In situ chemical composition measurement of individual cloud residue particles at a mountain site, southern China

Abstract. To investigate how atmospheric aerosol particles interact with chemical composition of cloud droplets, a ground-based counterflow virtual impactor (GCVI) coupled with a real-time single-particle aerosol mass spectrometer (SPAMS) was used to assess the chemical composition and mixing state of individual cloud residue particles in the Nanling Mountains (1690 m a. s. l. ), southern China, in January 2016. The cloud residues were classified into nine particle types: aged elemental carbon (EC), potassium-rich (K-rich), amine, dust, Pb, Fe, organic carbon (OC), sodium-rich (Na-rich) and Other. The largest fraction of the total cloud residues was the aged EC type (49.3 %), followed by the K-rich type (33.9 %). Abundant aged EC cloud residues that mixed internally with inorganic salts were found in air masses from northerly polluted areas. The number fraction (NF) of the K-rich cloud residues increased within southwesterly air masses from fire activities in Southeast Asia. When air masses changed from northerly polluted areas to southwesterly ocean and livestock areas, the amine particles increased from 0.2 to 15.1 % of the total cloud residues. The dust, Fe, Pb, Na-rich and OC particle types had a low contribution (0.5–4.1 %) to the total cloud residues. Higher fraction of nitrate (88–89 %) was found in the dust and Na-rich cloud residues relative to sulfate (41–42 %) and ammonium (15–23 %). Higher intensity of nitrate was found in the cloud residues relative to the ambient particles. Compared with nonactivated particles, nitrate intensity decreased in all cloud residues except for dust type. To our knowledge, this study is the first report on in situ observation of the chemical composition and mixing state of individual cloud residue particles in China.

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In situ chemical measurement of individual cloud residue particles at a mountain site, South China

10.5194/acp-2017-23 ◽

2017 ◽

Author(s):

Qinhao Lin ◽

Guohua Zhang ◽

Long Peng ◽

Xinhui Bi ◽

Xinming Wang ◽

...

Keyword(s):

Chemical Composition ◽

South China ◽

Chemical Properties ◽

In Situ Observation ◽

Mountain Range ◽

Mixing State ◽

Cloud Droplets ◽

Air Masses ◽

Aerosol Mass

Abstract. To estimate how atmospheric aerosol particles respond to chemical properties of cloud droplets, a ground-based counterflow virtual impactor (GCVI) coupled with a real-time single-particle aerosol mass spectrometer (SPAMS) was used to assess the chemical composition and mixing state of individual cloud residue particles in the Nanling Mountain Range (1,690 m a.s.l.), South China, in January 2016. The cloud residues were classified into nine particle types: Aged elemental carbon (EC), Potassium-rich (K-rich), Amine, Dust, Pb, Fe, Organic carbon (OC), Sodium-rich (Na-rich) and Other. The largest fraction of the cloud residues was the aged EC type (49.3 % by number), followed by the K-rich type (33.9 % by number). Abundant aged EC cloud residues that internally mixed with inorganic salts were found in air masses from northerly polluted areas. The number fraction (Nf) of the K-rich cloud residues significantly increased within southwesterly air masses from fire activities in Southeast Asia. In addition, the Amine particles represented 0.2 % to 15.1 % by number to the cloud residues when air masses changed from northerly to southwesterly sources. The Dust, Fe, Pb, Na-rich and OC particles had a low contribution (0.5–4.1 % by number) to the cloud residues. An analysis of the mixing state of cloud residues showed that the Dust and Na-rich cloud residues were highly associated with nitrate. Sulfate intensity increased in the aged EC and OC cloud residues and decreased in the Dust and Na-rich cloud residues relative to both ambient and interstitial particles. A comparison of cloud residues with interstitial particles indicated that a higher Nf for K-rich particles and a lower Nf for the aged EC particles were found in the cloud residues. Relative to the ambient and interstitial particles, the cloud residues exhibited larger size distributions. To our knowledge, this study is the first report on in situ observation of the chemical composition and mixing state of individual cloud residue particles in China. This study increases our understanding of the impacts of aerosols on cloud droplets in a remote area of China.

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The single-particle mixing state and cloud scavenging of black carbon: a case study at a high-altitude mountain site in southern China

Atmospheric Chemistry and Physics ◽

10.5194/acp-17-14975-2017 ◽

2017 ◽

Vol 17 (24) ◽

pp. 14975-14985 ◽

Cited By ~ 17

Author(s):

Guohua Zhang ◽

Qinhao Lin ◽

Long Peng ◽

Xinhui Bi ◽

Duohong Chen ◽

...

