Vertical characterization of highly oxygenated molecules (HOMs) below and above a boreal forest canopy

Zha, Qiaozhi; Yan, Chao; Junninen, Heikki; Riva, Matthieu; Sarnela, Nina; Aalto, Juho; Quéléver, Lauriane; Schallhart, Simon; Dada, Lubna; Heikkinen, Liine; Peräkylä, Otso; Zou, Jun; Rose, Clémence; Wang, Yonghong; Mammarella, Ivan; Katul, Gabriel; Vesala, Timo; Worsnop, Douglas R.; Kulmala, Markku; Petäjä, Tuukka; Bianchi, Federico; Ehn, Mikael

doi:10.5194/acp-18-17437-2018

Title: Vertical characterization of highly oxygenated molecules (HOMs) below and above a boreal forest canopy

Journal Article · 10 December 2018 · Atmospheric Chemistry and Physics (Online)

DOI: https://doi.org/10.5194/acp-18-17437-2018 · OSTI ID:1611630

^[1];

^[2]; Junninen, Heikki ^[2];

^[2]; Sarnela, Nina ^[2]; Aalto, Juho ^[2]; Quéléver, Lauriane ^[2]; Schallhart, Simon ^[2];

^[2];

^[2]; Zou, Jun ^[3]; Rose, Clémence ^[2];

^[2]; Mammarella, Ivan ^[2];

^[4]; Vesala, Timo ^[2]; Worsnop, Douglas R. ^[5];

^[2];

^[2] more »

Univ. of Helsinki (Finland). Inst. for Atmospheric and Earth System Research/Physics; DOE/OSTI
Univ. of Helsinki (Finland). Inst. for Atmospheric and Earth System Research/Physics
Nanjing Univ., Nanjing (China). CMA-NJU Joint Lab. for Climate Prediction Studies, Inst. for Climate and Global Change Research
Duke Univ., Durham, NC (United States)
Univ. of Helsinki (Finland). Inst. for Atmospheric and Earth System Research/Physics; Aerodyne Research, Inc., Billerica, MA (United States)

While the role of highly oxygenated molecules (HOMs) in new particle formation (NPF) and secondary organic aerosol (SOA) formation is not in dispute, the interplay between HOM chemistry and atmospheric conditions continues to draw significant research attention. During the Influence of Biosphere-Atmosphere Interactions on the Reactive Nitrogen budget (IBAIRN) campaign in September 2016, profile measurements of neutral HOMs below and above the forest canopy were performed for the first time at the boreal forest SMEAR II station. The HOM concentrations and composition distributions below and above the canopy were similar during daytime, supporting a well-mixed boundary layer approximation. However, much lower nighttime HOM concentrations were frequently observed at ground level, which was likely due to the formation of a shallow decoupled layer below the canopy. Near the ground HOMs were influenced by the changes in the precursors and oxidants and enhancement of the loss on surfaces in this layer, while the HOMs above the canopy top were not significantly affected. Our findings clearly illustrate that near-ground HOM measurements conducted under stably stratified conditions at this site might only be representative of a small fraction of the entire nocturnal boundary layer. This could, in turn, influence the growth of newly formed particles and SOA formation below the canopy where the large majority of measurements are typically conducted.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Duke Univ., Durham, NC (United States)

Sponsoring Organization:: Academy of Finland Center of Excellence in Atmospheric Science; European Research Council (ERC); National Science Foundation (NSF); USDOE Office of Science (SC); University of Helsinki; Vilho, Yrjö ja Kalle Väisälä Foundation

Grant/Contract Number:: SC0011461

OSTI ID:: 1611630

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 23 Vol. 18; ISSN 1680-7324

Publisher:: European Geosciences UnionCopyright Statement

Country of Publication:: United States

Language:: English

References (65)

