Oceanography and Atmospheric Sciences and Meteorology Commons^™

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 …

Improved Method For Quantifying The Air-Sea Flux Of Volatile And Semi-Volatile Organic Carbon, Emily Hauser, Rebecca M. Dickhut, Renee Falconer, Andrew S. Wozniak

Chemistry & Biochemistry Faculty Publications

A method for quantifying the diffusive air-sea exchange of gaseous organic carbon (OC) was developed. OC compounds were separated into two operational pools-those that were kinetically air limited in diffusion across the air-sea interface and those that were water limited-during simultaneous air/water sampling. The method separates OC compounds into low Henry's law constant (low-H) semivolatile OC (SOC) and high Henry's law constant (high-H) volatile OC (VOC) pools that can be categorized by relating diffusion kinetic parameters to Henry's Law constant. Air limited (low-H; H << similar to 0.1 L atm mol(^-1)) compounds were collected in pure water traps and were quantified as dissolved OC, whereas …

Ace-Fts Observations Of Pyrogenic Trace Species In Boreal Biomass Burning Plumes During Bortas, K. A. Tereszchuk, G. G. Abad, C. Clerbaux, J. Hadji-Lazaro, D. Hurtmans, P. F. Coheur, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

To further our understanding of the effects of biomass burning emissions on atmospheric composition, the BORTAS campaign (BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) was conducted on 12 July to 3 August 2011 during the boreal forest fire season in Canada. The simultaneous aerial, ground and satellite measurement campaign sought to record instances of boreal biomass burning to measure the tropospheric volume mixing ratios (VMRs) of short- and long-lived trace molecular species from biomass burning emissions. The goal was to investigate the connection between the composition and the distribution of these pyrogenic outflows and …

Stratospheric Lifetimes Of Cfc-12, Ccl4, Ch4, Ch3cl And N20 From Measurements Made By The Atmospheric Chemistry Experiment-Fourier Transform Spectrometer, A. T. Brown, C. M. Volk, M. R. Schoebert, C. D. Boone, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

Long lived halogen-containing compounds are important atmospheric constituents since they can act both as a source of chlorine radicals, which go on to catalyse ozone loss, and as powerful greenhouse gases. The long-term impact of these species on the ozone layer is dependent on their stratospheric lifetimes. Using observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) we present calculations of the stratospheric lifetimes of CFC-12, CCl₄, CH₄, CH₃Cl and N₂O. The lifetimes were calculated using the slope of the tracer-tracer correlation of these species with CFC-11 at the tropopause. The …

Harmonized Dataset Of Ozone Profiles From Satellite Limb And Occultation Measurements, V. F. Sofieva, N. Rahpoe, J. Tamminen, E. Kyrölä, N. Kalakoski, M. Weber, A. Rozanov, C. Von Savigny, A Laeng, T. Von Clarmann, P. Bernath, R. J. Hargreaves

Chemistry & Biochemistry Faculty Publications

In this paper, we present a HARMonized dataset of OZone profiles (HARMOZ) based on limb and occultation measurements from Envisat (GOMOS, MIPAS and SCIAMACHY), Odin (OSIRIS, SMR) and SCISAT (ACE-FTS) satellite instruments. These measurements provide high-vertical-resolution ozone profiles covering the altitude range from the upper troposphere up to the mesosphere in years 2001-2012. HARMOZ has been created in the framework of the European Space Agency Climate Change Initiative project. The harmonized dataset consists of original retrieved ozone profiles from each instrument, which are screened for invalid data by the instrument teams. While the original ozone profiles are presented in different …

Validation Of Stratospheric And Mesospheric Ozone Observed By Smiles From International Space Station, Y. Kasai, H. Sagawa, D. Kreyling, E. Dupuy, P. Baron, J. Mendrok, K Suzuki, T. O. Sato, T. Nishibori, S. Mizobuchi, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

We observed ozone O₃ in the vertical region between 250 and 0.0005 hPa (~ 12-96 km) using the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) on the Japanese Experiment Module (JEM) of the International Space Station (ISS) between 12 October 2009 and 21 April 2010. The new 4K superconducting heterodyne receiver technology of SMILES allowed us to obtain a one order of magnitude better signal-to-noise ratio for the O₃ line observation compared to past spaceborne microwave instruments. The non-sun-synchronous orbit of the ISS allowed us to observe O₃ at various local times. We assessed the quality of the vertical …

The Relation Between Atmospheric Humidity And Temperature Trends For Stratospheric Water, S. Fueglistaler, Y. S. Liu, T. J. Flannaghan, P. H. Haynes, D. P. Dee, W. J. Read, E. E. Remsberg, L. W. Thomason, D. F. Hurst, J. R. Lanzante, P. F. Bernath

