Supercooled Ternary Solution Research Articles

Antarctic Polar Stratospheric Cloud Analysis of ACE‐FTS Data From 2005 to 2023

AbstractWe present an analysis of Antarctic polar winters from 2005 to 2023 as observed by the Atmospheric Chemistry Experiment (ACE). The unique broad band infrared spectral features in ACE “residual” spectra are used to classify the spectra of polar aerosols by composition into polar stratospheric clouds (PSCs) and sulfate aerosols. The spectra of PSCs are further classified into nitric acid trihydrate, supercooled ternary solutions, supercooled nitric acid, ice‐mix, and mixtures of PSCs. A breakdown of PSC composition is presented for each year. Antarctic winter seasons with unusual compositions are: 2011, in which volcanic ash mixed with PSCs was observed from July to August; 2019, which experienced a stratospheric warming event; 2020, the PSC season following the Australian Black Summer pyrocumulonimbus event; and 2023, which had unusually large sulfate aerosols following the Honga‐Tonga Honga Ha'apai eruption of 2022.

Polar Stratospheric Cloud Observations at Concordia Station by Remotely Controlled Lidar Observatory

Polar stratospheric clouds (PSCs) form in polar regions, typically between 15 and 25 km above mean sea level, when the local temperature is sufficiently low. PSCs play an important role in the ozone chemistry and the dehydration and denitrification of the stratosphere. Lidars with a depolarization channel may be used to detect and classify different classes of PSCs. The main PSC classes are water ice, nitric acid trihydrate (NAT), and supercooled ternary solutions (STSs), the latter being liquid droplets consisting of water, nitric acid, and sulfuric acid. PSCs have been observed at the lidar observatory at Concordia Station from 2014 onward. The harsh environmental conditions at Concordia during winter render successful lidar operation difficult. To facilitate the operation of the observatory, several measures have been put in place to achieve an almost complete remote control of the system. PSC occurrence is strongly correlated with local temperatures and is affected by dynamics, as the PSC coverage during the observation season shows. PSC observations in 2021 are shown as an example of the capability and functionality of the lidar observatory. A comparison of the observations with the satellite-borne CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) lidar has been made to demonstrate the quality of the data and their representativeness for the Antarctic Plateau.

Antarctic polar stratospheric cloud composition as observed by ACE, CALIPSO and MIPAS

The composition of polar stratospheric clouds (PSCs) in the Antarctic is measured by infrared absorption spectroscopy by the Atmospheric Chemistry Experiment (ACE) satellite and compared to lidar (CALIPSO) and emission spectroscopy (MIPAS) results. ACE observations are compared first to CALIPSO for the period 2006–2020, then to MIPAS for the period 2005–2011, and then a set of triple coincidences is studied. In both CALIPSO-ACE and MIPAS-ACE comparisons, nitric acid trihydrate (NAT) detections are in excellent agreement (∼80 % of coincident compositions is found). Supercooled ternary solution (STS) detections are in good agreement for CALIPSO-ACE (∼60 %) but in poor agreement for MIPAS-ACE (39 %). This contrasts with ice detections, in poor agreement for CALIPSO-ACE (∼30 %) and in better agreement for MIPAS-ACE (45 %). Triple coincidences show that ACE STS detections are more reliable than MIPAS STS detections. The comparison between ACE observations and homogeneous CALIPSO PSCs shows that for 11 events, CALIPSO reports STS rather than supercooled nitric acid (SNA) clouds.

Statistical analysis of observations of polar stratospheric clouds with a lidar in Kiruna, northern Sweden

Abstract. In the present paper, we analyse 11 years of lidar measurements to derive general characteristics of polar stratospheric clouds (PSCs) and to examine how mountain lee waves influence PSC properties. Measurements of PSCs were made with a backscatter lidar located in Kiruna, northern Sweden, in the lee of the Scandinavian mountain range. The statistical analysis demonstrates that nearly half of all observed PSCs consisted of nitric acid trihydrate (NAT) particles, while ice clouds accounted for only a small fraction, and the remainder consisted of supercooled ternary solution (STS) and mixtures of different compositions. Most PSCs were observed around 22 km altitude. Mountain lee waves provide a distinct influence on PSC chemical composition and cloud height distribution. Ice PSCs were about 5 times as frequent, and NAT clouds were about half as frequent under wave conditions. PSCs were on average at 2 km higher altitudes when under the influence of mountain lee waves.

