scholarly journals Photomineralization mechanism changes the ability of dissolved organic matter to activate cloud droplets and to nucleate ice crystals

2019 ◽  
Author(s):  
Nadine Borduas-Dedekind ◽  
Rachele Ossola ◽  
Robert O. David ◽  
Lin S. Boynton ◽  
Vera Weichlinger ◽  
...  
Keyword(s):  
Organic Matter ◽  
Dissolved Organic Matter ◽  
Hydrological Cycle ◽  
Supercooled Liquid ◽  
Mixed Phase ◽  
Ice Crystals ◽  
Radiative Properties ◽  
Cloud Droplets ◽  
Photochemical Processing ◽  
Mixed Phase Clouds

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.

scholarly journals Photomineralization mechanism changes the ability of dissolved organic matter to activate cloud droplets and to nucleate ice crystals

2019 ◽  
Vol 19 (19) ◽  
pp. 12397-12412 ◽  
Author(s):  
Nadine Borduas-Dedekind ◽  
Rachele Ossola ◽  
Robert O. David ◽  
Lin S. Boynton ◽  
Vera Weichlinger ◽  
...  
Keyword(s):  
Organic Matter ◽  
Organic Carbon ◽  
Dissolved Organic Matter ◽  
Organic Acids ◽  
Liquid Water ◽  
Supercooled Liquid ◽  
Ice Nucleation ◽  
Ice Crystals ◽  
Cloud Droplets ◽  
Photochemical Processing

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.

scholarly journals Observing ice particle growth along fall streaks in mixed-phase clouds using spectral polarimetric radar data

2018 ◽  
Author(s):  
Lukas Pfitzenmaier ◽  
Christine M. H. Unal ◽  
Yann Dufournet ◽  
Herman J. W. Russchenberg
Keyword(s):  
Particle Growth ◽  
Supercooled Liquid ◽  
Radar Data ◽  
Detection Algorithm ◽  
Mixed Phase ◽  
Ice Crystals ◽  
Liquid Droplets ◽  
Growth Processes ◽  
Retrieval Technique ◽  
Mixed Phase Clouds

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.

scholarly journals In-situ Observation of Riming in Mixed-Phase Clouds using the PHIPS probe

2021 ◽  
Author(s):  
Fritz Waitz ◽  
Martin Schnaiter ◽  
Thomas Leisner ◽  
Emma Järvinen
Keyword(s):  
Liquid Water ◽  
Prediction Models ◽  
Supercooled Liquid ◽  
Liquid Water Content ◽  
Mixed Phase ◽  
Ice Crystals ◽  
The Arctic ◽  
In Situ Observation ◽  
Cloud Particle ◽  
Mixed Phase Clouds

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.

scholarly journals The contribution of black carbon to global ice nucleating particle concentrations relevant to mixed-phase clouds

2020 ◽  
Vol 117 (37) ◽  
pp. 22705-22711
Author(s):  
Gregory P. Schill ◽  
Paul J. DeMott ◽  
Ethan W. Emerson ◽  
Anne Marie C. Rauker ◽  
John K. Kodros ◽  
...  
Keyword(s):  
Black Carbon ◽  
Biomass Burning ◽  
Fossil Fuel ◽  
Supercooled Liquid ◽  
Mixed Phase ◽  
Radiative Properties ◽  
Prescribed Burns ◽  
Earth’S Climate ◽  
Mixed Phase Clouds ◽  
Fossil Fuel Emissions

Black carbon (BC) aerosol plays an important role in the Earth’s climate system because it absorbs solar radiation and therefore potentially warms the climate; however, BC can also act as a seed for cloud particles, which may offset much of its warming potential. If BC acts as an ice nucleating particle (INP), BC could affect the lifetime, albedo, and radiative properties of clouds containing both supercooled liquid water droplets and ice particles (mixed-phase clouds). Over 40% of global BC emissions are from biomass burning; however, the ability of biomass burning BC to act as an INP in mixed-phase cloud conditions is almost entirely unconstrained. To provide these observational constraints, we measured the contribution of BC to INP concentrations ([INP]) in real-world prescribed burns and wildfires. We found that BC contributes, at most, 10% to [INP] during these burns. From this, we developed a parameterization for biomass burning BC and combined it with a BC parameterization previously used for fossil fuel emissions. Applying these parameterizations to global model output, we find that the contribution of BC to potential [INP] relevant to mixed-phase clouds is ∼5% on a global average.

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
Keyword(s):  
Liquid Water ◽  
Supercooled Liquid ◽  
Mixed Phase ◽  
Ice Crystals ◽  
Radiation Budget ◽  
Doppler Spectrum ◽  
Droplet Growth ◽  
Liquid Droplets ◽  
Cloud Droplets ◽  
Ice Particles

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.

scholarly journals Scavenging of black carbon in mixed phase clouds at the high alpine site Jungfraujoch

2007 ◽  
Vol 7 (7) ◽  
pp. 1797-1807 ◽  
Author(s):  
J. Cozic ◽  
B. Verheggen ◽  
S. Mertes ◽  
P. Connolly ◽  
K. Bower ◽  
...  
Keyword(s):  
Black Carbon ◽  
Cloud Condensation Nuclei ◽  
Aerosol Particles ◽  
Liquid Water Content ◽  
Mixed Phase ◽  
Ice Crystals ◽  
Research Station ◽  
Liquid Droplets ◽  
Cloud Droplets ◽  
Mixed Phase Clouds

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.

scholarly journals Observing ice particle growth along fall streaks in mixed-phase clouds using spectral polarimetric radar data

2018 ◽  
Vol 18 (11) ◽  
pp. 7843-7862 ◽  
Author(s):  
Lukas Pfitzenmaier ◽  
Christine M. H. Unal ◽  
Yann Dufournet ◽  
Herman W. J. Russchenberg
Keyword(s):  
Particle Growth ◽  
Supercooled Liquid ◽  
Radar Data ◽  
Detection Algorithm ◽  
Mixed Phase ◽  
Ice Crystals ◽  
Liquid Droplets ◽  
Growth Processes ◽  
Retrieval Technique ◽  
Mixed Phase Clouds

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.

scholarly journals Scavenging of black carbon in mixed phase clouds at the high alpine site Jungfraujoch

2006 ◽  
Vol 6 (6) ◽  
pp. 11877-11912 ◽  
Author(s):  
J. Cozic ◽  
B. Verheggen ◽  
S. Mertes ◽  
P. Connolly ◽  
K. Bower ◽  
...  
Keyword(s):  
Black Carbon ◽  
Cloud Condensation Nuclei ◽  
Aerosol Particles ◽  
Liquid Water Content ◽  
Mixed Phase ◽  
Ice Crystals ◽  
Research Station ◽  
Liquid Droplets ◽  
Cloud Droplets ◽  
Mixed Phase Clouds

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 (drops and ice particles) as well as interstitial aerosol particles; an interstitial inlet which collected only interstitial (unactivated) 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 cloud 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~10% in mixed-phase clouds with IMF>0.2. This is 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.

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

2021 ◽  
Vol 21 (17) ◽  
pp. 13593-13608
Author(s):  
Haoran Li ◽  
Alexei Korolev ◽  
Dmitri Moisseev
Keyword(s):  
Spectral Analysis ◽  
Liquid Water ◽  
Supercooled Liquid ◽  
Mixed Phase ◽  
Ice Crystals ◽  
Doppler Spectrum ◽  
Liquid Droplets ◽  
Cloud Droplets ◽  
Ice Particles ◽  
Doppler Spectral Analysis

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.

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