scholarly journals Supercooled liquid water and secondary ice production in Kelvin–Helmholtz instability as revealed by radar Doppler spectra observations

2021 ◽  
Author(s):  
Haoran Li ◽  
Alexei Korolev ◽  
Dmitri Moisseev

Abstract. Mixed-phase clouds are globally omnipresent and play a major role in the Earth's radiation budget and precipitation formation. The existence of liquid droplets in presence of ice particles is microphysically unstable and depends on a delicate balance of several competing processes. Understanding mechanisms that govern ice initiation and moisture supply are important to understand the life-cycle of such clouds. This study presents observations that reveal the onset of drizzle inside a ∼600 m deep mixed-phase layer embedded in a stratiform precipitation system. Using Doppler spectra analysis, we show how large supercooled liquid droplets are generated in Kelvin-Helmholtz (K-H) instability despite ice particles falling from upper cloud layers. The spectral width of supercooled liquid water mode in radar Doppler spectrum is used to identify a region of increased turbulence. The observations show that large liquid droplets, characterized by reflectivity values larger than −20 dBZ, are generated in this region. In addition to cloud droplets, Doppler spectral analysis reveals the production of the columnar ice crystals in the K-H billows. The modelling study estimates that the concentration of these ice crystals is 3 ∼ 8 L−1, which is at least one order of magnitude higher than that of primary ice nucleating particles. Given the detail of the observations, we show that multiple populations of secondary ice particles are generated in regions where larger cloud droplets are produced and not at some constant level within the cloud. It is therefore hypothesized that K-H instability provides conditions favorable for enhanced droplet growth and formation of secondary ice particles.

2021 ◽  
Vol 21 (17) ◽  
pp. 13593-13608
Author(s):  
Haoran Li ◽  
Alexei Korolev ◽  
Dmitri Moisseev

Abstract. Mixed-phase clouds are globally omnipresent and play a major role in the Earth's radiation budget and precipitation formation. The existence of liquid droplets in the presence of ice particles is microphysically unstable and depends on a delicate balance of several competing processes. Understanding mechanisms that govern ice initiation and moisture supply are important to understand the life cycle of such clouds. This study presents observations that reveal the onset of drizzle inside a ∼ 600 m deep mixed-phase layer embedded in a stratiform precipitation system. Using Doppler spectral analysis, we show how large supercooled liquid droplets are generated in Kelvin–Helmholtz (K–H) instability despite ice particles falling from upper cloud layers. The spectral width of the supercooled liquid water mode in the radar Doppler spectrum is used to identify a region of increased turbulence. The observations show that large liquid droplets, characterized by reflectivity values larger than −20 dBZ, are generated in this region. In addition to cloud droplets, Doppler spectral analysis reveals the production of columnar ice crystals in the K–H billows. The modeling study estimates that the concentration of these ice crystals is 3–8 L−1, which is at least 1 order of magnitude higher than that of primary ice-nucleating particles. Given the detail of the observations, we show that multiple populations of secondary ice particles are generated in regions where larger cloud droplets are produced and not at some constant level within the cloud. It is, therefore, hypothesized that K–H instability provides conditions favorable for enhanced droplet growth and formation of secondary ice particles.


2019 ◽  
Vol 19 (19) ◽  
pp. 12397-12412 ◽  
Author(s):  
Nadine Borduas-Dedekind ◽  
Rachele Ossola ◽  
Robert O. David ◽  
Lin S. Boynton ◽  
Vera Weichlinger ◽  
...  

