Atmospheric Sciences Commons^™

Intercomparison And Evaluation Of Satellite Peroxyacetyl Nitrate Observations In The Upper Troposphere-Lower Stratosphere, Richard J. Pope, Nigel A. D. Richards, Martyn P. Chipperfield, David P. Moore, Sarah A. Monks, Stephen R. Arnold, Norbert Glatthor, Michael Kiefer, Tom J. Breider, Jeremy J. Harrison, Peter F. Bernath

Chemistry & Biochemistry Faculty Publications

Peroxyacetyl nitrate (PAN) is an important chemical species in the troposphere as it aids the long-range transport of NO_x and subsequent formation of O₃ in relatively clean remote regions. Over the past few decades observations from aircraft campaigns and surface sites have been used to better understand the regional distribution of PAN. However, recent measurements made by satellites allow for a global assessment of PAN in the upper troposphere-lower stratosphere (UTLS). In this study, we investigate global PAN distributions from two independent retrieval methodologies, based on measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, on …

Global Stratospheric Measurements Of The Isotopologues Of Methane From The Atmospheric Chemistry Experiment Fourier Transform Spectrometer, Eric M. Buzan, Chris A. Beale, Chris. D. Boone, Peter F. Bernath

Chemistry & Biochemistry Faculty Publications

This paper presents an analysis of observations of methane and its two major isotopologues, CH₃D and ¹³CH₄, from the Atmospheric Chemistry Experiment (ACE) satellite between 2004 and 2013. Additionally, atmospheric methane chemistry is modeled using the Whole Atmospheric Community Climate Model (WACCM). ACE retrievals of methane extend from 6 km for all isotopologues to 75 km for ¹²CH₄, 35 km for CH₃D, and 50 km for ¹³CH₄. While total methane concentrations retrieved from ACE agree well with the model, values of δD-CH₄ and δ¹³C-CH …

Detailed Source-Specific Molecular Composition Of Ambient Aerosol Organic Matter Using Ultrahigh Resolution Mass Spectrometry And H Nmr, Amanda S. Willoughby, Andrew S. Wozniak, Patrick G. Hatcher

Chemistry & Biochemistry Faculty Publications

Organic aerosols (OA) are universally regarded as an important component of the atmosphere that have far-ranging impacts on climate forcing and human health. Many of these impacts are related to OA molecular characteristics. Despite the acknowledged importance, current uncertainties related to the source apportionment of molecular properties and environmental impacts make it difficult to confidently predict the net impacts of OA. Here we evaluate the specific molecular compounds as well as bulk structural properties of total suspended particulates in ambient OA collected from key emission sources (marine, biomass burning, and urban) using ultrahigh resolution mass spectrometry (UHR-MS) and proton nuclear …

Upper Tropospheric Water Vapour Variability At High Latitudes- Part 1: Influence Of The Annular Modes, Christopher E. Sioris, Jason Zou, David A. Plummer, Chris D. Boone, C. Thomas Mcelroy, Patrick E. Sheese, Omid Moeini, Peter F. Bernath

Chemistry & Biochemistry Faculty Publications

Seasonal and monthly zonal medians of water vapour in the upper troposphere and lower stratosphere (UTLS) are calculated for both Atmospheric Chemistry Experiment (ACE) instruments for the northern and southern high-latitude regions (60-90° N and 60-90°S). Chosen for the purpose of observing high-latitude processes, the ACE orbit provides sampling of both regions in 8 of 12 months of the year, with coverage in all seasons. The ACE water vapour sensors, namely MAESTRO (Measurements of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation) and the Fourier Transform Spectrometer (ACE-FTS) are currently the only satellite instruments that can probe from …

Mipas Imk/Iaa Cfc-11 (Ccl3f) And Cfc-12 (Ccl2f2) Measurements: Accuracy, Precision And Long-Term Stability, E. Eckert, A. Laeng, S. Lossow, S. Kellmann, G. Stiller, T. Von Clarmann, N. Glatthor, M. Hopfner, M. Kiefer, H. Oelhaf, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

