J. V. Pittman

In‐situ observations of mid‐latitude forest fire plumes deep in the stratosphere

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 extratropical 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.

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.

The Stratosphere–Troposphere Analyses of Regional Transport 2008 Experiment

The Stratosphere–Troposphere Analyses of Regional Transport 2008 (START08) experiment investigated a number of important processes in the extratropical upper troposphere and lower stratosphere (UTLS) using the National Science Foundation (NSF)–NCAR Gulfstream V (GV) research aircraft. The main objective was to examine the chemical structure of the extratropical UTLS in relation to dynamical processes spanning a range of scales. The campaign was conducted during April–June 2008 from Broomfield, Colorado. A total of 18 research flights sampled an extensive geographical region of North America (25°–65°N, 80°–120°W) and a wide range of meteorological conditions. The airborne in situ instruments measured a comprehensive suite of chemical constituents and microphysical variables from the boundary layer to the lower stratosphere, with flights specifically designed to target key transport processes in the extratropical UTLS. The flights successfully investigated stratosphere–troposphere exchange (STE) processes, ...

New particle formation observed in the tropical//subtropical cirrus clouds

[1] Previous studies show that new particle formation takes place in the outflows of marine stratus and cumulus clouds. Here we show measurements of high concentrations of ultrafine particles, diameters (Dp) from 4 to 9 nm (N4–9), in interstitial cloud aerosol. These ultrafine particles indicate that in situ new particle formation occurs interstitially in cirrus clouds. Measurements were made at altitudes from 7 to 16 km over Florida with instruments on the WB-57F aircraft during Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiments (CRYSTAL-FACE) in July 2002. Sizeresolved ice crystal particle concentrations and water vapor concentrations were measured to help identify the presence of cirrus clouds. About 72% of the in-cloud samples showed new particle formation events with the average N4–9 of 3.0 10 3 cm 3 , whereas about 56% of the out-of-cloud samples had events with the lower N4–9of 1.3 10 3 cm 3 . The periods during which high N4–9 appeared were often associated with times of increasing ice water content (IWC) and high relative humidity with respect to ice (RHI); however, the measured N4–9was not quantitatively correlated to IWC. The magnitude and frequency of new particle formation events seen in cirrus clouds were also higher than those previously observed in the tropical/subtropical upper troposphere in the absence of clouds. These results suggest that cirrus clouds may provide favorable conditions for particle formation, such as low temperatures, high RHI, high OH production (due to high water vapor), cloud electricity, and atmospheric convection. At present, however, particle formation mechanisms in clouds are unidentified. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0320 Atmospheric Composition and Structure: Cloud physics and chemistry; 0335 Atmospheric Composition and Structure: Ion chemistry of the atmosphere (2419, 2427); 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; 0368 Atmospheric Composition and Structure: Troposphere—constituent transport and chemistry;

The NASA Airborne Tropical Tropopause Experiment: High-altitude aircraft measurements in the Tropical Western Pacific

AbstractThe February–March 2014 deployment of the National Aeronautics and Space Administration (NASA) Airborne Tropical Tropopause Experiment (ATTREX) provided unique in situ measurements in the western Pacific tropical tropopause layer (TTL). Six flights were conducted from Guam with the long-range, high-altitude, unmanned Global Hawk aircraft. The ATTREX Global Hawk payload provided measurements of water vapor, meteorological conditions, cloud properties, tracer and chemical radical concentrations, and radiative fluxes. The campaign was partially coincident with the Convective Transport of Active Species in the Tropics (CONTRAST) and the Coordinated Airborne Studies in the Tropics (CAST) airborne campaigns based in Guam using lower-altitude aircraft (see companion articles in this issue). The ATTREX dataset is being used for investigations of TTL cloud, transport, dynamical, and chemical processes, as well as for evaluation and improvement of global-model representations of TTL processes. The ATTREX da...

Validation of the Harvard Lyman-α in situ water vapor instrument: Implications for the mechanisms that control stratospheric water vapor

Building on previously published details of the laboratory calibrations of the Harvard Lyman-α photofragment fluorescence hygrometer (HWV) on the NASA ER-2 and WB-57 aircraft, we describe here the validation process for HWV, which includes laboratory calibrations and intercomparisons with other Harvard water vapor instruments at water vapor mixing ratios from 0 to 10 ppmv, followed by in-flight intercomparisons with the same Harvard hygrometers. The observed agreement exhibited in the laboratory and during intercomparisons helps corroborate the accuracy of HWV. In light of the validated accuracy of HWV, we present and evaluate a series of intercomparisons with satellite and balloon borne water vapor instruments made from the upper troposphere to the lower stratosphere in the tropics and midlatitudes. Whether on the NASA ER-2 or WB-57 aircraft, HWV has consistently measured about 1–1.5 ppmv higher than the balloon-borne NOAA/ESRL/GMD frost point hygrometer (CMDL), the NOAA Cryogenic Frost point Hygrometer (CFH), and the Microwave Limb Sounder (MLS) on the Aura satellite in regions of the atmosphere where water vapor is <10 ppmv. Comparisons in the tropics with the Halogen Occultation Experiment (HALOE) on the Upper Atmosphere Research Satellite show large variable differences near the tropopause that converge to ~10% above 460 K, with HWV higher. Results we show from the Aqua Validation and Intercomparison Experiment (AquaVIT) at the AIDA chamber in Karlsruhe do not reflect the observed in-flight differences. We illustrate that the interpretation of the results of comparisons between modeled and measured representations of the seasonal cycle of water entering the lower tropical stratosphere is dictated by which data set is used.