Keyword(s):

Black Carbon ◽

Single Particle ◽

Southern China ◽

Cloud Droplet ◽

Mixing State ◽

Cloud Droplets ◽

Aerosol Mass ◽

Mountain Site ◽

Cloud Scavenging ◽

Scavenging Efficiency

Abstract. In the present study, a ground-based counterflow virtual impactor (GCVI) was used to sample cloud droplet residual (cloud RES) particles, while a parallel PM2.5 inlet was used to sample cloud-free or cloud interstitial (cloud INT) particles. The mixing state of black carbon (BC)-containing particles and the mass concentrations of BC in the cloud-free, RES and INT particles were investigated using a single-particle aerosol mass spectrometer (SPAMS) and two aethalometers, respectively, at a mountain site (1690 m a. s. l. ) in southern China. The measured BC-containing particles were extensively internally mixed with sulfate and were scavenged into cloud droplets (with number fractions of 0.05–0.45) to a similar (or slightly lower) extent as all the measured particles (0.07–0.6) over the measured size range of 0.1–1.6 µm. The results indicate the preferential activation of larger particles and/or that the production of secondary compositions shifts the BC-containing particles towards larger sizes. BC-containing particles with an abundance of both sulfate and organics were scavenged less than those with sulfate but limited organics, implying the importance of the mixing state on the incorporation of BC-containing particles into cloud droplets. The mass scavenging efficiency of BC with an average of 33 % was similar for different cloud events independent of the air mass. This is the first time that both the mixing state and cloud scavenging of BC in China have been reported. Our results would improve the knowledge on the concentration, mixing state, and cloud scavenging of BC in the free troposphere.

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Enrichment of submicron sea-salt-containing particles in small cloud droplets based on single-particle mass spectrometry

Atmospheric Chemistry and Physics ◽

10.5194/acp-19-10469-2019 ◽

2019 ◽

Vol 19 (16) ◽

pp. 10469-10479 ◽

Cited By ~ 2

Author(s):

Qinhao Lin ◽

Yuxiang Yang ◽

Yuzhen Fu ◽

Guohua Zhang ◽

Feng Jiang ◽

...

Keyword(s):

Chemical Composition ◽

Organic Acids ◽

Single Particle ◽

Southern China ◽

Cloud Condensation Nuclei ◽

Sea Salt ◽

Cloud Droplets ◽

Organic Species ◽

Aerosol Mass ◽

Ccn Activity

Abstract. The effects of the chemical composition and size of sea-salt-containing particles on their cloud condensation nuclei (CCN) activity are incompletely understood. We used a ground-based counterflow virtual impactor (GCVI) coupled with a single-particle aerosol mass spectrometer (SPAMS) to characterize chemical composition of submicron (dry diameter of 0.2–1.0 µm) and supermicron (1.0–2.0 µm) sea-salt-containing cloud residues (dried cloud droplets) at Mount Nanling, southern China. Seven cut sizes (7.5–14 µm) of cloud droplets were set in the GCVI system. The highest number fraction of sea-salt-containing particles was observed at the cut size of 7.5 µm (26 %, by number), followed by 14 µm (17 %) and the other cut sizes (3 %–5 %). The submicron sea-salt-containing cloud residues contributed approximately 20 % (by number) at the cut size of 7.5 µm, which was significantly higher than the percentages at the cut sizes of 8–14 µm (below 2 %). This difference was likely involved in the change in the chemical composition. At the cut size of 7.5 µm, nitrate was internally mixed with over 90 % of the submicron sea-salt-containing cloud residues, which was higher than sulfate (20 %), ammonium (below 1 %), amines (6 %), hydrocarbon organic species (2 %), and organic acids (4 %). However, at the cut sizes of 8–14 µm, nitrate, sulfate, ammonium, amines, hydrocarbon organic species, and organic acids were internally mixed with > 90 %, > 80 %, 39 %–84 %, 71 %–86 %, 52 %–90 %, and 32 %–77 % of the submicron sea-salt-containing cloud residues. The proportion of sea-salt-containing particles in the supermicron cloud residues generally increased as a function of cut size, and their CCN activity was less influenced by chemical composition. This study provided a significant contribution towards a comprehensive understanding of sea-salt CCN activity.

