Abstract

Abstract. Aerosol particles form in the atmosphere via the clustering of certain atmospheric vapors. After growing into larger particles by the condensation of low-volatility gases, they can affect the Earth's climate by scattering light and acting as cloud condensation nuclei (CCN). Observations of low-volatility aerosol precursor gases have been reported around the world, but longer-term measurement series and any Arctic data sets showing seasonal variation are close to nonexistent. Here, we present ∼7 months of aerosol precursor gas measurements performed with a nitrate-based chemical ionization atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometer. We deployed our measurements ∼150 km north of the Arctic Circle at the SMEAR I (Station for Measuring Ecosystem–Atmosphere Relations) continental Finnish subarctic field station, located in the Värriö strict nature reserve. We report concentration measurements of the most common compounds related to new particle formation (NPF): sulfuric acid (SA), methane sulfonic acid (MSA), iodic acid (IA) and the total concentration of highly oxygenated organic molecules (HOMs). At this remote measurement site, SA originates from both anthropogenic and biological sources and has a clear diurnal cycle but no significant seasonal variation. MSA shows a more distinct seasonal cycle, with concentrations peaking in the summer. Of the measured compounds, IA concentrations are the most stable throughout the measurement period, except in April during which time the concentration of IA is significantly higher than during the rest of the year. Otherwise, IA has almost identical daily maximum concentrations in spring, summer and autumn, and on NPF event or non-event days. HOMs are abundant during the summer months and low in the autumn months. Due to their low autumn concentrations and high correlation with ambient air temperature, we suggest that most HOMs are products of biogenic emissions, most probably monoterpene oxidation products. NPF events at SMEAR I happen under relatively low-temperature (1–8 ∘C) conditions, with a fast temperature rise in the early morning hours as well as lower and decreasing relative humidity (RH, 55 % vs. 80 %) during NPF days compared with non-event days. NPF days have clearly higher global irradiance values (∼450 m−2 vs. ∼200 m−2) and about 10 ppbv higher ozone concentrations than non-event days. During NPF days, we have, on average, higher SA concentrations, peaking at noon; higher MSA concentrations in the afternoon; and slightly higher IA concentration than during non-event days. In summary, these are the first long-term measurements of aerosol-forming vapors from SMEAR I in the subarctic region, and the results of this work will help develop an understanding of atmospheric chemical processes and aerosol formation in the rapidly changing Arctic.

Highlights

  • The climate of the subarctic region is characterized by some of the most extreme temperature variations on Earth

  • We present the measurements of aerosol precursor molecules from the continental SMEAR I station, ∼ 150 km north of the Arctic Circle and ∼ 150 km from the Arctic Ocean

  • iodic acid (IA) data are missing from late July, as the peak could not be separated well enough from overlapping peaks in the spectra during this time

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Summary

Introduction

During the course of the 21st century, it is expected that the boreal forest will experience the largest temperature increases of all forest biomes (IPCC, 2013), making it the most vulnerable to climate change. On the other hand, during the polar night, air pollutants accumulate in the atmosphere due to a cold and stable atmospheric conditions, while turbulent mixing is inhibited, and the lack of removal processes lead to the formation of Arctic haze (Stohl, 2006). These features make the Arctic an interesting study region with respect to the photochemistry of reduced atmospheric compounds. A detailed understanding of the atmospheric processes leading to aerosol precursor formation and gas-to-particle conversion as well as their role in feedback mechanisms would help with assessing the future climate

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