Airborne in situ measurements of ice particles in the tropical tropopause layer

Ice clouds have a strong effect on the Earth-atmosphere radiative energy balance, on the distribution of condensable gases in the atmosphere, as well as on the chemical composition of the air. The ice particles in these clouds can take on a variety of shapes which makes the description of the cloud microphysical properties more difficult. In the tropical upper troposphere/lower stratosphere (UTLS), a region where ice cloud abundance is relatively high, different types of ice clouds can be observed. However, in situ measurements are rare due to the high altitude of these clouds and the few available research aircraft, only three worldwide, that can fly at such altitudes.rnThis work focuses on in situ measurements of the tropical UTLS clouds performedrnwith a Cloud Imaging Probe (CIP) and a Forward Scattering Spectrometer Probern(FSSP-100), whereof the CIP is the key instrument of this thesis. The CIP is anrnairborne in situ instrument that obtains two-dimensional shadow images of cloud particles. Several cloud microphysical parameters can be derived from these measurements, e.g. number concentrations and size distributions. In order to obtain a high quality data set, a careful image analysis and several corrections need to be applied to the CIP observations. These methods are described in detail.rnMeasurements within the tropical UTLS have been performed during two campaigns:rnSCOUT-O3, 2005 in Northern Australia and SCOUT-AMMA, 2006 inWest Africa. Thernobtained data set includes first observations of subvisible cirrus clouds over a continental area and observations of the anvils of deep convective clouds. The latter can be further divided into clouds in mesoscale convective system outflows of different ages and clouds in overshooting cloud turrets that even penetrated the stratosphere. The microphysical properties of these three cloud types are discussed in detail. Furthermore, the vertical structure of the ice clouds in the UTLS is investigated. The values of the microphysical parameters were found to decrease with increasing altitude in the upper troposphere. Particle numbers and maximum sizes were also decreasing with increasing age of the outflow clouds. Further differences between the deep convective clouds and subvisible cirrus were found in the particle morphology as well as in the ratio of the observed aerosol particles to cloud particles which indicates that the different freezing processes (deposition, contact, immersion freezing) play different roles in the formation of the respective clouds. For the achievementrnof a better microphysical characterisation and description numerical fits have been adjusted onto the cloud particle size distributions of the subvisible cirrus as well as on the size distributions of the clouds at different altitudes in the UTLS.

Micrometer-sized ice particles for planetary-science experiments – II. Bidirectional reflectance

We have measured the bidirectional reflectance of spherical micrometer-sized water-ice particles in the visible spectral range over a wide range of incidence and emission angles. The small ice spheres were produced by spraying fine water droplets directly into liquid nitrogen. The resulting mean particle radii are 1.47 + 0.96 - 0.58 μm. Such a material shares many properties with ice in comets and at the surface of icy satellites. Measurements show that the fresh sample material is highly backscattering, contrasting with natural terrestrial snow and frost. The formation of agglomerates of particles during the sample production results in a noticeable variability of the photometric properties of the samples in their initial state. We have also observed significant temporal evolutions of the scattering behavior of the samples, shifting towards more forward scattering within some tens of hours, resulting most likely from sintering processes. All reflectance data are fitted by the Hapke photometric model (1993 and 2002 formulation) with a one/two/three-parameter Henyey-Greenstein phase function and the resulting Hapke parameters are provided. These parameters can be used to compare laboratory results with the observed photometric behaviors of astronomical objects. We show, in particular, that the optical properties of the fresh micrometer-sized ice samples can be used to reproduce the predominant backscattering in the phase curves of Enceladus and Europa.

