HNO3 and PSC Measurements from the Transall: Sequestering of HNO3 in the Winter of 1994/95

In the winter of 1994/95 the TRANSALL research aircraft performed several flights in the region of the Arctic vortex during the period of low stratospheric temperatures. The results of simultaneous measurements of HNO3 column amounts by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and of aerosol backscatter profiles by the Ozone Lidar EXperiment (OLEX) are presented for two typical flight scenarios across the polar vortex boundary on December 17, 1994 and January 11/12, 1995. On December 17 and January 12, the column amounts of gaseous HNO3 decreased significantly in regions with low stratospheric temperatures. This decrease was correlated with the extent of the polar stratospheric clouds. Depolarisation measurements showed that type Ib PSCs were observed primarily, but equilibrium calculations for H2SO4/HNO3/H2O aerosols seem to underestimate the observed HNO3 sequestering.     

Vertical profiles of Volcanic Aerosol and Polar Stratospheric Clouds Above Kiruna, Sweden: Winters 1993 and 1995

Vertical profiles of aerosol were measured in February 1993, and January - March 1995 using balloon-borne particle counters released from Kiruna, Sweden. Condensation nuclei (CN) and aerosol with radii 0.15 - 10.0 µm were measured in 8-12 size classes. The three flights in 1993 were within the polar vortex. Temperatures were below polar stratospheric cloud (PSC) threshold temperatures on one flight and a thin PSC was observed. The volcanic aerosol in the 1993 vortex was similar to that in 1992. In 1993, surface areas were 10 - 20 µm2 cm-3 and volumes 1 - 3 µm3 cm-3. In 1995 three of five flights were within the polar vortex. The volcanic aerosol had decreased to 3 - 7 µm2 cm-3 and 0.1 - 0.4 µm3 cm-3. The top of the volcanic aerosol layer in both years was near 500 K potential temperature (~20 km). A thick nitric acid and water PSC was observed in January 1995. In the thickest region of this PSC nearly all CN were observed to be activated, and surface areas of 5 - 10 µm2 cm-3 were calculated. The volumes observed in this PSC were closer to what would be expected for particles composed of nitric acid trihydrate than for ternary solution droplets. In 1993 the opposite was observed, the volumes in the thin PSC were closer to what would be expected for ternary solution droplets.     

Clear‐sky closure studies of lower tropospheric aerosol and water vapor during ACE‐2 using airborne sunphotometer, airborne in‐situ, space‐borne, and ground‐based measurements

We report on clear‐sky column closure experiments (CLEARCOLUMN) performed in the Canary Islands during the second Aerosol Characterization Experiment (ACE‐2) in June/July 1997. We present CLEARCOLUMN results obtained by combining airborne sunphotometer and in‐situ (optical particle counter, nephelometer, and absorption photometer) measurements taken aboard the Pelican aircraft, space‐borne NOAA/AVHRR data and ground‐based lidar and sunphotometer measurements. During both days discussed here, vertical profiles flown in cloud‐free air masses revealed 3 distinctly different layers: a marine boundary layer (MBL) with varying pollution levels, an elevated dust layer, and a very clean layer between the MBL and the dust layer. A key result of this study is the achievement of closure between extinction or layer aerosol optical depth (AOD) computed from continuous in‐situ aerosol size‐distributions and composition and those measured with the airborne sunphotometer. In the dust, the agreement in layer AOD (λ=380–1060 nm) is 3–8%. In the MBL there is a tendency for the in‐situ results to be slightly lower than the sunphotometer measurements (10–17% at λ=525 nm), but these differences are within the combined error bars of the measurements and computations.     

Microphysical properties of stratocumulus clouds during ACE‐2

Microphysical measurements performed during 8 flights of the CLOUDYCOLUMN component of ACE‐2, with the Meteo‐France Merlin‐IV, are analyzed in terms of droplet number concentration and size. The droplet concentration is dependent upon the aerosol properties within the boundary layer. Its mean value over a flight varies from 55 cm⁻³, for the cleanest conditions, to 244 cm⁻³, for the most polluted one. For each flight, the variability of the concentration, in selected cloud regions that are not affected by mixing with dry air or drizzle scavenging, ranges from 0.5 to 1.5 of the mean value. The mean volume diameter increases with altitude above cloud base according to the adiabatic cloud model. The frequency distribution of mean droplet volume normalized by the adiabatic value, for the selected regions, shows the same dispersion as the distribution of normalized concentration. The values of droplet concentration versus mean volume diameter are then examined in sub‐adiabatic samples to characterize the effects of mixing and drizzle scavenging. Finally, the ratio of mean volume diameter to effective diameter is analyzed and a simple relationship between these 2 crucial parameters is proposed.     

