CCN properties of pollen from selected wind pollinated plants

Author(s):  
Sebastian Sonnenberg ◽  
Julia Burkart ◽  
Jürgen Gratzl

<p>Aerosol particles that act as cloud condensation nuclei (CCN) inuence cloud albedo and lifetime and thereby affect the planetary radiative balance. The indirect aerosol effect on climate is still one of the largest uncertainties and especially the role of biological particles is not yet well described. Pollen grains are primary biological particles that become airborne during the blooming season of plants. Pollen from wind pollinated plants represent a seasonally signifficant portion of the organic aerosol in the atmosphere. Intact pollen grains are rather large (10-100 µm) but under conditions of high humidity pollen grains have been shown to rupture and release cytoplasmic material including a large number of particles much smaller in size (0.5-5 µm).</p><p>In this study we extract soluble and insoluble material from several pollen samples (<em>Phleum,</em> <em>Betula</em>, <em>Artimesia</em>, <em>Poa</em>, <em>Corylus</em> and <em>Ambrosia</em>) and investigate the CCN activity of the extracts in a laboratory study. The main component of the experiment is the continuous-flow streamwise thermal-gradient cloud condensation nuclei counter (CCNC) from Droplet Measurement Technologies (DMT). The CCNC was calibrated with (NH<sub>4</sub>)2SO<sub>4</sub>. The activation behavior of (NH<sub>4</sub>)2SO<sub>4</sub> is theoretically well described by Kohler equation. For particles which consist of a multitude of organic components it is convenient to represent the chemical composition through the hygroscopicity parameter κ. In the first part of the experiment, we determine the activation diameter at 5 different supersaturations and calculate the kappa parameter for all pollen samples. We find that the values fall in the range from 0.1-0.2. which is typical for particles composed of organic substances. Extracts from <em>Betula</em> pollen show the highest hygroscopicity (κ = 0.18), while extracts from <em>Artimesia</em> exhibit the lowest hygroscopicity (κ = 0.13). In the second part of the experiment we will also investigate the CCN activity of the insoluble material.</p>

2012 ◽  
Vol 12 (8) ◽  
pp. 3783-3790 ◽  
Author(s):  
Q. Zhang ◽  
J. Meng ◽  
J. Quan ◽  
Y. Gao ◽  
D. Zhao ◽  
...  

Abstract. The impact of aerosol composition on cloud condensation nuclei (CCN) activity were analyzed in this study based on field experiments carried out at downtown Tianjin, China in September 2010. In the experiments, the CCN measurements were performed at supersaturation (SS) of 0.1%, 0.2% and 0.4% using a thermal-gradient diffusion chamber (DMT CCNC), whereas the aerosol size distribution and composition were simultaneously measured with a TSI SMPS and an Aerodyne Aerosol Mass Spectrometer (AMS), respectively. The results show that the influence of aerosol composition on CCN activity is notable under low SS (0.1%), and their influence decreased with increasing SS. For example, under SS of 0.1%, the CCN activity increases from 4.5±2.6% to 12.8±6.1% when organics fraction decrease from 30–40% to 10–20%. The rate of increase reached up to 184%. While under SS of 0.4%, the CCN activity increases only from 35.7±19.0% to 46.5±12.3% correspondingly. The calculated NCCN based on the size-resolved activation ratio and aerosol number size distribution correlated well with observed NCCN at high SS (0.4%), but this consistence decreased with the falling of SS. The slopes of linear fitted lines between calculated and observed NCCN are 0.708, 0.947, and 0.995 at SS of 0.1%, 0.2% and 0.4% respectively. Moreover, the stand deviation (SD) of calculated NCCN increased with the decreasing of SS. A case study of CCN closure analyses indicated that the calculated error of NCCN could reach up to 34% at SS of 0.1% if aerosol composition were not included, and the calculated error decreased with the raising of SS. It is decreased to 9% at SS of 0.2%, and further decreased to 4% at SS of 0.4%.


2018 ◽  
Vol 18 (10) ◽  
pp. 7345-7359 ◽  
Author(s):  
Mingjin Wang ◽  
Tong Zhu ◽  
Defeng Zhao ◽  
Florian Rubach ◽  
Andreas Wahner ◽  
...  

