Toward a novel high-resolution modeling approach for the study of chemical evolution of pollutant plumes during long-range transport

Abstract. An intensive field measurement was conducted at a remote, background, high-altitude site (Qomolangma Station, QOMS, 4276 m a.s.l.) in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) along with other collocated instruments. The field measurement was performed from 12 April to 12 May 2016 to chemically characterize the high time-resolved submicron particulate matter (PM1) and obtain the dynamic processes (emissions, transport, and chemical evolution) of biomass burning (BB), frequently transported from South Asia to the Himalayas during pre-monsoon season. Overall, the average (±1σ) PM1 mass concentration was 4.44 (±4.54) µg m−3 for the entire study, which is comparable with those observed at other remote sites worldwide. Organic aerosol (OA) was the dominant PM1 species (accounting for 54.3 % of total PM1 on average) followed by black carbon (BC) (25.0 %), sulfate (9.3 %), ammonium (5.8 %), nitrate (5.1 %), and chloride (0.4 %). The average size distributions of PM1 species all peaked at an overlapping accumulation mode (∼ 500 nm), suggesting that aerosol particles were internally well-mixed and aged during long-range transport. Positive matrix factorization (PMF) analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a BB-related OA (BBOA, 43.7 %), a nitrogen-containing OA (NOA, 13.9 %) and a more-oxidized oxygenated OA (MO-OOA, 42.4 %). Two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions from the west and southwest of QOMS during the study were observed. A typical BB plume was investigated in detail to illustrate the chemical evolution of aerosol characteristics under distinct air mass origins, meteorological conditions, and atmospheric oxidation processes.

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Black and White Episodes, Chemical Evolution of Eurasian Air Masses, and Long-Range Transport of Carbon to the Arctic

Particulate Carbon ◽

10.1007/978-1-4684-4154-3_19 ◽

1982 ◽

pp. 327-342 ◽

Cited By ~ 10

Author(s):

K. A. Rahn ◽

C. Brosset ◽

B. Ottar ◽

E. M. Patterson

Keyword(s):

Long Range ◽

Chemical Evolution ◽

The Arctic ◽

Long Range Transport ◽

Air Masses ◽

Black And White ◽

Range Transport

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The CHE global nature run: A high-resolution simulation providing realistic global carbon weather for the year of the Paris Agreement

10.5194/egusphere-egu21-12556 ◽

2021 ◽

Author(s):

Anna Agusti-Panareda ◽

Joe McNorton ◽

Keyword(s):

High Resolution ◽

Long Range ◽

Paris Agreement ◽

Surface Fluxes ◽

Long Range Transport ◽

Co2 Monitoring ◽

Range Transport ◽

Atmospheric Observations ◽

Independent Observations ◽

Total Column

High resolution simulations of carbon dioxide, methane and carbon monoxide (CO2, CH4 and CO) have been produced as part of the CO2 Human Emissions (CHE) project in order to assist carbon-cycle research and applications, such as the design of a CO2 Monitoring Verification Support (CO2MVS) capacity in support of the Paris Agreement. This dataset provides realistic variability of the carbon tracers in the atmosphere modulated by the weather and the underlying surface fluxes as shown by comparison with independent observations. It can therefore provide a reference for atmospheric inversion systems that use atmospheric observations from satellites and in situ networks to derive natural surface fluxes and anthropogenic emissions of CO2, CH4 and CO. Additional tagged tracers are used to identify the atmospheric enhancements associated with the different surface fluxes. These flux enhancements can shed light into the potential of new satellites to detect the emission signals in the atmosphere. As satellites observe the mean concentration of carbon tracers over a partial/total atmospheric column, the CHE nature run is also used here to assess the contribution of total column variability from different layers in the atmosphere. We find that the variability in the free troposphere is often dominating the variability of the total column for CO2, CH4 and CO, highlighting the role of long-range transport to represent variability of carbon tracers in the atmosphere, as well as the importance of assessing the accuracy of long-range transport in chemical transport models used in atmospheric inversions.

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Characterizing the long-range transport of black carbon aerosols during Transport and Chemical Evolution over the Pacific (TRACE-P) experiment

Environmental Monitoring and Assessment ◽

10.1007/s10661-008-0379-2 ◽

2008 ◽

Vol 154 (1-4) ◽

pp. 85-92 ◽

Cited By ~ 10

Author(s):

Sunita Verma ◽

John Worden ◽

Swagata Payra ◽

Line Jourdain ◽

Changsub Shim

Keyword(s):

Black Carbon ◽

Long Range ◽

Chemical Evolution ◽

Long Range Transport ◽

The Pacific ◽

Range Transport ◽

Carbon Aerosols ◽

Black Carbon Aerosols

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Chemical characterization and sources of submicron aerosols in the northeastern Qinghai-Tibet Plateau: insights from high-resolution mass spectrometry

10.5194/acp-2019-88 ◽

2019 ◽

Author(s):

Xinghua Zhang ◽

Jianzhong Xu ◽

Shichang Kang ◽

Qi Zhang

Keyword(s):