Chemistry & Biochemistry Faculty Publications

We analyze the relation between atmospheric temperature and water vapor-a fundamental component of the global climate system-for stratospheric water vapor (SWV). We compare measurements of SWV (and methane where available) over the period 1980-2011 from NOAA balloon-borne frostpoint hygrometer (NOAA-FPH), SAGE II, Halogen Occultation Experiment (HALOE), Microwave Limb Sounder (MLS)/Aura, and Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) to model predictions based on troposphere-to-stratosphere transport from ERA-Interim, and temperatures from ERA-Interim, Modern Era Retrospective- Analysis (MERRA), Climate Forecast System Reanalysis (CFSR), Radiosonde Atmospheric Temperature Products for Assessing Climate (RATPAC), HadAT2, and RICHv1.5. All model predictions are dry biased. The interannual …

Hydrocarbons In The Upper Troposphere And Lower Stratosphere Observed From Ace-Fts And Comparisons With Waccm, Mijeong Park, William J. Randel, Douglas E. Kinnison, Louisa K. Emmons, Peter F. Bernath, Kaley A. Walker, Chris D. Boone, Nathaniel J. Livesey

Chemistry & Biochemistry Faculty Publications

Satellite measurements from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) are used to examine the global, seasonal variations of several hydrocarbons, including carbon monoxide (CO), ethane (C₂H₆), acetylene (C₂H₂), and hydrogen cyanide (HCN). We focus on quantifying large-scale seasonal behavior from the middle troposphere to the stratosphere, particularly in the tropics, and furthermore make detailed comparisons with the Whole Atmosphere Community Climate Model (WACCM) chemistry climate model (incorporating tropospheric photochemistry, time-varying hydrocarbon emissions, and meteorological fields nudged from reanalysis). Comparisons with Microwave Limb Sounder (MLS) measurements of CO are also included …

Water Vapor And The Equatorial Mesospheric Semi-Annual Oscillation (Msao), R. L. Gattinger, E. Kyröla, C. D. Boone, W. F. J. Evans, K. A. Walker, I. C. Mcdade, P. F. Bernath, E. J. Llewellyn

Chemistry & Biochemistry Faculty Publications

Observations of the mesospheric semi-annual oscillation (MSAO) in the equatorial region have been reported dating back several decades. Seasonal variations in both species densities and airglow emissions are well documented. The extensive observations available offer an excellent case study for comparison with model simulations. The broad range of measurements is summarised with emphasis on the 80 to 100 km region. Photochemical model simulations are described for near-equinox and near solstice conditions, the two lines with notable differences in the observed MSAO parameters. Diurnal tides are included in order to facilitate comparisons of observations made at different local times. The roles …

A Preliminary Examination Of An In Situ Dual Dye Approach To Measuring Light Fluxes In Lotic Systems, Elizabeth C. Minor, Elizabeth James, Jay A. Austin, Veronica Nelson, Ryan Lusk, Kenneth Mopper

Chemistry & Biochemistry Faculty Publications

Light is a critical parameter in aquatic ecosystems, affecting primary production and in situ photochemistry. However, measuring light exposure for suspended particles or dissolved components in a dynamic water column can be challenging with existing Eulerian approaches. Here, we assess the simultaneous deployment of two dyes differing in photolability (rhodamine WT and fluorescein) as a Lagrangian measure of sunlight exposure in a lotic system. Fluorescein is sensitive to light exposure; rhodamine WT is relatively photostable. We examined dye fluorescence at various pH, salinity, and temperature conditions. We also tested dye photolability as a function of pH and wavelength range. In …

Uncertainties In Modelling Heterogeneous Chemistry And Arctic Ozone Depletion In The Winter 2009/2010, I. Wohltmann, T. Wegner, R. Müller, R. Lehmann, M. Rex, G. L. Manney, M. L. Santee, P. Bernath, O. Suminska-Ebersoldt

Chemistry & Biochemistry Faculty Publications

Stratospheric chemistry and denitrification are simulated for the Arctic winter 2009/2010 with the Lagrangian Chemistry and Transport Model ATLAS. A number of sensitivity runs is used to explore the impact of uncertainties in chlorine activation and denitrification on the model results. In particular, the efficiency of chlorine activation on different types of liquid aerosol versus activation on nitric acid trihydrate clouds is examined. Additionally, the impact of changes in reaction rate coefficients, in the particle number density of polar stratospheric clouds, in supersaturation, temperature or the extent of denitrification is investigated. Results are compared to satellite measurements of MLS and …

Global Variations Of Hdo And Hdo/H2o Ratios In The Upper Troposphere And Lower Stratosphere Derived From Ace-Fts Satellite Measurements, William J. Randel, Elisabeth Moyer, Mijeong Park, Eric Jensen, Peter Bernath