Abstract. An organic aerosol particle has a lifetime of approximately 1 week in the atmosphere during which it will be exposed to sunlight. However, the effect of photochemistry on the propensity of organic matter to participate in the initial cloud-forming steps is difficult to predict. In this study, we quantify on a molecular scale the effect of photochemical exposure of naturally occurring dissolved organic matter (DOM) and of a fulvic acid standard on its cloud condensation nuclei (CCN) and ice nucleation (IN) activity. We find that photochemical processing, equivalent to 4.6 d in the atmosphere, of DOM increases its ability to form cloud droplets by up to a factor of 2.5 but decreases its ability to form ice crystals at a loss rate of −0.04 ∘CT50 h−1 of sunlight at ground level. In other words, the ice nucleation activity of photooxidized DOM can require up to 4 ∘C colder temperatures for 50 % of the droplets to activate as ice crystals under immersion freezing conditions. This temperature change could impact the ratio of ice to water droplets within a mixed-phase cloud by delaying the onset of glaciation and by increasing the supercooled liquid fraction of the cloud, thereby modifying the radiative properties and the lifetime of the cloud. Concurrently, a photomineralization mechanism was quantified by monitoring the loss of organic carbon and the simultaneous production of organic acids, such as formic, acetic, oxalic and pyruvic acids, CO and CO2. This mechanism explains and predicts the observed increase in CCN and decrease in IN efficiencies. Indeed, we show that photochemical processing can be a dominant atmospheric ageing process, impacting CCN and IN efficiencies and concentrations. Photomineralization can thus alter the aerosol–cloud radiative effects of organic matter by modifying the supercooled-liquid-water-to-ice-crystal ratio in mixed-phase clouds with implications for cloud lifetime, precipitation patterns and the hydrological cycle.Highlights. During atmospheric transport, dissolved organic matter (DOM) within aqueous aerosols undergoes photochemistry. We find that photochemical processing of DOM increases its ability to form cloud droplets but decreases its ability to form ice crystals over a simulated 4.6 d in the atmosphere. A photomineralization mechanism involving the loss of organic carbon and the production of organic acids, CO and CO2 explains the observed changes and affects the liquid-water-to-ice ratio in clouds.


2018 ◽  
Author(s):  
Lukas Pfitzenmaier ◽  
Christine M. H. Unal ◽  
Yann Dufournet ◽  
Herman J. W. Russchenberg

Abstract. The growth of ice crystals in presence of super-cooled liquid droplets represents the most important process for precipitation formation in the mid-latitudes. Such mixed-phase interaction processes remain however pretty much unknown, as capturing the complexity in cloud dynamics and microphysical variabilities turns to be a real observational challenge. Ground-based radar systems equipped with fully polarimetric and Doppler capabilities in high temporal and spatial resolutions 5 such as the S-band Transportable Atmospheric Radar (TARA) are best suited to observe mixed-phase growth processes. In this paper, measurements are taken with the TARA radar during the ACCEPT campaign (Analysis of the Composition of Clouds with Extended Polarization Techniques). Besides the common radar observables, the 3D wind field is also retrieved due to TARA unique three beam configuration. The novelty of this paper is to combine all these observations with a particle evolution detection algorithm based on a new fall streak retrieval technique in order to study ice particle growth within complex 10 precipitating mixed-phased cloud systems. In the presented cases, three different growth processes of ice crystals, plate-like crystals, and needles, are detected and related to the presence of supercooled liquid water. Moreover, TARA observed signatures are assessed with co-located measurements obtained from a cloud radar and radiosondes. This paper shows that it is possible to observe ice particle growth processes within complex systems taking advantage of adequate technology and state of the art retrieval algorithms. A significant improvement is made towards a conclusive interpretation of ice particle growth processes 15 and their contribution to rain production using fall streak rearranged radar data.