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Enrichment of submicron sea salt-containing particles in small cloud droplets based on single particle mass spectrometry

10.5194/acp-2019-143 ◽

2019 ◽

Author(s):

Qinhao Lin ◽

Yuxiang Yang ◽

Yuzhen Fu ◽

Guohua Zhang ◽

Feng Jiang ◽

...

Keyword(s):

Chemical Composition ◽

Organic Acids ◽

Single Particle ◽

Southern China ◽

Cloud Condensation Nuclei ◽

Sea Salt ◽

Cloud Droplets ◽

Organic Species ◽

Aerosol Mass ◽

Ccn Activity

Abstract. The effects of chemical composition and size of sea salt-containing particles on their cloud condensation nuclei (CCN) activity are incompletely understood. We used a ground-based counterflow virtual impactor (GCVI) coupled with a single particle aerosol mass spectrometer (SPAMS) to characterize chemical composition of submicron (dry diameter of 0.2–1.0 μm) and supermicron (dry diameter of 1.0–2.0 μm) sea salt-containing cloud residues (dried cloud droplets) at Mount Nanling, southern China. Seven cut sizes (7.5–14 μm) of cloud droplets were set in the GCVI system. Approximately 20 % (by number) of the submicron cloud residues included sea salt-containing particles at the cut size of 7.5 μm, which was significantly higher than the percentages at the cut sizes of 8–14 μm (below 2 %). This difference was likely to be involved in the change in the chemical composition. For the cut size of 7.5 μm, nitrate was internally mixed with over 90 % of the submicron sea salt-containing cloud residues, which was higher than sulfate (20 %), ammonium (below 1 %), amines (6 %), hydrocarbon organic species (2 %), and organic acids (4 %). However, nitrate, sulfate, ammonium, amines, hydrocarbon organic species, and organic acids were internally mixed with over 90 %, over 80 %, 39–84 %, 71–86 %, 52–90 %, and 32–77 %, respectively, of the submicron sea salt-containing cloud residues for the cut sizes of 8–14 μm. The proportion of sea salt-containing particles in the supermicron cloud residues generally increased as a function of cut size, and their CCN activity was less influenced by chemical composition. This study highlights the different distribution of the submicron and supermicron sea salt-containing particles in various cloud droplets, which might further influence their atmospheric residence time.

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Relationship between the Optical Properties and Chemical Composition of Urban Aerosol Particles in Lithuania

Advances in Meteorology ◽

10.1155/2018/8674173 ◽

2018 ◽

Vol 2018 ◽

pp. 1-10 ◽

Cited By ~ 1

Author(s):

Julija Pauraite ◽

Kristina Plauškaitė ◽

Vadimas Dudoitis ◽

Vidmantas Ulevicius

Keyword(s):

Optical Properties ◽

Chemical Composition ◽

Organic Aerosol ◽

Single Scattering ◽

Chemical Compositions ◽

Spectra Analysis ◽

Average Value ◽

Aerosol Mass ◽

In Situ Investigation

In situ investigation results of aerosol optical properties (absorption and scattering) and chemical composition at an urban background site in Lithuania (Vilnius) are presented. Investigation was performed in May-June 2017 using an aerosol chemical speciation monitor (ACSM), a 7-wavelength Aethalometer and a 3-wavelength integrating Nephelometer. A positive matrix factorisation (PMF) was used for the organic aerosol mass spectra analysis to characterise the sources of ambient organic aerosol (OA). Five OA factors were identified: hydrocarbon-like OA (HOA), biomass-burning OA (BBOA), more and less oxygenated OA (LVOOA and SVOOA, respectively), and local hydrocarbon-like OA (LOA). The average absorption (at 470 nm) and scattering (at 450 nm) coefficients during the entire measurement campaign were 16.59 Mm−1 (standard deviation (SD) = 17.23 Mm−1) and 29.83 Mm−1 (SD = 20.45 Mm−1), respectively. Furthermore, the absorption and scattering Angström exponents (AAE and SAE, respectively) and single-scattering albedo (SSA) were calculated. The average AAE value at 470/660 nm was 0.97 (SD = 0.16) indicating traffic-related black carbon (BCtr) dominance. The average value of SAE (at 450/700 nm) was 1.93 (SD = 0.32) and could be determined by the submicron particle (PM1) dominance versus the supermicron ones (PM > 1 µm). The average value of SSA was 0.62 (SD = 0.13). Several aerosol types showed specific segregation in the SAE versus SSA plot, which underlines different optical properties due to various chemical compositions.

