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 ◽  
...  

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.

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.


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.


Author(s):  
Jeonghyun Kim ◽  
Yeseul Kim ◽  
Sung Eun Park ◽  
Tae-Hoon Kim ◽  
Bong-Guk Kim ◽  
...  

AbstractIn Jeju Island, multiple land-based aquafarms were fully operational along most coastal region. However, the effect of effluent on distribution and behaviours of dissolved organic matter (DOM) in the coastal water are still unknown. To decipher characteristics of organic pollution, we compared physicochemical parameters with spectral optical properties near the coastal aquafarms in Jeju Island. Absorption spectra were measured to calculate the absorption coefficient, spectral slope coefficient, and specific UV absorbance. Fluorescent DOM was analysed using fluorescence spectroscopy coupled with parallel factor analysis. Dissolved organic carbon (DOC) and total dissolved nitrogen (TDN) were measured using high-temperature catalytic oxidation. The DOC concentration near the discharge outlet was twice higher than that in natural groundwater, and the TDN concentration exponentially increased close to the outlet. These distribution patterns indicate that aquafarms are a significant source of DOM. Herein, principal component analysis was applied to categorise the DOM origins. There were two distinct groups, namely, aquaculture activity for TDN with humic-like and high molecular weights DOM (PC1: 48.1%) and natural biological activity in the coastal water for DOC enrichment and protein-like DOM (PC2: 18.8%). We conclude that the aquafarms significantly discharge organic nitrogen pollutants and provoke in situ production of organic carbon. Furthermore, these findings indicate the potential of optical techniques for the efficient monitoring of anthropogenic organic pollutants from aquafarms worldwide.


2008 ◽  
Vol 5 (2) ◽  
pp. 281-298 ◽  
Author(s):  
P. Raimbault ◽  
N. Garcia ◽  
F. Cerutti

Abstract. During the BIOSOPE cruise the RV Atalante was dedicated to study the biogeochemical properties in the South Pacific between the Marquesas Islands (141° W–8° S) and the Chilean upwelling (73° W–34° S). Over the 8000 km covered by the cruise, several different trophic situations were encountered, in particular strong oligotrophic conditions in the South Pacific Gyre (SPG, between 123° W and 101° W). In this isolated region, nitrate was undetectable between the surface and 160–180 m and only trace quantities (<20 nmoles l−1) of regenerated nitrogen (nitrite and ammonium) were detected, even in the subsurface maximum. Integrated nitrate over the photic layer, which reached 165 m, was close to zero. Despite this severe nitrogen-depletion, phosphate was always present in significant concentrations (≈0.1 μmoles l−1), while silicic acid was maintained at low but classical oceanic levels (≈1 μmoles l−1). In contrast, the Marquesas region (MAR) to the west and Chilean upwelling (UPW) to the east were characterized by high nutrient concentrations, one hundred to one thousand fold higher than in the SPG. The distribution of surface chlorophyll reflected the nitrate gradient, the lowest concentrations (0.023 nmoles l−1) being measured at the centre of the SPG, where integrated value throughout the photic layer was very low (≈ 10 mg m−2). However, due to the relatively high concentrations of chlorophyll-a encountered in the DCM (0.2 μg l−1), chlorophyll-a concentrations throughout the photic layer were less variable than nitrate concentrations (by a factor 2 to 5). In contrast to chlorophyll-a, integrated particulate organic matter (POM) remained more or less constant along the study area (500 mmoles m−2, 60 mmoles m−2 and 3.5 mmoles m−2 for particulate organic carbon, particulate organic nitrogen and particulate organic phosphorus, respectively), with the exception of the upwelling, where values were two fold higher. The residence time of particulate carbon in the surface water was only 4–5 days in the upwelling, but up to 30 days in the SPG, where light isotopic δ15N signal noted in the suspended POM suggests that N2-fixation provides a dominant supply of nitrogen to phytoplankton. The most striking feature was the large accumulation of dissolved organic matter (DOM) in the SPG compared to the surrounding waters, in particular dissolved organic carbon (DOC) where concentrations were at levels rarely measured in oceanic waters (>100 μmoles l−1). Due to this large pool of DOM in the SPG photic layer, integrated values followed a converse geographical pattern to that of inorganic nutrients with a large accumulation in the centre of the SPG. Whereas suspended particulate matter in the mixed layer had a C/N ratio largely conforming to the Redfield stochiometry (C/N≈6.6), marked deviations were observed in this excess DOM (C/N≈16 to 23). The marked geographical trend suggests that a net in situ source exists, mainly due to biological processes. Thus, in spite of strong nitrate-depletion leading to low chlorophyll biomass, the closed ecosystem of the SPG can accumulate large amounts of C-rich dissolved organic matter. The implications of this finding are examined, the conclusion being that, due to weak lateral advection, the biologically produced dissolved organic carbon can be accumulated and stored in the photic layer for very long periods. In spite of the lack of seasonal vertical mixing, a significant part of new production (up to 34%), which was mainly supported by dinitrogen fixation, can be exported to deep waters by turbulent diffusion in terms of DOC. The diffusive rate estimated in the SPG (134 μmolesC m−2 d−1), was quite equivalent to the particles flux measured by sediments traps.


