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Jucks, K. W.

Publications and source records attributed to Jucks, K. W..

Validation of Aura Microwave Limb Sounder HCl Measurements

The Earth Observing System (EOS) Microwave Limb Sounder (MLS) aboard the Aura satellite has provided daily global HCl profiles since August 2004. We provide a characterization of the resolution, random and systematic uncertainties, and known issues for the version 2.2 MLS HCl data. The MLS sampling allows for comparisons with many (~1500 to more than 3000) closely matched profiles from the Halogen Occultation Experiment (HALOE) and Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). These data sets provide HCl latitudinal distributions that are, overall, very similar to those from (coincident) MLS profiles, although there are some discrepancies in the upper stratosphere between the MLS and HALOE gradients. As found in previous work, MLS and ACE HCl profiles agree very well (within approximately 5%, on average), but the MLS HCl abundances are generally larger (by 10-20%) than HALOE HCl. The bias versus HALOE is unlikely to arise mostly from MLS, as a similar systematic bias (of order 15%) is not observed between average MLS and balloon-borne measurements of HCl, obtained over Fort Sumner, New Mexico, in 2004 and 2005. At the largest pressure (147 hPa) for MLS HCl, a high bias (approximately 0.2 ppbv) is apparent in analyses of low to midlatitude data versus in situ aircraft chemical ionization mass spectrometry (CIMS) HCl measurements from the Aura Validation Experiment (AVE) campaigns in 2004, 2005, and 2006; this bias is also observed in comparisons of MLS and aircraftHCl/O3 correlations. Good agreement between MLS and CIMS HCl is obtained at 100 to 68 hPa. The recommended pressure range for MLS HCl is from 100 to 0.15 hPa.

Earth Observing System (EOS)↗

Validation of the Aura Microwave Limb Sounder middle atmosphere water vapor and nitrous oxide measurements

The quality of the version 2.2 (v2.2) middle atmosphere water vapor and nitrous oxide measurements from the Microwave Limb Sounder (MLS) on the Earth Observing System (EOS) Aura satellite is assessed. The impacts of the various sources of systematic error are estimated by a comprehensive set of retrieval simulations. Comparisons with correlative data sets from ground-based, balloon and satellite platforms operating in the UV/visible, infrared and microwave regions of the spectrum are performed. Precision estimates are also validated, and recommendations are given on the data usage. The v2.2 H2O data have been improved over v1.5 by providing higher vertical resolution in the lower stratosphere and better precision above the stratopause. The single-profile precision is ~0.2–0.3 ppmv (4–9%), and the vertical resolution is ~3–4 km in the stratosphere. The precision and vertical resolution become worse with increasing height above the stratopause. Over the pressure range 0.1–0.01 hPa the precision degrades from 0.4 to 1.1 ppmv (6–34%), and the vertical resolution degrades to ~12–16 km. The accuracy is estimated to be 0.2–0.5 ppmv (4–11%) for the pressure range 68–0.01 hPa. The scientifically useful range of the H2O data is from 316 to 0.002 hPa, although only the 82–0.002 hPa pressure range is validated here. Substantial improvement has been achieved in the v2.2 N2O data over v1.5 by reducing a significant low bias in the stratosphere and eliminating unrealistically high biased mixing ratios in the polar regions. The single-profile precision is ~13–25 ppbv (7–38%), the vertical resolution is ~4–6 km and the accuracy is estimated to be 3–70 ppbv (9–25%) for the pressure range 100–4.6 hPa. The scientifically useful range of the N2O data is from 100 to 1 hPa.