Profiles of CFC-11 (CCl₃F) and CFC-12 (CCl₂F₂) of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) aboard the European satellite Envisat have been retrieved from versions MIPAS/4.61 to MI-PAS/4.62 and MIPAS/5.02 to MIPAS/5.06 level-1b data using the scientific level-2 processor run by Karlsruhe Institute of Technology (KIT), Institute of Meteorology and Climate Research (IMK) and Consejo Superior de Investigaciones Cientificas (CSIC), Instituto de Astrofisica de Andalucia (IAA). These profiles have been compared to measurements taken by the balloon-borne cryosampler, Mark IV (MkIV) and MIPAS-Balloon (MIPAS-B), the airborne MIPAS-STRatospheric aircraft (MIPAS-STR), the satellite-borne Atmospheric Chemistry …

Validation Of The Global Distribution Of Co2 Volume Mixing Ratio In The Mesosphere And Lower Thermosphere From Saber, L. Rezac, Y. Jian, J. Yue, J. M. Russell Iii, A. Kutepov, R. Garcia, K. Walker, P. Bernath

Chemistry & Biochemistry Faculty Publications

The Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) instrument on board the Thermosphere Ionosphere Mesosphere Energetics and Dynamics satellite has been measuring the limb radiance in 10 broadband infrared channels over the altitude range from ~ 400 km to the Earth's surface since 2002. The kinetic temperatures and CO₂ volume mixing ratios (VMRs) in the mesosphere and lower thermosphere have been simultaneously retrieved using SABER limb radiances at 15 and 4.3 μm under nonlocal thermodynamic equilibrium (non-LTE) conditions. This paper presents results of a validation study of the SABER CO₂ VMRs obtained with a two-channel, self-consistent …

Simulation Of Energetic Particle Precipitation Effects During The 2003-2004 Arctic Winter, C. E. Randall, V. L. Harvey, L. A. Holt, D. R. Marsh, D. Kinnison, B. Funke, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

Energetic particle precipitation (EPP) during the 2003-2004 Arctic winter led to the production and subsequent transport of reactive odd nitrogen (NO_x=NO+NO₂) from the mesosphere and lower thermosphere (MLT) into the stratosphere. This caused NO_x enhancements in the polar upper stratosphere in April 2004 that were unprecedented in the satellite record. Simulations of the 2003-2004 Arctic winter with the Whole Atmosphere Community Climate Model using Specified Dynamics (SD-WACCM) are compared to satellite measurements to assess our understanding of the observed NO_x enhancements. The comparisons show that SD-WACCM clearly displays the descent of NO_x produced …

Growth In Stratospheric Chlorine From Short-Lived Chemicals Not Controlled By The Montreal Protocol, R. Hossaoni, M. P. Chipperfield, A. Saiz-Lopez, J. J. Harrison, R. Von Glasow, R. Sommariva, E. Atlas, M. Navarro, S. A. Montzka, W. Feng, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

We have developed a chemical mechanism describing the tropospheric degradation of chlorine containing very short-lived substances (VSLS). The scheme was included in a global atmospheric model and used to quantify the stratospheric injection of chlorine from anthropogenic VSLS (Cl_y^VSLS) between 2005 and 2013. By constraining the model with surface measurements of chloroform (CHCl₃), dichloromethane (CH₂Cl₂), tetrachloroethene (C₂Cl₄), trichloroethene (C₂HCl₃), and 1,2-dichloroethane (CH₂ClCH₂Cl), we infer a 2013 Cl_y^VSLS mixing ratio of 123 parts per trillion (ppt). Stratospheric injection …