2018 ◽  
Author(s):  
Ulrike Lohmann ◽  
David Neubauer

Abstract. Clouds are important in the climate system because of their large influence on the radiation budget. On the one hand, they scatter solar radiation and with that cool the climate. On the other hand, they absorb and re-emit terrestrial radiation, which causes a warming. How clouds change in a warmer climate is one of the largest uncertainties for the equilibrium climate sensitivity (ECS). While a large spread in the cloud feedback arises from low-level clouds, it was recently shown that also mixed-phase clouds are important for ECS. If mixed-phase clouds in the current climate contain too few supercooled cloud droplets, too much ice will change to liquid water in a warmer climate. As shown by Tan et al. (2016), this overestimates the negative cloud phase feedback and underestimates ECS in the CAM global climate model (GCM). Here we are using the newest version of the ECHAM6-HAM2 GCM to investigate the importance of mixed-phase clouds for ECS. Although we also considerably underestimate the fraction of supercooled liquid water globally in the reference version of ECHAM6-HAM2 GCM, we do not obtain increases in ECS in simulations with more supercooled liquid water in the present-day climate, contrary to the findings by Tan et al. (2016). We hypothesize that it is not the global supercooled liquid water fraction that matters, but only how well low- and mid-level mixed-phase clouds with cloud top temperatures in the mixed-phase temperature range between 0 and −35 ºC are simulated. These occur most frequent in mid-latitudes, in particular over the Southern Ocean where they determine the amount of absorbed shortwave radiation. In ECHAM6-HAM2 the amount of absorbed shortwave radiation over the Southern Ocean is only overestimated if all clouds below 0 ºC consist exclusively of ice and only in this simulation is ECS is significantly smaller than in all other simulations. Hence, the negative cloud phase feedback seems to be important only if the optically thin low- and mid-level mid-latitude clouds have the wrong phase (ice instead of liquid water) in the absence of overlying clouds. In all other simulations, changes in cloud feedbacks associated with cloud amount and cloud top pressure, dominate.


2021 ◽  
Author(s):  
Fritz Waitz ◽  
Martin Schnaiter ◽  
Thomas Leisner ◽  
Emma Järvinen

Abstract. Mixed-phase clouds consist of both supercooled liquid water droplets and solid ice crystals. Despite having a significant impact on Earth‘s climate, mixed-phase clouds are poorly understood and not well represented in climate prediction models. One piece of the puzzle is understanding and parameterizing riming of mixed-phase cloud ice crystals, which is one of the main growth mechanisms of ice crystals via the accretion of small, supercooled droplets. Especially the extent of riming on ice crystals smaller than 500 μm is often overlooked in studies – mainly because observations are scarce. Here, we investigated riming in mixed-phase clouds during three airborne campaigns in the Arctic, the Southern Ocean and US east coast. Riming was observed from stereo-microscopic cloud particle images recorded with the Particle Habit Imaging and Polar Scattering (PHIPS) probe. We show that riming is most prevalent at temperatures around −7 °C, where, on average, 43 % of the investigated particles in a size range from 100 ≤ D ≤ 700 μm showed evidence of riming. We discuss the occurrence and properties of rimed ice particles and show correlation of the occurrence and the amount of riming with ambient meteorological parameters. We show that riming fraction increases with ice particle size (< 20 % for D ≤ 200 μm, 35–40 % for D ≥ 400 μm) and liquid water content (25 % for LWC ≤ 0.05 g m−3, up to 60 % for LWC = 0.5 g m−3). We investigate the ageing of rimed particles and the difference between "normal" and "epitaxial" riming based on a case study.


