Evidence of formation of submicrometer water-soluble organic aerosols at a deciduous forest site in northern Japan in summer

Abstract. To investigate the seasonal changes in biogenic water-soluble organic carbon (WSOC) aerosols in a boreal forest, aerosol samples were collected continuously in the canopy of a~deciduous forest in Northern Japan during 2009–2010. Stable carbon isotopic ratios of WSOC (δ13CWSOC) in aerosols exhibited a distinct seasonal cycle, with lower values from June through September (−25.5 ± 0.5‰). This cycle follows the net CO2 exchange between the forest ecosystem and the atmosphere, indicating that δ13CWSOC likely reflects the biological activity at the forest site. WSOC concentrations showed the highest values in early summer and autumn. Positive matrix factorization (PMF) analysis indicated that the factor in which biogenic secondary organic aerosols (BSOAs) dominated accounted for ~ 40% of the highest concentrations of WSOC, where BSOAs mostly consisted of α-/β-pinene SOA. In addition, primary biological aerosol particles (PBAPs) made similar contributions (~ 57%) to the WSOC near the canopy floor in early summer. This finding indicates that the production of both primary and secondary WSOC aerosols is important during the growing season in a deciduous forest. The methanesulfonic acid (MSA) maximum was also found in early summer and had a distinct vertical gradient with larger concentrations near the canopy floor. Together with the similar vertical gradients found for WSOC and δ13CWSOCas well as the α-/β-pinene SOA tracers, our results indicate that the forest floor, including ground vegetation and soil, acts as a significant source of the WSOC within a~forest canopy at the study site.

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Seasonal variations of stable carbon isotopic composition and biogenic tracer compounds of water-soluble organic aerosols in a deciduous forest

Atmospheric Chemistry and Physics ◽

10.5194/acp-12-1367-2012 ◽

2012 ◽

Vol 12 (3) ◽

pp. 1367-1376 ◽

Cited By ~ 55

Author(s):

Y. Miyazaki ◽

P. Q. Fu ◽

K. Kawamura ◽

Y. Mizoguchi ◽

K. Yamanoi

Keyword(s):

Isotopic Composition ◽

Forest Floor ◽

Deciduous Forest ◽

Carbon Isotopic Composition ◽

Organic Aerosols ◽

Early Summer ◽

Water Soluble ◽

Ground Vegetation ◽

Stable Carbon ◽

Carbon Isotopic

Abstract. To investigate the seasonal changes in biogenic water-soluble organic carbon (WSOC) aerosols in a boreal forest, aerosol samples were collected continuously in the canopy of a deciduous forest in northern Japan during 2009–2010. Stable carbon isotopic composition of WSOC (δ13CWSOC) in total suspended particulate matter (TSP) exhibited a distinct seasonal cycle, with lower values from June through September (−25.5±0.5 ‰). This cycle follows the net CO2 exchange between the forest ecosystem and the atmosphere, indicating that δ13CWSOC likely reflects the biological activity at the forest site. WSOC concentrations showed the highest values in early summer and autumn. Positive matrix factorization (PMF) analysis indicated that the factor in which biogenic secondary organic aerosols (BSOAs) dominated accounted for ~40 % of the highest concentrations of WSOC, where BSOAs mostly consisted of α-/β-pinene SOA. In addition, primary biological aerosol particles (PBAPs) made similar contributions (~57 %) to the WSOC near the forest floor in early summer. This finding indicates that the production of both primary and secondary WSOC aerosols is important during the growing season in a deciduous forest. The methanesulfonic acid (MSA) maximum was also found in early summer and had a distinct vertical gradient with larger concentrations near the forest floor. Together with the similar vertical gradients found for WSOC and δ13CWSOC as well as the α-/β-pinene SOA tracers, our results indicate that the forest floor, including ground vegetation and soil, acts as a significant source of WSOC in TSP within a forest canopy at the study site.

