T. Sugita

Denitrification observed inside the Arctic vortex in February 1995

Balloon-borne in situ measurements of total reactive nitrogen (NO,,) and nitrous oxide (N 2 O) were made from Kiruna (68°N, 21°E), Sweden on February 11, 1995. Ten hours later, N 2 O was again measured by an infrared spectrometer flown on another balloon launched from Kiruna. Both observations were made inside the polar vortex between 380 K (∼14 km) and at least 675 K (∼26 km). In the winter of 1994-1995, temperatures at 475 K (∼19 km) inside the vortex were extremely low, sometimes lower than ice frost point, especially from mid-December to mid-January. The NO y profiles obtained during both the ascent and descent revealed layered structures between 15 and 20 km with mixing ratios ranging from 2.7 to 9.3 parts per billion by volume (ppbv). The observed N 2 O profiles indicate significant downward transport of air due to diabatic cooling in the winter. To quantify the degree of irreversible removal of NO y (denitrification) between 12 and 28 km, the unperturbed values of NO y (i.e., NO * y ) were estimated from the observed N 2 O values using the NO y - N 2 O relationship obtained at midlatitudes by the atmospheric trace molecule spectroscopy ATLAS mission and in situ aircraft and balloon-borne measurements. The largest denitrification was observed at 19± 0.5 km, where the NO y values were lower than the NO * y values by ∼10 ppbv, corresponding to a 70% removal of NO y . In spite of the large uncertainty in NO * y the NO y values generally agreed well with the NO * y values at ∼14 km as well as between 3 and 28 km. The relationship between NO,, and N 2 O measured between 23 and 28 km agreed with that measured above 40 km at northern midlatitudes in fall, indicating that the air masses sampled at 23-28 km over Kiruna were transported from the midlatitude upper stratosphere followed by the descent inside the vortex.

NOy-N2O correlation observed inside the Arctic vortex in February 1997: Dynamical and chemical effects

Simultaneous balloon-borne in situ measurements of total reactive nitrogen (NO ) and nitrous oxide (N 2 O) were made up to 29 km over Kiruna, Sweden (68°N, 21°E) on February 10 and 25, 1997. Kiruna was located at the edge or inside of the Arctic vortex at potential temperatures between 475 (∼19 km) and 675 K (∼26 km). Below 500 K (∼21 km) the N 2 O values were >120 ppbv on both days, and the observed NO mixing ratios agreed well with those calculated using the NO y -N 2 O correlation previously obtained at northern midlatitudes. An exception was a sharp dip in NO at 445 K (18.4 km) observed on February 25. Back trajectory analyses indicate that this layer had experienced cold temperatures close to ice saturation, i.e., favorable conditions for denitrification. Between 500 and 600 K (∼24 km) the N 2 O values were <120 ppbv, and the observed NO y values were some 4-6 ppbv lower than those calculated using the midlatitude NO y -N 2 O correlation, which includes the NO reduction due to the N + NO reaction. The temperatures in the Arctic winter above 55 K were too high to cause extensive denitrification. The combined processes of (1) diabatic descent and (2) quasi-horizontal mixing of vortex air are likely causes of the anomalous NO y -N 2 O correlation. The CH 4 -N 2 O correlation obtained inside the Arctic vortex in February 1997 also supports this hypothesis. A similar anomalous NO y -N 2 O correlation was observed from the ER-2 measurements and from the atmospheric trace molecule spectroscopy ATLAS 2 measurements made inside the vortex in the winters of 1991-1992 and 1992-1993.

