scholarly journals Eddy covariance measurements with high-resolution time-of-flight aerosol mass spectrometry: a new approach to chemically resolved aerosol fluxes

2011 ◽  
Vol 4 (6) ◽  
pp. 1275-1289 ◽  
Author(s):  
D. K. Farmer ◽  
J. R. Kimmel ◽  
G. Phillips ◽  
K. S. Docherty ◽  
D. R. Worsnop ◽  
...  
Keyword(s):  
High Resolution ◽  
Eddy Covariance ◽  
Ammonium Sulphate ◽  
Ponderosa Pine ◽  
Particle Deposition ◽  
Deposition Velocity ◽  
Time Of Flight ◽  
Resolution Time ◽  
New Approach ◽  
Aerosol Mass

Abstract. Although laboratory studies show that biogenic volatile organic compounds (VOCs) yield substantial secondary organic aerosol (SOA), production of biogenic SOA as indicated by upward fluxes has not been conclusively observed over forests. Further, while aerosols are known to deposit to surfaces, few techniques exist to provide chemically-resolved particle deposition fluxes. To better constrain aerosol sources and sinks, we have developed a new technique to directly measure fluxes of chemically-resolved submicron aerosols using the high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) in a new, fast eddy covariance mode. This approach takes advantage of the instrument's ability to quantitatively identify both organic and inorganic components, including ammonium, sulphate and nitrate, at a temporal resolution of several Hz. The new approach has been successfully deployed over a temperate ponderosa pine plantation in California during the BEARPEX-2007 campaign, providing both total and chemically resolved non-refractory (NR) PM1 fluxes. Average deposition velocities for total NR-PM1 aerosol at noon were 2.05 ± 0.04 mm s−1. Using a high resolution measurement of the NH2+ and NH3+ fragments, we demonstrate the first eddy covariance flux measurements of particulate ammonium, which show a noon-time deposition velocity of 1.9 ± 0.7 mm s−1 and are dominated by deposition of ammonium sulphate.

scholarly journals Eddy covariance measurements with high-resolution time-of-flight aerosol mass spectrometry: a new approach to chemically-resolved aerosol fluxes

2010 ◽  
Vol 3 (6) ◽  
pp. 5867-5905 ◽  
Author(s):  
D. K. Farmer ◽  
J. R. Kimmel ◽  
G. Phillips ◽  
K. S. Docherty ◽  
D. R. Worsnop ◽  
...  
Keyword(s):  
High Resolution ◽  
Eddy Covariance ◽  
Ammonium Sulphate ◽  
Ponderosa Pine ◽  
Particle Deposition ◽  
Deposition Velocity ◽  
Time Of Flight ◽  
Resolution Time ◽  
New Approach ◽  
Aerosol Mass

Abstract. Although laboratory studies show that biogenic volatile organic compounds (VOCs) yield substantial secondary organic aerosol (SOA), production of biogenic SOA as indicated by upward fluxes has not been conclusively observed over forests. Further, while aerosols are known to deposit to surfaces, few techniques exist to provide chemically-resolved particle deposition fluxes. To better constrain aerosol sources and sinks, we have developed a new technique to directly measure fluxes of chemically-resolved submicron aerosols using the high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) in a new, fast eddy covariance mode. This approach takes advantage of the instrument's ability to quantitatively identify both organic and inorganic components, including ammonium, sulphate and nitrate, at a temporal resolution of several Hz. The new approach has been successfully deployed over a temperate ponderosa pine plantation in California during the BEARPEX-2007 campaign, providing both total and chemically resolved non-refractory (NR) PM1 fluxes. Average deposition velocity for total NR-PM1 aerosol at noon was 2.05 ± 0.04 mm/s. Using a high resolution measurement of the NH2+ and NH3+ fragments, we demonstrate the first eddy covariance flux measurements of particulate ammonium, which show a noon-time deposition velocity of 1.9 ± 0.7 mm/s and are dominated by deposition of ammonium sulphate.

scholarly journals Characterization of the sources and processes of organic and inorganic aerosols in New York City with a high-resolution time-of-flight aerosol mass spectrometer