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Different characteristics of new particle formation between urban and deciduous forest sites in Northern Japan during the summers of 2010–2011

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-12-14043-2012 ◽

2012 ◽

Vol 12 (6) ◽

pp. 14043-14087

Author(s):

J. Jung ◽

Y. Miyazaki ◽

K. Kawamura

Keyword(s):

Wind Direction ◽

Deciduous Forest ◽

Particle Formation ◽

Urban Site ◽

Forest Site ◽

New Particle Formation ◽

Air Masses ◽

Nucleation Mode ◽

Prevailing Wind Direction ◽

Northern Japan

Abstract. To investigate new particle formation (NPF) events in urban and forest environments, number size distributions of ultrafine particles were measured at an urban site and a deciduous forest site in Sapporo, Northern Japan, during the summers of 2011 and 2010, respectively. The burst of nucleation mode particles at the urban site typically started in the morning (7:00–11:30 local time, LT) with simultaneous increases in SO2 and O3 concentrations and the UV index under clear (sunny) weather conditions. The growth rates of nucleated particles at the urban site ranged from 5.0 to 7.8 nm h−1 with an average of 6.3 ± 1.1 nm h−1. NPF events at the urban site were separated into events with or without subsequent particle growth after the burst of nucleation mode particles. This division was related to prevailing wind direction as the subsequent growth of freshly nucleated particles typically occurred when wind direction shifted to northwesterly (from residential and public park areas), whereas it did not occur under southeasterly winds (from the downtown area). During the periods with NPF events, elevated concentrations of non-methane hydrocarbons (NMHC) were obtained under conditions of northwesterly winds when compared to southeasterly winds, whereas no difference in SO2 levels was recorded. These results suggest that variations in NMHC concentration may play an important role in the growth of freshly nucleated particles at the urban site. The burst of nucleation mode particles at the forest site typically started around noon (10:30–14:30 LT), which was 3–4 h later than that at the urban site. Interestingly, at the forest site the burst of nucleation mode particles usually started when air masses originating from urban Sapporo arrived at the forest site. The present study indicates that the inflow of these urban air masses acted as a trigger for the initiation of the burst of nucleation mode particles in the deciduous forest.

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Different characteristics of new particle formation between urban and deciduous forest sites in Northern Japan during the summers of 2010–2011

Atmospheric Chemistry and Physics ◽

10.5194/acp-13-51-2013 ◽

2013 ◽

Vol 13 (1) ◽

pp. 51-68 ◽

Cited By ~ 22

Author(s):

J. Jung ◽

Y. Miyazaki ◽

K. Kawamura

Keyword(s):

Wind Direction ◽

Deciduous Forest ◽

Particle Formation ◽

Urban Site ◽

Forest Site ◽

New Particle Formation ◽

Air Masses ◽

Nucleation Mode ◽

Prevailing Wind Direction ◽

Northern Japan

Abstract. To investigate new particle formation (NPF) events in urban and forest environments, number size distributions of ultrafine particles were measured at an urban site and a deciduous forest site in Sapporo, Northern Japan, during the summers of 2011 and 2010, respectively. The burst of nucleation mode particles at the urban site typically started in the morning (07:00–11:30 local time, LT) with simultaneous increases in SO2 and O3 concentrations and the UV index under clear (sunny) weather conditions. The growth rates of nucleated particles at the urban site ranged from 5.0 to 7.8 nm h−1 with an average of 6.3 ± 1.1 nm h−1. NPF events at the urban site were separated into events with or without subsequent particle growth after the burst of nucleation mode particles. This division was found to relate to prevailing wind direction because the subsequent growth of freshly nucleated particles typically occurred when wind direction shifted to northwesterly (from residential and public park areas), whereas it did not occur under southeasterly winds (from the downtown area). During the periods with NPF events, elevated concentrations of non-methane hydrocarbons (NMHC) were obtained under conditions of northwesterly winds when compared to southeasterly winds, whereas no difference in SO2 levels was recorded. These results suggest that variations in NMHC concentration may play an important role in the growth of freshly nucleated particles at the urban site. The burst of nucleation mode particles at the forest site typically started around noon (10:30–14:30 LT), which was 3–4 h later than that at the urban site. Interestingly, at the forest site the burst of nucleation mode particles usually started when air masses originating from urban Sapporo arrived at the forest site. The present study indicates that the inflow of these urban air masses acted as a trigger for the initiation of the burst of nucleation mode particles in the deciduous forest.