Abstract. Condensation of carboxylic acids on mineral particles leads to coatings and impacts the particles' potential to act as cloud condensation nuclei (CCN). To determine how the CCN activity of mineral particles is impacted by carboxylic acid coatings, the CCN activities of CaCO3 particles and CaCO3 particles with oleic acid and malonic acid coatings were compared in this study. The results revealed that small amounts of oleic acid coating (volume fraction (vf) ≤4.3 %) decreased the CCN activity of CaCO3 particles, while more oleic acid coating (vf ≥16 %) increased the CCN activity of CaCO3 particles. This phenomenon has not been reported before. In contrast, the CCN activity of CaCO3 particles coated with malonic acid increased with the thickness of the malonic acid coating (vf =0.4–40 %). Even the smallest amounts of malonic acid coating (vf =0.4 %) significantly enhanced the CCN activity of CaCO3 particles from κ=0.0028±0.0001 to κ=0.0123±0.0005. This indicates that a small amount of water-soluble organic acid coating may significantly enhance the CCN activity of mineral particles. The presence of water vapor during the coating process with malonic acid additionally increased the CCN activity of the coated CaCO3 particles, probably because more CaCO3 reacts with malonic acid when sufficient water is available.


2019 ◽  
Vol 19 (24) ◽  
pp. 15545-15567 ◽  
Author(s):  
Franz Friebel ◽  
Prem Lobo ◽  
David Neubauer ◽  
Ulrike Lohmann ◽  
Saskia Drossaart van Dusseldorp ◽  
...  

Abstract. The largest contributors to the uncertainty in assessing the anthropogenic contribution in radiative forcing are the direct and indirect effects of aerosol particles on the Earth's radiative budget. Soot particles are of special interest since their properties can change significantly due to aging processes once they are emitted into the atmosphere. Probably the largest obstacle for the investigation of these processes in the laboratory is the long atmospheric lifetime of 1 week, requiring tailored experiments that cover this time span. This work presents results on the ability of two types of soot, obtained using a miniCAST soot generator, to act as cloud condensation nuclei (CCN) after exposure to atmospherically relevant levels of ozone (O3) and humidity. Aging times of up to 12 h were achieved by successful application of the continuous-flow stirred tank reactor (CSTR) concept while allowing for size selection of particles prior to the aging step. Particles of 100 nm diameter and rich in organic carbon (OC) that were initially CCN inactive showed significant CCN activity at supersaturations (SS) down to 0.3 % after 10 h of exposure to 200 ppb of O3. While this process was not affected by different levels of relative humidity in the range of 5 %–75 %, a high sensitivity towards the ambient/reaction temperature was observed. Soot particles with a lower OC content required an approximately 4-fold longer aging duration to show CCN activity at the same SS. Prior to the slow change in the CCN activity, a rapid increase in the particle diameter was detected which occurred within several minutes. This study highlights the applicability of the CSTR approach for the simulation of atmospheric aging processes, as aging durations beyond 12 h can be achieved in comparably small aerosol chamber volumes (<3 m3). Implementation of our measurement results in a global aerosol-climate model, ECHAM6.3-HAM2.3, showed a statistically significant increase in the regional and global CCN burden and cloud droplet number concentration.


2019 ◽  
Author(s):  
Franz Friebel ◽  
Prem Lobo ◽  
David Neubauer ◽  
Ulrike Lohmann ◽  
Saskia Drossaart van Dusseldorp ◽  
...  

Abstract. The largest contributors to the uncertainty in assessing the anthropogenic contribution in radiative forcing are the direct and indirect effects of aerosol particles on the Earth's radiative budget. Soot particles are of special interest since their properties can change significantly due to aging processes once they are emitted to the atmosphere. Probably the largest obstacle for the investigation of these processes in the laboratory is the long atmospheric lifetime of one week, demanding tailored experiments that cover this time span. This work presents results on the ability of two types of soot to act as cloud condensation nuclei (CCN) after exposure to atmospherically relevant levels of ozone and humidity. Aging times of up to 12 h were achieved by successful application of the continuous-flow stirred tank reactor (CSTR) concept while allowing for size-selection of particles prior to the aging step. 100 nm particles rich in organic carbon (OC) that were initially CCN-inactive showed significant CCN-activity at supersaturations (SS) down to 0.3 % after 10 h of exposure to 200 ppb of ozone. While this process was not affected by different levels of relative humidity in the range 5–75 %, a high sensitivity towards the ambient/reaction temperature was observed. Soot particles with a lower OC-content demanded an approximately four-fold longer aging duration to show CCN-activity for the same SS. Prior to the slow change in the CCN-activity, a rapid increase in the particle diameter was detected which occurred within several minutes. This study highlights the applicability of the CSTR-approach for the simulation of atmospheric aging processes, as aging durations beyond 12 h can be achieved in comparably small aerosol chamber volumes (


2011 ◽  
Vol 11 (17) ◽  
pp. 8913-8928 ◽  
Author(s):  
A. T. Lambe ◽  
T. B. Onasch ◽  
P. Massoli ◽  
D. R. Croasdale ◽  
J. P. Wright ◽  
...  