The Influence of Hilly Terrain on Canopy-Atmosphere Carbon Dioxide Exchange Katul, G. G.; Finnigan, J. J.; Poggi, D. Boundary-Layer Meteorology, Vol. 118, Issue 1 https://doi.org/10.1007/s10546-005-6436-2	journal	January 2006
A large source of low-volatility secondary organic aerosol Ehn, Mikael; Thornton, Joel A.; Kleist, Einhard Nature, Vol. 506, Issue 7489 https://doi.org/10.1038/nature13032	journal	February 2014
The role of low-volatility organic compounds in initial particle growth in the atmosphere Tröstl, Jasmin; Chuang, Wayne K.; Gordon, Hamish Nature, Vol. 533, Issue 7604 https://doi.org/10.1038/nature18271	journal	May 2016
Determining the contribution of vertical advection to the net ecosystem exchange at Hyytiälä forest, Finland Mammarella, I.; Kolari, P.; Rinne, J. Tellus B: Chemical and Physical Meteorology, Vol. 59, Issue 5 https://doi.org/10.1111/j.1600-0889.2007.00306.x	journal	January 2007
New particle formation in the free troposphere: A question of chemistry and timing Bianchi, F.; Trostl, J.; Junninen, H. Science, Vol. 352, Issue 6289 https://doi.org/10.1126/science.aad5456	journal	May 2016
On the formation, growth and composition of nucleation mode particles Kulmala, M.; Maso, M. Dal; Mäkelä, J. M. Tellus B: Chemical and Physical Meteorology, Vol. 53, Issue 4 https://doi.org/10.3402/tellusb.v53i4.16622	journal	January 2001
Physical characterization of aerosol particles during nucleation events Aalto, Pasi; Hämeri, Kaarle; Becker, Edo Tellus B: Chemical and Physical Meteorology, Vol. 53, Issue 4 https://doi.org/10.3402/tellusb.v53i4.17127	journal	January 2001
Composition and temporal behavior of ambient ions in the boreal forest Ehn, M.; Junninen, H.; Petäjä, T. Atmospheric Chemistry and Physics, Vol. 10, Issue 17 https://doi.org/10.5194/acp-10-8513-2010	journal	January 2010
Ozone deposition into a boreal forest over a decade of observations: evaluating deposition partitioning and driving variables Rannik, Ü.; Altimir, N.; Mammarella, I. Atmospheric Chemistry and Physics, Vol. 12, Issue 24 https://doi.org/10.5194/acp-12-12165-2012	journal	January 2012
Formation of highly oxidized multifunctional compounds: autoxidation of peroxy radicals formed in the ozonolysis of alkenes – deduced from structure–product relationships Mentel, T. F.; Springer, M.; Ehn, M. Atmospheric Chemistry and Physics, Vol. 15, Issue 12 https://doi.org/10.5194/acp-15-6745-2015	journal	January 2015
Long-term analysis of clear-sky new particle formation events and nonevents in Hyytiälä Dada, Lubna; Paasonen, Pauli; Nieminen, Tuomo Atmospheric Chemistry and Physics, Vol. 17, Issue 10 https://doi.org/10.5194/acp-17-6227-2017	journal	January 2017
Observations of ozone depletion events in a Finnish boreal forest Chen, Xuemeng; Quéléver, Lauriane L. J.; Fung, Pak L. Atmospheric Chemistry and Physics, Vol. 18, Issue 1 https://doi.org/10.5194/acp-18-49-2018	journal	January 2018
Technical Note: Quantitative long-term measurements of VOC concentrations by PTR-MS – measurement, calibration, and volume mixing ratio calculation methods Taipale, R.; Ruuskanen, T. M.; Rinne, J. Atmospheric Chemistry and Physics, Vol. 8, Issue 22 https://doi.org/10.5194/acp-8-6681-2008	journal	January 2008
Rapid Autoxidation Forms Highly Oxidized RO ₂ Radicals in the Atmosphere Jokinen, Tuija; Sipilä, Mikko; Richters, Stefanie Angewandte Chemie International Edition, Vol. 53, Issue 52 https://doi.org/10.1002/anie.201408566	journal	October 2014
Accretion Product Formation from Self- and Cross-Reactions of RO ₂ Radicals in the Atmosphere Berndt, Torsten; Scholz, Wiebke; Mentler, Bernhard Angewandte Chemie International Edition, Vol. 57, Issue 14 https://doi.org/10.1002/anie.201710989	journal	March 2018
Highly Oxygenated Molecules from Atmospheric Autoxidation of Hydrocarbons: A Prominent Challenge for Chemical Kinetics Studies: HIGHLY OXYGENATED MOLECULES FROM ATMOSPHERIC AUTOXIDATION OF HYDROCARBONS Ehn, Mikael; Berndt, Torsten; Wildt, Jürgen International Journal of Chemical Kinetics, Vol. 49, Issue 11 https://doi.org/10.1002/kin.21130	journal	September 2017