Microphysical properties of cold frontal rainbands

Observations have been obtained within an intense (precipitation rates > 50 mm h−1 ) narrow cold-frontal rainband (NCFR) embedded within a broader region of stratiform precipitation. In situ data were obtained from an aircraft which flew near a steerable dual-polarisation Doppler radar. The observations were obtained to characterise the microphysical properties of cold frontal clouds, with an emphasis on ice and precipitation formation and development. Primary ice nucleation near cloud top (−55◦ C) appeared to be enhanced by convective features. However, ice multiplication led to the largest ice particle number concentrations being observed at relatively high temperatures (> −10◦ C). The multiplication process (most likely rime splintering) occurs when stratiform precipitation interacts with supercooled water generated in the NCFR. Graupel was notably absent in the data obtained. Ice multiplication processes are known to have a strong impact in glaciating isolated convective clouds, but have rarely been studied within larger organised convective systems such as NCFRs. Secondary ice particles will impact on precipitation formation and cloud dynamics due to their relatively small size and high number density. Further modelling studies are required to quantify the effects of rime splintering on precipitation and dynamics in frontal rainbands. Available parametrizations used to diagnose the particle size distributions do not account for the influence of ice multiplication. This deficiency in parametrizations is likely to be important in some cases for modelling the evolution of cloud systems and the precipitation formation. Ice multiplication has significant impact on artefact removal from in situ particle imaging probes.

Impact of biomass burning aerosols on precipitation in the Amazon: A modeling case study

A study of the potential role of aerosols in modifying clouds and precipitation is presented using a numerical atmospheric model. Measurements of cloud condensation nuclei (CCN) and cloud size distribution properties taken in the southwestern Amazon region during the transition from dry to wet seasons were used as guidelines to define the microphysical parameters for the simulations. Numerical simulations were carried out using the Brazilian Development on Regional Atmospheric Modeling System, and the results presented considerable sensitivity to changes in these parameters. High CCN concentrations, typical of polluted days, were found to result in increases or decreases in total precipitation, depending on the level of pollution used as a reference, showing a complexity that parallels the aerosol-precipitation interaction. Our results show that on the grids evaluated, higher CCN concentrations reduced low-to-moderate rainfall rates and increased high rainfall rates. The principal consequence of the increased pollution was a change from a warm to a cold rain process, which affected the maximum and overall mean accumulated precipitation. Under polluted conditions, cloud cover diminished, allowing greater amounts of solar radiation to reach the surface. Aerosol absorption of radiation in the lower layers of the atmosphere delayed convective evolution but produced higher maximum rainfall rates due to increased instability. In addition, the intensity of the surface sensible heat flux, as well as that of the latent heat flux, was reduced by the lower temperature difference between surface and air, producing greater energy stores at the surface.

Observations of ice multiplication in a weakly convective cell embedded in supercooled mid-level stratus

Simultaneous observations of cloud microphysical properties were obtained by in-situ aircraft measurements and ground based Radar/Lidar. Widespread mid-level stratus cloud was present below a temperature inversion (~5 °C magnitude) at 3.6 km altitude. Localised convection (peak updraft 1.5 m s−1) was observed 20 km west of the Radar station. This was associated with convergence at 2.5 km altitude. The convection was unable to penetrate the inversion capping the mid-level stratus. The mid-level stratus cloud was vertically thin (~400 m), horizontally extensive (covering 100 s of km) and persisted for more than 24 h. The cloud consisted of supercooled water droplets and small concentrations of large (~1 mm) stellar/plate like ice which slowly precipitated out. This ice was nucleated at temperatures greater than −12.2 °C and less than −10.0 °C, (cloud top and cloud base temperatures, respectively). No ice seeding from above the cloud layer was observed. This ice was formed by primary nucleation, either through the entrainment of efficient ice nuclei from above/below cloud, or by the slow stochastic activation of immersion freezing ice nuclei contained within the supercooled drops. Above cloud top significant concentrations of sub-micron aerosol were observed and consisted of a mixture of sulphate and carbonaceous material, a potential source of ice nuclei. Particle number concentrations (in the size range 0.1Ice crystal concentrations in the cloud were constant at around 0.2 L−1. It is estimated that entrainment of aerosol particles into cloud cannot replenish the loss of ice nuclei from the cloud layer via precipitation. Precipitation from the mid-level stratus evaporated before reaching the surface, whereas rates of up to 1 mm h−1 were observed below the convective feature. There is strong evidence for the Hallett-Mossop (HM) process of secondary ice particle production leading to the formation of the precipitation observed. This includes (1) Ice concentrations in the convective feature were more than an order of magnitude greater than the concentration of primary ice in the overlaying stratus, (2) Large concentrations of small pristine columns were observed at the ~−5 °C level together with liquid water droplets and a few rimed ice particles, (3) Columns were larger and increasingly rimed at colder temperatures. Calculated ice splinter production rates are consistent with observed concentrations if the condition that only droplets greater than 24 μm are capable of generating secondary ice splinters is relaxed. This case demonstrates the importance of understanding the formation of ice at slightly supercooled temperatures, as it can lead to secondary ice production and the formation of precipitation in clouds which may not otherwise be considered as significant precipitation sources.

