Hope A. Michelsen

Stratospheric water vapor increases over the past half‐century

Ten data sets covering the period 1954–2000 are analyzed to show a 1%/yr increase in stratospheric water vapor. The trend has persisted for at least 45 years, hence is unlikely the result of a single event, but rather indicative of long-term climate change. A long-term change in the transport of water vapor into the stratosphere is the most probable cause.

Correlations of stratospheric abundances of NO y , O3, N2O, and CH4 derived from ATMOS measurements

Correlations are presented for [NO y ] relative to [N 2 O] and [O 3 ] derived from measurements from the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument from a wide range of altitudes and latitudes, including the tropics for which previous analyses have not extended above ∼20 km. Relationships for [O 3 ] versus [N 2 O] are also given. The results are shown to be in good agreement with aircraft- and balloon-based observations. Distinct correlations are observed for the tropics, the springtime polar vortex, and the extratropics-extravortex regions. These correlations demonstrate rapid production of NO y and O 3 in the tropical middle stratosphere and episodic export of air from this region to higher latitudes. Isolation of air within the developing polar vortices in the fall is also shown. Arctic vortex data from April 1993 appear to indicate denitrification of 25-30%, which is evident as a 3.0-4.5 ppb deficit in [NO,] when the vortex [NO y ]:[N 2 O] correlation is compared with the extravortex correlation. A mixture of air descended from above 40 km with air from lower altitudes can fully account for this deficit in [NO y ], in addition to approximately half of an apparent Arctic ozone loss of 50-60%, as inferred by comparison of the vortex and extravortex [O 3 ]:[N 2 O] correlations. Comparison of Antarctic vortex and extravortex correlations from November 1994 similarly show a 60-80% deficit in [NO y ] and 80-100% deficit in [O 3 ]; at least half of this apparent denitrification and ozone loss can be attributed to mixing of air descended from higher altitudes with air from lower altitudes.

Atmospheric Trace Molecule Spectroscopy (ATMOS) Experiment Version 3 data retrievals

Version 3 of the Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment data set for some 30 trace and minor gas profiles is available. From the IR solar-absorption spectra measured during four Space Shuttle missions (in 1985, 1992, 1993, and 1994), profiles from more than 350 occultations were retrieved from the upper troposphere to the lower mesosphere. Previous results were unreliable for tropospheric retrievals, but with a new global-fitting algorithm profiles are reliably returned down to altitudes as low as 6.5 km (clouds permitting) and include notably improved retrievals of H2O, CO, and other species. Results for stratospheric water are more consistent across the ATMOS spectral filters and do not indicate a net consumption of H2 in the upper stratosphere. A new sulfuric-acid aerosol product is described. An overview of ATMOS Version 3 processing is presented with a discussion of estimated uncertainties. Differences between these Version 3 and previously reported Version 2 ATMOS results are discussed. Retrievals are available at http://atmos.jpl.nasa.gov/atmos.

Polar vortex dynamics during spring and fall diagnosed using trace gas observations from the Atmospheric Trace Molecule Spectroscopy instrument

Trace gases measured by the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument during three Atmospheric Laboratory for Applications and Science (ATLAS) space-shuttle missions, in March/April 1992 (AT-1), April 1993 (AT-2), and November 1994 (AT-3) have been mapped into equivalent latitude/potential temperature (EqL/θ) coordinates. The asymmetry of the spring vortices results in coverage of subtropical to polar EqLs. EqL/θ fields of long-lived tracers in spring in both hemispheres show the net effects of descent at high EqL throughout the winter, reflecting strong descent in the upper stratosphere, decreasing descent at lower altitudes, and evidence of greater descent at the edge of the lower stratospheric vortex than in the vortex center; these results are consistent with trajectory calculations examining the history of the air measured by ATMOS in the month prior to each mission. EqL/θ tracer fields, the derived fields CH 4 -CH * 4 (CH * 4 is the expected CH 4 calculated from a prescribed relationship with N 2 O for fall) and NO y -NO * y (analogous to CH * 4 ), and parcel histories all indicate regions of strong mixing in the 1994 Southern Hemisphere (SH) spring vortex above 500 K, with the strongest mixing confined to the vortex edge region between 500 and 700 K, and mixing throughout the Northern Hemisphere (NH) spring vortex in 1993 below about 850 K. Parcel histories indicate mixing of extravortex air with air near the vortex edge below 500 K in the SH but not with air in the vortex core; they show extravortex air mixing well into the vortex above ∼450 K in the NH and into the vortex edge region below. The effects of severe denitrification are apparent in EqL/θ HNO 3 in the SH lower stratospheric spring vortex. The morphology of HNO 3 in the Arctic spring lower stratospheric vortex is consistent with the effects of descent. EqL/θ fields of ATMOS NO y -NO * y show decreases consistent with the effects of mixing throughout the NH lower stratospheric vortex. The EqL/θ-mapped ATMOS data thus indicate no significant denitrification during the 1992-1993 NH winter. Examination of H 2 O+2CH 4 shows that dehydration in SH spring 1994 extended up to ∼600 K; it also suggests the possibility of a small amount of dehydration in the NH 1993 spring vortex below ∼465 K. Ozone depletion is evident in the spring vortices in both hemispheres. Differences in autumn EqL/θ tracer fields between the missions reflect the fact that each succeeding mission took place ∼2 weeks later in the season, when the vortex had developed further. There was greater average descent and greater isolation of air in the developing vortex during each succeeding mission, consistent with progressively larger downward excursions of long-lived tracer contours observed in the upper stratosphere at high EqL.