High Resolution ◽

Long Range ◽

Biomass Burning ◽

Tibet Plateau ◽

Source Analysis ◽

Long Range Transport ◽

Aerosol Mass ◽

Range Transport ◽

Qinghai Tibet Plateau ◽

Mass Concentrations

Abstract. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed along with other online instruments to study the highly time-resolved chemistry and sources of submicron aerosols (PM1) at Waliguan (WLG) Baseline Observatory, a high-altitude (3816 m a.s.l.) background station located at the northeastern edge of Qinghai-Tibet Plateau (QTP), during 1–31 July 2017. The average PM1 mass concentration during this study was 9.1 μg m−3 (ranging from 0.3 to 28.1 μg m−3), which was distinct higher than those (2.0–5.7 μg m−3) measured with Aerodyne AMS at other high-elevation sites in the southern or central QTP. Sulfate showed dominant contribution (38.1 %) to PM1 at WLG following by organics (34.5 %), ammonium (15.2 %), nitrate (8.1 %), BC (3.0 %) and chloride (1.1 %). Accordingly, bulk aerosols appeared to be slightly acidic throughout this study mainly related to the enhanced sulfate contribution. All chemical species peaked at the accumulation mode, indicating the well mixed and highly aged aerosol particles at WLG from long-range transport. Positive matrix factorization (PMF) on the high-resolution organic mass spectra resolved four distinct organic aerosol (OA) components, including a traffic-related hydrocarbon-like OA (HOA), a relatively fresh biomass burning OA (BBOA), an aged biomass burning OA (agBBOA) and a more-oxidized oxygenated OA (OOA). On average, the two relatively oxidized OAs, OOA and agBBOA, contributed 34.4 % and 40.4 % of organics, respectively, while the rest were 18.4 % for BBOA and 6.8 % for HOA. Source analysis for air masses displayed higher mass concentrations of PM1 and enhanced contributions of sulfate and biomass burning related OA components (agBBOA + BBOA) were from northeast of the WLG with shorter transport distance, whereas lower PM1 mass concentrations with enhanced OOA contribution were from west after long-range transport, suggesting their distinct aerosol sources and significant impacts of regional transport to aerosol mass loadings and chemistry at WLG.

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Chemical characterization and sources of submicron aerosols in the northeastern Qinghai–Tibet Plateau: insights from high-resolution mass spectrometry

Atmospheric Chemistry and Physics ◽

10.5194/acp-19-7897-2019 ◽

2019 ◽

Vol 19 (11) ◽

pp. 7897-7911 ◽

Cited By ~ 5

Author(s):

Xinghua Zhang ◽

Jianzhong Xu ◽

Shichang Kang ◽

Qi Zhang ◽

Junying Sun

Keyword(s):

High Resolution ◽

Long Range ◽

Biomass Burning ◽

Tibet Plateau ◽

Source Analysis ◽

Long Range Transport ◽

Aerosol Mass ◽

Range Transport ◽

Qinghai Tibet Plateau ◽

Mass Concentrations

Abstract. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed along with other online instruments to study the highly time resolved chemistry and sources of submicron aerosols (PM1) at Waliguan (WLG) Baseline Observatory, a high-altitude (3816 m a.s.l.) background station located at the northeast edge of the Qinghai–Tibet Plateau (QTP), during 1–31 July 2017. The average PM1 mass concentration during this study was 9.1 µg m−3 (ranging from 0.3 to 28.1 µg m−3), which was distinctly higher than those (2.0–5.7 µg m−3) measured with the Aerodyne AMS at other high-elevation sites in the southern or central QTP. Sulfate showed a dominant contribution (38.1 %) to PM1 at WLG followed by organics (34.5 %), ammonium (15.2 %), nitrate (8.1 %), BC (3.0 %) and chloride (1.1 %). Accordingly, bulk aerosols appeared to be slightly acidic throughout this study, mainly related to the enhanced sulfate contribution. All chemical species peaked at the accumulation mode, indicating the well-mixed and highly aged aerosol particles at WLG from long-range transport. Positive matrix factorization (PMF) on the high-resolution organic mass spectra resolved four distinct organic aerosol (OA) components, including a traffic-related hydrocarbon-like OA (HOA), a relatively fresh biomass burning OA (BBOA), an aged biomass burning OA (agBBOA) and a more-oxidized oxygenated OA (OOA). On average, the two relatively oxidized OAs, OOA and agBBOA, contributed 34.4 % and 40.4 % of organics, respectively, while the rest were 18.4 % for BBOA and 6.8 % for HOA. Source analysis for air masses showed that higher mass concentrations of PM1 and enhanced contributions of sulfate and biomass-burning-related OA components (agBBOA + BBOA) were from the northeast of the WLG with shorter transport distance, whereas lower PM1 mass concentrations with enhanced OOA contribution were from the west after long-range transport, suggesting their distinct aerosol sources and significant impacts of regional transport on aerosol mass loadings and chemistry at WLG.

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