Ground‐based lidar measurements of aerosols during ACE‐2: instrument description, results, and comparisons with other ground‐based and airborne measurements

A micro‐pulse lidar system (MPL) was used to measure the vertical and horizontal distribution of aerosols during the Aerosol Characterization Experiment 2 (ACE‐2) in June and July of 1997. The MPL measurements were made at the Izaña observatory (IZO), a weather station located on a mountain ridge (28°18' N, 16°30' W, 2367 m asl) near the center of the island of Tenerife, Canary Islands. The MPL was used to acquire aerosol backscatter, extinction, and optical depth profiles for normal background periods and periods influenced by Saharan dust from North Africa. System tests and calibration procedures are discussed, and an analysis of aerosol optical profiles acquired during ACE‐2 is presented. MPL data taken during normal IZO conditions (no dust) showed that upslope aerosols appeared during the day and dissipated at night and that the layers were mostly confined to altitudes a few hundred meters above IZO. MPL data taken during a Saharan dust episode on 17 July showed that peak aerosol extinction values were an order of magnitude greater than molecular scattering over IZO, and that the dust layers extended to 5 km asl. The value of the dust backscatter–extinction ratio was determined to be 0.027±0.007 sr⁻¹. Comparisons of the MPL data with data from other co‐located instruments showed good agreement during the dust episode.     

Polarising properties of the aerosols in the north‐eastern tropical Atlantic Ocean, with emphasis on the ACE‐2 period

Measurements of the polarisation state of the atmosphere were performed at Tenerife in June–July 1997, in the framework of ACE‐2 (second Aerosol Characterization Experiment), by 2 ground‐based instruments: RefPol (a LOA prototype) which took measurements at 445, 665, 870, 1610 nm in the solar principal plane; and an automatic CIMEL (CE 318) sun/sky‐photometer which measured polarised radiation at 870 nm in the same observational geometry. Measurements acquired during the campaign, as well as AERONET (AErosol RObotic NETwork) measurements acquired at the sites of Cape Verde and M'Bour, are processed with an algorithm determining the polarised single‐scattering sky‐radiance due to aerosols, directly proportional to the aerosol polarised phase function (representing the probability to scatter polarised radiation in the direction of the scattering angle). A good correlation between the Ångström exponent α, representing the spectral dependence of the extinction measurements, and the polarised phase function is observed on each set of data. The uncertainty of retrievals at 445 nm makes the determination of the spectral dependence of polarisation inconclusive but does not prevent confirming the dependence of the aerosol polarised phase function on α, at all wavelengths. An Ångström exponent of 1 corresponds to a polarised phase function of around 0.1 (±0.04), at 870 nm and at a scattering angle of 60°. For α between 0 and 0.4, the average value of the polarised phase function is 0.05. The correlation shows that polarisation is more sensitive to small particles than to large particles. The discrepancy between retrievals and Mie calculations from an AERONET size distribution, inverted from Izaña measurements acquired during a dust event, suggests the presence of small particles, not detected by total sky‐radiance measurements.     

Size‐segregated chemical, gravimetric and number distribution‐derived mass closure of the aerosol in Sagres, Portugal during ACE‐2