Odin/SMR limb observations of stratospheric trace gases: Validation of N2O

The Sub-Millimetre Radiometer (Odin/SMR) on board the Odin satellite, launched on 20 February 2001, performs regular measurements of the global distribution of stratospheric nitrous oxide (N2O) using spectral observations of the J = 20R 19 rotational transition centered at 502.296 GHz. We present a quality assessment for the retrieved N2O profiles (level 2 product) by comparison with independent balloonborne and aircraftborne validation measurements as well as by cross-comparing with preliminary results from other satellite instruments. An agreement with the airborne validation experiments within 28 ppbv in terms of the root mean square (RMS) deviation is found for all SMR data versions (v222, v223, and v1.2) under investigation. More precisely, the agreement is within 19 ppbv for N2O volume mixing ratios (VMR) lower than 200 ppbv and within 10% for mixing ratios larger than 150 ppbv. Given the uncertainties due to atmospheric variability inherent to such comparisons, these values should be interpreted as upper limits for the systematic error of the Odin/SMR N2O measurements. Odin/SMR N2O mixing ratios are systematically slightly higher than nonvalidated data obtained from the Improved Limb Atmospheric Spectrometer-II (ILAS-II) on board the Advanced Earth Observing Satellite-II (ADEOS-II). Root mean square deviations are generally within 23 ppbv (or 20% for VMR-N2O > 100 ppbv) for versions 222 and 223. The comparison with data obtained from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on the Envisat satellite yields a good agreement within 9-17 ppbv (or 10% for VMR-N2O > 100 ppbv) for the same data versions. Odin/SMR version 1.2 data show somewhat larger RMS deviations and a higher positive bias.

Ozone profiles in the high-latitude stratosphere and lower mesosphere measured by the Improved Limb Atmospheric Spectrometer (ILAS)-II: comparison with other satellite sensors and ozonesondes

A solar occultation sensor, the Improved Limb Atmospheric Spectrometer (ILAS)-II, measured 5890 vertical profiles of ozone concentrations in the stratosphere and lower mesosphere and of other species from January to October 2003. The measurement latitude coverage was 54–71°N and 64–88°S, which is similar to the coverage of ILAS (November 1996 to June 1997). One purpose of the ILAS-II measurements was to continue such high-latitude measurements of ozone and its related chemical species in order to help accurately determine their trends. The present paper assesses the quality of ozone data in the version 1.4 retrieval algorithm, through comparisons with results obtained from comprehensive ozonesonde measurements and four satellite-borne solar occultation sensors. In the Northern Hemisphere (NH), the ILAS-II ozone data agree with the other data within ±10% (in terms of the absolute difference divided by its mean value) at altitudes between 11 and 40 km, with the median coincident ILAS-II profiles being systematically up to 10% higher below 20 km and up to 10% lower between 21 and 40 km after screening possible suspicious retrievals. Above 41 km, the negative bias between the NH ILAS-II ozone data and the other data increases with increasing altitude and reaches 30% at 61–65 km. In the Southern Hemisphere, the ILAS-II ozone data agree with the other data within ±10% in the altitude range of 11–60 km, with the median coincident profiles being on average up to 10% higher below 20 km and up to 10% lower above 20 km. Considering the accuracy of the other data used for this comparative study, the version 1.4 ozone data are suitably used for quantitative analyses in the high-latitude stratosphere in both the Northern and Southern Hemisphere and in the lower mesosphere in the Southern Hemisphere.

Longitudinally Dependent Ozone Increase in the Antarctic Polar Vortex Revealed by Balloon and Satellite Observations

The horizontal structure of processes causing increases in ozone in the Antarctic polar vortex was examined using data measured in 2003 from an ozonesonde observation campaign at Syowa Station (39.68E, 69.08S) and from the Improved Limb Atmospheric Spectrometer II (ILAS-II) onboard the Advanced Earth Observing Satellite II. The ILAS-II data are daily and distributed uniformly at 14 points in the zonal direction, mostly at polar latitudes. The Antarctic ozone hole that developed in 2003 was one of the largest recorded. The period of focus in this study is 26 September through 24 October, when a strong polar vortex was situated in the stratosphere. An ozone mixing ratio contour (1.0 ppmv) moved downward near a height of 20 km during the period of focus. This increase in ozone is likely to result from downward transport of ozone-rich air originating from lower latitudes by Brewer‐Dobson circulation. First, the descent rate of the mixing ratio contour was estimated by taking the geometric height as the vertical coordinate for the deep vortex interior around 20 km. A significant longitudinal dependence was observed. An analysis using ECMWF operational data shows that this dependence can be approximately explained by longitudinally dependent vertical movements of the isentropes caused by a zonal wavenumber-1 quasi-stationary planetary wave with amplitude and phases varying on a seasonal time scale. Next, the descent rate was calculated around 500 K (around 20 km) by taking the potential temperature (isentrope) as the vertical coordinate. The longitudinal dependence was still present using this coordinate, meaning that the ozone mixing ratio and its increase are not constant on the isentropic layer even in the interior of the polar vortex. A backward trajectory analysis showed that air parcels with large ozone mixing ratios were mostly transported from the polar vortex boundary region. This result suggests that lateral transport/mixing is important even before the breakup of the polar vortex. Results from a tracer‐tracer correlation analysis of O3 and long-lived constituent N2O were also consistent with this inference. The contribution of lateral mixing to the increase in ozone was estimated at about 17% 6 4% that of the Brewer‐Dobson circulation around 20 km, using the calculated descent rates. The results of this study also imply that Lagrangian downward motions in the vortex interior are not correctly estimated without accounting for lateral mixing, even if the polar vortex is dynamically stable.