A study of optical scattering modelling for mixed-phase polar stratospheric clouds

Abstract. Scattering codes are used to study the optical properties of polar stratospheric clouds (PSCs). Particle backscattering and depolarization coefficients can be computed with available scattering codes once the particle size distribution (PSD) is known and a suitable refractive index is assumed. However, PSCs often appear as external mixtures of supercooled ternary solution (STS) droplets, solid nitric acid trihydrate (NAT) and possibly ice particles, making the assumption of a single refractive index and a single morphology to model the scatterers questionable. Here we consider a set of 15 coincident measurements of PSCs above McMurdo Station, Antarctica, using ground-based lidar, a balloon-borne optical particle counter (OPC) and in situ observations taken by a laser backscattersonde and OPC during four balloon stratospheric flights from Kiruna, Sweden. This unique dataset of microphysical and optical observations allows us to test the performances of optical scattering models when both spherical and aspherical scatterers of different composition and, possibly, shapes are present. We consider particles as STS if their radius is below a certain threshold value Rth and NAT or possibly ice if it is above it. The refractive indices are assumed known from the literature. Mie scattering is used for the STS, assumed spherical. Scattering from NAT particles, considered spheroids of different aspect ratio (AR), is treated with T-matrix results where applicable. The geometric-optics–integral-equation approach is used whenever the particle size parameter is too large to allow for a convergence of the T-matrix method. The parameters Rth and AR of our model have been varied between 0.1 and 2 µm and between 0.3 and 3, respectively, and the calculated backscattering coefficient and depolarization were compared with the observed ones. The best agreement was found for Rth between 0.5 and 0.8 µm and for AR less than 0.55 and greater than 1.5. To further constrain the variability of AR within the identified intervals, we have sought an agreement with the experimental data by varying AR on a case-by-case basis and further optimizing the agreement by a proper choice of AR smaller than 0.55 and greater than 1.5 and Rth within the interval 0.5 and 0.8 µm. The ARs identified in this way cluster around the values 0.5 and 2.5. The comparison of the calculations with the measurements is presented and discussed. The results of this work help to set limits to the variability of the dimensions and asphericity of PSC solid particles, within the limits of applicability of our model based on the T-matrix theory of scattering and on assumptions on a common particle shape in a PSD and a common threshold radius for all the PSDs.

14 years of lidar measurements of polar stratospheric clouds at the French Antarctic station Dumont d'Urville

Abstract. Polar stratospheric clouds (PSCs) play a critical role in the stratospheric ozone depletion processes. The last 30 years have seen significant improvements in our understanding of the PSC processes but PSC parametrization in global models still remains a challenge due to the necessary trade-off between the complexity of PSC microphysics and model parametrization constraints. The French Antarctic station Dumont d'Urville (DDU, 66.6∘ S, 140.0∘ E) has one of the few high latitude ground-based lidars in the Southern Hemisphere that has been monitoring PSCs for decades. This study focuses on the PSC data record during the 2007–2020 period. First, the DDU lidar record is analysed through three established classification schemes that prove to be mutually consistent: the PSC population observed above DDU is estimated to be of 30 % supercooled ternary solutions, more than 60 % nitric acid trihydrate mixtures and less than 10 % of water–ice dominated PSC. The Cloud–Aerosol Lidar with Orthogonal Polarization PSC detection around the station are compared to DDU PSC datasets and show a good agreement despite more water–ice PSC detection. Detailed 2015 lidar measurements are presented to highlight interesting features of PSC fields above DDU. Then, combining a temperature proxy to lidar measurements, we build a trend of PSC days per year at DDU from ERA5 (the fifth generation of European ReAnalysis) and NCEP (National Centers for Environment Protection reanalysis) reanalyses fitted on lidar measurements operated at the station. This significant 14-year trend of −4.6 PSC days per decade is consistent with recent temperature satellite measurements at high latitudes. Specific DDU lidar measurements are presented to highlight fine PSC features that are often sub-scale to global models and spaceborne measurements.

