The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), on-board the European ENVIronmental SATellite (ENVISAT) launched on 1 March 2002, is a middle infrared Fourier Transform spectrometer measuring the atmospheric emission spectrum in limb sounding geometry. The instrument is capable to retrieve the vertical distribution of temperature and trace gases, aiming at the study of climate and atmospheric chemistry and dynamics, and at applications to data assimilation and weather forecasting. MIPAS operated in its standard observation mode for approximately two years, from July 2002 to March 2004, with scans performed at nominal spectral resolution of 0.025 cm⁻¹ and covering the altitude range from the mesosphere to the upper troposphere with relatively high vertical resolution (about 3 km in the stratosphere). Only reduced spectral resolution measurements have been performed subsequently. MIPAS data were re-processed by ESA using updated versions of the Instrument Processing Facility (IPF v4.61 and v4.62) and provided a complete set of level-2 operational products (geo-located vertical profiles of temperature and volume mixing ratio of H₂O, O₃, HNO₃, CH₄, N₂O and NO₂) with quasi continuous and global coverage in the period of MIPAS full spectral resolution mission. In this paper, we report a detailed description of the validation of MIPAS-ENVISAT operational ozone data, that was based on the comparison between MIPAS v4.61 (and, to a lesser extent, v4.62) O₃ VMR profiles and a comprehensive set of correlative data, including observations from ozone sondes, ground-based lidar, FTIR and microwave radiometers, remote-sensing and in situ instruments on-board stratospheric aircraft and balloons, concurrent satellite sensors and ozone fields assimilated by the European Center for Medium-range Weather Forecasting. A coordinated effort was carried out, using common criteria for the selection of individual validation data sets, and similar methods for the comparisons. This enabled merging the individual results from a variety of independent reference measurements of proven quality (i.e. well characterized error budget) into an overall evaluation of MIPAS O₃ data quality, having both statistical strength and the widest spatial and temporal coverage. Collocated measurements from ozone sondes and ground-based lidar and microwave radiometers of the Network for the Detection Atmospheric Composition Change (NDACC) were selected to carry out comparisons with time series of MIPAS O₃ partial columns and to identify groups of stations and time periods with a uniform pattern of ozone differences, that were subsequently used for a vertically resolved statistical analysis. The results of the comparison are classified according to synoptic and regional systems and to altitude intervals, showing a generally good agreement within the comparison error bars in the upper and middle stratosphere. Significant differences emerge in the lower stratosphere and are only partly explained by the larger contributions of horizontal and vertical smoothing differences and of collocation errors to the total uncertainty. Further results obtained from a purely statistical analysis of the same data set from NDACC ground-based lidar stations, as well as from additional ozone soundings at middle latitudes and from NDACC ground-based FTIR measurements, confirm the validity of MIPAS O₃ profiles down to the lower stratosphere, with evidence of larger discrepancies at the lowest altitudes. The validation against O₃ VMR profiles using collocated observations performed by other satellite sensors (SAGE II, POAM III, ODIN-SMR, ACE-FTS, HALOE, GOME) and ECMWF assimilated ozone fields leads to consistent results, that are to a great extent compatible with those obtained from the comparison with ground-based measurements. Excellent agreement in the full vertical range of the comparison is shown with respect to collocated ozone data from stratospheric aircraft and balloon instruments, that was mostly obtained in very good spatial and temporal coincidence with MIPAS scans. This might suggest that the larger differences observed in the upper troposphere and lowermost stratosphere with respect to collocated ground-based and satellite O₃ data are only partly due to a degradation of MIPAS data quality. They should be rather largely ascribed to the natural variability of these altitude regions and to other components of the comparison errors. By combining the results of this large number of validation data sets we derived a general assessment of MIPAS v4.61 and v4.62 ozone data quality. A clear indication of the validity of MIPAS O₃ vertical profiles is obtained for most of the stratosphere, where the mean relative difference with the individual correlative data sets is always lower than ±10%. Furthermore, these differences always fall within the combined systematic error (from 1 hPa to 50 hPa) and the standard deviation is fully consistent with the random error of the comparison (from 1 hPa to ~30–40 hPa). A degradation in the quality of the agreement is generally observed in the lower stratosphere and upper troposphere, with biases up to 25% at 100 hPa and standard deviation of the global mean differences up to three times larger than the combined random error in the range 50–100 hPa. The larger differences observed at the bottom end of MIPAS retrieved profiles can be associated, as already noticed, to the effects of stronger atmospheric gradients in the UTLS that are perceived differently by the various measurement techniques. However, further components that may degrade the results of the comparison at lower altitudes can be identified as potentially including cloud contamination, which is likely not to have been fully filtered using the current settings of the MIPAS cloud detection algorithm, and in the linear approximation of the forward model that was used for the a priori estimate of systematic error components. The latter, when affecting systematic contributions with a random variability over the spatial and temporal scales of global averages, might result in an underestimation of the random error of the comparison and add up to other error sources, such as the possible underestimates of the p and T error propagation based on the assumption of a 1 K and 2% uncertainties, respectively, on MIPAS temperature and pressure retrievals. At pressure lower than 1 hPa, only a small fraction of the selected validation data set provides correlative ozone data of adequate quality and it is difficult to derive quantitative conclusions about the performance of MIPAS O₃ retrieval for the topmost layers.