Validation of the Improved Limb Atmospheric Spectrometer‐II (ILAS‐II) Version 1.4 nitrous oxide and methane profiles

This study assesses polar stratospheric nitrous oxide (N(2)O) and methane (CH(4)) data from the Improved Limb Atmospheric Spectrometer-II (ILAS-II) on board the Advanced Earth Observing Satellite-II (ADEOS-II) retrieved by the Version 1.4 retrieval algorithm. The data were measured between January and October 2003. Vertical profiles of ILAS-II volume mixing ratio (VMR) data are compared with data from two balloon-borne instruments, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) and the MkIV instrument, as well as with two satellite sensors, the Odin Sub-Millimetre Radiometer (SMR) for N(2)O and the Halogen Occultation Experiment (HALOE) for CH(4). Relative percentage differences between the ILAS-II and balloon/satellite data and their median values are calculated in 10-ppbv-wide bins for N(2)O (from 0 to 400 ppbv) and in 0.05-ppmv-wide bins for CH(4) (from 0 to 2 ppmv) in order to assess systematic differences between the ILAS-II and balloon/satellite data. According to this study, the characteristics of the ILAS-II Version 1.4 N(2)O and CH(4) data differ between hemispheres. For ILAS-II N(2)O VMR larger than 250 ppbv, the ILAS-II N(2)O agrees with the balloon/SMR N(2)O within +/- 20% in both hemispheres. The ILAS-II N(2)O in the VMR range from 30-50 to 250 ppbv (corresponding to altitudes of similar to 17-30 km in the Northern Hemisphere (NH, mainly outside the polar vortex) and similar to 13-21 km in the Southern Hemisphere (SH, mainly inside the polar vortex) is smaller by similar to 10-30% than the balloon/SMR N(2)O. For ILAS-II N(2)O VMR smaller than 30 ppbv (>similar to 21 km) in the SH, the differences between the ILAS-II and SMR N(2)O are within +/- 10 ppbv. For ILAS-II CH(4) VMR larger than 1 ppmv ( similar to 30 km) and the ILAS-II CH(4) for its VMR smaller than 1 ppmv (>similar to 25 km) only in the NH, are abnormally small compared to the balloon/satellite data.

ILAS-II instrument and data processing system for stratospheric ozone layer monitoring

The Improved Limb Atmospheric Spectrometer-II (ILAS-II) is a satellite-borne solar occultation sensor developed by the Environment Agency of Japan for measuring ozone, other gas species, and aerosols/PSCs that are related to the ozone chemistry in the stratosphere. The ILAS-II instrument will be installed on board the ADEOS-II satellite that will be put into a sun-synchronous polar orbit by the National Space Development Agency of Japan (NASDA) in November 2001. The ILAS-II measurement is a continuation of that of ILAS on board ADEOS, which obtained data from November 1996 to June 1997. The main components of ILAS-II are four spectrometers and a sun-edge sensor. The spectrometers include an infrared spectrometer to cover about 6 to 12 micrometer in wavelength, a mid-infrared spectrometer 3 to 5.7 micrometer, a narrow band spectrometer around 12.8 micrometer, and a visible spectrometer 753 to 784 nm. The first two spectrometers are used for measuring gas and aerosol/PSC profiles, while the third is for ClONO2 measurements. The visible spectrometer is used for pressure/temperature measurements as well as aerosol/PSC extinction coefficients. The ILAS_II instrument has already completed its development and environment tests, and now is undergoing satellite system environment tests at NASDA. This paper outlines the characteristics and performance results from laboratory tests along with the present status of development of its data processing algorithm and operational software.

