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Title: Long-term real-time chemical characterization of submicron aerosols at Montsec (southern Pyrenees, 1570 m a.s.l.)

Abstract

Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols (particles with an aerodynamic diameter of less than 1 μm) from a continental background site (Montsec, MSC, 1570 m a.s.l.) in the western Mediterranean Basin (WMB) were conducted for 10 months (July 2011–April 2012). An aerosol chemical speciation monitor (ACSM) was co-located with other online and offline PM 1 measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here, for the first time, for this region. Seasonal trends in PM 1 components are attributed to variations in evolution of the planetary boundary layer (PBL) height, air mass origin, and meteorological conditions. In summer, the higher temperature and solar radiation increases convection, enhancing the growth of the PBL and the transport of anthropogenic pollutants towards high altitude sites. Furthermore, the regional recirculation of air masses over the WMB creates a continuous increase in the background concentrations of PM 1 components and causes the formation of reservoir layers at relatively high altitudes. The combination of all these atmospheric processes results in a high variability of PM 1 components, with poorly defined daily patterns, except for the organic aerosols (OA). OA was mostly composed (upmore » to 90%) of oxygenated organic aerosol (OOA), split in two types: semivolatile (SV-OOA) and low-volatility (LV-OOA), the rest being hydrocarbon-like OA (HOA). The marked diurnal cycles of OA components regardless of the air mass origin indicates that they are not only associated with anthropogenic and long-range-transported secondary OA (SOA) but also with recently produced biogenic SOA. Very different conditions drive the aerosol phenomenology in winter at MSC. The thermal inversions and the lower vertical development of the PBL leave MSC in the free troposphere most of the day, being affected by PBL air masses only after midday, when the mountain breezes transport emissions from the adjacent valleys and plains to the top of the mountain. This results in clear diurnal patterns of both organic and inorganic concentrations. OA was also mainly composed (71%) of OOA, with contributions from HOA (5%) and biomass burning OA (BBOA; 24%). Moreover, in winter sporadic long-range transport from mainland Europe is observed. The results obtained in the present study highlight the importance of SOA formation processes at a remote site such as MSC, especially in summer. Furthermore, additional research is needed to characterize the sources and processes of SOA formation at remote sites.« less