During the ACE‐2 field campaign in the summer of 1997 an intensive, ground‐based physical and chemical characterisation of the clean marine and continentally polluted aerosol was performed at Sagres, Portugal. Number size distributions of the dry aerosol in the size range 3–10 000 nm were continuously measured using DMPS and APS systems. Impactor samples were regularly taken at 60% relative humidity (RH) to obtain mass size distributions by weighing the impactor foils, and to derive a chemical mass balance by ion and carbon analysis. Hygroscopic growth factors of the metastable aerosol at 60% RH were determined to estimate the number size distribution at a relative humidity of 60%. A size segregated 3‐way mass closure study was performed in this investigation for the first time. Mass size distributions at 60% RH derived from number size distribution measurements and impactors samples (weighing and chemical analysis) are compared. A good agreement was found for the comparison of total gravimetrically‐determined mass with both number distribution‐derived (slope=1.23/1.09; R²>0.97; depending on the parameters humidity growth and density) and chemical mass concentration (slope=1.02; R²= 0.79) for particles smaller than 3 μm in diameter. Except for the smallest impactor size range relatively good correlations (slope=0.86–1.42) with small deviations (R²=0.76–0.98) for the different size fractions were found. Since uncertainties in each of the 3 methods are about 20% the observed differences in the size‐segregated mass fractions can be explained by the measurement uncertainties. However, the number distribution‐derived mass is mostly higher than the chemically and gravimetrically determined mass, which can be explained by sampling losses of the impactor, but as well with measurement uncertainties as, e.g., the sizing of the DMPS/APS.     

Meteorological conditions and polar stratospheric clouds over Yakutsk in winter 2004/05

Regular observations of polar stratospheric clouds were started at a lidar stratospheric station in the city of Yakutsk. According to lidar measurements in the winter of 2004/05, thick aerosol layers in the lower stratosphere appeared over this region quite frequently. They were episodically observed as pearl clouds. In November 2004, polar stratospheric clouds were observed at the stratospheric temperatures that were much higher than those at which particles of the polar stratospheric clouds could condense. Analysis of air-mass trajectories that simultaneously passed over Yakutsk at different altitudes on the days of polar stratospheric cloud observations showed that clouds could be formed over the Norwegian Sea at altitudes of about 18–21 km, where the stratosphere was the coldest, and then were transported to Yakutsk by wind during 4–5 days.     

Observation of the Stratospheric NO2 Latitudinal Distribution in the Northern Winter Hemisphere

During a series of flights in the winters 1991/92 to 1994/95 total stratospheric NO2 was measured by means of the DOAS (Differential Optical Absorption Spectroscopy) technique on board a C160 (Transall) aircraft. In an area covering 60°W to 60°E, and 16°N to 86°N, the total stratospheric NO2 was observed to vary markedly with latitude and season (winter and spring). In the mid-winter Arctic vortex extremely low total stratospheric NO2 (< 3.1014/cm2) was always found, generally larger amounts of NO2 occurred outside the vortex in winter and towards the spring both inside and outside the vortex. This behaviour of stratospheric NO2 can be explained by the denoxification of the wintertime polar stratosphere. Ambient to the vortex in mid-winter however, sudden increases of total stratospheric NO2 by about a factor of 3 were observed. These sudden increases in stratospheric NO2 coincide with a change in the wavenumber 2 of the geopotential height at 60°N, which indicates that most likely the events are caused by planetary waves efficiently transporting air masses rich in NOx from lower to higher latitudes. The monitoring of stratospheric NO2, during latitudinal traverses ranging from the Arctic (80°N) to the Subtropics (18°N) in spring also unexpectedly showed a large variability in total stratospheric NO2 at mid-latitudes. Since photochemistry almost certainly can be excluded, it is proposed that the observed variability may be due to the planetary wave activity of the stratospheric surf zone, known to dynamically connect the tropical and the polar stratosphere.     

Groundbased Doas UV/visible measurements at Kiruna (Sweden) during the sesame winters 1993/94 and 1994/95.

Zenith sky observations of O3, NO2, OClO and BrO are reported, which were performed at Kiruna (67.9°N, 21.1°E) within the SESAME winters 1993/1994 and 1994/95. For both winters large total amounts of OClO were observed inside the polar vortex at twilight, indicating the degree and the temporal variation of the halogen activation of the polar stratosphere. Occasionally OClO could also be observed outside the polar vortex, most likely due to export of halogen activated vortex air masses into the ambient stratosphere. BrO could also be detected in winter 1994/95, with the largest slant column amounts (5·1014/cm2) occuring in the polar vortex in mid-winter. Similar abundances of stratospheric BrO were observed at dusk and dawn, for both, air masses inside and outside the vortex. This observation is in reasonable agreement with previous studies on stratospheric BrO (observations and models) of Wahner et al. (1992), Arpag et al. (1994), Krug et al. (1996), and Lary et al. (1996a,b), but partly in disagreement with those of Solomon et al. (1989), Fish et al. (1995), and Sessler et al. (1996).     