Deep convection in the Asian summer monsoon is a significant transport process for lifting pollutants from the planetary boundary layer to the tropopause level. This process enables efficient injection into the stratosphere of reactive species such as chlorinated very short-lived substances (Cl-VSLSs) that deplete ozone. Past studies of convective transport associated with the Asian summer monsoon have focused mostly on the south Asian summer monsoon. Airborne observations reported in this work identify the East Asian summer monsoon convection as an effective transport pathway that carried record-breaking levels of ozone-depleting Cl-VSLSs (mean organic chlorine from these VSLSs ~500 ppt) to the base of the stratosphere. These unique observations show total organic chlorine from VSLSs in the lower stratosphere over the Asian monsoon tropopause to be more than twice that previously reported over the tropical tropopause. Considering the recently observed increase in Cl-VSLS emissions and the ongoing strengthening of the East Asian summer monsoon under global warming, our results highlight that a reevaluation of the contribution of Cl-VSLS injection via the Asian monsoon to the total stratospheric chlorine budget is warranted.

The second Radiative Heating in Underexplored Bands Campaign (RHUBC‐II) was conducted in 2009 by the U.S. Department of Energy Atmospheric Radiation Measurement program to improve water vapor spectroscopy in the far‐infrared spectral region. RHUBC‐II was located in an extremely dry region of Chile to ensure very low opacities in this spectral region. Spectrally resolved measurements by a far‐infrared spectrometer and a submillimeter interferometer from RHUBC‐II are compared with line‐by‐line radiative transfer model calculations. Water vapor amounts and temperatures used in the calculations come from collocated radiosondes, with extensive adjustments to correct for issues due to the campaign's dry conditions and mountainous terrain. A reanalysis is also performed of far‐infrared measurements taken at the Atmospheric Radiation Measurement North Slope of Alaska site before and during the first RHUBC campaign. These analyses determine that differences between the measurements and model calculations using existing spectroscopic parameters are significant in the far‐infrared and submillimeter regions, leading to the derivation of improved water vapor continuum absorption coefficients and air‐broadened widths of 74 water vapor lines. The foreign continuum is increased by more than 50% in part of the far‐infrared and the widths of more than 20 lines are changed by more than 10%. The uncertainty in the foreign continuum coefficients is estimated as greater than 20% in some spectral regions, primarily a consequence of the uncertainty in the specification of water vapor. The improved far‐infrared spectroscopic parameters have a notable impact on calculated spectral radiances and a modest impact on broadband radiative fluxes and heating rates.

We report the most accurate measurement of the helium fine structure splitting. The $2{}_{}{}^3{}_{}{}^{}P_0^{}{}_{}{}^{}-2{}_{}{}^3{}_{}{}^{}P_1^{}{}_{}{}^{}$ energy splitting is $29616949.7\pm 2.0\mathrm{kHz}$. Laser saturation spectroscopy, heterodyne pure frequency determination, and fluorescence detection were combined in a novel experimental approach. The absence of external perturbing magnetic fields, used in earlier experiments, lends confidence to our determined value and allows us to discriminate between contradictory results previously reported. This result, when combined with expected advances in theory, should yield a new value of the fine structure $\alpha$, which may help clarify a presently puzzling experimental situation.

Water vapor and clouds are among the most important greenhouse components whose radiative features cover all the broad spectral range of the thermal emission of the atmosphere. Typically more than 40% of the total thermal emission of Earth occurs in the far-infrared (FIR) spectral region from 100 to 667 cm−1 (wavelengths from 100 to 15 µm). Nevertheless, this spectral region has not ever been fully covered down to 100 cm−1 by space missions, and only a few ground-based experiments exist because of the difficulty of performing measurements from high altitude and very dry locations where the atmosphere is sufficiently transparent to observe the FIR emission features. To cover this lack of observations, the Italian experiment “Radiative Properties of Water Vapor and Clouds in Antarctica” has collected a 2-yr dataset of spectral measurements of the radiance emitted by the atmosphere and by clouds, such as cirrus and polar stratospheric clouds, from 100 to 1,400 cm−1 (100–7 µm of wavelength), including the underexplored FIR region, along with polarization-sensitive lidar observations, daily radiosondes, and other ancillary information to characterize the atmosphere above the site. Measurements have been performed almost continuously with a duty cycle of 6 out of 9 h, from the Italian–French base of Concordia at Dome C over the Antarctic Plateau at 3,230 m MSL, in all-sky conditions since 2012. Because of the uniqueness of the observations, this dataset will be extremely valuable for evaluating the accuracy of atmospheric absorption models (both gas and clouds) in the underexplored FIR and to detect possible daily, seasonal, and annual climate signatures.

The ENVISAT validation programme for the atmospheric instruments MIPAS, SCIAMACHY and GOMOS is based on a number of balloon-borne, aircraft, satellite and ground-based correlative measurements. In particular the activities of validation scientists were coordinated by ESA within the ENVISAT Stratospheric Aircraft and Balloon Campaign or ESABC. As part of a series of similar papers on other species [this issue] and in parallel to the contribution of the individual validation teams, the present paper provides a synthesis of comparisons performed between MIPAS CH₄ and N₂O profiles produced by the current ESA operational software (Instrument Processing Facility version 4.61 or IPF v4.61, full resolution MIPAS data covering the period 9 July 2002 to 26 March 2004) and correlative measurements obtained from balloon and aircraft experiments as well as from satellite sensors or from ground-based instruments. In the middle stratosphere, no significant bias is observed between MIPAS and correlative measurements, and MIPAS is providing a very consistent and global picture of the distribution of CH₄ and N₂O in this region. In average, the MIPAS CH₄ values show a small positive bias in the lower stratosphere of about 5%. A similar situation is observed for N₂O with a positive bias of 4%. In the lower stratosphere/upper troposphere (UT/LS) the individual used MIPAS data version 4.61 still exhibits some unphysical oscillations in individual CH₄ and N₂O profiles caused by the processing algorithm (with almost no regularization). Taking these problems into account, the MIPAS CH₄ and N₂O profiles are behaving as expected from the internal error estimation of IPF v4.61 and the estimated errors of the correlative measurements.