The Influence of Hilly Terrain on Canopy-Atmosphere Carbon Dioxide Exchange Katul, G. G.; Finnigan, J. J.; Poggi, D. Boundary-Layer Meteorology, Vol. 118, Issue 1 https://doi.org/10.1007/s10546-005-6436-2	journal	January 2006
Nocturnal subcanopy flow regimes and missing carbon dioxide Vickers, Dean; Irvine, James; Martin, Jonathan G. Agricultural and Forest Meteorology, Vol. 152 https://doi.org/10.1016/j.agrformet.2011.09.004	journal	January 2012
Partitioning ozone fluxes between canopy and forest floor by measurements and a multi-layer model Launiainen, S.; Katul, G. G.; Grönholm, T. Agricultural and Forest Meteorology, Vol. 173 https://doi.org/10.1016/j.agrformet.2012.12.009	journal	May 2013
Evolution of the nocturnal decoupled layer in a pine forest canopy Alekseychik, P.; Mammarella, I.; Launiainen, S. Agricultural and Forest Meteorology, Vol. 174-175 https://doi.org/10.1016/j.agrformet.2013.01.011	journal	June 2013
Modeling the Charging of Highly Oxidized Cyclohexene Ozonolysis Products Using Nitrate-Based Chemical Ionization Hyttinen, Noora; Kupiainen-Määttä, Oona; Rissanen, Matti P. The Journal of Physical Chemistry A, Vol. 119, Issue 24 https://doi.org/10.1021/acs.jpca.5b01818	journal	May 2015
The Formation of Highly Oxidized Multifunctional Products in the Ozonolysis of Cyclohexene Rissanen, Matti P.; Kurtén, Theo; Sipilä, Mikko Journal of the American Chemical Society, Vol. 136, Issue 44 https://doi.org/10.1021/ja507146s	journal	October 2014
Rate Constants for the Reactions of XO ₃ ^- (H ₂ O) _n (X = C, HC, and N) and NO ₃ ^- (HNO ₃ ) _n with H ₂ SO ₄ : Implications for Atmospheric Detection of H ₂ SO ₄ Viggiano, A. A.; Seeley, John V.; Mundis, Paul L. The Journal of Physical Chemistry A, Vol. 101, Issue 44 https://doi.org/10.1021/jp971768h	journal	October 1997
Autoxidation of Organic Compounds in the Atmosphere Crounse, John D.; Nielsen, Lasse B.; Jørgensen, Solvejg The Journal of Physical Chemistry Letters, Vol. 4, Issue 20 https://doi.org/10.1021/jz4019207	journal	September 2013
Nocturnal Boundary-Layer Regimes Mahrt, L. Boundary-Layer Meteorology, Vol. 88, Issue 2 https://doi.org/10.1023/A:1001171313493	journal	August 1998
Shallow Drainage Flows Mahrt, L.; Vickers, Dean; Nakamura, Reina Boundary-Layer Meteorology, Vol. 101, Issue 2 https://doi.org/10.1023/A:1019273314378	journal	November 2001
On the formation, growth and composition of nucleation mode particles Kulmala, M.; Maso, M. Dal; MÄKelÄ, J. M. Tellus B, Vol. 53, Issue 4 https://doi.org/10.1034/j.1600-0889.2001.d01-33.x	journal	September 2001
A large source of low-volatility secondary organic aerosol Ehn, Mikael; Thornton, Joel A.; Kleist, Einhard Nature, Vol. 506, Issue 7489 https://doi.org/10.1038/nature13032	journal	February 2014
Ion-induced nucleation of pure biogenic particles Kirkby, Jasper; Duplissy, Jonathan; Sengupta, Kamalika Nature, Vol. 533, Issue 7604 https://doi.org/10.1038/nature17953	journal	May 2016
The role of low-volatility organic compounds in initial particle growth in the atmosphere Tröstl, Jasmin; Chuang, Wayne K.; Gordon, Hamish Nature, Vol. 533, Issue 7604 https://doi.org/10.1038/nature18271	journal	May 2016
Laboratory studies of organic peroxy radical chemistry: an overview with emphasis on recent issues of atmospheric significance Orlando, John J.; Tyndall, Geoffrey S. Chemical Society Reviews, Vol. 41, Issue 19 https://doi.org/10.1039/c2cs35166h	journal	January 2012
Two phenomenological constants explain similarity laws in stably stratified turbulence Katul, Gabriel G.; Porporato, Amilcare; Shah, Stimit Physical Review E, Vol. 89, Issue 2 https://doi.org/10.1103/PhysRevE.89.023007	journal	February 2014