Atlas, E.↗

Observed and Modeled HOCl Profiles in the Midlatitude Stratosphere: Implication for Ozone Loss

Vertical profiles of stratospheric HOCl calculated with a diurnal steady-state photochemical model that uses currently recommended reaction rates and photolysis cross sections underestimate observed profiles of HOCl obtained by two balloon-borne instruments, FIRS-2 (a far-infrared emission spectrometer) and MkIV (a mid-infrared, solar absorption spectrometer). Considerable uncertainty (a factor of two) persists in laboratory measurements of the rate constant (k(sub 1)) for the reaction ClO + HO2 yields HOCl + O2. Agreement between modeled and measured HOCl can be attained using a value of k(sub 1) from Stimpfle et al. (1979) that is about a factor-of-two faster than the currently recommended rate constant. Comparison of modeled and measured HOCl suggests that models using the currently recommended value for k(sub 1) may underestimate the role of the HOCl catalytic cycle for ozone depletion, important in the midlatitude lower stratosphere.

temperature dependence↗

Measured and modeled HOCl profiles in the mid-latitude stratosphere : implication for ozone loss

The HOCl catalytic cycle is an efficient ozone loss mechanism in the lower mid-latitude stratosphere. We use a diurnal steady-state photochemical model to calculate profiles of HOCl for conditions encountered by a number of high-altitude balloon flights. To assess how well this model represents ozone loss by the HOCl cycle, we compare our calculations of HOCl and its precursors Cl0 and HO2 with measurements obtained by an FTIR solar absorption spectrometer (MkIV), a far-infrared emission spectrometer (FIRS-2), and a submillimetenvave limb sounder (SLS). We then evaluate these comparisons in light of a number of recent laboratory studies of the main formation mechanism of HOCl, the reaction of Cl0 + HO2. Those studies measured both the reaction rate constant and the quantum yield for a second product pathway, formation of HCl.

stratosphere↗

An Examination of the Inorganic Chlorine Budget in the Lower Stratosphere

We use the first simultaneous in situ measurements of ClONO2, ClO, and HCl acquired using the NASA ER-2 aircraft during the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) mission to test whether these three compounds quantitatively account for total inorganic chlorine (Cly) in the lower stratosphere in 1997. We find (ClO + ClONO2 + HCl)/Cly = 0.92 +/- 0.10, where Cly is inferred from in situ measurements of organic chlorine source gases. These observations are consistent with our current understanding of the budget and partitioning of Cly in the lower stratosphere. We find no evidence in support of missing inorganic chlorine species that compose a significant fraction of Cly. We apply the analysis to earlier ER-2 observations dating from 1991 to investigate possible causes of previously observed discrepancies in the inorganic chlorine budget. Using space shuttle, satellite, balloon, and aircraft measurements in combination with ER-2 data, we find that the discrepancy is unlikely to have been caused by missing chlorine species or an error in the photolysis rate of chlorine nitrate. We also find that HCl/Cly is not significantly controlled by aerosol surface area density in the lower stratosphere.

Bonne, G. P.↗

Growth of Lower Stratospheric HCl/Cly Since 1993: Observations from Aircraft (ALIAS), Balloon (MarkIV, FIRS-2), Space Shuttle (ATMOS), and Satellite (HALOE) Measurements

Measurements of HCl in the lower stratosphere (15-21 km) from aircraft, balloon, Space Shuttle, and satellite reveal a growth in its mean abundance relative to that of total inorganic chlorine (Cly) from HCl/Cly = 57(+/-5)% in early 1993 to 75(+/-7)% by the end of 1997.

HCl lower stratosphere inorganic chlorine ATMOS HA↗

Ozone Budgets from a Global Chemistry/Transport Model and Comparison to Observations from POLARIS