Relative Drifts And Biases Between Six Ozone Limb Satellite Measurements From The Last Decade, N. Rahpoe, M. Weber, A. V. Rozanov, K. Weigel, H. Bovensmann, J. P. Burrows, A. Laeng, G. Stiller, T. Von Clarmann, E. Kyrölä, V. F. Sofieva, J. Tamminen, K. Walker, D. Degenstein, A. E. Bourassa, R. Hargreaves, P. Bernath, J. Urban, D. P. Murtagh

Chemistry & Biochemistry Faculty Publications

As part of European Space Agency's (ESA) climate change initiative, high vertical resolution ozone profiles from three instruments all aboard ESA's Envisat (GOMOS, MIPAS, SCIAMACHY) and ESA's third party missions (OSIRIS, SMR, ACE-FTS) are to be combined in order to create an essential climate variable data record for the last decade. A prerequisite before combining data is the examination of differences and drifts between the data sets. In this paper, we present a detailed analysis of ozone profile differences based on pairwise collocated measurements, including the evolution of the differences with time. Such a diagnosis is helpful to identify strengths …

Retrieval And Validation Of Carbon Dioxide, Methane, And Water Vapor For The Canary Islands Ir-Laser Occultation Experiment, V. Proschek, G. Kirchengast, S. Schweitzer, J.S. A. Brooke, P. F. Bernath, C. B. Thomas, J. G. Wang, K. A. Tereszchuk, G. González Abad, R. J. Hargreaves, C. A. Beale, J. J. Harrison, P. A. Martin, V. L. Kasyutich, C. Gerbig, O. Kolle, A. Loescher

Chemistry & Biochemistry Faculty Publications

The first ground-based experiment to prove the concept of a novel space-based observation technique for microwave and infrared-laser occultation between low-Earthorbit satellites was performed in the Canary Islands between La Palma and Tenerife. For two nights from 21 to 22 July 2011 the experiment delivered the infrared-laser differential transmission principle for the measurement of greenhouse gases (GHGs) in the free atmosphere. Such global and long-term stable measurements of GHGs, accompanied also by measurements of thermodynamic parameters and line-of-sight wind in a self-calibrating way, have become very important for climate change monitoring. The experiment delivered promising initial data for demonstrating the …

Decrease Of Carbon Tetrachloride (Ccl⁴) Over 2004-2013 As Inferred From Global Occultation Measurements With Ace-Fts, E. Mahieu, Peter F. Bernath, Christopher D. Boone, Kaley A. Walker

Chemistry & Biochemistry Faculty Publications

In this contribution, we use infrared solar occultation measurements performed by the ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) instrument onboard the SCISAT-1 Canadian satellite (Bernath et al., 2005). Since its launch in August 2003, this spectrometer has been in continuous operation with no significant degradation of its performance, and global measurements are available from late February 2004 onwards, spanning now more than a decade.

Global Ozone Chemistry And Related Trace Gas Data Records For The Stratosphere (Gozcards): Methodology And Sample Results With A Focus On Hcl, H20, And 03, L. Froidevaux, J. Anderson, H. J. Wang, R. A. Fuller, M. J. Schwartz, M. L. Santee, N. J. Livesey, H. C. Pumphrey, P. F. Bernath, J. M. Russell Iii, M. P. Mccormick

Chemistry & Biochemistry Faculty Publications

We describe the publicly available data from the Global OZone Chemistry And Related trace gas Data records for the Stratosphere (GOZCARDS) project and provide some results, with a focus on hydrogen chloride (HCl), water vapor (H₂O), and ozone (O₃). This data set is a global long-term stratospheric Earth system data record, consisting of monthly zonal mean time series starting as early as 1979. The data records are based on high-quality measurements from several NASA satellite instruments and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on SCISAT. We examine consistency aspects between the various data sets. …

Recent Increase Of Ethane Detected In The Remote Atmosphere Of The Northern Hemisphere, Bruno Franco, Whitney Bader, Benoît Bovy, Emmanuel Mahieu, Emily V. Fischer, Kimberly Strong, Stephanie Conway, James W. Hannigan, Eric Nussbaumer, Peter F. Bernath, Chris D. Boone, Kaley A. Walker

Chemistry & Biochemistry Faculty Publications

Ethane (C₂H₆) has a large impact on tropospheric composition and air quality because of its involvement in the global VOC (volatile organic compound) – HO_x – NO_x chemistry responsible for generating and destroying tropospheric ozone. By acting as a major sink for tropospheric OH radicals, the abundance of C₂H₆ influences the atmospheric content of carbon monoxide and impacts the lifetime of methane. Moreover, it is an important source of PAN, a thermally unstable reservoir for NOx radicals.