Infrared transmittance spectra of polar stratospheric clouds

Polar stratospheric clouds (PSCs) are responsible for polar ozone depletion. Infrared transmittance spectra of PSCs recorded by the Fourier transform spectrometer (FTS) on the Atmospheric Chemistry Experiment (ACE) satellite were used to determine the composition and properties of PSCs. These unique broad band infrared spectra identify PSCs as nitric acid trihydrate (NAT), supercooled ternary solutions (STS) of nitric and sulfuric acid, and ice, as expected. Quantitative modeling of these PSC spectra shows that supercooled nitric acid (SNA) is also common, i.e., “STS” with no observable sulfuric acid in their infrared spectra. ACE-FTS observations therefore classify PSCs into 4 basic spectral types, NAT, STS, SNA and ice, as well as their mixtures. As an example, this classification scheme was applied to the Antarctic for July to September 2019. The composition and particularly the phase of PSCs are critical to the understanding and detailed chemical modeling of polar stratospheric ozone depletion.

Comparison of Coincident Optical Particle Counter and Lidar Measurements of Polar Stratospheric Clouds Above McMurdo (77.85°S, 166.67°E) From 1994 to 1999

AbstractMacroscopic stratospheric aerosol properties such as surface area density (SAD) and volume density (VD) are required by modern chemistry climate models. These quantities are in continuous need of validation by observations. Direct observation of these parameters is not possible, but they can be derived from optical particle counters (OPCs) which provide concentration (number density) and size distributions of aerosol particles, and possibly from ground‐based and satellite‐borne lidar observations of particle backscatter coefficients and aerosol type. When such measurements are obtained simultaneously by OPCs and lidars, they can be used to calculate backscatter and extinction coefficients, as well as SAD and VD. Empirical relations can thus be derived between particle backscatter coefficient, extinction coefficient, and SAD and VD for a variety of aerosols (desert dust, maritime aerosols, stratospheric aerosols) and be used to approximate SAD and VD from lidar measurements. Here we apply this scheme to coincident measurements of polar stratospheric clouds above McMurdo Station, Antarctica, by ground‐based lidar and balloon‐borne OPCs. The relationships derived from these measurements will provide a means to obtain values of SAD and VD for supercooled ternary solutions (STS) and nitric acid trihydrate (NAT) PSCs from the backscatter coefficients measured by lidar. Coincident lidar and OPC measurements provided 15 profile comparisons. Empirical expressions of SAD and VD as a function of particle backscatter coefficient, β, were calculated from fits of the form log(SAD/VD) = A + B log(β) using β from the lidar and SAD/VD from the OPC. The PSCs were classified as STS and NAT mixtures, ice being absent.

A new method to detect and classify polar stratospheric nitric acid trihydrate clouds derived from radiative transfer simulations and its first application to airborne infrared limb emission observations

Abstract. Polar stratospheric clouds (PSCs) play an important role in the spatial and temporal evolution of trace gases inside the polar vortex due to different processes, such as chlorine activation and NOy redistribution. As there are still uncertainties in the representation of PSCs in model simulations, detailed observations of PSCs and information on their type – nitric acid trihydrate (NAT), supercooled ternary solution (STS), and ice – are desirable. The measurements inside PSCs made by the CRISTA-NF (CRyogenic Infrared Spectrometers and Telescope for the Atmosphere – New Frontiers) airborne infrared limb sounder during the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions) aircraft campaign showed a spectral peak at about 816 cm−1. This peak is shifted compared with the known peak at about 820 cm−1, which is recognised as being caused by the emission of radiation by small NAT particles. To investigate the reason for this spectral difference, we performed a large set of radiative transfer simulations of infrared limb emission spectra in the presence of various PSCs (NAT, STS, ice, and mixtures) for the airborne viewing geometry of CRISTA-NF. NAT particles can cause different spectral features in the 810–820 cm−1 region. The simulation results show that the appearance of the feature changes with an increasing median radius of the NAT particle size distribution, from a peak at 820 cm−1 to a shifted peak and, finally, to a step-like feature in the spectrum, caused by the increasing contribution of scattering to the total extinction. Based on the appearance of the spectral feature, we defined different colour indices to detect PSCs containing NAT particles and to subgroup them into three size regimes under the assumption of spherical particles: small NAT (≤ 1.0 µm), medium NAT (1.5–4.0 µm), and large NAT (≥ 3.5 µm). Furthermore, we developed a method to detect the bottom altitude of a cloud by using the cloud index (CI), a colour ratio indicating the optical thickness, and the vertical gradient of the CI. Finally, we applied the methods to observations of the CRISTA-NF instrument during one local flight of the RECONCILE aircraft campaign and found STS and medium-sized NAT.