The objective of the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) field mission was to obtain data to better characterize the summertime seasonal decrease of ozone at mid to high latitudes. The decrease in ozone occurs mainly in the lower stratosphere and is expected to result from in situ chemical destruction. Instrumented balloons and aircraft were used in POLARIS, along with satellites, to measure ozone and chemical species which are involved with stratospheric ozone chemistry. In order to close the seasonal ozone budget, however, ozone transport must also be estimated. Comparison to a global chemistry and transport model (CTM) of the stratosphere indicates how well the summertime ozone loss processes are simulated and thus how well we can predict the ozone response to changing amounts of chemical source gases. Moreover, the model gives insight into the possible relative magnitude of transport contributions to the seasonal ozone decline. Initial comparison to the Goddard CTM, which uses transport winds and temperatures from meteorological data assimilation, shows a high ozone bias in the model and an attenuated summertime ozone loss cycle. Comparison of the model chemical partitioning and ozone catalytic loss rates to those derived from measurements shows fairly close agreement both at ER-2 altitudes (20 km) and higher. This suggests that the model transport is too active in resupplying ozone to the high latitude region, although chemistry failings cannot be completely ruled out. Comparison of ozone and related species will be shown along with a full diagnosis of the model ozone budget and its possible sources of error.

Kawa, S. Randolph↗

Smithsonian stratospheric far-infrared spectrometer and data reduction system

The Smithsonian far-infrared spectrometer (FIRS) is a remote sensing Fourier transform spectrometer that measures the mid- and far-infrared thermal emission spectrum of the stratosphere from balloon and aircraft platforms. The spectrometer has had nine successful balloon flights from 1987 to 1994, flying at float altitudes of 36 - 39 km and collecting 131 hours of midlatitude stratospheric limb spectra. The spectrometer also flew on a NASA CD-8 aircraft, as part of the second Airborne Arctic Stratospheric Expedition (AASE-2), collecting 140 hours of overhead spectra at latitudes ranging from the equator to the north pole. We present here a brief description of the instrument, a discussion of data reduction procedures, an estimation of both random and systematic errors, an outline of the procedure for retrieving mixing ratio profiles, and an explanation of the method of deriving temperature and pressure from the far- and mid-infrared spectra.

Johnson, D. G.↗

Comparison of column abundances from three infrared spectrometers during AASE 2

Three Fourier transform infrared (FTIR) spectromenters were based on board the NASA DC-8 during the second Airborne Arctic Stratospheric Expedition (AASE II) in 1992. Two FTIRs used solar absorption and one used thermal emission. We compare over 2000 measurements from these 3 FTIRs, on 12 DC-8 flights, for closely coincident air masses and times, both inside and outside the polar vortex. In the majority of cases the offset biases are quite small, in the range 1-4%, and comparable to the absolute precisions expected. In most cases the rms scatter is in the range 4-11%; this scatter is unlikely to be geophysical, but rather is probably instrumental or analytical in origin.

Traub, W. A.↗

Upper limit for stratospheric HBr using far-infrared thermal emission spectroscopy

An upper limit is measured for stratospheric HBr from three balloon flights. The observations were made with the FIRS-2 far-infrared Fourier transform spectrometer. The 1sigma upper limits from the 1988, 1989, and 1990 balloon flights are 13 pptv at 35 km, 7 pptv at 32 km, and 3 pptv at 31 km, respectively. Combining all 3 flights, the weighted average 1sigma upper limit for HBr is 4 pptv at 32 km. This value is significantly smaller than the only other previously published spectroscopic value of 20 +/- 7 pptv (2sigma), but is consistent with a theoretical estimate which predicts roughly 0.4 pptv at this altitude.

Traub, W. A.↗

Measurement of the stratospheric hydrogen peroxide concentration profile using far infrared thermal emission spectroscopy

The first unequivocal measurement of hydrogen peroxide in the stratosphere have been made, a concentration profile obtained from a balloon platform using Fourier transform thermal emission spectroscopy in the far infrared. Measurements were made using the 112/cm R-Q5 branch of the rotational-torsional spectrum, with some confirmation from the 94/cm R-Q4 branch. The volume mixing ratio of H2O2 is 1.6 x 10 to the -10th at 38.4 km, decreasing to 0.6 x 10 to the -10th at 23.8 km, with uncertainties of about 16 percent. These measurements are compared to a recent stratospheric model calculation.

Chance, K. V.↗