On a global scale, the main sources of C₂H₆ are leakage from the production, transport of natural gas loss, biofuel consumption …

Assessment Of Water Vapor Isotopologue Measurements By Ace-Fts And Odin-Smr, Ralf Bauer, Patrick Sheese, Kaley Walker, Joachim Urban, Donal Murtagh, Chris Boone, Peter Bernath, Gloria Manney

Chemistry & Biochemistry Faculty Publications

[Introduction] Knowing the isotopic composition of trace gases can improve our understanding of processes in the Earth's atmosphere causing isotopic fractionation. In many studies, isotopologue (molecules of identical chemical but different isotopic composition) amounts are primarily discussed as δ values, which are defined relative to a standard, e.g.:

Ace-Fts And Haloe Observations Of Hydrogen Fluoride (Hf) And Their Comparison With Slimcat Chemical Transport Model Calculations, Jeremy Harrison, Martyn Chipperfield, Chris Boone, Peter Bernath, Lucien Froidevaux, John Anderson, James Russell Iii

Chemistry & Biochemistry Faculty Publications

The majority of fluorine in the atmosphere has resulted from the anthropogenic emission of chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), and hydrofluorocarbons (HFCs). Most tropospheric fluorine is present in its emitted 'organic' form due to the molecules having long lifetimes (up to a decade or longer). Thus they are able to reach the stratosphere where they are broken down, liberating fluorine. The principal degradation products are carbonyl fluoride (COF2), carbonyl chloride fluoride (COClF), and hydrogen fluoride (HF); of these HF is the most abundant. In fact at the top of the stratosphere most of the fluorine is present as HF, which, due …

Comparison Of Upper Tropospheric Carbon Monoxide From Mopitt, Ace-Fts, And Hippo-Qcls, Sara Martínez-Alonzo, Merritt N. Deeter, Helen M. Worden, John C. Gille, Louisa K. Emmons, Laura L. Pan, Mijeong Park, Gloria L. Manney, Peter F. Bernath, Chris D. Boone

Chemistry & Biochemistry Faculty Publications

Products from the Measurements Of Pollution In The Troposphere (MOPITT) instrument are regularly validated using in situ airborne measurements. However, few of these measurements reach into the upper troposphere, thus hindering MOPITT validation in that region. Here we evaluate upper tropospheric (~500 hPa to the tropopause) MOPITT CO profiles by comparing them to satellite Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) retrievals and to measurements from the High-performance Instrumented Airborne Platform for Environmental Research Pole to Pole Observations (HIPPO) Quantum Cascade Laser Spectrometer (QCLS). Direct comparison of colocated v5 MOPITT thermal infrared-only retrievals, v3.0 ACE-FTS retrievals, and HIPPO-QCLS measurements shows …

Distinguishing Molecular Characteristics Of Aerosol Water Soluble Organic Matter From The 2011 Trans-North Atlantic Us Geotraces Cruise, A. S. Wozniak, A. S. Willoughby, S. C. Gurganus, Patrick G. Hatcher

Chemistry & Biochemistry Faculty Publications

The molecular characteristics of aerosol organic matter (OM) determines to a large extent its impacts on the atmospheric radiative budget and ecosystem function in terrestrial and aquatic environments, yet the OM molecular details of aerosols from different sources are not well established. Aerosol particulate samples with North American-influenced, North African-influenced, and marine (minimal recent continental influence) air mass back trajectories were collected as part of the 2011 trans-North Atlantic US GEOTRACES cruise and analyzed for their water soluble OM (WSOM) molecular characteristics using electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Principal component analysis (PCA) separated the samples into …