2010 ◽  
Vol 10 (10) ◽  
pp. 22669-22723 ◽  
Author(s):  
Y.-L. Sun ◽  
Q. Zhang ◽  
J. J. Schwab ◽  
K. L. Demerjian ◽  
W.-N. Chen ◽  
...  
Keyword(s):  
New York ◽  
New York City ◽  
High Resolution ◽  
Mass Spectrometer ◽  
York City ◽  
Time Of Flight ◽  
Resolution Time ◽  
Aerosol Mass Spectrometer ◽  
Spectral Pattern ◽  
Aerosol Mass

Abstract. Submicron aerosol particles (PM1) were measured in-situ using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) during the summer 2009 Field Intensive Study at Queens College in New York City. Organic aerosol (OA) and sulfate are the two dominant species, accounting for 54% and 24%, respectively, of total PM1 mass on average. The average mass size distribution of OA presents a small mode peaking at ~150 nm (Dva) in addition to an accumulation mode (~550 nm) that is internally mixed with sulfate, nitrate, and ammonium. The diurnal cycles of sulfate and OA both show pronounced peaks between 01:00–02:00 p.m. EST due to photochemical production. The average (±1σ) oxygen-to-carbon (O/C), hydrogen-to-carbon (H/C), and nitrogen-to-carbon (N/C) ratios of OA in NYC are 0.36 (±0.09), 1.49 (±0.08), and 0.012(±0.005), respectively, corresponding to an average organic mass-to-carbon (OM/OC) ratio of 1.62(±0.11). Positive matrix factorization (PMF) of the high resolution mass spectra identified five OA components: a hydrocarbon-like OA (HOA), two types of oxygenated OA (OOA) including a low-volatility OOA (LV-OOA) and a semi-volatile OOA (SV-OOA), a cooking-emission related OA (COA), and a unique nitrogen-enriched OA (NOA). HOA appears to represent primary OA (POA) from urban traffic emissions. It comprises primarily of reduced species (H/C=1.83; O/C=0.06) and shows a mass spectral pattern very similar to those of POA from fossil fuel combustion, and correlates tightly with traffic emission tracers including elemental carbon and NOx. LV-OOA, which is highly oxidized (O/C=0.63) and correlates well with sulfate, appears to be representative for regional, aged secondary OA (SOA). SV-OOA, which is less oxidized (O/C=0.38) and correlates well with non-refractory chloride, likely represents less photo-chemically aged, semi-volatile SOA. COA shows a similar spectral pattern to the reference spectra of POA from cooking emissions and a distinct diurnal pattern peaking around local lunch and dinner times. In addition, NOA is characterized with prominent CxH2x+2N+ peaks likely from amine compounds. Our results indicate that cooking-related activities are a major source of POA in NYC, releasing comparable amounts of POA as traffic emissions. POA=HOA+COA) on average accounts for ~30% of the total OA mass during this study while SOA dominates the OA composition with SV-OOA and LV-OOA on average accounting for 34% and 30%, respectively, of the total OA mass. The chemical evolution of SOA in NYC involves a~continuous oxidation from SV-OOA to LV-OOA, which is further supported by a gradual increase of O/C ratio and a simultaneous decrease of H/C ratio in total OOA. Detailed analysis of NOA (5.8% of OA) presents evidence that nitrogen-containing organic species such as amines might have played an important role in the atmospheric processing of OA in NYC, likely involving acid-base chemistry. Analysis of air mass trajectories and satellite imagery of aerosol optical depth (AOD) indicates that the high potential source regions of secondary sulfate and aged OA are mainly located in regions to the west and southwest of the city.