Evaluation of polar stratospheric clouds in the global chemistry–climate model SOCOLv3.1 by comparison with CALIPSO spaceborne lidar measurements

Abstract. Polar stratospheric clouds (PSCs) contribute to catalytic ozone destruction by providing surfaces for the conversion of inert chlorine species into active forms and by denitrification. The latter describes the removal of HNO3 from the stratosphere by sedimenting PSC particles, which hinders chlorine deactivation by the formation of reservoir species. Therefore, an accurate representation of PSCs in chemistry–climate models (CCMs) is of great importance to correctly simulate polar ozone concentrations. Here, we evaluate PSCs as simulated by the CCM SOCOLv3.1 for the Antarctic winters 2006, 2007 and 2010 by comparison with backscatter measurements by CALIOP on board the CALIPSO satellite. The year 2007 represents a typical Antarctic winter, while 2006 and 2010 are characterized by above- and below-average PSC occurrence. The model considers supercooled ternary solution (STS) droplets, nitric acid trihydrate (NAT) particles, water ice particles and mixtures thereof. PSCs are parameterized in terms of temperature and partial pressures of HNO3 and H2O, assuming equilibrium between the gas and particulate phase. The PSC scheme involves a set of prescribed microphysical parameters, namely ice number density, NAT particle radius and maximum NAT number density. In this study, we test and optimize the parameter settings through several sensitivity simulations. The choice of the value for the ice number density affects simulated optical properties and dehydration, while modifying the NAT parameters impacts stratospheric composition via HNO3 uptake and denitrification. Depending on the NAT parameters, reasonable denitrification can be modeled. However, its impact on ozone loss is minor. The best agreement with the CALIOP optical properties and observed denitrification was for this case study found with the ice number density increased from the hitherto used value of 0.01 to 0.05 cm−3 and the maximum NAT number density from 5×10-4 to 1×10-3 cm−3. The NAT radius was kept at the original value of 5 µm. The new parameterization reflects the higher importance attributed to heterogeneous nucleation of ice and NAT particles following recent new data evaluations of the state-of-the-art CALIOP measurements. A cold temperature bias in the polar lower stratosphere results in an overestimated PSC areal coverage in SOCOLv3.1 by up to 40 %. Offsetting this cold bias by +3 K delays the onset of ozone depletion by about 2 weeks, which improves the agreement with observations. Furthermore, the occurrence of mountain-wave-induced ice, as observed mainly over the Antarctic Peninsula, is continuously underestimated in the model due to the coarse model resolution (T42L39) and the fixed ice number density. Nevertheless, we find overall good temporal and spatial agreement between modeled and observed PSC occurrence and composition. This work confirms previous studies indicating that simplified PSC schemes, which avoid nucleation and growth calculations in sophisticated but time-consuming microphysical process models, may also achieve good approximations of the fundamental properties of PSCs needed in CCMs.

Ice Particle Formation in the Lower Stratosphere

Field observation data on aerosol ice particles in the lower stratosphere and the results of laboratory modeling of their microphysics are considered. A model of ice particle formation in the lower stratosphere is described using classical nucleation theory. The results of computational experiments indicate that the formation of the ice phase in supercooled ternary solutions can occur only if these liquid particles are supercooled (~3 K), which is consistent with the data from field observation data.

Widespread polar stratospheric ice clouds in the 2015–2016 Arctic winter – implications for ice nucleation