Chemistry & Biochemistry Faculty Publications

High-quality satellite observations of water and deuterated water in the upper troposphere and lower stratosphere (UTLS) from the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) are used to map global climatological behavior. Spatial and temporal variability in these data suggest that convection plays a significant role in setting water vapor isotopic composition in these regions. In many instances, enhancements in HDO/H₂O (i.e., δD) are closely tied to patterns of climatological deep convection and uncorrelated with water vapor, although convection appears to have different isotopic effects in different locations. The ACE-FTS data reveal seasonal variations in the tropics …

Technical Note: A Trace Gas Climatology Derived From The Atmospheric Chemistry Experiment Fourier Transform Spectrometer (Ace-Fts) Data Set, A. Jones, K. A. Walker, J. J. Jin, J. R. Taylor, C. D. Boone, P. F. Bernath, S. Brohede, G. L. Manney, S. Mcleod, R. Hughes, W. H. Daffer

Chemistry & Biochemistry Faculty Publications

The Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) aboard the Canadian satellite SCISAT (launched in August 2003) was designed to investigate the composition of the upper troposphere, stratosphere, and mesosphere. ACE-FTS utilizes solar occultation to measure temperature and pressure as well as vertical profiles of over thirty chemical species including O₃, H₂O, CH₄, N₂O, CO, NO, NO₂, N₂O₅, HNO₃, HCl, ClONO₂, CCl₃F, CCl₂F₂, and HF. Global coverage for each species is obtained approximately over a three month …

Greenhouse Gas Measurements Over A 144 Km Open Path In The Canary Islands, J.S. A. Brooke, P. F. Bernath, G. Kirchengast, C. B. Thomas, J. G. Wang, K. A. Tereszchuk, G. González Abad, R. J. Hargreaves, C. A. Beale, J. J. Harrison

Chemistry & Biochemistry Faculty Publications

A new technique for the satellite remote sensing of greenhouse gases in the atmosphere via the absorption of short-wave infrared laser signals transmitted between counter-rotating satellites in low Earth orbit has recently been proposed; this would enable the acquisition of a long-term, stable, global set of altitude-resolved concentration measurements. We present the first ground-based experimental demonstration of this new infrared-laser occultation method, in which the atmospheric absorption of CO₂ near 2.1µm was measured over a ∼144km path length between two peaks in the Canary Islands (at an altitude of ∼2.4 km), using relatively low power diode lasers (∼4 to …

Isotopic Characterization Of Aerosol Organic Carbon Components Over The Eastern United States, Andrew S. Wozniak, James E. Bauer, Rebecca M. Dickhut, Xu Li, Ann P. Mcnichol

Chemistry & Biochemistry Faculty Publications

Carbon isotopic signatures (δ¹³C, Δ¹⁴C) of aerosol particulate matter total organic carbon (TOC) and operationally defined organic carbon (OC) components were measured in samples from two background sites in the eastern U.S. TOC and water-soluble OC (WSOC)δ¹³C values (−27 to −24‰) indicated predominantly terrestrial C₃ plant and fossil derived sources. Total solvent extracts (TSE) and their aliphatic, aromatic, and polar OC components were depleted in δ¹³C (−30 to −26‰) relative to TOC and WSOC. Δ¹⁴C signatures of aerosol TOC and TSE (−476 to +25‰) suggest variable fossil contributions (∼5–50%) …

Process-Evaluation Of Tropospheric Humidity Simulated By General Circulation Models Using Water Vapor Isotopologues: 1. Comparison Between Models And Observations, Camille Risi, David Noone, John Worden, Christian Frankenberg, Gabriele Stiller, Michael Kiefer, Bernd Funke, Kaley Walker, Peter Bernath, Matthias Schneider, Debra Wunch, Vanessa Sherlock, Nicholas Deutscher, David Griffith, Paul O. Wennberg, Kimberly Strong, Dan Smale, Emmanuel Mahieu, Sabine Barthlott, Frank Hase, Omaira García, Justus Notholt, Thorsten Warneke, Geoffrey Toon, David Sayres, Sandrine Bony, Jeonghoon Lee, Derek Brown, Ryu Uemura, Christophe Sturm

Chemistry & Biochemistry Faculty Publications

The goal of this study is to determine how H₂O and HDO measurements in water vapor can be used to detect and diagnose biases in the representation of processes controlling tropospheric humidity in atmospheric general circulation models (GCMs). We analyze a large number of isotopic data sets (four satellite, sixteen ground-based remote-sensing, five surface in situ and three aircraft data sets) that are sensitive to different altitudes throughout the free troposphere. Despite significant differences between data sets, we identify some observed HDO/H₂O characteristics that are robust across data sets and that can be used to evaluate …