2021 ◽  
Author(s):  
Florian Tornow ◽  
Andrew S. Ackerman ◽  
Ann M. Fridlind

Abstract. Marine cold air outbreaks (CAOs) commonly form overcast cloud decks that transition into broken cloud fields downwind, dramatically altering the local radiation budget. In this study, we investigate the impact of frozen hydrometeors on these transitions. We focus on a CAO case in the NW Atlantic, the location of the multi-year flight campaign ACTIVATE. We use MERRA-2 reanalysis fields to drive large-eddy simulations with mixed-phase two-moment microphysics in a Lagrangian framework. We find that transitions are triggered by substantial rain (rainwater paths > 25 g m−2) and only simulations that allow for aerosol depletion result in sustained breakups as observed. Using a range of diagnostic ice nucleating particle concentrations, Ninp, we find that increasing ice progressively accelerates transitions, thus abbreviating the overcast state. Ice particles affect the cloud-topped boundary layer evolution primarily through riming-related processes prior to substantial rain, leading to (1) reduction in cloud liquid water, (2) early consumption of cloud condensation nuclei, and (3) early and light precipitation cooling and moistening below cloud. We refer to these three effects collectively as preconditioning by riming. Greater boundary layer aerosol concentrations delay the onset of substantial rain. However, cloud breakup and low-aerosol concentration final stages are found to be inevitable in this case owing primarily to liquid water path buildup. To address prevailing uncertainties in the model representation of mixed-phase processes, the magnitude of ice formation and riming impacts and, thereby, the strength of an associated negative cloud-climate feedback process, requires further observational evaluation by targeting riming hotspots with in situ imaging probes that allow both for characterization of ice particles and abundance of supercooled droplets.


2018 ◽  
Vol 75 (4) ◽  
pp. 1045-1062 ◽  
Author(s):  
M. Pinsky ◽  
A. Khain ◽  
A. Korolev

Abstract The process of ice–liquid water interaction in the unsaturated environment is explored both analytically and with the help of a numerical simulation. Ice–liquid water interaction via the condensation–evaporation mechanism is considered in relation to the problem of homogeneous mixing in an unmovable air volume. The process is separated into three stages: the homogenization stage, during which the rapid alignment of thermodynamic and microphysical parameters in the mixing volume takes place; the glaciation stage, during which the liquid droplets evaporate; and the ice stage, which leads to attaining a thermodynamic equilibrium. Depending on the initial temperature, humidity, and mixing ratios of liquid water and of ice water, the third stage may result in two outcomes: existence of ice particles under zero supersaturation with respect to ice or a complete disappearance of ice particles. Three characteristic times are associated with the microphysical stages: the phase relaxation time associated with droplets, the glaciation time determined by the Wegener–Bergeron–Findeisen process, and the phase relaxation time associated with ice. Since the duration of the second and third microphysical stages may be of the same order as the homogenization time or even longer, the homogeneous mixing scenario is more probable in mixed-phase clouds than in liquid clouds. It is shown that mixing of a mixed-phase cloud with a dry environment accelerates cloud glaciation, leading to a decrease in the glaciation time by more than 2 times. The conditions of fast ice particles’ disappearance due to sublimation are analyzed as well.


2019 ◽  
Author(s):  
Nadine Borduas-Dedekind ◽  
Rachele Ossola ◽  
Robert O. David ◽  
Lin S. Boynton ◽  
Vera Weichlinger ◽  
...  

Abstract. An organic aerosol particle has a lifetime of approximately one week in the atmosphere during which it will be exposed to sunlight. Yet, the effect of photochemistry on the propensity of organic matter to participate in the initial cloud-forming steps is difficult to predict. In this study, we quantify on a molecular scale the effect of photochemical exposure of naturally occurring dissolved organic matter (DOM) and of a fulvic acid standard on its ability to form mixed-phase clouds, by acting as cloud condensation nuclei (CCN) and by acting as ice nucleating particles (INPs). We find that photochemical processing, equivalent to 4.6 days in the atmosphere, of DOM increases its ability to form cloud droplets by up to a factor of 2.5 but decreases its ability to form ice crystals at a loss rate of −0.04°CT50 h−1 of sunlight at ground level. In other words, the ice nucleation activity of photooxidized DOM can require up to 4 degrees colder temperatures for 50 % of the droplets to activate as ice crystals under immersion freezing conditions. This temperature change could impact the ratio of ice to water droplets within a mixed phase cloud by delaying the onset of glaciation and by increasing the supercooled liquid fraction of the cloud, thereby modifying the radiative properties and the lifetime of the cloud. Concurrently, a photomineralization mechanism was quantified by monitoring the loss of organic carbon and the simultaneous production of organic acids, such as formic, acetic, oxalic and pyruvic acids, CO and CO2. This mechanism explains and predicts the observed increase in CCN and decrease in INP efficiencies. Indeed, we show that photochemical processing can be a dominant atmospheric aging process, impacting CCN and INP efficiencies and concentrations. Photomineralization can thus alter the aerosol-cloud radiative effects of organic matter by modifying the supercooled liquid water-to-ice crystal ratio in mixed-phase clouds with implications for cloud lifetime, precipitation patterns and the hydrological cycle.