Validation Of Mipas Imk/Iaa V5r_O3_224 Ozone Profiles, A. Laeng, U. Grabowski, T. Von Clarmann, G. Stiller, N. Glatthor, M. Höpfner, S. Kellmann, M. Kiefer, A. Linden, S. Lossow, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

We present the results of an extensive validation program of the most recent version of ozone vertical profiles retrieved with the IMK/IAA (Institute for Meteorology and Climate Research/Instituto de Astrofisica de Andalucia) MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) research level 2 processor from version 5 spectral level 1 data. The time period covered corresponds to the reduced spectral resolution period of the MIPAS instrument, i.e., January 2005-April 2012. The comparison with satellite instruments includes all post-2005 satellite limb and occultation sensors that have measured the vertical profiles of tropospheric and stratospheric ozone: ACE-FTS, GOMOS, HALOE, HIRDLS, MLS, OSIRIS, POAM, …

Global Stratospheric Fluorine Inventory For 2004-2009 From Atmospheric Chemistry Experiment Fourier Transform Spectrometer (Ace-Fts) Measurements And Slimcat Model Simulations, A. T. Brown, M. P. Chipperfield, N. A. D. Richards, C. Boone, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

Fluorine-containing species can be extremely effective atmospheric greenhouse gases. We present fluorine budgets using organic and inorganic species retrieved by the ACE-FTS satellite instrument supplemented with output from the SLIMCAT 3-D chemical transport model. The budgets are calculated between 2004 and 2009 for a number of latitude bands: 70-30 °N, 30-00 °N, 00 °N-30 °S, and 30-70°S. At lower altitudes total fluorine profiles are dominated by the contribution from CFC-12, up to an altitude of 20 km in the extra-tropics and 29 km in the tropics; above these altitudes the profiles are dominated by hydrogen fluoride (HF). Our data show …

Technical Note: Swift - A Fast Semi-Empirical Model For Polar Stratospheric Ozone Loss, M. Rex, S. Kremser, P. Huck, G. Bodeker, I. Wohltmann, M. L. Santee, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

An extremely fast model to estimate the degree of stratospheric ozone depletion during polar winters is described. It is based on a set of coupled differential equations that simulate the seasonal evolution of vortex-averaged hydrogen chloride (HCl), nitric acid (HNO3), chlorine nitrate (ClONO₂), active forms of chlorine (ClO_x = Cl+ClO+2ClOOCl) and ozone (O₃) on isentropic levels within the polar vortices. Terms in these equations account for the chemical and physical processes driving the time rate of change of these species. Eight empirical fit coefficients associated with these terms are derived by iteratively fitting the equations …

Derivation Of Tropospheric Methane From Tccon Ch4 And Hf Total Column Observations, K. M. Saad, D. Wunch, P. Bernath, C. Boone, B. Connor, N. M. Deutscher, D.W.T. Griffith, R. Kivi, J. Notholt, C. Roehl, M. Schneider, V. Sherlock, P. O. Wennberg

Chemistry & Biochemistry Faculty Publications

The Total Carbon Column Observing Network (TCCON) is a global ground-based network of Fourier transform spectrometers that produce precise measurements of column-averaged dry-air mole fractions of atmospheric methane (CH₄). Temporal variability in the total column of CH₄ due to stratospheric dynamics obscures fluctuations and trends driven by tropospheric transport and local surface fluxes that are critical for understanding CH₄ sources and sinks. We reduce the contribution of stratospheric variability from the total column average by subtracting an estimate of the stratospheric CH₄ derived from simultaneous measurements of hydrogen fluoride (HF). HF provides a proxy for …

Middle Atmospheric Changes Caused By The January And March 2012 Solar Proton Events, C. H. Jackman, C. E. Randall, V. L. Harvey, S. Wang, E. L. Fleming, M. López-Puertas, B. Funke, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