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The single-particle mixing state and cloud scavenging of black carbon at a high-altitude mountain site in southern China

10.5194/acp-2017-785 ◽

2017 ◽

Author(s):

Guohua Zhang ◽

Qinhao Lin ◽

Long Peng ◽

Xinhui Bi ◽

Duohong Chen ◽

...

Keyword(s):

Black Carbon ◽

Single Particle ◽

Southern China ◽

Climate Impacts ◽

Limited Information ◽

Mixing State ◽

Cloud Droplets ◽

Mountain Site ◽

Cloud Scavenging ◽

Scavenging Efficiency

Abstract. In the present study, a ground-based counterflow virtual impactor (GCVI) was used to sample cloud droplet residual (cloud RES) particles, while a parallel PM2.5 inlet was used to sample cloud-free or cloud interstitial (cloud INT) particles. The mixing state of black carbon (BC)-containing particles in a size range of 0.1–1.6 µm and the mass concentrations of BC in the cloud-free, RES and INT particles were investigated using a single particle aerosol mass spectrometer (SPAMS) and two aethalometers, respectively, at a mountain site (1690 m a.s.l.) in southern China. The measured BC-containing particles were internally mixed extensively with sulfate, and were activated into cloud droplets to the same extent as all the measured particles. The results indicate the preferential activation of larger particles and/or that the production of secondary compositions shifts the BC-containing particles towards larger sizes. BC-containing particles with an abundance of both sulfate and organics were activated less than those with sulfate but limited organics, implying the importance of the mixing state on the incorporation of BC-containing particles into cloud droplets. The mass scavenging efficiency of BC with an average of 33 % was similar for different cloud events independent of the air mass. This is the first time that both the mixing state and cloud scavenging of BC in China have been reported. Since limited information on BC-containing particles in the free troposphere is available, the results also provide an important reference for the representation of BC concentrations, properties, and climate impacts in modeling studies.

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Processing of biomass burning aerosol in the Eastern Mediterranean during summertime

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-13-25969-2013 ◽

2013 ◽

Vol 13 (10) ◽

pp. 25969-25999 ◽

Cited By ~ 2

Author(s):

A. Bougiatioti ◽

I. Stavroulas ◽

E. Kostenidou ◽

P. Zarmpas ◽

C. Theodosi ◽

...

Keyword(s):

Chemical Composition ◽

Biomass Burning ◽

Eastern Mediterranean ◽

Late Summer ◽

Organic Aerosol ◽

High Temporal Resolution ◽

Night Time ◽

Air Masses ◽

Aerosol Mass ◽

Atmospheric Processing

Abstract. The aerosol chemical composition in air masses affected by wildfires from the Greek islands of Chios, Euboea and Andros, the Dalmatian Coast and Sicily, during late summer of 2012 was characterized at the remote background site of Finokalia, Crete. Air masses were transported several hundreds of kilometers, arriving at the measurement station after approximately half a day of transport, mostly during night-time. The chemical composition of the particulate matter was studied by different high temporal resolution instruments, including an Aerosol Chemical Speciation Monitor (ACSM) and a seven-wavelength aethalometer. Despite the large distance from emission and long atmospheric processing, a clear biomass burning organic aerosol (BBOA) profile containing characteristic markers is derived from BC measurements and Positive Matrix Factorization (PMF) analysis of the ACSM mass spectra. The ratio of fresh to aged BBOA decreases with increasing atmospheric processing time and BBOA components appear to be converted to oxygenated organic aerosol (OOA). Given that the smoke was mainly transported overnight, it appears that the processing can take place in the dark. These results show that a significant fraction of the BBOA loses its characteristic AMS signature and is transformed to OOA in less than a day. This implies that biomass burning can contribute almost half of the organic aerosol mass in the area during summertime.