2007 ◽  
Vol 7 (7) ◽  
pp. 1797-1807 ◽  
Author(s):  
J. Cozic ◽  
B. Verheggen ◽  
S. Mertes ◽  
P. Connolly ◽  
K. Bower ◽  
...  

Abstract. The scavenging of black carbon (BC) in liquid and mixed phase clouds was investigated during intensive experiments in winter 2004, summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m a.s.l., Switzerland). Aerosol residuals were sampled behind two well characterized inlets; a total inlet which collected cloud particles (droplets and ice particles) as well as interstitial (unactivated) aerosol particles; an interstitial inlet which collected only interstitial aerosol particles. BC concentrations were measured behind each of these inlets along with the submicrometer aerosol number size distribution, from which a volume concentration was derived. These measurements were complemented by in-situ measurements of cloud microphysical parameters. BC was found to be scavenged into the condensed phase to the same extent as the bulk aerosol, which suggests that BC was covered with soluble material through aging processes, rendering it more hygroscopic. The scavenged fraction of BC (FScav,BC), defined as the fraction of BC that is incorporated into cloud droplets and ice crystals, decreases with increasing cloud ice mass fraction (IMF) from FScav,BC=60% in liquid phase clouds to FScav,BC~5–10% in mixed-phase clouds with IMF>0.2. This can be explained by the evaporation of liquid droplets in the presence of ice crystals (Wegener-Bergeron-Findeisen process), releasing BC containing cloud condensation nuclei back into the interstitial phase. In liquid clouds, the scavenged BC fraction is found to decrease with decreasing cloud liquid water content. The scavenged BC fraction is also found to decrease with increasing BC mass concentration since there is an increased competition for the available water vapour.


2018 ◽  
Vol 18 (11) ◽  
pp. 7843-7862 ◽  
Author(s):  
Lukas Pfitzenmaier ◽  
Christine M. H. Unal ◽  
Yann Dufournet ◽  
Herman W. J. Russchenberg

Abstract. The growth of ice crystals in presence of supercooled liquid droplets represents the most important process for precipitation formation in the mid-latitudes. However, such mixed-phase interaction processes remain relatively unknown, as capturing the complexity in cloud dynamics and microphysical variabilities turns to be a real observational challenge. Ground-based radar systems equipped with fully polarimetric and Doppler capabilities in high temporal and spatial resolutions such as the S-band transportable atmospheric radar (TARA) are best suited to observe mixed-phase growth processes. In this paper, measurements are taken with the TARA radar during the ACCEPT campaign (analysis of the composition of clouds with extended polarization techniques). Besides the common radar observables, the 3-D wind field is also retrieved due to TARA unique three beam configuration. The novelty of this paper is to combine all these observations with a particle evolution detection algorithm based on a new fall streak retrieval technique in order to study ice particle growth within complex precipitating mixed-phased cloud systems. In the presented cases, three different growth processes of ice crystals, plate-like crystals, and needles are detected and related to the presence of supercooled liquid water. Moreover, TARA observed signatures are assessed with co-located measurements obtained from a cloud radar and radiosondes. This paper shows that it is possible to observe ice particle growth processes within complex systems taking advantage of adequate technology and state of the art retrieval algorithms. A significant improvement is made towards a conclusive interpretation of ice particle growth processes and their contribution to rain production using fall streak rearranged radar data.


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