A modelling study on the activation of small Aitken‐mode aerosol particles during CIME 97

During February 1997, one of the 2 observational periods of CIME ( c loud i ce m ountain e xperiment), a joint field experiment funded by the European Commission, took place on the summit of the Puy de Dōme in the centre of France. During this experiment the droplet spectra were measured with an FSSP and the aerosol particles in the drops and in the interstitial particle phase were measured with a counterflow virtual impactor and a round jet impactor inside a windtunnel. Very low aerosol particle and drop concentrations were observed and particles as small as 25 nm in diameter were found to activate. Two datasets obtained on 15 February and 17 February were used to study the activation of the small Aitken‐mode particles and the spectral form of the droplet spectrum and the scavenging fraction. Numerous sensitivity studies were performed investigating the rôle of the number density and chemical composition of the aerosol particles. The rôle of mixing inside the orographic cloud was studied by using a new technique. It considers the fact that the air arriving on the summit of the Puy de Dôme is a mixture of air of different origins. Thus, it weighs the results of a spectral scavenging model (DESCAM or EXMIX) calculated along a number of individual trajectories. The weighing function is derived from tracer and trajectory studies with a 3‐dimensional mesoscale model. The model was able to reproduce the activation of aerosol particles as small as 25 nm. It was caused by the low aerosol particle number concentrations. In general, we can conclude that the variability found in the sensitivity tests of the dynamical and chemical factors allows to reproduce the shape of the observed results. As too many free parameters exit at the moment we cannot quantify the contribution of each factor studied to the observed scavenging fraction, however, it seems that dynamics dominates.     

An overview of the ACE‐2 CLOUDYCOLUMN closure experiment

CLOUDYCOLUMN is one of the 6 ACE‐2 projects which took place in June‐July 1997, between Portugal and the Canary Islands. It was specifically dedicated to the study of changes of cloud radiative properties resulting from changes in the properties of those aerosols which act as cloud condensation nuclei. This process is also refered to as the aerosol indirect effect on climate. CLOUDYCOLUMN is focused on the contribution of stratocumulus clouds to that process. In addition to the basic aerosol measurements performed at the ground stations of the ACE‐2 project, 5 instrumented aircraft carried out in situ characterization of aerosol physical, chemical and nucleation properties and cloud dynamical and microphysical properties. Cloud radiative properties were also measured remotely with radiometers and a lidar. 11 case studies have been documented, from pure marine to significantly polluted air masses. The simultaneity of the measurements with the multi‐aircraft approach provides a unique data set for closure experiments on the aerosol indirect effect. In particular CLOUDYCOLUMN provided the 1st experimental evidence of the existence of the indirect effect in boundary layer clouds forming in polluted continental outbreacks. This paper describes the objectives of the project, the instrumental setup and the sampling strategy. Preliminary results published in additional papers are briefly summarized.     

ACE‐2 multiple angle micro‐pulse lidar observations from Las Galletas, Tenerife, Canary Islands

Multiple‐angle micro‐pulse lidar (MPL) observations were made at Las Galletas on Tenerife, Canary Islands during the Aerosol Characterization Experiment‐2 (ACE‐2) conducted June–July, 1997. A principal objective of the MPL observations was to characterize the temporal/spatial distributions of aerosols in the region, particularly to identify and profile elevated Saharan dust layers which occur intermittently during the June–July time period. Vertical and slant angle measurements taken 16 and 17 July characterize such an occurrence, providing aerosol backscatter, extinction, and optical depth profiles of the dust layer between 1 and 5 km above mean sea level (MSL). Additionally, horizontal measurements taken in Las Galletas throughout the 6‐week period provide a time profile of the varying aerosol extinction at the surface. This profile exhibits the alternating periods of clean maritime air and pollution outbreaks that typified the region. Horizontal measurements also provide some evidence suggesting the possible influx of Saharan dust from the free troposphere to the surface. This paper presents estimates of aerosol optical properties retrieved from the multi‐angle MPL measurements in addition to an outline of the methodologies employed to obtain these results.     