Temperature and pressure retrievals from O2 A-band absorption measurements made by ILAS: retrieval algorithm and error analyses

A visible grating spectrometer of the Improved Limb Atmospheric Spectrometer (ILAS) aboard the Advanced Earth Observing Satellite (ADEOS) measured atmospheric absorption spectra at a wavelength region from 753 nm to 784 nm, including the molecular oxygen (O2) A-band centered at 762 nm, with a spectral resolution of 0.17 nm. Temperature and pressure profiles throughout the stratosphere were retrieved from the satellite solar occultation measurements of the O2 A-band absorption spectra. Based on simulation studies, root-sum-square errors associated with several systematic uncertainties in spectroscopic databases and instrument functions were estimated to be 4 K for temperature and 4% for pressure in the stratosphere. Current problems in this retrieval are also presented through comparisons with correlative temperature measurements.

ILAS data processing for stratospheric gas and aerosol retrievals with aerosol physical modeling: Methodology and validation of gas retrievals

This paper presents initial results of simultaneous gas and aerosol retrievals from Improved Limb Atmospheric Spectrometer (ILAS) observations taken between November 1996 and June 1997. The solar occultation measurements were processed by an inversion method that included aerosol physical modeling and permitted simultaneous retrieval of O 3 , HNO 3 , CH 4 , H 2 O, NO 2 , N 2 O, N 2 O S , ClONO 2 , CFC-11, and CFC-12 trace species and particle volume size distributions for key aerosol/polar stratospheric cloud (PSC) components such as liquid ternary solution, nitric acid trihydrate, nitric acid dihydrate, and water ice. The retrieval method was designed for the version 7.0 ILAS data processing algorithm. Gas retrieval results for the entire ILAS data set were compared to results from the earlier version 6.0 retrieval algorithm that was based on aerosol/PSC contribution estimates in the gas window channel. Gas data from nearby balloon-borne validation measurements and new data on the aerosol retrievals helped explain discrepancies between the two algorithms. The new version 7.0 methodology proved effective for simultaneous retrievals of all trace gases and showed a significant advantage when retrieving CH 4 , H 2 O, NO 2 , N 2 O, and CFC-12 from PSC observations.

Interpretation of nitric oxide profile observed in January 1992 over Kiruna

NO mixing ratios measured from Kiruna (68°N, 20°E), Sweden, on January 22, 1992, revealed values much smaller than those observed at midlatitude near equinox and had a sharper vertical gradient around 25 km. Location of the measurements was close to the terminator and near the edge of the polar vortex, which is highly distorted from concentric flow by strong planetary wave activities. These conditions necessitate accurate calculation, properly taking into account the transport and photochemical processes, in order to quantitatively explain the observed NO profile. A three-dimensional chemistry and transport model (CTM) and a trajectory model (TM) were used to interpret the profile observations within their larger spatial, temporal, and chemical context. The NOy profile calculated by the CTM is in good agreement with that observed on January 31, 1992. In addition, model NOy profiles show small variabilities depending on latitudes, and they change little between January 22 and 31. The TM uses the observed NOy values. The NO values calculated by the CTM and TM agree with observations up to 27 km. Between 20 and 27 km the NO values calculated by the trajectory model including only gas phase chemistry are much larger than those including heterogeneous chemistry, indicating that NO mixing ratios were reduced significantly by heterogeneous chemistry on sulfuric acid aerosols. Very little sunlight to generate NOx from HNO3 was available, also causing the very low NO values. The good agreement between the observed and modeled NO profiles indicates that models can reproduce the photochemical and transport processes in the region where NO values have a sharp horizontal gradient. Moreover, CTM and TM model results show that even when the NOy gradients are weak, the model NO depends upon accurate calculation of the transport and insolation for several days.