ALBERT

Description: This paper presents extensive {bias determination} analyses of ozone observations from the Atmospheric Chemistry Experiment (ACE) satellite instruments: the ACE Fourier Transform Spectrometer (ACE-FTS) and the Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (ACE-MAESTRO) instrument. Here we compare the latest ozone data products from ACE-FTS and ACE-MAESTRO with coincident observations from nearly 20 satellite-borne, airborne, balloon-borne and ground-based instruments, by analysing volume mixing ratio profiles and partial column densities. The ACE-FTS version 2.2 Ozone Update product reports more ozone than most correlative measurements from the upper troposphere to the lower mesosphere. At altitude levels from 16 to 44 km, the average values of the mean relative differences are nearly all within +1 to +8%. At higher altitudes (4560 km), the ACE-FTS ozone amounts are significantly larger than those of the comparison instruments, with mean relative differences of up to +40% (about +20% on average). For the ACE-MAESTRO version 1.2 ozone data product, mean relative differences are within ±10% (average values within ±6%) between 18 and 40 km for both the sunrise and sunset measurements. At higher altitudes (~3555 km), systematic biases of opposite sign are found between the ACE-MAESTRO sunrise and sunset observations. While ozone amounts derived from the ACE-MAESTRO sunrise occultation data are often smaller than the coincident observations (with mean relative differences down to −10%), the sunset occultation profiles for ACE-MAESTRO show results that are qualitatively similar to ACE-FTS, indicating a large positive bias (mean relative differences within +10 to +30%) in the 4555 km altitude range. In contrast, there is no significant systematic difference in bias found for the ACE-FTS sunrise and sunset measurements.

Description: Chemical ozone loss in the Arctic stratosphere was investigated for the twelve years between 1991 and 2003 employing the ozone-tracer correlation method. For this method, the change in the relation between ozone and a long-lived tracer is considered for all twelve years over the lifetime of the polar vortex to calculate chemical ozone loss. Both the accumulated local ozone loss in the lower stratosphere and the column ozone loss were derived consistently, mainly on the basis of HALOE satellite observations. HALOE measurements do not cover the polar region homogeneously over the course of the winter. Thus, to derive an early winter reference function for each of the twelve years, all available measurements were additionally used; for two winters climatological considerations were necessary. Moreover, a detailed quantification of uncertainties was performed. This study further demonstrates the interaction between meteorology and ozone loss. The connection between temperature conditions and chlorine activation, and in turn, the connection between chlorine activation and ozone loss, becomes obvious in the HALOE HCl measurements. Additionally, the degree of homogeneity of ozone loss within the vortex was shown to depend on the meteorological conditions. Results derived here are in general agreement with the results obtained by other methods for deducing polar ozone loss. Differences occur mainly owing to different time periods considered in deriving accumulated ozone loss. However, very strong ozone losses as deduced from SAOZ for January in winters 1993-1994 and 1995-1996 cannot be identified using available HALOE observations in the early winter. In general, strong accumulated ozone loss was found to occur in conjunction with a strong cold vortex containing a large volume of possible PSC existence (VPSC), whereas moderate ozone loss was found if the vortex was less strong and moderately warm. Hardly any ozone loss was calculated for very warm winters with small amounts of VPSC during the entire winter. This study supports the linear relationship between VPSC and the accumulated ozone loss reported by Rex et al. (2004) if VPSC was averaged over the entire winter period. Here, further meteorological factors controlling ozone loss were additionally identified if VPSC was averaged over the same time interval as that for which the accumulated ozone loss was deduced. A significant difference in ozone loss (of ≈36DU) was found due to the different duration of solar illumination of the polar vortex of at maximum 4 hours per day in the observed years. Further, the increased burden of aerosols in the atmosphere after the Pinatubo volcanic eruption in 1991 significantly increased the extent of chemical ozone loss.

Description: This paper describes a methodology for water vapor retrieval in the mesosphere-lower thermosphere (MLT) using 6.6 μm daytime broadband emissions measured by SABER, the limb scanning infrared radiometer on board the TIMED satellite. Particular attention is given to accounting for the non-local thermodynamic equilibrium (non-LTE) nature of the H2O 6.6 μm emission in the MLT. The non-LTE H2O(ν2) vibrational level populations responsible for this emission depend on energy exchange processes within the H2O vibrational system as well as on interactions with vibrationally excited states of the O2, N2, and CO2 molecules. The rate coefficients of these processes are known with large uncertainties that undermines the reliability of the H2O retrieval procedure. We developed a methodology of finding the optimal set of rate coefficients using the nearly coincidental solar occultation H2O density measurements by the ACE-FTS satellite and relying on the better signal-to-noise ratio of SABER daytime 6.6 μm measurements. From this comparison we derived an update to the rate coefficients of the three most important processes that affect the H2O(ν2) populations in the MLT: a) the vibrational-vibrational (V–V) exchange between the H2O and O2 molecules; b) the vibrational-translational (V–T) process of the O2(1) level quenching by collisions with atomic oxygen, and c) the V–T process of the H2O(010) level quenching by collisions with N2, O2, and O. Using the advantages of the daytime retrievals in the MLT, which are more stable and less susceptible to uncertainties of the radiance coming from below, we demonstrate that applying the updated H2O non-LTE model to the SABER daytime radiances makes the retrieved H2O vertical profiles in 50–85 km region consistent with climatological data and model predictions. The H2O retrieval uncertainties in this approach are about 10% at and below 70 km, 20% at 80 km, and 30% at 85 km altitude.

Description: This study focuses on the effects of polar mesospheric cloud (PMC) formation on the chemical environment of the mesosphere and lower thermosphere. Of specific interest is how the dehydration due to mesospheric ice particle formation leads to significant seasonal decreases in the atomic hydrogen near the mesopause at middle to high latitudes. Using a three-dimensional whole atmosphere coupled chemistry/dynamics model, we simulate the effects of this dehydration, and via comparisons with three data sets taken from two NASA satellites, we quantify the perturbations to atomic hydrogen and water vapor. We also identify a local ozone maximum that results from the PMC-induced decrease in atomic hydrogen. Further, the large interannual variability in the onset of the Southern Hemisphere PMC season correlates well with the interannual variability of early summer atomic hydrogen at 95 km. Since the PMC onset is known to be controlled by interannual variations in the Southern Hemisphere stratospheric polar vortex, this correlation indicates a coupling between the stratosphere and the chemistry of the mesosphere and lower thermosphere. Finally, our model results suggest that the seasonal biteout in atomic hydrogen propagates up into the thermosphere and to lower latitudes. This raises the intriguing possibility that PMC formation might play a role in modulating the escape of hydrogen from the atmosphere. ©2018. American Geophysical Union. All Rights Reserved.

Description: We describe the publicly available dataset from the Global OZone Chemistry And Related Datasets for the Stratosphere (GOZCARDS) project, and provide some results, with a~focus on hydrogen chloride (HCl), water vapor (H2O), and ozone (O3). This dataset is a global long-term stratospheric Earth System Data Record (ESDR), 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 ACE-FTS on SCISAT. We examine consistency aspects between the various datasets. To merge ozone records, the time series are debiased by calculating average offsets with respect to SAGE II during periods of measurement overlap, whereas for other species, the merging derives from an averaging procedure based on overlap periods. The GOZCARDS files contain mixing ratios on a common pressure/latitude grid, as well as standard errors and other diagnostics; we also present estimates of systematic uncertainties in the merged products. Monthly mean temperatures for GOZCARDS were also produced, based directly on data from the Modern-Era Retrospective analysis for Research and Applications (MERRA). The GOZCARDS HCl merged product comes from HALOE, ACE-FTS and (for the lower stratosphere) Aura MLS data. After a~rapid rise in upper stratospheric HCl in the early 1990s, the rate of decrease in this region for 1997–2010 was between 0.4 and 0.7% yr−1. On shorter timescales (6 to 8 years), the rate of decrease peaked in 2004–2005 at about 1% yr−1, and has since levelled off, at ~0.5 yr−1. With a delay of 6–7 years, these changes roughly follow total surface chlorine, whose behavior vs. time arises from inhomogeneous changes in the source gases. Since the late 1990s, HCl decreases in the lower stratosphere have occurred with pronounced latitudinal variability at rates sometimes exceeding 1–2 yr−1. There has been a significant reversal in the changes of lower stratospheric HCl abundances and columns for 2005–2010, in particular at northern midlatitudes and in the deep tropics, where short-term increases are observed. However, lower stratospheric HCl tendencies appear to be reversing after about 2011, with (short-term) decreases at northern midlatitudes and some increasing tendencies at southern midlatitudes. For GOZCARDS H2O, covering the stratosphere and mesosphere, the same instruments as for HCl are used, along with UARS MLS stratospheric H2O data (1991–1993). We display seasonal to decadal-type variability in H2O from 22 years of data. In the upper mesosphere, the anti-correlation between H2O and solar flux is now clearly visible over two full solar cycles. Lower stratospheric tropical H2O has exhibited two periods of increasing values, followed by fairly sharp drops, the well-documented 2000–2001 decrease, and another recent decrease in 2011–2013. Tropical decadal variability peaks just above the tropopause. Between 1991 and 2013, both in the tropics and on a near-global basis, H2O has decreased by ~ 5–10% in the lower stratosphere, but about a 10% increase is observed in the upper stratosphere and lower mesosphere. However, recent tendencies may not hold for the long-term, and the addition of a few years of data can significantly modify trend results. For ozone, we used SAGE I, SAGE II, HALOE, UARS and Aura MLS, and ACE-FTS data to produce a~merged record from late 1979 onward, using SAGE II as the primary reference for aligning (debiasing) the other datasets. Other adjustments were needed in the upper stratosphere to circumvent temporal drifts in SAGE II O3 after June 2000, as a result of the (temperature-dependent) data conversion from a density/altitude to a mixing ratio/pressure grid. Unlike the 2 to 3% increase in near-global column ozone after the late 1990s reported by some, GOZCARDS stratospheric column O3 values do not show a recent upturn of more than 0.5 to 1%; continuing studies of changes in global ozone profiles, as well as ozone columns, are warranted. A brief mention is also made of other currently available, commonly-formatted GOZCARDS satellite data records for stratospheric composition, namely those for N2O and HNO3.

Description: Measurement of atmospheric temperature as a function of pressure, T(P), is key to understanding many atmospheric processes and a prerequisite for retrieving gas mixing ratios and other parameters from solar occultation measurements. This paper gives a brief overview of the solar occultation measurement technique followed by a detailed discussion of the mechanisms that make the measurement sensitive to temperature. Methods for retrieving T(P) using both broadband transmittance and refraction are discussed. Investigations using measurements of broadband transmittance in two CO2 absorption bands (the 4.3 and 2.7 μm bands) and refractive bending are then presented. These investigations include sensitivity studies, simulated retrieval studies, and examples from SOFIE.

Description: SCIAMACHY limb scatter ozone profiles from 2002 to 2008 have been compared with MLS (2005–2008), SABER (2002–2008), SAGE II (2002–2005), HALOE (2002–2005) and ACE-FTS (2004–2008) measurements. The comparison is performed for global zonal averages and heights from 10 to 50 km in one km steps. The validation was performed by comparing monthly mean zonal means and by comparing averages over collocated profiles within a zonal band and month. Both approaches yield similar results. For most of the stratosphere SCIAMACHY agrees to within 10 % or better with other correlative data. A systematic bias of SCIAMACHY ozone of up to 100 % between 10 and 20 km in the tropics points to some remaining issues with regard to convective cloud interference. Statistical hypothesis testing reveals at which altitudes and in which region differences between SCIAMACHY and other satellite data are statistically significant. We also estimated linear trends from monthly mean data for different periods where SCIAMACHY has common observations with other satellite data using a classical trend model with QBO and seasonal terms in order to draw conclusions on potential instrumental drifts as a function of latitude and altitude. SCIAMACHY exhibits a statistically significant negative trend in the range of of about 1–3 % per year depending on latitude during the period 2002–2005 (overlapping with HALOE and SAGE II) and somewhat less during 2002–2008 (overlapping with SABER) in the altitude range of 30–40 km, while in the period 2004–2008 (overlapping with MLS and ACE-FTS) no significant trends are observed. The statistically significant negative trends only observed with SCIAMACHY data point at some residual effects from errors in the tangent height registration.