Measurements of the Total Water Content of Cirrus Clouds. Part I: Instrument Details and Calibration

Abstract This paper describes an instrument designed to measure the sum of gas phase and solid phase water, or total water, in cirrus clouds, and to be mounted in a pallet in the underbelly of the NASA WB-57 research aircraft. The ice water content of cirrus is determined by subtracting water vapor measured simultaneously by the Harvard water vapor instrument on the aircraft. The total water instrument uses an isokinetic inlet to maintain ambient particle concentrations as air enters the instrument duct, a 600-W heater mounted directly in the flow to evaporate the ice particles, and a Lyman-α photofragment fluorescence technique for detection of the total water content of the ambient air. Isokinetic flow is achieved with an actively controlled roots pump by referencing aircraft pressure, temperature, and true airspeed, together with instrument flow velocity, temperature, and pressure. Laboratory calibrations that utilize a water vapor addition system that adds air with a specific humidity tied to the vapo...

Measurements of the Total Water Content of Cirrus Clouds. Part II: Instrument Performance and Validation

Abstract This paper describes the performance and in-flight validation of an instrument mounted in a pallet on the NASA WB-57 research aircraft that measures the sum of gas phase and solid phase water, or total water, in cirrus clouds. Using a heated isokinetic inlet and a Lyman-α photofragment fluorescence technique for detection, measurements of total water have been made over three orders of magnitude. During the Cirrus Regional Study of Tropical Anvils and Cirrus Layers Florida Area Cirrus Experiment (CRYSTAL FACE), the instrument operated at duct temperatures sufficiently warms to completely evaporate particles up to 150-μm diameter. Laboratory calibrations, in-flight diagnostics, intercomparison with water vapor measured by absorption in flight, and intercomparisons in clear air with the Harvard water vapor instrument validate the detection sensitivity of the instrument and illustrate the minimal hysteresis from instrument surface contamination. The Harvard total water and water vapor instruments to...

Ozone Profile Retrieval from an Advanced Infrared Sounder: Experiments with Tropopause-Based Climatology and Optimal Estimation Approach

Abstract Motivated by a significant potential for retrieving atmospheric ozone profile information from advanced satellite infrared sounders, this study investigates various methods to optimize ozone retrievals. A set of retrieval experiments has been performed to assess the impact of different background states (or the a priori states) and retrieval algorithms on the retrieved ozone profiles in the upper troposphere and lower stratosphere (UTLS) using Atmospheric Infrared Sounder (AIRS) measurements. A new tropopause-based ozone climatology, using publicly available global ozonesonde data to construct the a priori state, is described. Comparisons are made with the AIRS version 5 (v5) ozone climatology. The authors also present the result of a newly implemented optimal estimation (OE) algorithm and compare it to the current AIRS science team (AST) algorithm used in version 5. The ozone climatology using tropopause-referenced coordinates better preserves the shape and the magnitude of the ozone gradient ac...

A new Differential Optical Absorption Spectroscopy instrument to study atmospheric chemistry from a high- altitude unmanned aircraft

Observations of atmospheric trace gases in the tropical upper troposphere (UT), tropical tropopause layer (TTL), and lower stratosphere (LS) require dedicated measurement platforms and instrumentation. Here we present a new limb-scanning Differential Optical Absorption Spectroscopy (DOAS) instrument developed for NASA’s Global Hawk (GH) unmanned aerial system and deployed during the Airborne Tropical TRopopause EXperiment (ATTREX). The mini-DOAS system is designed for automatic operation under unpressurized and unheated conditions at 14–18 km altitude, collecting scattered sunlight in three wavelength windows: UV (301–387 nm), visible (410–525 nm), and near infrared (900–1700 nm). A telescope scanning unit allows selection of a viewing angle around the limb, as well as realtime correction of the aircraft pitch. Due to the high altitude, solar reference spectra are measured using diffusors and direct sunlight. The DOAS approach allows retrieval of slant column densities (SCDs) of O3, O4, NO2, and BrO with relative errors similar to other aircraft DOAS systems. Radiative transfer considerations show that the retrieval of trace gas mixing ratios from the observed SCD based on O4 observations, the most common approach for DOAS measurements, is inadequate for high-altitude observations. This is due to the frequent presence of low-altitude clouds, which shift the sensitivity of the O4 SCD into the lower atmosphere and make it highly dependent on cloud coverage. A newly developed technique that constrains the radiative transfer by comparing in situ and DOAS O3 observations overcomes this issue. Extensive sensitivity calculations show that the novel O3-scaling technique allows the retrieval of BrO and NO2 mixing ratios at high accuracies of 0.5 and 15 ppt, respectively. The BrO and NO2 mixing ratios and vertical profiles observed during ATTREX thus provide new insights into ozone and halogen chemistry in the UT, TTL, and LS.