Abstract. Low planetary wave activity led to a stable vortex with exceptionally cold temperatures in the 2015–2016 Arctic winter. Extended areas with temperatures below the ice frost point temperature Tice persisted over weeks in the Arctic stratosphere as derived from the 36-year temperature climatology of the ERA-Interim reanalysis data set of the European Centre for Medium-Range Weather Forecasts (ECMWF). These extreme conditions promoted the formation of widespread polar stratospheric ice clouds (ice PSCs). The space-borne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument on board the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) satellite continuously measured ice PSCs for about a month with maximum extensions of up to 2×106 km2 in the stratosphere. On 22 January 2016, the WALES (Water Vapor Lidar Experiment in Space – airborne demonstrator) lidar on board the High Altitude and Long Range Research Aircraft HALO detected an ice PSC with a horizontal length of more than 1400 km. The ice PSC extended between 18 and 24 km altitude and was surrounded by nitric acid trihydrate (NAT) particles, supercooled ternary solution (STS) droplets and particle mixtures. The ice PSC occurrence histogram in the backscatter ratio to particle depolarization ratio optical space exhibits two ice modes with high or low particle depolarization ratios. Domain-filling 8-day back-trajectories starting in the high particle depolarization (high-depol) ice mode are continuously below the NAT equilibrium temperature TNAT and decrease below Tice∼10 h prior to the observation. Their matches with CALIPSO PSC curtain plots demonstrate the presence of NAT PSCs prior to high-depol ice, suggesting that the ice had nucleated on NAT. Vice versa, STS or no PSCs were detected by CALIPSO prior to the ice mode with low particle depolarization ratio. In addition to ice nucleation in STS potentially having meteoric inclusions, we find evidence for ice nucleation on NAT in the Arctic winter 2015–2016. The observation of widespread Arctic ice PSCs with high or low particle depolarization ratios advances our understanding of ice nucleation in polar latitudes. It further provides a new observational database for the parameterization of ice nucleation schemes in atmospheric models.

The MIPAS/Envisat climatology (2002–2012) of polar stratospheric cloud volume density profiles

Abstract. A global data set of vertical profiles of polar stratospheric cloud (PSC) volume density has been derived from Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) space-borne infrared limb measurements between 2002 and 2012. To develop a well characterized and efficient retrieval scheme, systematic tests based on limb-radiance simulations for PSCs from in situ balloon observations have been performed. The finally selected wavenumber range was 831–832.5 cm−1. Optical constants of nitric acid trihydrate (NAT) have been used to derive maximum and minimum profiles of volume density which are compatible with MIPAS observations under the assumption of small, non-scattering and larger, scattering PSC particles. These max/min profiles deviate from their mean value at each altitude by about 40 %–45 %, which is attributed as the maximum systematic error of the retrieval. Further, the retrieved volume density profiles are characterized by a random error due to instrumental noise of 0.02–0.05 µm3 cm−3, a detection limit of about 0.1–0.2 µm3 cm−3 and a vertical resolution of around 3 km. Comparisons with coincident observations by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) on the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) satellite showed good agreement regarding the vertical profile shape. Quantitatively, in the case of supercooled ternary solution (STS) PSCs, the CALIOP dataset fits to the MIPAS retrievals obtained under the assumptions of small particles. Unlike for STS and NAT, in the case of ice PSCs the MIPAS retrievals are limited by the clouds becoming optically thick in the limb-direction. In these cases, the MIPAS volume densities represent lower limits. Among other interesting features, this climatology helps to study quantitatively the on-set of PSC formation very near to the South Pole and the large variability of the PSC volume densities between different Arctic stratospheric winters.

Accuracy and precision of polar lower stratospheric temperatures from reanalyses evaluated from A-Train CALIOP and MLS, COSMIC GPS RO, and the equilibrium thermodynamics of supercooled ternary solutions and ice clouds