Authors:
 [1]; ORCiD logo [2];  [3];  [4];  [4];  [5];  [5];  [5];  [2]; ORCiD logo [2]
  1. Institute of Environmental Assessment and Water Research (IDAEA-CSIC), Barcelona (Spain); Univ. of Barcelona, Barcelona (Spain)
  2. Institute of Environmental Assessment and Water Research (IDAEA-CSIC), Barcelona (Spain)
  3. Aix-Marseille Univ., Marseille (France)
  4. Univ. of Colorado, Boulder, CO (United States)
  5. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
Publication Date:
Research Org.:
Univ. of Colorado, Boulder, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1455232
Grant/Contract Number:  
SC0011105
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Volume: 15; Journal Issue: 6; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ripoll, Anna, Minguillon, M. C., Pey, J., Jimenez, J. L., Day, D. A., Sosedova, Y., Canonaco, F., Prevot, A. S. H., Querol, X., and Alastuey, A. Long-term real-time chemical characterization of submicron aerosols at Montsec (southern Pyrenees, 1570 m a.s.l.). United States: N. p., 2015. Web. doi:10.5194/acp-15-2935-2015.
Ripoll, Anna, Minguillon, M. C., Pey, J., Jimenez, J. L., Day, D. A., Sosedova, Y., Canonaco, F., Prevot, A. S. H., Querol, X., & Alastuey, A. Long-term real-time chemical characterization of submicron aerosols at Montsec (southern Pyrenees, 1570 m a.s.l.). United States. doi:10.5194/acp-15-2935-2015.
Ripoll, Anna, Minguillon, M. C., Pey, J., Jimenez, J. L., Day, D. A., Sosedova, Y., Canonaco, F., Prevot, A. S. H., Querol, X., and Alastuey, A. Mon . "Long-term real-time chemical characterization of submicron aerosols at Montsec (southern Pyrenees, 1570 m a.s.l.)". United States. doi:10.5194/acp-15-2935-2015. https://www.osti.gov/servlets/purl/1455232.
@article{osti_1455232,
title = {Long-term real-time chemical characterization of submicron aerosols at Montsec (southern Pyrenees, 1570 m a.s.l.)},
author = {Ripoll, Anna and Minguillon, M. C. and Pey, J. and Jimenez, J. L. and Day, D. A. and Sosedova, Y. and Canonaco, F. and Prevot, A. S. H. and Querol, X. and Alastuey, A.},
abstractNote = {Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols (particles with an aerodynamic diameter of less than 1 μm) from a continental background site (Montsec, MSC, 1570 m a.s.l.) in the western Mediterranean Basin (WMB) were conducted for 10 months (July 2011–April 2012). An aerosol chemical speciation monitor (ACSM) was co-located with other online and offline PM1 measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here, for the first time, for this region. Seasonal trends in PM1 components are attributed to variations in evolution of the planetary boundary layer (PBL) height, air mass origin, and meteorological conditions. In summer, the higher temperature and solar radiation increases convection, enhancing the growth of the PBL and the transport of anthropogenic pollutants towards high altitude sites. Furthermore, the regional recirculation of air masses over the WMB creates a continuous increase in the background concentrations of PM1 components and causes the formation of reservoir layers at relatively high altitudes. The combination of all these atmospheric processes results in a high variability of PM1 components, with poorly defined daily patterns, except for the organic aerosols (OA). OA was mostly composed (up to 90%) of oxygenated organic aerosol (OOA), split in two types: semivolatile (SV-OOA) and low-volatility (LV-OOA), the rest being hydrocarbon-like OA (HOA). The marked diurnal cycles of OA components regardless of the air mass origin indicates that they are not only associated with anthropogenic and long-range-transported secondary OA (SOA) but also with recently produced biogenic SOA. Very different conditions drive the aerosol phenomenology in winter at MSC. The thermal inversions and the lower vertical development of the PBL leave MSC in the free troposphere most of the day, being affected by PBL air masses only after midday, when the mountain breezes transport emissions from the adjacent valleys and plains to the top of the mountain. This results in clear diurnal patterns of both organic and inorganic concentrations. OA was also mainly composed (71%) of OOA, with contributions from HOA (5%) and biomass burning OA (BBOA; 24%). Moreover, in winter sporadic long-range transport from mainland Europe is observed. The results obtained in the present study highlight the importance of SOA formation processes at a remote site such as MSC, especially in summer. Furthermore, additional research is needed to characterize the sources and processes of SOA formation at remote sites.},
doi = {10.5194/acp-15-2935-2015},
journal = {Atmospheric Chemistry and Physics (Online)},
issn = {1680-7324},
number = 6,
volume = 15,
place = {United States},
year = {2015},
month = {3}
}

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Works referenced in this record:

O/C and OM/OC Ratios of Primary, Secondary, and Ambient Organic Aerosols with High-Resolution Time-of-Flight Aerosol Mass Spectrometry
journal, June 2008

  • Aiken, Allison C.; DeCarlo, Peter F.; Kroll, Jesse H.
  • Environmental Science & Technology, Vol. 42, Issue 12
  • DOI: 10.1021/es703009q

Regional modeling of carbonaceous aerosols over Europe—focus on secondary organic aerosols
journal, November 2008

  • Bessagnet, Bertrand; Menut, Laurent; Curci, Gabriele
  • Journal of Atmospheric Chemistry, Vol. 61, Issue 3
  • DOI: 10.1007/s10874-009-9129-2

Intercomparison of an Aerosol Chemical Speciation Monitor (ACSM) with ambient fine aerosol measurements in downtown Atlanta, Georgia
journal, January 2014

  • Budisulistiorini, S. H.; Canagaratna, M. R.; Croteau, P. L.
  • Atmospheric Measurement Techniques, Vol. 7, Issue 7
  • DOI: 10.5194/amt-7-1929-2014

Real-Time Continuous Characterization of Secondary Organic Aerosol Derived from Isoprene Epoxydiols in Downtown Atlanta, Georgia, Using the Aerodyne Aerosol Chemical Speciation Monitor
journal, May 2013

  • Budisulistiorini, Sri Hapsari; Canagaratna, Manjula R.; Croteau, Philip L.
  • Environmental Science & Technology, Vol. 47, Issue 11
  • DOI: 10.1021/es400023n

Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer
journal, January 2007

  • Canagaratna, M. R.; Jayne, J. T.; Jimenez, J. L.
  • Mass Spectrometry Reviews, Vol. 26, Issue 2
  • DOI: 10.1002/mas.20115

Chemical Characterization of Submicron Aerosol Particles in Santiago de Chile
journal, January 2013

  • Carbone, Samara; Saarikoski, Sanna; Frey, Anna
  • Aerosol and Air Quality Research, Vol. 13, Issue 2
  • DOI: 10.4209/aaqr.2012.10.0261

3-year chemical composition of free tropospheric PM1 at the Mt. Cimone GAW global station – South Europe – 2165 m a.s.l.
journal, April 2014


Influence of altitude on ozone levels and variability in the lower troposphere: a ground-based study for western Europe over the period 2001–2004
journal, January 2007

  • Chevalier, A.; Gheusi, F.; Delmas, R.
  • Atmospheric Chemistry and Physics, Vol. 7, Issue 16
  • DOI: 10.5194/acp-7-4311-2007

Chemical composition of free tropospheric aerosol for PM1 and coarse mode at the high alpine site Jungfraujoch
journal, January 2008

  • Cozic, J.; Verheggen, B.; Weingartner, E.
  • Atmospheric Chemistry and Physics, Vol. 8, Issue 2
  • DOI: 10.5194/acp-8-407-2008

Organic aerosol components derived from 25 AMS data sets across Europe using a consistent ME-2 based source apportionment approach
journal, January 2014

  • Crippa, M.; Canonaco, F.; Lanz, V. A.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 12
  • DOI: 10.5194/acp-14-6159-2014

Organic Aerosols in the Earth’s Atmosphere
journal, October 2009

  • De Gouw, Joost; Jimenez, Jose L.
  • Environmental Science & Technology, Vol. 43, Issue 20
  • DOI: 10.1021/es9006004

Contribution of fungi to primary biogenic aerosols in the atmosphere: wet and dry discharged spores, carbohydrates, and inorganic ions
journal, January 2007

  • Elbert, W.; Taylor, P. E.; Andreae, M. O.
  • Atmospheric Chemistry and Physics, Vol. 7, Issue 17
  • DOI: 10.5194/acp-7-4569-2007

Seasonal variations in aerosol particle composition at the puy-de-Dôme research station in France
journal, January 2011

  • Freney, E. J.; Sellegri, K.; Canonaco, F.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 24
  • DOI: 10.5194/acp-11-13047-2011

ACTRIS ACSM intercomparison – Part 2: Intercomparison of ME-2 organic source apportionment results from 15 individual, co-located aerosol mass spectrometers
journal, January 2015

  • Fröhlich, R.; Crenn, V.; Setyan, A.
  • Atmospheric Measurement Techniques Discussions, Vol. 8, Issue 2
  • DOI: 10.5194/amtd-8-1559-2015

The formation, properties and impact of secondary organic aerosol: current and emerging issues
journal, January 2009

  • Hallquist, M.; Wenger, J. C.; Baltensperger, U.
  • Atmospheric Chemistry and Physics, Vol. 9, Issue 14
  • DOI: 10.5194/acp-9-5155-2009

Quantification of topographic venting of boundary layer air to the free troposphere
journal, January 2004

  • Henne, S.; Furger, M.; Nyeki, S.
  • Atmospheric Chemistry and Physics, Vol. 4, Issue 2
  • DOI: 10.5194/acp-4-497-2004

Ambient aerosol sampling using the Aerodyne Aerosol Mass Spectrometer
journal, January 2003


Evolution of Organic Aerosols in the Atmosphere
journal, December 2009


Overview of the meteorology and transport patterns during the DAURE field campaign and their impact to PM observations
journal, October 2013


Chemistry of secondary organic aerosol: Formation and evolution of low-volatility organics in the atmosphere
journal, May 2008


The chemical and microphysical properties of secondary organic aerosols from Holm Oak emissions
journal, January 2010

  • Lang-Yona, N.; Rudich, Y.; Mentel, Th. F.
  • Atmospheric Chemistry and Physics, Vol. 10, Issue 15
  • DOI: 10.5194/acp-10-7253-2010