Time-resolved laser-induced incandescence of soot: the influence of experimental factors and microphysical mechanisms

We present a data set for testing models of time-resolved laser-induced incandescence of soot. Measurements were made in a laminar ethene diffusion flame over a wide range of laser fluences at 532 nm. The laser was seeded to provide a smooth temporal profile, and the beam was spatially filtered and imaged into the flame to provide a homogeneous spatial profile. The particle incandescence was imaged onto a fast photodiode. The measurements are compared with the standard Melton model [Appl. Opt. 23,2201 (1984)] and with a new model that incorporates physical mechanisms not included in the Melton model.

Time-Resolved Laser-Induced Incandescence and Laser Elastic Scattering Measurements in a Propane Diffusion Flame

Laser-induced incandescence (LII) and laser elastic-scattering measurements have been obtained with subnanosecond time resolution from a propane diffusion flame. Results show that the peak and time-integrated values of the LII signal increase with increasing laser fluence to maxima at the time of the onset of significant vaporization, beyond which they both decrease rapidly with further increases in fluence. This latter behavior for the time-integrated value is known to be characteristic for a laser beam with a rectangular spatial profile and is attributed to soot mass loss from vaporization. However, there is no apparent explanation for the corresponding large decrease in the peak value. Analysis shows that the peak value occurs at the time in the laser pulse when the time-integrated fluence reaches approximately 0.2 J/cm(2) and that the magnitude of the peak value is strongly dependent on the rate of energy deposition. One possible explanation for this behavior is that, at high laser fluences, a cascade ionization phenomenon leads to the formation of an absorptive plasma that strongly perturbs the LII process.

Correlations of stratospheric abundances of CH4 and N2O derived from ATMOS measurements

ATMOS measurements made over a wide range of altitudes and latitudes demonstrate compact correlations between mixing ratios of CH4 and N2O. Tight but distinct correlations are observed for the tropics, the springtime Arctic vortex, and the extra-tropics/extra-vortex regions, indicating dynamical isolation between these regions. Little variability is apparent in correlations between [CH4] and [N2O] from measurements made in different years (1992, 1993, and 1994), seasons (March/April and November), and hemispheres.

Tropical entrainment time scales inferred from stratospheric N2O and CH4 observations

Simultaneous in situ measurements of N_2O and CH_4 were made with a tunable diode laser spectrometer (ALIAS II) aboard the Observations from the Middle Stratosphere (OMS) balloon platform from New Mexico, Alaska, and Brazil during 1996 and 1997. We find different compact relationships of CH_4 with N_2O in the tropics and extra-tropics because mixing is slow between these regions. Transport into the extra-tropics from the tropics or the polar vortex leads to deviations from the normal compact relationship. We use measured N_2O and CH_4 and a simple model to quantify entrainment of mid-latitude stratospheric air into the tropics. The entrainment time scale is estimated to be 16 (+17, −8) months for altitudes between 20 and 28 km. The fraction of tropical air entrained from the extra-tropical stratosphere is 50% (+18%, −30%) at 20 km, increasing to 78% (+11%, −19%) at 28 km.

A laser and molecular beam mass spectrometer study of low-pressure dimethyl ether flames

The oxidation of dimethyl ether (DME) is studied in low-pressure flames using new molecular beam mass spectrometer and laser diagnostics. Two 30.0-Torr, premixed DME/oxygen/argon flames are investigated with stoichiometries of 0.98 and 1.20. The height above burner profiles of nine stable species and two radicals are measured. These results are compared to the detailed chemical reaction mechanism of Curran and coworkers. Generally good agreement is found between the model and data. The largest discrepancies are found for the methyl radical profiles where the model predicts qualitatively different trends in the methyl concentration with stoichiometry than observed in the experiment.

Particle formation from pulsed laser irradiation of soot aggregates studied with a scanning mobility particle sizer, a transmission electron microscope, and a scanning transmission x-ray microscope

We investigated the physical and chemical changes induced in soot aggregates exposed to laser radiation using a scanning mobility particle sizer, a transmission electron microscope, and a scanning transmission x-ray microscope to perform near-edge x-ray absorption fine structure spectroscopy. Laser-induced nanoparticle production was observed at fluences above 0.12 J/cm(2) at 532 nm and 0.22 J/cm(2) at 1064 nm. Our results indicate that new particle formation proceeds via (1) vaporization of small carbon clusters by thermal or photolytic mechanisms, followed by homogeneous nucleation, (2) heterogeneous nucleation of vaporized carbon clusters onto material ablated from primary particles, or (3) both processes.