BCC_AGCM2.1模式对平流层环流变化特征的数值模拟及其模式评估

使用国家气候中心大气环流模式BCC_AGCM2.1的30年模拟试验资料,对平流层纬向环流场、高空急流、极涡及爆发性增温过程进行了数值模拟研究,并使用欧洲中期天气预报中心（ECMWF）和美国国家环境预报中心（NCEP）的再分析资料对模式输出结果进行了对比、分析。结果表明：（1） 在观测海温、二氧化碳、气溶胶等外强迫地驱动下,BCC模式能够很好地再现出与再分析资料一致的平流层纬向平均风场、温度场的分布特征和季节变化过程;模拟得到的温度廓线和高空急流与再分析资料的主要差别出现在南、北半球冬季的中高纬度地区;模拟得到的平流层温度普遍偏低,主要的差异位于对流层顶区域和平流层高层。（2） 模拟的对流层上层的副热带急流位置偏南、强度也偏弱,而平流层中的绕极极夜急流则位置偏北、强度更大。这样的急流分布特征使模拟的行星波向赤道的波导更强,向极的波导偏弱;同时由于模式中本身可以形成的行星波就比再分析资料弱,因此导致模拟结果中北半球冬季的平流层极涡更加稳定、极区温度更低。（3） BCC模式对于平流层极涡的季节变化特征模拟得较好,但对强极涡扰动过程,即北半球冬季的平流层爆发性增温（SSW）事件则模拟效果不佳,不论是增温事件出现的频率,还是增温的时间、强度,模拟结果和再分析资料都还存在一定偏差,需要在今后的工作中逐步改善。     

Evolution of boundary‐layer aerosol particles due to in‐cloud chemical reactions during the 2nd Lagrangian experiment of ACE‐2

The second Aerosol Characterisation Experiment (ACE‐2) was aimed at investigating the physical, chemical and radiative properties of aerosol and their evolution in the North Atlantic region. In the 2nd "Lagrangian" experiment, an air mass was tracked over a 30‐h period during conditions of extensive stratocumulus cover. Boundary‐layer measurements of the aerosol size distribution obtained with a passive cavity aerosol spectrometer probe (PCASP) during the experiment show a gradual growth in size of particles in the 0.1–0.2 μm diameter mode. Simultaneously, SO₂ concentrations were found to decrease sharply from 800 to 20 ppt. The fraction of sulphate in aerosol ionic mass increased from 0.68±0.07 to 0.82±0.09 for small particles (diameter below 1.7 μm) and from 0.21±0.04 to 0.34±0.03 for large particles (diameter above 1.7 μm). The measurements were compared with a multicyclic parcel model of gas phase diffusion into cloud droplets and aqueous phase chemical reactions. The model was able to broadly reproduce the observed transformation in the aerosol spectra and the timescale for the transformation of SO₂ to sulphate aerosol. The modelled SO₂ concentration in the boundary layer fell to below half its initial value over a 6.5‐h time period due to a combination of the entrainment of cleaner tropospheric air and cloud chemical reactions. NH₃ and HCl gas were also found to play an important rôle in cloud processing in the model.     

MIPAS-Transall Observations of the Variability of CLONO2 during the Arctic Winter of 1994/95

In the winter of 1994/95 the German Transall research aircraft performed 5 campaigns in the European Arctic with 22 flights altogether. An extensive dataset of HNO3, ClONO2 and O3 column amounts was obtained by MIPAS-FT (Michelson Interferometer for Passive Atmospheric Sounding - Flugzeug Transall) onboard the aircraft. In this paper we present the variability of the ClONO2 reservoir gas in the course of the winter. We include groundbased FTIR measurements of HF, HCl and ClONO2 to discuss the airborne observations with regard to the partitioning of inorganic chlorine.From mid-December until the end of January, MIPAS measured a stable ClONO2 collar with constantly low column amounts inside the polar vortex and maxima at the edge. This observation reflected widespread conversion of ClONO2 to reactive chlorine inside the vortex for at least six weeks. In good accordance, the ground stations measured low in-vortex HCl and ClONO2 column amounts and conversion of HCl into ClONO2 in the region of the ClONO2 maxima. In the first week of February the ClONO2 amounts started to increase in the edge region as well as inside the vortex. Between March 21 and 27, just one week after the last cold period, MIPAS observed exclusively high ClONO2 column amounts inside the vortex, indicating fast deactivation of active chlorine. In the same period the ground stations measured an excess of ClONO2 over HCl. Further, the high ClONO2 implies that the polar vortex was renoxified in March. Lower ClONO2 values, observed inside the vortex on the flights of April 5 and 8, and an increased HCl/ClONO2 ratio, measured from ground, marked the starting redistribution within the chlorine reservoir species to the photochemically more stable HCl.In February, March and April, MIPAS observed mixing of ClONO2-rich air masses with midlatitude air at the vortex edge. A very clear event happened on March 27. On this flight a distinct ClONO2 minimum was measured at the vortex edge, which was closely correlated with a filament of midlatitude air observed by OLEX (Ozone Lidar EXperiment) onboard the Transall.     