Abstract. We investigate the accuracy and precision of polar lower stratospheric temperatures (100–10 hPa during 2008–2013) reported in several contemporary reanalysis datasets comprising two versions of the Modern-Era Retrospective analysis for Research and Applications (MERRA and MERRA-2), the Japanese 55-year Reanalysis (JRA-55), the European Centre for Medium-Range Weather Forecasts (ECMWF) interim reanalysis (ERA-I), and the National Oceanic and Atmospheric Administration (NOAA) National Centers for Environmental Prediction (NCEP) Climate Forecast System Reanalysis (NCEP-CFSR). We also include the Goddard Earth Observing System model version 5.9.1 near-real-time analysis (GEOS-5.9.1). Comparisons of these datasets are made with respect to retrieved temperatures from the Aura Microwave Limb Sounder (MLS), Constellation Observing System for Meteorology, Ionosphere and Climate (COSMIC) Global Positioning System (GPS) radio occultation (RO) temperatures, and independent absolute temperature references defined by the equilibrium thermodynamics of supercooled ternary solutions (STSs) and ice clouds. Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) observations of polar stratospheric clouds are used to determine the cloud particle types within the Aura MLS geometric field of view. The thermodynamic calculations for STS and the ice frost point use the colocated MLS gas-phase measurements of HNO3 and H2O. The estimated bias and precision for the STS temperature reference, over the 68 to 21 hPa pressure range, are 0.6–1.5 and 0.3–0.6 K, respectively; for the ice temperature reference, they are 0.4 and 0.3 K, respectively. These uncertainties are smaller than those estimated for the retrieved MLS temperatures and also comparable to GPS RO uncertainties (bias < 0.2 K, precision > 0.7 K) in the same pressure range. We examine a case study of the time-varying temperature structure associated with layered ice clouds formed by orographic gravity waves forced by flow over the Palmer Peninsula and compare how the wave amplitudes are reproduced by each reanalysis dataset. We find that the spatial and temporal distribution of temperatures below the ice frost point, and hence the potential to form ice polar stratospheric clouds (PSCs) in model studies driven by the reanalyses, varies significantly because of the underlying differences in the representation of mountain wave activity. High-accuracy COSMIC temperatures are used as a common reference to intercompare the reanalysis temperatures. Over the 68–21 hPa pressure range, the biases of the reanalyses with respect to COSMIC temperatures for both polar regions fall within the narrow range of −0.6 K to +0.5 K. GEOS-5.9.1, MERRA, MERRA-2, and JRA-55 have predominantly cold biases, whereas ERA-I has a predominantly warm bias. NCEP-CFSR has a warm bias in the Arctic but becomes substantially colder in the Antarctic. Reanalysis temperatures are also compared with the PSC reference temperatures. Over the 68–21 hPa pressure range, the reanalysis temperature biases are in the range −1.6 to −0.3 K with standard deviations ∼ 0.6 K for the CALIOP STS reference, and in the range −0.9 to +0.1 K with standard deviations ∼ 0.7 K for the CALIOP ice reference. Comparisons of MLS temperatures with the PSC reference temperatures reveal vertical oscillations in the MLS temperatures and a significant low bias in MLS temperatures of up to 3 K.

Development of a Polar Stratospheric Cloud Model Within the Community Earth System Model: Assessment of 2010 Antarctic Winter

AbstractTo simulate polar stratospheric clouds (PSCs) during the Antarctic winter of 2010, we have developed a PSC model within the Community Earth System Model framework that includes detailed microphysics of sulfuric aerosols and three types of PSCs: supercooled ternary solution (STS), nitric acid trihydrate (NAT), and ice. Our model includes two major NAT formation mechanisms, both of which are essential to reproduce the PSC and gas phase chemical features in the 2010 Antarctic winter. Homogeneous nucleation of NAT from STS produces NAT particles with sizes near 8 μm, which are important to properly simulate denitrification and the gas phase HNO3 observed by the Microwave Limb Sounder (MLS). Heterogeneous nucleation of NAT on ice particles or ice particles on NAT and subsequent evaporation of the ice produces NAT particles with sizes from submicrometers to a few micrometers. These particles account for the large backscattering ratio from NAT observed by the Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observations satellite, especially in the midwinter season. Adding temperature fluctuations from gravity waves is important to produce larger number density and higher backscattering ratio from ice and NAT particles. However, our model needs a better representation of waves to improve the backscattering ratio and gas phase HNO3 compared with observations. Our model also includes homogeneous nucleation of ice from STS and heterogeneous nucleation of ice on NAT. The model reproduces the gas phase H2O during the winter within the uncertainty of the MLS observations.

Comparing simulated PSC optical properties with CALIPSO observations during the 2010 Antarctic winter