The recent 23-30 January and 7-11 March 2012 solar proton event (SPE) periods were substantial and caused significant impacts on the middle atmosphere. These were the two largest SPE periods of solar cycle 24 so far. The highly energetic solar protons produced considerable ionization of the neutral atmosphere as well as HOx (H, OH, HO2) and NOx (N, NO, NO2). We compute a NOx production of 1.9 and 2.1 Gigamoles due to these SPE periods in January and March 2012, respectively, which places these SPE periods among the 12 largest in the past 50 yr. Aura Microwave Limb Sounder (MLS) …

A Molecular-Level Approach For Characterizing Water-Insoluble Components Of Ambient Organic Aerosol Particulates Using Ultrahigh-Resolution Mass Spectrometry, A. S. Willoughby, A. S. Wozniak, Patrick G. Hatcher

Chemistry & Biochemistry Faculty Publications

The chemical composition of organic aerosols in the atmosphere is strongly influenced by human emissions. The effect these have on the environment, human health, and climate change is determined by the molecular nature of these chemical species. The complexity of organic aerosol samples limits the ability to study the chemical composition, and therefore the associated properties and the impacts they have. Many studies have addressed the watersoluble fraction of organic aerosols and have had much success in identifying specific molecular formulas for thousands of compounds present. However, little attention is given to the water-insoluble portion, which can contain most of …

Retrievals Of Carbonyl Fluoride (Cof₂) From Ace-Fts And Mipas Spectra And Their Comparison With Slimcat Ctm Calculations, Jeremy Harrison, Shaomin Cai, Anu Dudhia, Martyn Chipperfield, Chris Boone, Peter Bernath

Chemistry & Biochemistry Faculty Publications

The majority of fluorine in the atmosphere has resulted from the anthropogenic emission of chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), and hydrofluorocarbons (HFCs). Most tropospheric fluorine is present in its emitted 'organic' form due to the molecules having long lifetimes. At the top of the stratosphere most of the fluorine is present as the 'inorganic' product HF, which, due to its extreme stability, is an almost permanent reservoir of stratospheric fluorine. The second most abundant stratospheric 'inorganic' fluorine reservoir is carbonyl fluoride (COF₂). The major sources of COF₂ are from the atmospheric degradation of CFC-12 (CCl₂F₂), which is now banned under the …

Hci And Cio Profiles Inside The Antarctic Vortex As Observed By Smiles In November 2009: Comparisons With Mls And Ace-Fts Instruments, T. Sugita, Y. Kasai, Y. Terao, S. Hayashida, G. L. Manney, W. H. Daffer, H. Sagawa, M. Suzuki, M. Shiotani, K. A. Walker, C. D. Boone, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

We present vertical profiles of hydrogen chloride (HCl) and chlorine monoxide (ClO) as observed by the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) on the International Space Station (ISS) inside the Antarctic vortex on 19-24 November 2009. The SMILES HCl value reveals 2.8-3.1 ppbv between 450K and 500K levels in potential temperature (PT). The high value of HCl is highlighted since it is suggested that HCl is a main component of the total inorganic chlorine Cl_y, defined as Cl_y similar or equal to HCl + ClO + chlorine nitrate ClONO₂, inside the Antarctic vortex in spring, owing …

Stratospheric Loss And Atmospheric Lifetimes Of Cfc-11 And Cfc-12 Derived From Satellite Observations, K. Minschwaner, L. Hoffmann, A. Brown, M. Riese, R. Müller, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

The lifetimes of CFC-11 and CFC-12 have been evaluated using global observations of their stratospheric distributions from satellite-based instruments over the time period from 1992 to 2010. The chlorofluorocarbon (CFC) datasets are from the Cryogen Limb Array Etalon Spectrometer (CLAES), the Cryogenic Infrared Spectrometers and Telescopes for the Atmosphere (CRISTA-1 and CRISTA-2), the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), and the Atmospheric Chemistry Experiment (ACE). Stratospheric loss rates were calculated using an ultraviolet radiative transfer code with updated cross section and solar irradiance data. Mean steady-state lifetimes based on these observations are 44.7 (36-58) yr for CFC-11 and 106.6 …