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On the relationship of NDVI with leaf area index in a deciduous forest site

Remote Sensing of Environment ◽

10.1016/j.rse.2004.10.006 ◽

2005 ◽

Vol 94 (2) ◽

pp. 244-255 ◽

Cited By ~ 283

Author(s):

Quan Wang ◽

Samuel Adiku ◽

John Tenhunen ◽

André Granier

Keyword(s):

Leaf Area Index ◽

Leaf Area ◽

Deciduous Forest ◽

Forest Site ◽

Area Index ◽

Relationship Of ◽

The Relationship

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Multidimensional Analytical Characterization of Water-Soluble Organic Aerosols: Challenges and New Perspectives

Applied Sciences ◽

10.3390/app11062539 ◽

2021 ◽

Vol 11 (6) ◽

pp. 2539

Author(s):

Regina M. B. O. Duarte ◽

João T. V. Matos ◽

Armando C. Duarte

Keyword(s):

High Resolution ◽

High Resolution Mass Spectrometry ◽

Organic Aerosols ◽

Analytical Techniques ◽

Water Soluble ◽

Chemical Complexity ◽

Molecular Features ◽

High Resolution Mass ◽

Analytical Strategies ◽

Resolution Mass

Water-soluble organic aerosols (OA) are an important component of air particles and one of the key drivers that impact both climate and human health. Understanding the processes involving water-soluble OA depends on how well the chemical composition of this aerosol component is decoded. Yet, obtaining detailed information faces several challenges, including water-soluble OA collection, extraction, and chemical complexity. This review highlights the multidimensional non-targeted analytical strategies that have been developed and employed for providing new insights into the structural and molecular features of water-soluble organic components present in air particles. First, the most prominent high-resolution mass spectrometric methods for near real-time measurements of water-soluble OA and their limitations are discussed. Afterward, a special emphasis is given to the degree of compositional information provided by offline multidimensional analytical techniques, namely excitation–emission (EEM) fluorescence spectroscopy, high-resolution mass spectrometry and two-dimensional nuclear magnetic resonance (NMR) spectroscopy and their hyphenation with chromatographic systems. The major challenges ahead on the application of these multidimensional analytical strategies for OA research are also addressed so that they can be used advantageously in future studies.

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Characterisation of water-soluble organic aerosols at a site on the southwest coast of India

Journal of Atmospheric Chemistry ◽

10.1007/s10874-015-9322-4 ◽

2015 ◽

Vol 73 (2) ◽

pp. 181-205 ◽

Cited By ~ 8

Author(s):

Prashant Hegde ◽

Kimitaka Kawamura ◽

I. A. Girach ◽

Prabha R. Nair

Keyword(s):

Organic Aerosols ◽

Water Soluble ◽

Southwest Coast Of India ◽

Southwest Coast ◽

A Site

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Exploring water-soluble organic aerosols structures in urban atmosphere using advanced solid-state 13C NMR spectroscopy

Atmospheric Environment ◽

10.1016/j.atmosenv.2020.117503 ◽

2020 ◽

Vol 230 ◽

pp. 117503

Author(s):

Regina M.B.O. Duarte ◽

Pu Duan ◽

Jingdong Mao ◽

Wenying Chu ◽

Armando C. Duarte ◽

...

Keyword(s):

Solid State ◽

Nmr Spectroscopy ◽

13C Nmr ◽

Organic Aerosols ◽

13C Nmr Spectroscopy ◽

Water Soluble ◽

Urban Atmosphere ◽

Solid State 13C Nmr

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Contribution of dissolved organic matter to submicron water-soluble organic aerosols in the marine boundary layer over the eastern equatorial Pacific

10.5194/acp-2016-164 ◽

2016 ◽

Cited By ~ 1

Author(s):

Yuzo Miyazaki ◽

Sean Coburn ◽

Kaori Ono ◽

David T. Ho ◽

R. Bradley Pierce ◽

...