AbstractWe simulate polar stratospheric clouds (PSCs) during the Antarctic winter of 2010 using the Specified Dynamics version of the Whole Atmosphere Community Climate Model/Community Aerosol and Radiation Model for Atmospheres (SD‐WACCM/CARMA) model. The current PSC model contains microphysical schemes for supercooled ternary solutions (STS) and nitric acid trihydrate (NAT) particles, as well as a prognostic treatment for PSC ice particles and dehydration. Our simulations and CALIPSO satellite data suggest two major NAT particle formation mechanisms. The first mechanism is the nucleation of NAT from STS. Our model, with homogeneous nucleation rates of NAT from STS constrained by observations from the Arctic winter of 2010–2011, reproduces optical properties observed by CALIPSO over Antarctica in May and the timing of denitrification observed by the Microwave Limb Sounder within their uncertainties. On the other hand, the CALIPSO data indicate that our simulations are missing clouds containing small NAT particles with large number densities. We suggest these particles are most likely to form from ice clouds or STS in gravity waves, as found by previous investigations. The simulated cloud coverage agrees with the CALIPSO cloud coverage within a few percent on average with a correlation coefficient of 0.83. However, using the CALIPSO classification algorithm, simulated ice clouds often fall into Mix categories under the denitrified and dehydrated conditions. The model needs an improved ice microphysical representation, not only to allow ice particles to be a source of NAT but also to provide information on ice cloud particle number and size so that ice cloud optical properties can be more precisely calculated for comparison with CALIPSO data.

Interannual variations of early winter Antarctic polar stratospheric cloud formation and nitric acid observed by CALIOP and MLS

Abstract. We use satellite-borne measurements collected over the last decade (2006–2015) from the Aura Microwave Limb Sounder (MLS) and the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) to investigate the nitric acid distribution and the properties of polar stratospheric clouds (PSCs) in the early winter Antarctic vortex. Frequently, at the very start of the winter, we find that synoptic-scale depletion of HNO3 can be detected in the inner vortex before the first lidar detection of geophysically associated PSCs. The generation of "sub-visible" PSCs can be explained as arising from the development of a solid particle population with low number densities and large particle sizes. Assumed to be composed of nitric acid trihydrate (NAT), the sub-visible PSCs form at ambient temperatures well above the ice frost point, but also above the temperature at which supercooled ternary solution (STS) grows out of the background supercooled binary solution (SBS) distribution. The temperature regime of their formation, inferred from the simultaneous uptake of ambient HNO3 into NAT and their Lagrangian temperature histories, is at a depression of a few kelvin with respect to the NAT existence threshold, TNAT. Therefore, their nucleation requires a considerable supersaturation of HNO3 over NAT, and is consistent with a recently described heterogeneous nucleation process on solid foreign nuclei immersed in liquid aerosol. We make a detailed investigation of the comparative limits of detection of PSCs and the resulting sequestration of HNO3 imposed by lidar, mid-infrared, and microwave techniques. We find that the temperature history of air parcels, in addition to the local ambient temperature, is an important factor in the relative frequency of formation of liquid/solid PSCs. We conclude that the initiation of NAT nucleation and the subsequent development of large NAT particles capable of sedimentation and denitrification in the early winter do not emanate from an ice-seeding process. Finally, we investigate the patterns of interannual variability and compare the relative formation frequency of liquid and solid PSCs in the Antarctic lower polar stratosphere using the results of a cluster analysis to synthesize the combined CALIOP and MLS measurements into a relatively small number of interrelated categories.

A multi-wavelength classification method for polar stratospheric cloud types using infrared limb spectra

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument on board the ESA Envisat satellite operated from July 2002 until April 2012. The infrared limb emission measurements represent a unique dataset of daytime and night-time observations of polar stratospheric clouds (PSCs) up to both poles. Cloud detection sensitivity is comparable to space-borne lidars, and it is possible to classify different cloud types from the spectral measurements in different atmospheric windows regions. Here we present a new infrared PSC classification scheme based on the combination of a well-established two-colour ratio method and multiple 2-D brightness temperature difference probability density functions. The method is a simple probabilistic classifier based on Bayes' theorem with a strong independence assumption. The method has been tested in conjunction with a database of radiative transfer model calculations of realistic PSC particle size distributions, geometries, and composition. The Bayesian classifier distinguishes between solid particles of ice and nitric acid trihydrate (NAT), as well as liquid droplets of super-cooled ternary solution (STS). The classification results are compared to coincident measurements from the space-borne lidar Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument over the temporal overlap of both satellite missions (June 2006–March 2012). Both datasets show a good agreement for the specific PSC classes, although the viewing geometries and the vertical and horizontal resolution are quite different. Discrepancies are observed between the CALIOP and the MIPAS ice class. The Bayesian classifier for MIPAS identifies substantially more ice clouds in the Southern Hemisphere polar vortex than CALIOP. This disagreement is attributed in part to the difference in the sensitivity on mixed-type clouds. Ice seems to dominate the spectral behaviour in the limb infrared spectra and may cause an overestimation in ice occurrence compared to the real fraction of ice within the PSC area in the polar vortex. The entire MIPAS measurement period was processed with the new classification approach. Examples like the detection of the Antarctic NAT belt during early winter, and its possible link to mountain wave events over the Antarctic Peninsula, which are observed by the Atmospheric Infrared Sounder (AIRS) instrument, highlight the importance of a climatology of 9 Southern Hemisphere and 10 Northern Hemisphere winters in total. The new dataset is valuable both for detailed process studies, and for comparisons with and improvements of the PSC parameterizations used in chemistry transport and climate models.