Aerosol Chemical Composition in Cloud Events by High Resolution Time-of-Flight Aerosol Mass Spectrometry

2013 ◽  
Vol 47 (6) ◽  
pp. 2645-2653 ◽  
Author(s):  
Liqing Hao ◽  
Sami Romakkaniemi ◽  
Aki Kortelainen ◽  
Antti Jaatinen ◽  
Harri Portin ◽  
...  
Keyword(s):  
Mass Spectrometry ◽  
Chemical Composition ◽  
High Resolution ◽  
Time Of Flight ◽  
Resolution Time ◽  
Aerosol Mass ◽  
Aerosol Mass Spectrometry ◽  
Aerosol Chemical Composition

Field-Deployable, High-Resolution, Time-of-Flight Aerosol Mass Spectrometer

2006 ◽  
Vol 78 (24) ◽  
pp. 8281-8289 ◽  
Author(s):  
Peter F. DeCarlo ◽  
Joel R. Kimmel ◽  
Achim Trimborn ◽  
Megan J. Northway ◽  
John T. Jayne ◽  
...  
Keyword(s):  
High Resolution ◽  
Mass Spectrometer ◽  
Time Of Flight ◽  
Resolution Time ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass

O/C and OM/OC Ratios of Primary, Secondary, and Ambient Organic Aerosols with High-Resolution Time-of-Flight Aerosol Mass Spectrometry

2008 ◽  
Vol 42 (12) ◽  
pp. 4478-4485 ◽  
Author(s):  
Allison C. Aiken ◽  
Peter F. DeCarlo ◽  
Jesse H. Kroll ◽  
Douglas R. Worsnop ◽  
J. Alex Huffman ◽  
...  
Keyword(s):  
Mass Spectrometry ◽  
High Resolution ◽  
Time Of Flight ◽  
Organic Aerosols ◽  
Resolution Time ◽  
Aerosol Mass ◽  
Aerosol Mass Spectrometry

scholarly journals Evaluating the degree of oxygenation of organic aerosol during foggy and hazy days in Hong Kong using high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS)

2013 ◽  
Vol 13 (2) ◽  
pp. 3533-3573 ◽  
Author(s):  
Y. J. Li ◽  
B. Y. L. Lee ◽  
J. Z. Yu ◽  
N. L. Ng ◽  
C. K. Chan
Keyword(s):  
Mass Spectrometry ◽  
Hong Kong ◽  
High Resolution ◽  
Time Of Flight ◽  
Organic Aerosol ◽  
Present Observation ◽  
Particle Phase ◽  
Resolution Time ◽  
Aerosol Mass ◽  
Aerosol Mass Spectrometry

Abstract. The chemical characteristics of organic aerosol (OA) are still poorly constrained. Here we present observation results of the degree of oxygenation of OA based on high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) measurements made at a coastal site in Hong Kong from late April to the end of May in 2011. Two foggy periods and one hazy period were chosen for detailed analysis to compare the changes in the degree of oxygenation of OA due to different processes. The Extended Aerosol Inorganic Model (E-AIM) predicted a fine particle liquid water content (LWCfp) up to 85 μg m−3 during the foggy days. Particle concentration as measured by HR-ToF-AMS was up to 60 μg m−3 during the hazy days and up to 30 μg m−3 during the foggy days. The degree of oxygenation of OA, as indicated by several parameters including the fraction of m/z 44 in organic mass spectra (f44), the elemental ratio of oxygen to carbon (O : C), and the carbon oxidation state (OSc), was evaluated against the odd oxygen (Ox) concentration, LWCfp, ionic strength (IS), and in-situ pH (pHis). Results suggest that the high concentration of OA (on average 11 μg m−3) and the high degree of oxygenation (f44 = 0.15, O : C = 0.51, and OSc = −0.31) during the hazy period were mainly due to gas-phase oxidation. During the foggy periods with low photochemical activities, the degree of oxygenation of OA was almost as high as that on the hazy days and significantly higher than that during non-foggy/non-hazy days. However, the OA evolved quite differently in the two foggy periods. The first foggy period in late April saw a larger LWCfp and a lower Ox concentration and the OA was made up of ~ 20% semi-volatile oxygenated organic aerosol (SVOOA) as resolved by positive matrix factorization (PMF). In the second foggy period in mid-May, higher Ox concentration and lower LWCfp were observed, and the OA was found to contain >50% low-volatility oxygenated organic aerosols (LVOOA). An examination of the particle-phase constituents suggests that partitioning may have been the dominating process through which oxygenated species were incorporated into the particle phase during the first foggy period, while oxidation in the aqueous phase may have been the dominating process during the second foggy period. Both physical and chemical processes were found to be important for oxygenated OA formation.

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