Observations Of Peroxyacetyl Nitrate (Pan) In The Upper Troposphere By The Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (Ace-Fts), K. A. Tereszchuk, D. P. Moore, J. J. Harrison, C. D. Boone, M. Park, J. J. Remedios, W. J. Randel, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

Peroxyacetyl nitrate (CH₃CO·O₂NO₂, abbreviated as PAN) is a trace molecular species present in the troposphere and lower stratosphere due primarily to pollution from fuel combustion and the pyrogenic outflows from biomass burning. In the lower troposphere, PAN has a relatively short lifetime and is principally destroyed within a few hours through thermolysis, but it can act as a reservoir and carrier of NO_x in the colder temperatures of the upper troposphere, where UV photolysis becomes the dominant loss mechanism. Pyroconvective updrafts from large biomass burning events can inject PAN into the upper troposphere …

Production Mechanisms, Number Concentration, Size Distribution, Chemical Composition, And Optical Properties Of Sea Spray Aerosols, Nicholas Meskhidze, Markus D. Petters, Kostas Tsigaridis, Tim Bates, Colin O'Dowd, Jeff Reid, Ernie R. Lewis, Brett Gantt, Magdalena D. Anguelova, Prakash V. Bhave, Andrew Wozniak

Chemistry & Biochemistry Faculty Publications

(First paragraph)

The impact of sea spray aerosols on global climate remains one of the most uncertain components of the aerosol–radiation–climate problem, but has received less attention than the impacts of terrestrial and anthropogenic aerosols. The last decade has produced a large body of information regarding the sources and composition of marine aerosols, resulting in a reassessment of the complex role that sea spray particles play in climate and various geophysical phenomena. As sea spray aerosol contributes substantially to the preindustrial, natural background which provides the baseline on top of which anthropogenic forcing should be quantified, and because the ocean …

Ace-Fts Observations Of Acetonitrile In The Lower Stratosphere, J. J. Harrison, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

This work reports the first infrared satellite remote-sensing measurements of acetonitrile (CH₃CN) in the Earth's atmosphere using solar occultation measurements made by the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) between 2004 and 2011. The retrieval scheme uses new quantitative laboratory spectroscopic measurements of acetonitrile (Harrison and Bernath, 2012). Although individual ACE-FTS profile measurements are dominated by measurement noise, median profiles in 10 degrees latitude bins show a steady decline in volume mixing ratio from similar to 150 ppt (parts per trillion) at 11.5 km to < 40 ppt at 25.5-29.5 km. These new measurements agree well with the scant available air-and balloon-borne data in the lower stratosphere. An acetonitrile stratospheric lifetime of 73 ± 20 yr has been determined.

Quantifying The Impact Of Boreal Forest Fires On Tropospheric Oxidants Over The Atlantic Using Aircraft And Satellites (Bortas) Experiment: Design, Execution And Science Overview, P. I. Palmer, M. Parrington, J. D. Lee, A, C. Lewis, A. R. Rickard, P. F. Bernath, T. J. Duck, D. L. Waugh, D. W. Tarasick, S. Andrews

Chemistry & Biochemistry Faculty Publications

We describe the design and execution of the BORTAS (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) experiment, which has the overarching objective of understanding the chemical aging of air masses that contain the emission products from seasonal boreal wildfires and how these air masses subsequently impact downwind atmospheric composition. The central focus of the experiment was a two-week deployment of the UK BAe-146-301 Atmospheric Research Aircraft (ARA) over eastern Canada, based out of Halifax, Nova Scotia. Atmospheric ground-based and sonde measurements over Canada and the Azores associated with the planned …