Ice formation and development in aged, wintertime cumulus over the UK: observations and modelling

In situ high resolution aircraft measurements of cloud microphysical properties were made in coordination with ground based remote sensing observations of a line of small cumulus clouds, using Radar and Lidar, as part of the Aerosol Properties, PRocesses And InfluenceS on the Earth's climate (APPRAISE) project. A narrow but extensive line (~100 km long) of shallow convective clouds over the southern UK was studied. Cloud top temperatures were observed to be higher than −8 °C, but the clouds were seen to consist of supercooled droplets and varying concentrations of ice particles. No ice particles were observed to be falling into the cloud tops from above. Current parameterisations of ice nuclei (IN) numbers predict too few particles will be active as ice nuclei to account for ice particle concentrations at the observed, near cloud top, temperatures (−7.5 °C). The role of mineral dust particles, consistent with concentrations observed near the surface, acting as high temperature IN is considered important in this case. It was found that very high concentrations of ice particles (up to 100 L−1) could be produced by secondary ice particle production providing the observed small amount of primary ice (about 0.01 L−1) was present to initiate it. This emphasises the need to understand primary ice formation in slightly supercooled clouds. It is shown using simple calculations that the Hallett-Mossop process (HM) is the likely source of the secondary ice. Model simulations of the case study were performed with the Aerosol Cloud and Precipitation Interactions Model (ACPIM). These parcel model investigations confirmed the HM process to be a very important mechanism for producing the observed high ice concentrations. A key step in generating the high concentrations was the process of collision and coalescence of rain drops, which once formed fell rapidly through the cloud, collecting ice particles which caused them to freeze and form instant large riming particles. The broadening of the droplet size-distribution by collision-coalescence was, therefore, a vital step in this process as this was required to generate the large number of ice crystals observed in the time available. Simulations were also performed with the WRF (Weather, Research and Forecasting) model. The results showed that while HM does act to increase the mass and number concentration of ice particles in these model simulations it was not found to be critical for the formation of precipitation. However, the WRF simulations produced a cloud top that was too cold and this, combined with the assumption of continual replenishing of ice nuclei removed by ice crystal formation, resulted in too many ice crystals forming by primary nucleation compared to the observations and parcel modelling.

Li distribution characterization in Li-ion batteries positive electrodes containing LixNi0.8Co0.15Al0.05O2 secondary particles

The elemental distribution of as-received (non-charged) and charged Li-ion battery positive electrodes containing LixNi0.8Co0.15Al0.05O2 (0.75 ? x ? 1.0) microparticles as active material is characterized by combining μ-PIXE and μ-PIGE techniques. PIGE measurements evidence that the Li distribution is inhomogeneous (existence of Li-rich and Li-depleted regions) in as-received electrodes corresponding with the distribution of secondary particles but it is homogeneous within the studied individual secondary micro-particles. The dependence of the Li distribution on electrode thickness and on charging conditions is characterized by measuring the Li distribution maps in specifically fabricated cross-sectional samples. These data show that decreasing the electrode thickness down to 35 μm and charging the batteries at slow rate give rise to more homogeneous Li depth profiles.

Theory and observations of ice particle evolution in cirrus using Doppler radar: evidence for aggregation

Vertically pointing Doppler radar has been used to study the evolution of ice particles as they sediment through a cirrus cloud. The measured Doppler fall speeds, together with radar-derived estimates for the altitude of cloud top, are used to estimate a characteristic fall time tc for the `average' ice particle. The change in radar reflectivity Z is studied as a function of tc, and is found to increase exponentially with fall time. We use the idea of dynamically scaling particle size distributions to show that this behaviour implies exponential growth of the average particle size, and argue that this exponential growth is a signature of ice crystal aggregation.

