Semi-volatile and highly oxygenated gaseous and particulate organic compounds observed above a boreal forest canopy

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Lee , B H , Lopez-Hilfiker , F D , D'Ambro , E L , Zhou , P , Boy , M , Petäjä , T , Hao , L , Virtanen , A & Thornton , J A 2018 , ' Semi-volatile and highly oxygenated gaseous and particulate organic compounds observed above a boreal forest canopy ' , Atmospheric Chemistry and Physics , vol. 18 , no. 15 , pp. 11547-11562 . https://doi.org/10.5194/acp-18-11547-2018

Title: Semi-volatile and highly oxygenated gaseous and particulate organic compounds observed above a boreal forest canopy
Author: Lee, Ben H.; Lopez-Hilfiker, Felipe D.; D'Ambro, Emma L.; Zhou, Putian; Boy, Michael; Petäjä, Tuukka; Hao, Liqing; Virtanen, Annele; Thornton, Joel A.
Contributor: University of Helsinki, INAR Physics
University of Helsinki, Institute for Atmospheric and Earth System Research (INAR)
University of Helsinki, Institute for Atmospheric and Earth System Research (INAR)
Date: 2018-08-15
Language: eng
Number of pages: 16
Belongs to series: Atmospheric Chemistry and Physics
ISSN: 1680-7316
URI: http://hdl.handle.net/10138/276981
Abstract: We present hourly online observations of molecular compositions (CxHyOzN0-1) and abundances of oxygenated organic species in gas and submicron particle phases from April to June of 2014 as part of the Biogenic Aerosols-Effects on Cloud and Climate (BAECC) campaign. Measurements were made using the Filter Inlet for Gases and AEROsols coupled to a high-resolution time-of-flight iodide-adduct ionization mass spectrometer (FIGAERO-CIMS) located atop a 35m tall tower, about 10m above a boreal forest canopy at the SMEAR II research station in Hyytiala, Finland. Semi-volatile and highly oxygenated multifunctional (HOM) organic species possessing from 1 up to 20 carbon atoms, and with as few as 2 and as many as 16 oxygen atoms, were routinely observed. Utilizing non-negative matrix factorization, we determined that > 90 and > 99% of the organic mass in the gas and particle phases, respectively, exhibited one of three distinct diel trends: one in which abundances were enhanced at daytime, another in the early morning hours, and thirdly during nighttime. Particulate organic nitrates contributed similar to 35% to the total organic aerosol mass loading at night during BAECC, much higher than observed by the same instrument package at a mixed-deciduous forest site in the southeastern US that experienced higher nighttime concentrations of nitrogen oxides. Unique HOM monomers (defined here as those with 10 carbon and 7 or more oxygen atoms) and dimers (at least 16 carbon atoms), with and without a nitrogen atom, were found in most of the three subgroups of both phases. We show the potential to connect these groupings of compounds based on their distinct behavior in time to the expected chemical conditions (biogenic VOC precursor, oxidant type, etc.) responsible for their production. A suite of nitrated dimer-like compounds was detected in both the gas and particle phases, suggesting a potential role for the formation of low-volatility organics from NO3-radical-driven, as well as daytime NO-influenced, monoterpene chemistry.
Subject: POSITIVE MATRIX FACTORIZATION
AEROSOL FORMATION
MASS-SPECTROMETER
HIGH-RESOLUTION
MOLECULAR COMPOSITION
BIOGENIC EMISSIONS
CLIMATE-CHANGE
AMBIENT IONS
OXIDATION
ISOPRENE
1172 Environmental sciences
114 Physical sciences
116 Chemical sciences
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