Determining the contribution of vertical advection to the net ecosystem exchange at Hyytiälä forest, Finland Mammarella, I.; Kolari, P.; Rinne, J. Tellus B: Chemical and Physical Meteorology, Vol. 59, Issue 5 https://doi.org/10.1111/j.1600-0889.2007.00306.x	journal	January 2007
H ₂ O and CO ₂ fluxes at the floor of a boreal pine forest Kulmala, Liisa; Launiainen, Samuli; Pumpanen, Jukka Tellus B: Chemical and Physical Meteorology, Vol. 60, Issue 2 https://doi.org/10.1111/j.1600-0889.2007.00327.x	journal	January 2008
Direct Observations of Atmospheric Aerosol Nucleation Kulmala, M.; Kontkanen, J.; Junninen, H. Science, Vol. 339, Issue 6122 https://doi.org/10.1126/science.1227385	journal	February 2013
New particle formation in the free troposphere: A question of chemistry and timing Bianchi, F.; Trostl, J.; Junninen, H. Science, Vol. 352, Issue 6289 https://doi.org/10.1126/science.aad5456	journal	May 2016
Turbulence in and above Plant Canopies Raupach, M. R.; Thom, A. S. Annual Review of Fluid Mechanics, Vol. 13, Issue 1 https://doi.org/10.1146/annurev.fl.13.010181.000525	journal	January 1981
On the formation, growth and composition of nucleation mode particles Kulmala, M.; Maso, M. Dal; Mäkelä, J. M. Tellus B: Chemical and Physical Meteorology, Vol. 53, Issue 4 https://doi.org/10.3402/tellusb.v53i4.16622	journal	January 2001
Physical characterization of aerosol particles during nucleation events Aalto, Pasi; Hämeri, Kaarle; Becker, Edo Tellus B: Chemical and Physical Meteorology, Vol. 53, Issue 4 https://doi.org/10.3402/tellusb.v53i4.17127	journal	January 2001
Determining the contribution of vertical advection to the net ecosystem exchange at Hyytiälä forest, Finland Mammarella, I.; Kolari, P.; Rinne, J. Tellus B, Vol. 59, Issue 5 https://doi.org/10.3402/tellusb.v59i5.17068	journal	November 2007
H ₂ O and CO ₂ fluxes at the floor of a boreal pine forest Kulmala, Liisa; Launiainen, Samuli; Pumpanen, Jukka Tellus B, Vol. 60, Issue 2 https://doi.org/10.3402/tellusb.v60i2.16912	journal	April 2008
Ion-induced nucleation of pure biogenic particles Kirkby, Jasper; Frege, Carla; Tröstl, Jasmin ETH Zurich https://doi.org/10.3929/ethz-b-000117259	text	January 2016
Formation of highly oxygenated organic molecules from aromatic compounds Molteni, Ugo; Bianchi, Frederico; Klein, Felix ETH Zurich https://doi.org/10.3929/ethz-b-000342128	text	January 2018
Composition and temporal behavior of ambient ions in the boreal forest Ehn, M.; Junninen, H.; Petäjä, T. Atmospheric Chemistry and Physics, Vol. 10, Issue 17 https://doi.org/10.5194/acp-10-8513-2010	journal	January 2010
Ozone deposition into a boreal forest over a decade of observations: evaluating deposition partitioning and driving variables Rannik, Ü.; Altimir, N.; Mammarella, I. Atmospheric Chemistry and Physics, Vol. 12, Issue 24 https://doi.org/10.5194/acp-12-12165-2012	journal	January 2012
Atmospheric sulphuric acid and neutral cluster measurements using CI-APi-TOF Jokinen, T.; Sipilä, M.; Junninen, H. Atmospheric Chemistry and Physics, Vol. 12, Issue 9 https://doi.org/10.5194/acp-12-4117-2012	journal	January 2012
Gas phase formation of extremely oxidized pinene reaction products in chamber and ambient air Ehn, M.; Kleist, E.; Junninen, H. Atmospheric Chemistry and Physics, Vol. 12, Issue 11 https://doi.org/10.5194/acp-12-5113-2012	journal	January 2012
Characterization of a boreal convective boundary layer and its impact on atmospheric chemistry during HUMPPA-COPEC-2010 Ouwersloot, H. G.; Vilà-Guerau de Arellano, J.; Nölscher, A. C. Atmospheric Chemistry and Physics, Vol. 12, Issue 19 https://doi.org/10.5194/acp-12-9335-2012	journal	January 2012
Dependence of particle nucleation and growth on high-molecular-weight gas-phase products during ozonolysis of α-pinene Zhao, J.; Ortega, J.; Chen, M. Atmospheric Chemistry and Physics, Vol. 13, Issue 15 https://doi.org/10.5194/acp-13-7631-2013	journal	January 2013