Effects of polar stratospheric clouds in the Nimbus 7 LIMS Version 6 data set

Abstract. The historic Limb Infrared Monitor of the Stratosphere (LIMS) measurements of 1978–1979 from the Nimbus 7 satellite were re-processed with Version 6 (V6) algorithms and archived in 2002. The V6 data set employs updated radiance registration methods, improved spectroscopic line parameters, and a common vertical resolution for all retrieved parameters. Retrieved profiles are spaced about every 1.6° of latitude along orbits and include the additional parameter of geopotential height. Profiles of O3 are sensitive to perturbations from emissions of polar stratospheric clouds (PSCs). This work presents results of implementing a first-order screening for effects of PSCs using simple algorithms based on vertical gradients of the O3 mixing ratio. Their occurrences are compared with the co-located, retrieved temperatures and related to the temperature thresholds needed for saturation of H2O and/or HNO3 vapor onto PSC particles. Observed daily locations where the major PSC screening criteria are satisfied are validated against PSCs observed with the Stratospheric Aerosol Monitor (SAM) II experiment also on Nimbus 7. Remnants of emissions from PSCs are characterized for O3 and HNO3 following the screening. PSCs may also impart a warm bias in the co-located LIMS temperatures, but by no more than 1–2 K at the altitudes of where effects of PSCs are a maximum in the ozone; thus, no PSC screening was applied to the V6 temperatures. Minimum temperatures vary between 187 and 194 K and often occur 1 to 2 km above where PSC effects are first identified in the ozone (most often between about 21 and 28 hPa). Those temperature–pressure values are consistent with conditions for the existence of nitric acid trihydrate (NAT) mixtures and to a lesser extent of super-cooled ternary solution (STS) droplets. A local, temporary uptake of HNO3 vapor of order 1–3 ppbv is indicated during mid-January for the 550 K surface. Seven-month time series of the distributions of LIMS O3 and HNO3 are shown based on their gridded Level 3 data following the PSC screening. Zonal coefficients of both species are essentially free of effects from PSCs on the 550 K surface, based on their average values along PV contours and in terms of equivalent latitude. Remnants of PSCs are still present in O3 on the 450 K surface during mid-January. It is judged that the LIMS Level 3 data are of good quality for analyzing the larger-scale, stratospheric chemistry and transport processes during the Arctic winter of 1978–1979.

The role of sulfate aerosol in the formation of cloudiness over the sea

We estimate the impact of sulfate aerosols on cloudiness formation over the sea in the middle troposphere and the involvement of these particles in the formation of polar stratospheric clouds (PSCs) in the lower stratosphere. The first of these problems is solved using a combined model of moist convection and the formation of cloudiness and sulfate aerosols in the troposphere and lower stratosphere over the sea, incorporating natural emissions of sulfur-containing compounds. We have found that a significant source of condensation nuclei in the troposphere is the photochemical transformation of biogenic dimethyl sulfide (in addition to NaCl). The results of numerical experiments indicate that the absence of sulfate aerosols hinders the cloudiness formation over the sea in the middle and upper troposphere. The problem of sulfate aerosol involvement in the formation of supercooled ternary solutions (STSs) (PSC Type Ib) in the lower stratosphere is solved using a mathematical model of global transport of multicomponent gas pollutants and aerosols in the atmosphere. Using the combined model, numerical experiments were performed for the winter season in both hemispheres. Sulfate aerosols were found to really participate in the formation of STS particles. Without their participation, the formation of STS particles in the lower stratosphere would be hindered. We present the results of numerical calculations and discuss the distribution of concentrations of gaseous nitric and sulfuric acids, as well as mass concentrations of these components in STS particles.