Observations of the depth of ice particle evaporation beneath frontal cloud to improve NWP modelling

The evaporation (sublimation) of ice particles beneath frontal ice cloud can provide a significant source of diabatic cooling which can lead to enhanced slantwise descent below the frontal surface. The strength and vertical extent of the cooling play a role in determining the dynamic response of the atmosphere, and an adequate representation is required in numerical weather-prediction (NWP) models for accurate forecasts of frontal dynamics. In this paper, data from a vertically pointing 94 GHz radar are used to determine the characteristic depth-scale of ice particle sublimation beneath frontal ice cloud. A statistical comparison is made with equivalent data extracted from the NWP mesoscale model operational at the Met Office, defining the evaporation depth-scale as the distance for the ice water content to fall to 10% of its peak value in the cloud. The results show that the depth of the ice evaporation zone derived from observations is less than 1 km for 90% of the time. The model significantly overestimates the sublimation depth-scales by a factor of between two and three, and underestimates the local ice water content by a factor of between two and four. Consequently the results suggest the model significantly underestimates the strength of the evaporative cooling, with implications for the prediction of frontal dynamics. A number of reasons for the model discrepancy are suggested. A comparison with radiosonde relative humidity data suggests part of the overestimation in evaporation depth may be due to a high RH bias in the dry slot beneath the frontal cloud, but other possible reasons include poor vertical resolution and deficiencies in the evaporation rate or ice particle fall-speed parametrizations.

The retrieval of ice water content from radar reflectivity factor and temperature and its use in evaluating a mesoscale model

Ice clouds are an important yet largely unvalidated component of weather forecasting and climate models, but radar offers the potential to provide the necessary data to evaluate them. First in this paper, coordinated aircraft in situ measurements and scans by a 3-GHz radar are presented, demonstrating that, for stratiform midlatitude ice clouds, radar reflectivity in the Rayleigh-scattering regime may be reliably calculated from aircraft size spectra if the "Brown and Francis" mass-size relationship is used. The comparisons spanned radar reflectivity values from -15 to +20 dBZ, ice water contents (IWCs) from 0.01 to 0.4 g m(-3), and median volumetric diameters between 0.2 and 3 mm. In mixed-phase conditions the agreement is much poorer because of the higher-density ice particles present. A large midlatitude aircraft dataset is then used to derive expressions that relate radar reflectivity and temperature to ice water content and visible extinction coefficient. The analysis is an advance over previous work in several ways: the retrievals vary smoothly with both input parameters, different relationships are derived for the common radar frequencies of 3, 35, and 94 GHz, and the problem of retrieving the long-term mean and the horizontal variance of ice cloud parameters is considered separately. It is shown that the dependence on temperature arises because of the temperature dependence of the number concentration "intercept parameter" rather than mean particle size. A comparison is presented of ice water content derived from scanning 3-GHz radar with the values held in the Met Office mesoscale forecast model, for eight precipitating cases spanning 39 h over Southern England. It is found that the model predicted mean I WC to within 10% of the observations at temperatures between -30 degrees and - 10 degrees C but tended to underestimate it by around a factor of 2 at colder temperatures.

Using Doppler radar with a simple explicit microphysics model to diagnose problems with ice sublimation depth-scales in forecast models

Several previous studies have attempted to assess the sublimation depth-scales of ice particles from clouds into clear air. Upon examining the sublimation depth-scales in the Met Office Unified Model (MetUM), it was found that the MetUM has evaporation depth-scales 2–3 times larger than radar observations. Similar results can be seen in the European Centre for Medium-Range Weather Forecasts (ECMWF), Regional Atmospheric Climate Model (RACMO) and Météo-France models. In this study, we use radar simulation (converting model variables into radar observations) and one-dimensional explicit microphysics numerical modelling to test and diagnose the cause of the deep sublimation depth-scales in the forecast model. The MetUM data and parametrization scheme are used to predict terminal velocity, which can be compared with the observed Doppler velocity. This can then be used to test the hypothesis as to why the sublimation depth-scale is too large within the MetUM. Turbulence could lead to dry air entrainment and higher evaporation rates; particle density may be wrong, particle capacitance may be too high and lead to incorrect evaporation rates or the humidity within the sublimating layer may be incorrectly represented. We show that the most likely cause of deep sublimation zones is an incorrect representation of model humidity in the layer. This is tested further by using a one-dimensional explicit microphysics model, which tests the sensitivity of ice sublimation to key atmospheric variables and is capable of including sonde and radar measurements to simulate real cases. Results suggest that the MetUM grid resolution at ice cloud altitudes is not sufficient enough to maintain the sharp drop in humidity that is observed in the sublimation zone.