Formation of highly oxidized multifunctional compounds: autoxidation of peroxy radicals formed in the ozonolysis of alkenes – deduced from structure–product relationships Mentel, T. F.; Springer, M.; Ehn, M. Atmospheric Chemistry and Physics, Vol. 15, Issue 12 https://doi.org/10.5194/acp-15-6745-2015	journal	January 2015
Source characterization of highly oxidized multifunctional compounds in a boreal forest environment using positive matrix factorization Yan, Chao; Nie, Wei; Äijälä, Mikko Atmospheric Chemistry and Physics, Vol. 16, Issue 19 https://doi.org/10.5194/acp-16-12715-2016	journal	January 2016
Observation of new particle formation and measurement of sulfuric acid, ammonia, amines and highly oxidized organic molecules at a rural site in central Germany Kürten, Andreas; Bergen, Anton; Heinritzi, Martin Atmospheric Chemistry and Physics, Vol. 16, Issue 19 https://doi.org/10.5194/acp-16-12793-2016	journal	January 2016
The role of highly oxygenated molecules (HOMs) in determining the composition of ambient ions in the boreal forest Bianchi, Federico; Garmash, Olga; He, Xucheng Atmospheric Chemistry and Physics, Vol. 17, Issue 22 https://doi.org/10.5194/acp-17-13819-2017	journal	January 2017
Long-term analysis of clear-sky new particle formation events and nonevents in Hyytiälä Dada, Lubna; Paasonen, Pauli; Nieminen, Tuomo Atmospheric Chemistry and Physics, Vol. 17, Issue 10 https://doi.org/10.5194/acp-17-6227-2017	journal	January 2017
Formation of highly oxygenated organic molecules from aromatic compounds Molteni, Ugo; Bianchi, Federico; Klein, Felix Atmospheric Chemistry and Physics, Vol. 18, Issue 3 https://doi.org/10.5194/acp-18-1909-2018	journal	January 2018
Observations of ozone depletion events in a Finnish boreal forest Chen, Xuemeng; Quéléver, Lauriane L. J.; Fung, Pak L. Atmospheric Chemistry and Physics, Vol. 18, Issue 1 https://doi.org/10.5194/acp-18-49-2018	journal	January 2018
Contribution of mixing in the ABL to new particle formation based on observations Lauros, J.; Nilsson, E. D.; Dal Maso, M. Atmospheric Chemistry and Physics, Vol. 7, Issue 18 https://doi.org/10.5194/acp-7-4781-2007	journal	January 2007
Technical Note: Quantitative long-term measurements of VOC concentrations by PTR-MS – measurement, calibration, and volume mixing ratio calculation methods Taipale, R.; Ruuskanen, T. M.; Rinne, J. Atmospheric Chemistry and Physics, Vol. 8, Issue 22 https://doi.org/10.5194/acp-8-6681-2008	journal	January 2008
Vertical advection and nocturnal deposition of ozone over a boreal pine forest Rannik, Ü.; Mammarella, I.; Keronen, P. Atmospheric Chemistry and Physics, Vol. 9, Issue 6 https://doi.org/10.5194/acp-9-2089-2009	journal	January 2009
VOC measurements within a boreal forest during spring 2005: on the occurrence of elevated monoterpene concentrations during night time intense particle concentration events Eerdekens, G.; Yassaa, N.; Sinha, V. Atmospheric Chemistry and Physics, Vol. 9, Issue 21 https://doi.org/10.5194/acp-9-8331-2009	journal	January 2009
A high-resolution mass spectrometer to measure atmospheric ion composition Junninen, H.; Ehn, M.; Petäjä, T. Atmospheric Measurement Techniques, Vol. 3, Issue 4 https://doi.org/10.5194/amt-3-1039-2010	journal	January 2010
Characterization of the mass-dependent transmission efficiency of a CIMS Heinritzi, Martin; Simon, Mario; Steiner, Gerhard Atmospheric Measurement Techniques, Vol. 9, Issue 4 https://doi.org/10.5194/amt-9-1449-2016	journal	January 2016
Chemodiversity of a Scots pine stand and implications for terpene air concentrations Bäck, J.; Aalto, J.; Henriksson, M. Biogeosciences, Vol. 9, Issue 2 https://doi.org/10.5194/bg-9-689-2012	journal	January 2012
Data For "Vertical Characterization Of Highly Oxygenated Molecules (Homs) Below And Above A Boreal Forest Canopy" Qiaozhi, Zha Zenodo https://doi.org/10.5281/zenodo.1489078	dataset	January 2018
Data For "Vertical Characterization Of Highly Oxygenated Molecules (Homs) Below And Above A Boreal Forest Canopy" Qiaozhi, Zha Zenodo https://doi.org/10.5281/zenodo.1489079	dataset	January 2018