Abstract. Secondary organic aerosol (SOA) and oxidized primary organic aerosol (OPOA) were produced in laboratory experiments from the oxidation of fourteen precursors representing atmospherically relevant biogenic and anthropogenic sources. The SOA and OPOA particles were generated via controlled exposure of precursors to OH radicals and/or O3 in a Potential Aerosol Mass (PAM) flow reactor over timescales equivalent to 1–20 days of atmospheric aging. Aerosol mass spectra of SOA and OPOA were measured with an Aerodyne aerosol mass spectrometer (AMS). The fraction of AMS signal at m/z = 43 and m/z = 44 (f43, f44), the hydrogen-to-carbon (H/C) ratio, and the oxygen-to-carbon (O/C) ratio of the SOA and OPOA were obtained, which are commonly used to characterize the level of oxidation of oxygenated organic aerosol (OOA). The results show that PAM-generated SOA and OPOA can reproduce and extend the observed f44–f43 composition beyond that of ambient OOA as measured by an AMS. Van Krevelen diagrams showing H/C ratio as a function of O/C ratio suggest an oxidation mechanism involving formation of carboxylic acids concurrent with fragmentation of carbon-carbon bonds. Cloud condensation nuclei (CCN) activity of PAM-generated SOA and OPOA was measured as a function of OH exposure and characterized as a function of O/C ratio. CCN activity of the SOA and OPOA, which was characterized in the form of the hygroscopicity parameter κorg, ranged from 8.4×10−4 to 0.28 over measured O/C ratios ranging from 0.05 to 1.42. This range of κorg and O/C ratio is significantly wider than has been previously obtained. To first order, the κorg-to-O/C relationship is well represented by a linear function of the form κorg = (0.18±0.04) ×O/C + 0.03, suggesting that a simple, semi-empirical parameterization of OOA hygroscopicity and oxidation level can be defined for use in chemistry and climate models.


2012 ◽  
Vol 12 (18) ◽  
pp. 8377-8388 ◽  
Author(s):  
X. Tang ◽  
D. R. Cocker ◽  
A. Asa-Awuku

Abstract. Secondary organic aerosol (SOA) was formed in an environmental reaction chamber from the ozonolysis of β-caryophyllene (β-C) at low concentrations (5 ppb or 20 ppb). Experimental parameters were varied to characterize the effects of hydroxyl radicals, light and the presence of lower molecular weight terpene precursor (isoprene) for β-C SOA formation and cloud condensation nuclei (CCN) characteristics. Changes in β-C SOA chemicophysical properties (e.g., density, volatility, oxidation state) were explored with online techniques to improve our predictive understanding of β-C CCN activity. In the absence of OH scavenger, light intensity had negligible impacts on SOA oxidation state and CCN activity. In contrast, when OH reaction was effectively suppressed (> 11 ppm scavenger), SOA showed a much lower CCN activity and slightly less oxygenated state consistent with previously reported values. Though there is significant oxidized material present (O / C > 0.25), no linear correlation existed between the mass ratio ion fragment 44 in the bulk organic mass (f44) and O / C for the β-C-O3 system. No direct correlations were observed with other aerosol bulk ion fragment fraction (fx) and κ as well. A mixture of β-C and lower molecular weight terpenes (isoprene) consumed more ozone and formed SOA with distinct characteristics dependent on isoprene amounts. The addition of isoprene also improved the CCN predictive capabilities with bulk aerosol chemical information. The β-C SOA CCN activity reported here is much higher than previous studies (κ < 0.1) that use higher precursor concentration in smaller environmental chambers; similar results were only achieved with significant use of OH scavenger. Results show that aerosol formed from a mixture of low and high molecular weight terpene ozonolysis can be hygroscopic and can contribute to the global biogenic SOA CCN budget.


