Abstract

Abstract. An Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed at the peak of Whistler Mountain (2182 m above sea level), British Columbia, from 19 April to 16 May 2006, as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign. The mass concentrations and size distributions of non-refractory submicron particle (NR-PM1) species (i.e., sulfate, nitrate, ammonium, chloride, and organics) were measured in situ at 10-min time resolution. The HR-ToF-AMS results agreed well with collocated measurements. The average concentration of non-refractory submicron particulate matter (NR-PM1; 1.9 μg m−3) is similar to those observed at other remote, high elevation sites in North America. Episodes of enhanced aerosol loadings were observed, due to influences of regional and trans-Pacific transport of air pollution. Organics and sulfate were the dominant species, on average accounting for 55% and 30%, respectively, of the NR-PM1 mass. The average size distributions of sulfate and ammonium both showed an accumulation mode peaking at ~500 nm in vacuum aerodynamic diameter (Dva) while those of organic aerosol (OA) and nitrate peaked at ~300 nm. The size differences suggested that sulfate and OA were mostly present in external mixtures from different source origins. We also quantitatively determined the elemental composition of OA using the high resolution mass spectra. Overall, OA at Whistler Peak was highly oxygenated, with an average organic-mass-to-organic-carbon ratio (OM/OC) of 2.28±0.23 and an atomic ratio of oxygen-to-carbon (O/C) of 0.83±0.17. The nominal formula for OA was C1H1.66N0.03O0.83 for the entire study. Two significant trans-Pacific dust events originated from Asia were observed at Whistler Peak during this study. While both events were characterized with significant enhancements of coarse mode particles and mineral contents, the composition and characteristics of NR-PM1 were significantly different between them. One trans-Pacific event occurred on 15 May 2006, during which ammonium sulfate contributed >90% of the total NR-PM1 mass. This event was followed by a high OA episode likely associated with regional emissions. In total, three enhanced regional OA events, each of which lasted 2–3 days, were observed during this study. In contrast to the two dust events, the regional OA events were generally characterized with higher OA/sulfate ratio, less oxidized OA, and lower OM/OC ratio.

Highlights

  • Aerosol particles are an important component of the Earth’s atmosphere, playing significant roles in atmospheric chemistry, climate change and public health

  • MOUDI measurements at Whistler Peak indicate that the mass fractions of sulfate and ammonium were significantly enhanced in particles >1 μm during periods influenced by trans-Pacific dust events (Leaitch et al, 2008)

  • These observations, as well as the temporal variation patterns of aerosol species, suggest that Whistler Peak – a representative upper boundary layer/lower free troposphere site for Pacific northwest – is subject to the influences of air masses transported from different source regions, some of which are enriched with organic aerosol (OA) and to a lesser extent nitrate while others are dominated with aerosols mainly composed of ammonium sulfates

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Summary

Introduction

Aerosol particles are an important component of the Earth’s atmosphere, playing significant roles in atmospheric chemistry, climate change and public health. Asian emissions can be transported across the Pacific Ocean through midlatitude cyclonic system (Yienger, 2000), affecting air quality and regional climate in North America (Jaffe et al, 1999; Bailey and Barrie, 2000; Jacob et al, 2003; Liang et al, 2004). A key component of the Canadian INTEX-B measurement activities was the deployment of a High Resolution Timeof-Flight Aerosol Mass Spectrometer (HR-ToF-AMS; Aerodyne Research Inc.) at the peak of Whistler Mountain from 19 April–16 May 2006. Recent model studies (Heald et al, 2006) and analysis of aircraft observations (van Donkelaar et al, 2008) indicate that trans-Pacific transport of Asian anthropogenic aerosol is most significant in the layer between 700– 900 hPa, in which Whistler Peak is located. A detailed case study is performed on a significant trans-Pacific dust event observed on 15 May 2006 and a regional OA event that immediately followed

Sampling site and time
Description of the HR-ToF-AMS
HR-ToF-AMS operation and calibrations
Collocated and nearby measurements
Standard HR-ToF-AMS data analysis
Air mass trajectory analysis
Inter-comparisons of collocated measurements
Temporal variations of NR-PM1 species
Average composition and size distributions of submicron aerosol species
Aerosol acidity
Organic aerosol characteristics and elemental composition
50 Pacific Ocean
Characteristics of aerosols associated with different events
A case study of sulfate to organic transition at Whistler
Conclusions
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