochemical model simulations using standard gas phase kinetics and established relationships between total inorganic chlorine and CFC-11. Our observations suggest that short-lived organic chlorinated compounds and HCI carried across the tropical tropopause may provide an important source of inorganic chlorine to the tropical lower stratosphere that has been largely unappreciated in previous studies. The entrainment timescale found here is considerably less than the value found by a similar study that focused on observations obtained in the lower stratosphere during 1994. Several possible explanations for this difference are discussed.