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A GCM study of organic matter in marine aerosol and its potential contribution to cloud drop activation

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-7-5675-2007 ◽

2007 ◽

Vol 7 (2) ◽

pp. 5675-5700

Author(s):

G. J. Roelofs

Keyword(s):

Organic Matter ◽

Chemical Composition ◽

Dimethyl Sulfide ◽

Climate Model ◽

Organic Aerosol ◽

Potential Contribution ◽

Marine Aerosol ◽

Mixing State ◽

Cloud Drop ◽

Aerosol Mass

Abstract. With the global aerosol-climate model ECHAM5-HAM we investigate the potential influence of organic aerosol originating from the ocean on aerosol mass and chemical composition and the droplet concentration and size of marine clouds. We present sensitivity simulations in which the uptake of organic matter in the marine aerosol is prescribed for each aerosol mode with varying organic mass and mixing state, and with a geographical distribution and seasonality similar to the oceanic emission of dimethyl sulfide. Measurements of aerosol mass and chemical composition serve to evaluate the representativity of the model initializations. Good agreement with the measurements is obtained when organic matter is added to the Aitken, accumulation and coarse modes simultaneously. Representing marine organics in the model leads to higher cloud drop number concentrations, smaller cloud drop effective radii, and a better agreement with remote sensing measurements. The mixing state of the organics and the other aerosol matter, i.e., internal or external depending on the formation process of aerosol organics, is an important factor for this. We estimate that globally about 75 Tg C yr−1 of organic matter from marine origin enters the aerosol phase. An approximate 35% of this occurs through formation of secondary organic aerosol and 65% through emission of primary particles.

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Quantitative determination of carbonaceous particle mixing state in Paris using single particle mass spectrometer and aerosol mass spectrometer measurements

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-13-10345-2013 ◽

2013 ◽

Vol 13 (4) ◽

pp. 10345-10393

Author(s):

R. M. Healy ◽

J. Sciare ◽

L. Poulain ◽

M. Crippa ◽

A. Wiedensohler ◽

...

Keyword(s):

Chemical Composition ◽

Mass Spectrometer ◽

Single Particle ◽

Organic Aerosol ◽

Particle Mass ◽

Mixing State ◽

Aerosol Mass Spectrometer ◽

Aerosol Mass ◽

Particle Mixing ◽

Mixing States

Abstract. Single particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been estimated using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulphate and potassium were compared with concurrent measurements from an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal/optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived mass concentrations reproduced the variability of these species well (R2 = 0.67–0.78), and ten discrete mixing states for carbonaceous particles were identified and quantified. Potassium content was used to identify particles associated with biomass combustion. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorization, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulphate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA/EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidized OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the heterogeneity of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal behaviour and chemical composition of the ATOFMS classes also enabled estimation of the relative contribution of transported emissions of each chemical species and total particle mass in the size range investigated. Only 22% of the total ATOFMS-derived particle mass was apportioned to fresh, local emissions, with 78% apportioned to regional/continental scale emissions.

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Chemical composition of the ATAL aerosol measured by in-situ particle mass spectrometry

10.5194/egusphere-egu2020-9949 ◽

2020 ◽

Author(s):

Oliver Appel ◽

Andreas Hünig ◽

Antonis Dragoneas ◽

Sergej Molleker ◽

Frank Drewnick ◽

...

Keyword(s):

Mass Spectrometry ◽

Laser Ablation ◽

Chemical Composition ◽

Particle Diameter ◽

Aerosol Layer ◽

Aerosol Mass Spectrometer ◽

High Particle ◽

Aerosol Mass ◽

Ionisation Mass Spectrometry

The Asian Tropopause Aerosol Layer (ATAL) has been found to be an aerosol layer with exceptionally high particle number concentrations in the UT/LS altitude range. During the StratoClim 2017 field campaign in Nepal we deployed the novel in-situ aerosol mass spectrometer ERICA (ERC Instrument for Chemical composition of Aerosols). It combines the methods of laser ablation mass spectrometry with flash vaporization/electron impact ionisation mass spectrometry in a single instrument to analyse the chemical composition of individual aerosol particles or small particle ensembles in the particle diameter range from 100 nm to 2 &#181;m.The quantitative analysis shows a strong contribution of ammonium nitrate (AN) to the ATAL aerosol concentration. In this layer, the AN concentrations can be as high as 1.5 &#181;g per standard cubic meter. We present the vertical distribution of the mass concentrations of AN as well as other contributing species like sulphate and organics.The single particle data from the laser ablation module of ERICA show a distinct particle type with nitrate and sulphate ions without the typical components of primary aerosol (soot, dust, metals) within the ATAL, indicating that a significant fraction of the ATAL aerosol consists of secondary particles formed in the upper troposphere.

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