Atmospheric Effects Of Energetic Particle Precipitation In The Arctic Winter 1978-1979 Revisted, L. A. Holt, C. E. Randall, V. L. Harvey, E. E. Remsberg, G. P. Stiller, B. Funke, P. F. Bernath, K. A. Walker

Chemistry & Biochemistry Faculty Publications

[1] The Limb Infrared Monitor of the Stratosphere (LIMS) measured polar stratospheric enhancements of NO₂ mixing ratios due to energetic particle precipitation (EPP) in the Arctic winter of 1978–1979. Recently reprocessed LIMS data are compared to more recent measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) to place the LIMS measurements in the context of current observations. The amount of NO_x (NO + NO₂) entering the stratosphere that has been created by EPP in the mesosphere and lower thermosphere (EPP-NO_x) has been quantified …

First Remote Sensing Observations Of Trifluoromethane (Hfc-23) In The Upper Troposphere And Lower Stratosphere, Jeremy J. Harrison, Christopher D. Boone, Alexander T. Brown, Nicholas D. C. Allen, Geoffrey C. Toon, Peter F. Bernath

Chemistry & Biochemistry Faculty Publications

This work reports the first remote sensing measurements of atmospheric HFC-23 (CHF₃) using solar occultation measurements made by the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) and the Jet Propulsion Laboratory Mark IV (MkIV) balloon interferometer. A total of 8809 ACE occultations measured between 2004 and 2010 have been processed, along with 24 MkIV occultations measured between 1989 and 2007. ACE data (yearly averages over the 10-25 km altitude range) in the tropics/subtropics (40°S-40°N) reveal a trend of 4.0 ± 1.6% per year in the growth of HFC-23 for 2004-2009 (or 3.9 ± 1.2% per year for 2004-2010), …

Analysis Of Iasi Tropospheric O₃ Data Over The Arctic During Polarcat Campaigns In 2008, M. Pommier, C. Clerbaux, K. S. Law, G. Ancellet, P. Bernath, P.-F. Coheur, J. Hadji-Lazaro, D. Hurtmans, P. Nédélec, J.-D. Paris, F. Ravetta, T. B. Ryerson, H. Schlager, A. J. Weinheimer

Chemistry & Biochemistry Faculty Publications

Ozone data retrieved in the Arctic region from infrared radiance spectra recorded by the Infrared Atmospheric Sounding Interferometer (IASI) on board the MetOp-A European satellite are presented. They are compared with in situ and lidar observations obtained during a series of aircraft measurement campaigns as part of the International Polar Year POLARCAT activities in spring and summer 2008. Different air masses were sampled during the campaigns including clean air, polluted plumes originating from anthropogenic sources, forest fire plumes from the three northern continents, and stratospheric-influenced air masses. The comparison between IASI O₃ [0–8 km], [0–12 km] partial columns and …

Process-Evaluation Of Tropospheric Humidity Simulated By General Circulation Models Using Water Vapor Isotopic Observations: 2. Using Isotopic Diagnostics To Understand The Mid And Upper Tropospheric Moist Bias In The Tropics And Subtropics, Camille Risi, David Noone, John Worden, Christian Frankenberg, Gabriele Stiller, Michael Kiefer, Bernd Funke, Kaley Walker, Peter Bernath, Matthias Schneider, Sandrine Bony, Jeonghoon Lee, Derek Brown, Christophe Sturm

Chemistry & Biochemistry Faculty Publications

Evaluating the representation of processes controlling tropical and subtropical tropospheric relative humidity (RH) in atmospheric general circulation models (GCMs) is crucial to assess the credibility of predicted climate changes. GCMs have long exhibited a moist bias in the tropical and subtropical mid and upper troposphere, which could be due to the mis-representation of cloud processes or of the large-scale circulation, or to excessive diffusion during water vapor transport. The goal of this study is to use observations of the water vapor isotopic ratio to understand the cause of this bias. We compare the three-dimensional distribution of the water vapor isotopic …

Characterization Of Heterogeneities And Domains In Aquatic And Sedimentary Organic Matter By 1 H Spin Diffusion: Potential For Elucidating The Formation Mechanisms, Jingdong Mao, Xiaoyan Cao

Chemistry & Biochemistry Faculty Publications

Although the information on domains and heterogeneities of natural organic matter (NOM) can provide insights into its formation mechanisms, the appropriate solid-state NMR technique for measuring them is still lacking. The traditional technique requires mobility differences in NOM whereas NOM components are primarily rigid. We introduced a new ¹H spin diffusion technique, ¹H-¹³C two-dimensional heteronuclear correlation (2D HETCOR) NMR with ¹H spin diffusion, for characterization of domains and heterogeneities in aquatic and sedimentary organic matter. It was achieved by collecting a series of 2D HETCOR spectra with a variable mixing time, t_m', and …