Keyword(s):

Boundary Layer ◽

Organic Carbon ◽

Marine Boundary Layer ◽

Organic Aerosols ◽

Equatorial Pacific ◽

Water Soluble ◽

Total Carbon ◽

Stable Carbon ◽

Study Region ◽

Eastern Equatorial Pacific

Abstract. Stable carbon isotopic compositions of water-soluble organic carbon (WSOC) and organic molecular markers were measured to investigate the relative contributions of the sea-surface sources to the water-soluble fraction of submicron organic aerosols collected over the eastern equatorial Pacific during the Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOCs (TORERO)/KA-12-01 cruise. On average, the water-soluble organic fraction of the total carbon (TC) mass in submicron aerosols was ~ 30–35 % in the open oceans, whereas it was ~ 60 % in the coastal oceans. The average stable carbon isotope ratio of WSOC (δ13CWSOC) was −19.8 ± 2.0 ‰, which was systematically higher than that of TC (δ13CTC) (−21.8 ± 1.4 ‰). We found that in both coastal and open oceans, the δ13CWSOC was close to the typical values of δ13C for dissolved organic carbon (DOC), ranging from −22 ‰ to −20 ‰ in surface seawater of tropical Pacific oceans. This suggests an enrichment of marine biological products in WSOC aerosols in the study region regardless of the oceanic area. In particular, enhanced levels of WSOC and biogenic organic marker compounds together with high values of WSOC/TC (~ 60 %) and δ13CWSOC were observed over upwelling areas and phytoplankton blooms, which was attributed to planktonic tissues being more enriched in δ13C. The δ13C analysis estimated that on average, marine sources contribute ~ 90 ± 25 % of the aerosol carbon, indicating the predominance of marine-derived carbon in the submicron WSOC. This conclusion is supported by Lagrangian trajectory analysis, which suggests that the majority of the sampling points on the ship had been exposed to marine boundary layer air for more than 80 % of the time during the previous 7 days. The combined analysis of the δ13C and monosaccharides, such as glucose and fructose, indicated that DOC concentration was the major factor controlling the concentration levels of the submicron WSOC regardless of the oceanic areas over the study region.

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High time-resolved measurement of stable carbon isotope composition in water-soluble organic aerosols: method optimization and a case study during winter haze in East China

10.5194/acp-2018-1056 ◽

2018 ◽

Author(s):

Wenqi Zhang ◽

Yan-Lin Zhang ◽

Fang Cao ◽

Yankun Xiang ◽

Yuanyuan Zhang ◽

...

Keyword(s):

Organic Carbon ◽

Carbon Isotope ◽

Isotope Composition ◽

Stable Carbon Isotope ◽

Organic Aerosols ◽

Carbon Isotope Composition ◽

Water Soluble ◽

High Time ◽

Stable Carbon ◽

Air Mass

Abstract. Water soluble organic carbon (WSOC) is a significant fraction of organic carbon (OC) in atmospheric aerosols. WSOC is of great interest due to its significant effects on atmospheric chemistry, the Earth’s climate and human health. Stable carbon isotope (δ13C) can be used to track the potential sources and investigate atmospheric processes of organic aerosols. In this study, a method of simultaneously measuring the mass concentration and δ13C values of WSOC from aerosol samples is established by coupling the Gas Bench II preparation device with isotopic ratio mass spectrometry. The precision and accuracy of isotope determination is better than 0.17 ‰ and 0.5 ‰, respectively, for samples containing carbon larger than 5 μg. This method is then applied for the high time-resolution aerosol samples during a severe wintertime haze period in Nanjing, East China. WSOC varies between 3–32 μg m−3, whereas δ13C-WSOC ranges from −26.24 ‰ to −23.35 ‰. Three different episodes (e.g., namely the Episode 1, the Episode 2, the Episode 3) are identified in the sampling period, showing a different tendency of δ13C-WSOC with the accumulation process of WSOC aerosols. The increases in both the WSOC mass concentrations and the δ13C-WSOC values in the Episode 1 indicate that WSOC is subject to a substantial photochemical aging during the air mass transport. In the Episode 2, the decline of the δ13C-WSOC is accompanied by the increase in the WSOC mass concentrations, which is associated with regional-transported biomass burning emissions. In the Episode 3, heavier isotope (13C) is exclusively enriched in total carbon (TC) compares to WSOC aerosols. This suggests that water-insoluble carbon may contain 13C-enriched components such as dust carbonate which is supported by the enhanced Ca2+ concentrations and air mass trajectories analysis. The present study provides a novel method to determine stable carbon isotope composition of WSOC and it offers a great potential to better understand the source emission, the atmospheric aging and the secondary production of water soluble organic aerosols.

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