Cited By (4)

Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol Bianchi, Federico; Kurtén, Theo; Riva, Matthieu Chemical Reviews, Vol. 119, Issue 6 https://doi.org/10.1021/acs.chemrev.8b00395	journal	January 2019
Alkyl nitrates in the boreal forest: formation via the NO₃-, OH- and O₃-induced oxidation of biogenic volatile organic compounds and ambient lifetimes Liebmann, Jonathan; Sobanski, Nicolas; Schuladen, Jan Atmospheric Chemistry and Physics, Vol. 19, Issue 15 https://doi.org/10.5194/acp-19-10391-2019	journal	January 2019
Vertical profiles of sub-3 nm particles over the boreal forest Leino, Katri; Lampilahti, Janne; Poutanen, Pyry Atmospheric Chemistry and Physics, Vol. 19, Issue 6 https://doi.org/10.5194/acp-19-4127-2019	journal	January 2019
A novel approach for simple statistical analysis of high-resolution mass spectra Zhang, Yanjun; Peräkylä, Otso; Yan, Chao Atmospheric Measurement Techniques, Vol. 12, Issue 7 https://doi.org/10.5194/amt-12-3761-2019	journal	January 2019

Similar Records

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

Journal Article · 2018 · Atmospheric Chemistry and Physics (Online) · OSTI ID:1464654

Lee, Ben H.; Lopez-Hilfiker, Felipe D.; D'Ambro, Emma L.; +6 more

Nocturnal CO₂ exchange over a tall forest canopy associated with intermittent low-level jet activity

Journal Article · 2006 · Theoretical and Applied Climatology · OSTI ID:929545

Karipot, A.; Leclerc, M. Y.; Zhang, G.; +5 more

Nocturnal CO₂ exchange over a tall forest canopy associated with intermittent low-level jet activity

Journal Article · 2006 · Theoretical and Applied Climatology · OSTI ID:1009439

Karipot, A.; Leclerc, M. Y.; Zhang, G.; +5 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Environmental Sciences & Ecology
Meteorology & Atmospheric Sciences

Title: Vertical characterization of highly oxygenated molecules (HOMs) below and above a boreal forest canopy

Citation Formats

References (65)

Cited By (4)

Similar Records

Related Subjects