Advancements in the estimation of ice particle fall speeds using laboratory and field measurements

Accurate estimates for the fall speed of natural hydrometeors are vital if their evolution in clouds is to be understood quantitatively. In this study, laboratory measurements of the terminal velocity vt for a variety of ice particle models settling in viscous fluids, along with wind-tunnel and field measurements of ice particles settling in air, have been analyzed and compared to common methods of computing vt from the literature. It is observed that while these methods work well for a number of particle types, they fail for particles with open geometries, specifically those particles for which the area ratio Ar is small (Ar is defined as the area of the particle projected normal to the flow divided by the area of a circumscribing disc). In particular, the fall speeds of stellar and dendritic crystals, needles, open bullet rosettes, and low-density aggregates are all overestimated. These particle types are important in many cloud types: aggregates in particular often dominate snow precipitation at the ground and vertically pointing Doppler radar measurements. Based on the laboratory data, a simple modification to previous computational methods is proposed, based on the area ratio. This new method collapses the available drag data onto an approximately universal curve, and the resulting errors in the computed fall speeds relative to the tank data are less than 25% in all cases. Comparison with the (much more scattered) measurements of ice particles falling in air show strong support for this new method, with the area ratio bias apparently eliminated.

Evidence that ice forms primarily in supercooled liquid clouds at temperatures > -27C

Using 4 years of radar and lidar observations of layer clouds from the Chilbolton Observatory in the UK, we show that almost all (95%) ice particles formed at temperatures >-20°C appear to originate from supercooled liquid clouds. At colder temperatures, there is a monotonic decline in the fraction of liquid-topped ice clouds: 50% at -27°C, falling to zero at -37°C (where homogeneous freezing of water droplets occurs). This strongly suggests that deposition nucleation plays a relatively minor role in the initiation of ice in mid-level clouds. It also means that the initial growth of the ice particles occurs predominantly within a liquid cloud, a situation which promotes rapid production of precipitation via the Bergeron-Findeison mechanism.

A comparison among four different retrieval methods for ice-cloud properties using data from CloudSat, CALIPSO, and MODIS

The A-Train constellation of satellites provides a new capability to measure vertical cloud profiles that leads to more detailed information on ice-cloud microphysical properties than has been possible up to now. A variational radar–lidar ice-cloud retrieval algorithm (VarCloud) takes advantage of the complementary nature of the CloudSat radar and Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) lidar to provide a seamless retrieval of ice water content, effective radius, and extinction coefficient from the thinnest cirrus (seen only by the lidar) to the thickest ice cloud (penetrated only by the radar). In this paper, several versions of the VarCloud retrieval are compared with the CloudSat standard ice-only retrieval of ice water content, two empirical formulas that derive ice water content from radar reflectivity and temperature, and retrievals of vertically integrated properties from the Moderate Resolution Imaging Spectroradiometer (MODIS) radiometer. The retrieved variables typically agree to within a factor of 2, on average, and most of the differences can be explained by the different microphysical assumptions. For example, the ice water content comparison illustrates the sensitivity of the retrievals to assumed ice particle shape. If ice particles are modeled as oblate spheroids rather than spheres for radar scattering then the retrieved ice water content is reduced by on average 50% in clouds with a reflectivity factor larger than 0 dBZ. VarCloud retrieves optical depths that are on average a factor-of-2 lower than those from MODIS, which can be explained by the different assumptions on particle mass and area; if VarCloud mimics the MODIS assumptions then better agreement is found in effective radius and optical depth is overestimated. MODIS predicts the mean vertically integrated ice water content to be around a factor-of-3 lower than that from VarCloud for the same retrievals, however, because the MODIS algorithm assumes that its retrieved effective radius (which is mostly representative of cloud top) is constant throughout the depth of the cloud. These comparisons highlight the need to refine microphysical assumptions in all retrieval algorithms and also for future studies to compare not only the mean values but also the full probability density function.