Author(s):  
E. F. Mikhailov ◽  
O. A. Ivanova ◽  
E. Yu. Nebosko ◽  
S. S. Vlasenko ◽  
T. I. Ryshkevich

Bioparticles represent a significant fraction of the total atmospheric aerosol. Their size range varies from nanometers (macromolecules) to hundreds of micrometers (plant pollen, vegetation residues) and like other atmospheric aerosol particles, the degree of involvement of bioaerosols in atmospheric processes largely de- pends on their hygroscopic and cloud condensation nuclei properties. In this paper the ability of the pine, birch and rape subpollen particles to act as cloud condensation nuclei are considered. Submicron particles were obtained by aqueous extraction of biological material from pollen grains and subsequent solidification of the atomized liquid droplets. The parameters of cloud activation are determined in the size range of 20-270 nm in the range of water vapor supersaturations 0.1-1.1%. Based on experimental results, the hygroscopicity parameter, characterizing the effect of the chemical composition of the subparticles on their con- densation properties, is determined. The range of the hygroscopic parameter changes was 0.12-0.13. In general, the results of measurements showed that the condensation activity of the subpollen particles is comparable with the condensation activity of secondary organic aerosols and weakly depends on the type of the primary pollen.


2012 ◽  
Vol 12 (1) ◽  
pp. 1493-1516
Author(s):  
Q. Zhang ◽  
J. Meng ◽  
J. Quan ◽  
Y. Gao ◽  
D. Zhao ◽  
...  

Abstract. The impact of aerosol composition on cloud condensation nuclei (CCN) activity was analyzed in this study based on field experiments carried out at downtown Tianjin, China, in September 2010. In the experiments, the CCN measurements were performed at supersaturation (SS) of 0.1%, 0.2% and 0.4% using a thermal-gradient diffusion chamber (DMT CCNC), whereas the aerosol size distribution and composition were simultaneously measured with a TSI SMPS and an Aerodyne Aerosol Mass Spectrometer (AMS), respectively. The results show that the influence of aerosol composition on CCN activity is notable under low SS (0.1%), and their influence decreased with increasing SS. For example, under SS of 0.1%, the CCN activity increases from 4.5 ± 2.6% to 12.8 ± 6.1% when organics fraction decrease from 30–40% to 10–20%. The rate of increase reaches up to 184%. While under SS of 0.4%, the CCN activity increases only from 35.7 ± 19.0% to 46.5 ± 12.3%, correspondingly. The calculated NCCN based on the size-resolved activation ratio and aerosol number size distribution correlates well with observed NCCN at high SS (0.4%), but this correlation decreases with the falling of SS. The slopes of linear fitted lines between calculated and observed NCCN are 0.708, 0.947, and 0.995 at SS of 0.1%, 0.2% and 0.4%, respectively. Moreover, the standard deviation (SD) of calculated NCCN increases with the decreasing of SS. A case study of CCN closure analyses indicates that the calculated error of NCCN can reach up to 34% at SS of 0.1% if aerosol composition is not included, and the calculated error decreases with the raising of SS. It decreases to 9% at SS of 0.2%, and further decreases to 4% at SS of 0.4%.


2012 ◽  
Vol 12 (4) ◽  
pp. 8547-8577 ◽  
Author(s):  
X. Tang ◽  
D. R. Cocker III ◽  
A. Asa-Awuku

Abstract. Secondary organic aerosol (SOA) was formed in an environmental reaction chamber from the ozonolysis of β-caryophyllene (β-C) at very low concentrations (5 ppb or 20 ppb) near ambient conditions. Experimental parameters were varied to characterize the effects of hydroxyl radicals, light and the presence of lower molecular weight terpene precursor (isoprene) for β-C SOA formation and Cloud Condensation Nuclei (CCN) characteristics. Changes in β-C SOA chemicophysical properties (e.g. density, volatility, oxidation state) were explored with online techniques to improve our predictive understanding of β-C CCN activity. In the absence of OH scavenger, light intensity had negligible impacts on SOA oxidation state and CCN activity. In contrast, when OH reaction was effectively suppressed (>11ppm scavenger), SOA showed a much lower CCN activity and slightly less oxygenated state consistent with previously reported values. Though there is significant oxidized material present (O/C>0.25), no linear correlation existed between the mass ratio ion fragment 44 in the bulk organic mass (f44) and O/C for the β-C-O3 system. No direct correlations were observed with other aerosol bulk ion fragment fraction (fx) and κ as well. A mixture of β-C and lower molecular weight terpenes (isoprene) consumed more ozone and formed SOA with distinct characteristics dependent on isoprene amounts. The addition of isoprene also improved the CCN predictive capabilities with bulk aerosol chemical information. The β-C SOA CCN activity reported here is much higher than previous studies (κ>0.1) that use higher precursor concentration in smaller environmental chambers; similar results were only achieved with significant use of OH scavenger. Results show that aerosol formed from a mixture of low and high molecular weight terpene ozonolysis can be hygroscopic and can contribute to the global biogenic SOA CCN budget.


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