2014 ◽  
Vol 11 (10) ◽  
pp. 14097-14132 ◽  
Author(s):  
L. Tremblay ◽  
J. Caparros ◽  
K. Leblanc ◽  
I. Obernosterer

Abstract. Natural iron fertilization of high-nutrient low-chlorophyll (HNLC) waters induces annually occurring spring phytoplankton blooms off Kerguelen Islands (Southern Ocean). To examine the origin and fate of particulate and dissolved organic matter (POM and DOM), D- and L-amino acids (AA) were quantified at bloom and HNLC stations. Total hydrolysable AA accounted for 21–25% of surface particulate organic carbon (%POCAA) at the bloom sites, but for 10% at the HNLC site. A marked decrease in %POCAA with depth was observed at the most productive stations leading to values between 3 and 5% below 300 m depth. AA contributed to only 0.9–4.4% of dissolved organic carbon (%DOCAA) at all stations. The only consistent vertical trend was observed at the most productive station (A3-2) where %DOCAA decreased from ∼2% in the surface waters to 0.9% near 300 m. These AA yields and other markers revealed that POM and DOM were more rapidly altered or mineralized at the bloom sites compared to the HNLC site. Different molecular markers indicated that POM mostly originated from diatoms and bacteria. The estimated average proportion of POM from intact phytoplankton cells in surface waters was 45% at the bloom station A3-2, but 14% at the HNLC site. Estimates based on D-AA yields indicated that ∼15% of POM and ∼30% of DOM was of bacterial origin (cells and cell fragments) at all stations. Surprisingly, the DOM in HNLC waters appeared less altered than the DOM from the bloom, had slightly higher dissolved AA concentrations, and showed no sign of alteration within the water column. Unfavorable conditions for bacterial degradation in HNLC regions can explain these findings. In contrast, large inputs of labile organic molecules and iron, likely stimulate the degradation of organic matter (priming effect) and the production of more recalcitrant DOM (microbial carbon pump) during iron-fertilized blooms.


Fisheries ◽  
2020 ◽  
Vol 2020 (5) ◽  
pp. 25-29
Author(s):  
Anatoliy Sadchikov ◽  
Sergey Ostroumov

The role of algae and bacteria in the consumption and mineralization of dissolved organic matter (DOM) in a highly trophic aquatic ecosystem was studied. The phytoplankton and bacterioplankton community consumed 60% of added DOM in August and 56% of DOM in September. Of the uptaken DOM, a significant amount of organic carbon was mineralized. In August 42.7% and in September 29% of organic carbon (of the consumed organic matter) were used for respiration.


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