Characterization of aerosol chemical composition with aerosol mass spectrometry in Central Europe: an overview
journal, January 2010

  • Lanz, V. A.; Prévôt, A. S. H.; Alfarra, M. R.
  • Atmospheric Chemistry and Physics, Vol. 10, Issue 21
  • DOI: 10.5194/acp-10-10453-2010

Evaluation of Composition-Dependent Collection Efficiencies for the Aerodyne Aerosol Mass Spectrometer using Field Data
journal, March 2012


Photooxidant dynamics in the Mediterranean basin in summer: Results from European research projects
journal, April 1997

  • Millán, M. M.; Salvador, R.; Mantilla, E.
  • Journal of Geophysical Research: Atmospheres, Vol. 102, Issue D7
  • DOI: 10.1029/96JD03610

Fossil versus contemporary sources of fine elemental and organic carbonaceous particulate matter during the DAURE campaign in Northeast Spain
journal, January 2011

  • Minguillón, M. C.; Perron, N.; Querol, X.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 23
  • DOI: 10.5194/acp-11-12067-2011

Chemical characterization of submicron regional background aerosols in the Western Mediterranean using an Aerosol Chemical Speciation Monitor
journal, January 2015

  • Minguillón, M. C.; Ripoll, A.; Pérez, N.
  • Atmospheric Chemistry and Physics Discussions, Vol. 15, Issue 1
  • DOI: 10.5194/acpd-15-965-2015

Characterization and intercomparison of aerosol absorption photometers: result of two intercomparison workshops
journal, January 2011

  • Müller, T.; Henzing, J. S.; de Leeuw, G.
  • Atmospheric Measurement Techniques, Vol. 4, Issue 2
  • DOI: 10.5194/amt-4-245-2011

Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry
journal, January 2010

  • Ng, N. L.; Canagaratna, M. R.; Zhang, Q.
  • Atmospheric Chemistry and Physics, Vol. 10, Issue 10
  • DOI: 10.5194/acp-10-4625-2010

Changes in organic aerosol composition with aging inferred from aerosol mass spectra
journal, January 2011

  • Ng, N. L.; Canagaratna, M. R.; Jimenez, J. L.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 13
  • DOI: 10.5194/acp-11-6465-2011

Real-Time Methods for Estimating Organic Component Mass Concentrations from Aerosol Mass Spectrometer Data
journal, February 2011

  • Ng, N. L.; Canagaratna, M. R.; Jimenez, J. L.
  • Environmental Science & Technology, Vol. 45, Issue 3
  • DOI: 10.1021/es102951k

An Aerosol Chemical Speciation Monitor (ACSM) for Routine Monitoring of the Composition and Mass Concentrations of Ambient Aerosol
journal, July 2011


Warming-induced increase in aerosol number concentration likely to moderate climate change
journal, April 2013

  • Paasonen, Pauli; Asmi, Ari; Petäjä, Tuukka
  • Nature Geoscience, Vol. 6, Issue 6
  • DOI: 10.1038/ngeo1800

The Multilinear Engine: A Table-Driven, Least Squares Program for Solving Multilinear Problems, including the n-Way Parallel Factor Analysis Model
journal, December 1999

  • Paatero, Pentti
  • Journal of Computational and Graphical Statistics, Vol. 8, Issue 4
  • DOI: 10.2307/1390831

Effects of sources and meteorology on particulate matter in the Western Mediterranean Basin: An overview of the DAURE campaign: An overview of the DAURE campaign
journal, April 2014

  • Pandolfi, M.; Querol, X.; Alastuey, A.
  • Journal of Geophysical Research: Atmospheres, Vol. 119, Issue 8
  • DOI: 10.1002/2013JD021079

Climatology of aerosol optical properties and black carbon mass absorption cross section at a remote high-altitude site in the western Mediterranean Basin
journal, January 2014

  • Pandolfi, M.; Ripoll, A.; Querol, X.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 12
  • DOI: 10.5194/acp-14-6443-2014

Multi-angle absorption photometry—a new method for the measurement of aerosol light absorption and atmospheric black carbon
journal, April 2004


Recommendations for reporting "black carbon" measurements
journal, January 2013

  • Petzold, A.; