ALBERT

Description: This article presents our implementation of a non-LTE solver in spherical symmetry for molecular rotational transition in static or expanding atmospheres. The new open-source code relies on the Gauss–Seidel Accelerated Lambda Iteration methodology that provides a rapid and accurate convergence of the non-LTE problems, which is now routinely used in astrophysical and planetary research. The non-LTE code is interfaced with the widely used package, the Atmospheric Radiative Transfer Simulator (ARTS), to facilitate spectral line simulations for various viewing geometries. In this paper we describe the numerical implementation, provide the first validation results for the populations against two other non-LTE codes, and then discuss the possible application. The quantitative comparisons are performed using an established ortho-water non-LTE model applied to cases of optical thick and thin conditions of Ganymede’s atmosphere. The differences in populations expressed as excitation temperatures show very good agreement in both cases. Finally, we also apply this model to a sample of data from the Microwave Instrument for the Rosetta Orbiter (MIRO) instrument. The new non-LTE package is demonstrated to be fast and accurate, and we hope that it will be a useful addition to the planetary community. In addition, being open source and part of the ARTS, it will be further improved and developed.

Description: Hydrogen chloride (HCl) and hydrogen fluoride (HF) are respectively the main chlorine and fluorine reservoirs in the Earth's stratosphere. Their buildup resulted from the intensive use of man-made halogenated source gases, in particular CFC-11 (CCl3F) and CFC-12 (CCl2F2), during the second half of the 20th century. It is important to continue monitoring the evolution of these source gases and reservoirs, in support of the Montreal Protocol and also indirectly of the Kyoto Protocol. The Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) is a space-based instrument that has been performing regular solar occultation measurements of over 30 atmospheric gases since early 2004. In this validation paper, the HCl, HF, CFC-11 and CFC-12 version 2.2 profile data products retrieved from ACE-FTS measurements are evaluated. Volume mixing ratio profiles have been compared to observations made from space by MLS and HALOE, and from stratospheric balloons by SPIRALE, FIRS-2 and Mark-IV. Partial columns derived from the ACE-FTS data were also compared to column measurements from ground-based Fourier transform instruments operated at 12 sites. ACE-FTS data recorded from March 2004 to August 2007 have been used for the comparisons. These data are representative of a variety of atmospheric and chemical situations, with sounded air masses extending from the winter vortex to summer sub-tropical conditions. Typically, the ACE-FTS products are available in the 10–50 km altitude range for HCl and HF, and in the 7–20 and 7–25 km ranges for CFC-11 and CFC-12, respectively. For both reservoirs, comparison results indicate an agreement generally better than 5–10%, when accounting for the known offset affecting HALOE measurements of HCl and HF. Larger positive differences are however found for comparisons with single profiles from FIRS-2 and SPIRALE. For CFCs, the few coincident measurements available suggest that the differences probably remain within ±20%.

Description: The Atmospheric Chemistry Experiment (ACE) satellite was launched on 12 August 2003. Its two instruments measure vertical profiles of over 30 atmospheric trace gases by analyzing solar occultation spectra in the ultraviolet/visible and infrared wavelength regions. The reservoir gases HNO3, ClONO2, and N2O5 are three of the key species provided by the primary instrument, the ACE Fourier Transform Spectrometer (ACE-FTS). This paper describes the ACE-FTS version 2.2 data products, including the N2O5 update, for the three species and presents validation comparisons with available observations. We have compared volume mixing ratio (VMR) profiles of HNO3, ClONO2, and N2O5 with measurements by other satellite instruments (SMR, MLS, MIPAS), aircraft measurements (ASUR), and single balloon-flights (SPIRALE, FIRS-2). Partial columns of HNO3 and ClONO2 were also compared with measurements by ground-based Fourier Transform Infrared (FTIR) spectrometers. Overall the quality of the ACE-FTS v2.2 HNO3 VMR profiles is good from 18 to 35 km. For the statistical satellite comparisons, the mean absolute differences are generally within ±1 ppbv (±20%) from 18 to 35 km. For MIPAS and MLS comparisons only, mean relative differences lie within ±10% between 10 and 36 km. ACE-FTS HNO3 partial columns (~15–30 km) show a slight negative bias of −1.3% relative to the ground-based FTIRs at latitudes ranging from 77.8° S–76.5° N. Good agreement between ACE-FTS ClONO2 and MIPAS, using the Institut für Meteorologie und Klimaforschung and Instituto de Astrofísica de Andalucía (IMK-IAA) data processor is seen. Mean absolute differences are typically within ±0.01 ppbv between 16 and 27 km and less than +0.09 ppbv between 27 and 34 km. The ClONO2 partial column comparisons show varying degrees of agreement, depending on the location and the quality of the FTIR measurements. Good agreement was found for the comparisons with the midlatitude Jungfraujoch partial columns for which the mean relative difference is 4.7%. ACE-FTS N2O5 has a low bias relative to MIPAS IMK-IAA, reaching −0.25 ppbv at the altitude of the N2O5 maximum (around 30 km). Mean absolute differences at lower altitudes (16–27 km) are typically −0.05 ppbv for MIPAS nighttime and ±0.02 ppbv for MIPAS daytime measurements.

Description: This paper presents extensive validation 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. The ACE satellite instruments operate in the mid-infrared and ultraviolet-visible-near-infrared spectral regions using the solar occultation technique. In order to continue the long-standing record of solar occultation measurements from space, a detailed quality assessment is required to evaluate the ACE data and validate their use for scientific purposes. Here we compare the latest ozone data products from ACE-FTS and ACE-MAESTRO with coincident observations from 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 mean differences range generally between 0 and +10% with a slight but systematic positive bias (typically +5%). At higher altitudes (45–60 km), the ACE-FTS ozone amounts are significantly larger than those of the comparison instruments by up to ~40% (typically +20%). For the ACE-MAESTRO version 1.2 ozone data product, agreement within ±10% (generally better than ±5%) is found between 18 and 40 km for the sunrise and sunset measurements. At higher altitudes (45–55 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 (by as much as −10%), the sunset occultation profiles for ACE-MAESTRO show results that are qualitatively similar to ACE-FTS and indicate a large positive bias (+10 to +30%) in this altitude range. In contrast, there is no significant difference in bias found for the ACE-FTS sunrise and sunset measurements. These systematic effects in the ozone profiles retrieved from the measurements of ACE-FTS and ACE-MAESTRO are being investigated. This work shows that the ACE instruments provide reliable, high quality measurements from the tropopause to the upper stratosphere and can be used with confidence in this vertical domain.

Description: We estimate the concentration changes, caused by a single streamer in sprites, of ozone and related minor species as odd nitrogen (NOx) and hydrogen (HOx) families in the upper stratosphere and mesosphere. The streamer has an intense electric field and high electron density at its head where a large number of chemically-radical ions and atoms are produced through electron impact on neutral molecules. After propagation of the streamer, the densities of minor species can be perturbed through ion-neutral chemical reactions initiated by the relaxation of these radical products. We evaluate the production rates of ions and atoms using electron kinetics model and assuming the electric field and electron density in the streamer head. We calculate the density variations mainly for NOx, Ox, and HOx species using a one-dimensional model of the neutral and ion composition of the middle atmosphere, including the effect of the sprite streamer. Results at the nighttime condition show that the densities of NO, O3, H, and OH increase suddenly through reactions triggered by firstly produced atomic nitrogen and oxygen, and electrons just after streamer initiation. It is shown that NO and NO2 still remain for 1 h by a certain order of increase with their source-sink balance predominantly around 60 km; for other species, increases in O3, OH, HO2, and H2O2 still remain in the range of 40–70 km. From this affirmative result of long time behavior previously not presented, we emphasize that sprites would have a power to impact on local chemistry at night. We also discuss comparison with previous studies and suggestion for satellite observations.

Description: It is important to obtain the year-to-year trend of stratospheric minor species in the context of global changes. An important example is the trend in global ozone depletion. The purpose of this paper is to report the accuracy and precision of measurements of stratospheric chemical species that are made at our Poker Flat site in Alaska (65° N, 147° W). Since 1999, minor atmospheric molecules have been observed using a Fourier-Transform solar-absorption infrared Spectrometer (FTS) at Poker Flat. Vertical profiles of the abundances of ozone, HNO3, HCl, and HF for the period from 2001 to 2003 were retrieved from the FTS spectra by using Rodgers' formulation of the Optimal Estimation Method (OEM). The accuracy and precision of the retrievals were estimated by formal error analysis. Errors for the total column were estimated to be 5.3%, 3.4%, 5.9%, and 5.3% for ozone, HNO3, HCl, and HF, respectively. The ozone vertical profiles were in good agreement with profiles derived from collocated ozonesonde measurements that were smoothed with averaging kernel functions that had been obtained with the retrieval procedure used in the analysis of spectra from the ground-based FTS (gb-FTS). The O3, HCl, and HF columns that were retrieved from the FTS measurements were consistent with Earth Probe/Total Ozone Mapping Spectrometer (TOMS) and HALogen Occultation Experiment (HALOE) data over Alaska within the error limits of all the respective datasets. This is the first report from the Poker Flat FTS observation site on a number of stratospheric gas profiles including a comprehensive error analysis.

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 (45–60 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 (~35–55 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 45–55 km altitude range. In contrast, there is no significant systematic difference in bias found for the ACE-FTS sunrise and sunset measurements.

Description: The diurnal variation of HOCl and the related species ClO, HO2 and HCl measured by satellites has been compared with the results of a one-dimensional photochemical model. The study compares the data from various limb-viewing instruments with model simulations from the middle stratosphere to the lower mesosphere. Data from three sub-millimetre instruments and two infrared spectrometers are used, namely from the Sub-Millimetre Radiometer (SMR) on board Odin, the Microwave Limb Sounder (MLS) on board Aura, the Superconducting Submillimeter-wave Limb-Emission Sounder (SMILES) on the International Space Station, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on board ENVISAT, and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on board SCISAT. Inter-comparison of the measurements from instruments on sun-synchronous satellites (SMR, MLS, MIPAS) and measurements from solar occultation instruments (ACE-FTS) is challenging since the measurements correspond to different solar zenith angles (or local times). However, using a model which covers all solar zenith angles and data from the SMILES instrument which measured at all local times over a period of several months provides the possibility to verify the model and to indirectly compare the diurnally variable species. The satellite data were averaged for latitudes of 20° S to 20° N for the SMILES observation period from November 2009 to April 2010 and were compared at three altitudes: 35, 45 and 55 km. Besides presenting the SMILES data, the study also shows a first comparison of the latest MLS data (version 3.3) of HOCl, ClO, and HO2 with other satellite observations, as well as a first evaluation of HO2 observations made by Odin/SMR. The MISU-1D model has been carefully initialised and run for conditions and locations of the observations. The diurnal cycle features for the species investigated here are generally well reproduced by the model. The satellite observations and the model agree well in terms of absolute mixing ratios. The differences between the day and night values of the model are in good agreement with the observations although the amplitude of the HO2 diurnal variation is 10–20% lower in the model than in the observations. In particular, the data offered the opportunity to study the reaction ClO+HO2 → HOCl+O2 in the lower mesosphere at 55 km. At this altitude the HOCl night-time variation depends only on this reaction. The result of this analysis points towards a value of the rate constant within the range of the JPL 2006 recommendation and the upper uncertainty limit of the JPL 2011 recommendation at 55 km.

Description: It is important to obtain the year-to-year trend of stratospheric minor species in the context of global changes. An important example is the trend in global ozone depletion. The purpose of this paper is to report the accuracy and precision of measurements of stratospheric chemical species that are made at our Poker Flat site in Alaska (65° N, 147° W). Since 1999, minor atmospheric molecules have been observed using a Fourier-Transform solar-absorption infrared Spectrometer (FTS) at Poker Flat. Vertical profiles of the abundances of ozone, HNO3, HCl, and HF for the period from 2001 to 2003 were retrieved from FTS spectra using Rodgers' formulation of the Optimal Estimation Method (OEM). The accuracy and precision of the retrievals were estimated by formal error analysis. Errors for the total column were estimated to be 5.3%, 3.4%, 5.9%, and 5.3% for ozone, HNO3, HCl, and HF, respectively. The ozone vertical profiles were in good agreement with profiles derived from collocated ozonesonde measurements that were smoothed with averaging kernel functions that had been obtained with the retrieval procedure used in the analysis of spectra from the ground-based FTS (gb-FTS). The O3, HCl, and HF columns that were retrieved from the FTS measurements were consistent with Earth Probe/Total Ozone Mapping Spectrometer (TOMS) and HALogen Occultation Experiment (HALOE) data over Alaska within the error limits of all the respective datasets. This is the first report from the Poker Flat FTS observation site on a number of stratospheric gas profiles including a comprehensive error analysis.