Measurements of aerosol optical depth above 3570 m asl in the North Atlantic free troposphere: results from ACE‐2

As part of the 2nd A erosol C haracterisation E xperiment (ACE‐2), conducted during summer 1997 in the North Atlantic region between the Canary Islands and Portugal, we measured aerosol optical depths (AOD) at a mid‐tropospheric site, near the top of the volcanic mountain "El Teide"(28°16'N, 16°36' W, 3570 m asl). Our instrument was located at the highest altitude in a network of sunphotometers that extended down to sea level. Clear conditions dominated the ACE‐2 period, and, although suggested by back‐trajectories at 300 hPa, no evidence of anthropogenic pollution was found in our data. Three distinct dust episodes were observed. Vertical soundings and back trajectories suggested mineral dust from the Sahel region as a source. During these episodes, AOD increased an order of magnitude with respect to background conditions (from 0.017 up to 0.19 at λ=500 nm). A shift towards neutrality of the extinction spectral dependence (Ångstrom exponent α down to 0.13), indicated that the coarse mode (particle diameter >2 μm) dominated the aerosol size distribution. For 6 days during the episodes of mineral dust, a monomodal size distribution between 2 and 20 μm diameter was obtained from Mie based size distribution calculations. Estimates, at 500 nm, of the single scattering albedo ω₀(0.87–0.96), and the aerosol asymmetry parameter g (0.72–0.73) suggest that the dust layer causes a net cooling forcing at the top of the atmosphere.     

Observation of polar stratospheric clouds over Obninsk in December 2012

In late December 2012 a blocking anticyclone followed by the event of minor stratospheric warming, set in the troposphere over West Siberia and, after that, over the European part of Russia. As a result of the deformation of a polar stratospheric vortex, the temperature in the lower stratosphere over Obninsk dropped below the threshold of the formation of polar stratospheric clouds. The lidar measurements of temperature, ozone values, and aerosol characteristics in the middle atmosphere were carried out at the lidar station during this atmospheric event. In three cases, polar stratospheric clouds (PSCs) referred to NAT I_a type according to the sounding results, were registered at the height of about 20 km. No considerable decrease in the ozone concentration in the area of PSC formation was revealed in these measurements.     

Stratospheric Polar Vortex Splitting in December 2009

Abstract

The 2009–10 Arctic stratospheric winter, in comparison with other recent winters, is mainly characterized by a major Sudden Stratospheric Warming (SSW) in late January associated with planetary wavenumber 1. This event led to a large increase in the temperature of the polar stratosphere and to the reversal of the zonal wind. Unlike other major SSW events in recent winters, after the major SSW in January 2010 the westerlies and polar vortex did not recover to their pre-SSW strength until the springtime transition. As a result, the depletion of the ozone layer inside the polar vortex over the entire winter was relatively small over the past 20 years. The other distinguishing feature of the 2010 winter was the splitting of the stratospheric polar vortex into two lobes in December. The vortex splitting was accompanied by an increase in the temperature of the polar stratosphere and a weakening of the westerlies but with no reversal. The splitting occurred when, in addition to the high-pressure system over northeastern Eurasia and the northern Pacific Ocean, the tropospheric anticyclone over Europe amplified and extended to the lower stratosphere. Analysis of wave activity in the extratropical troposphere revealed that two Rossby wave trains propagated eastward to the North Atlantic several days prior to the vortex splitting. The first wave train propagated from the subtropics and mid-latitudes of the eastern Pacific Ocean over North America and the second one propagated from the northern Pacific Ocean. These wave trains contributed to an intensification of the tropospheric anticyclone over Europe and to the splitting of the stratospheric polar vortex.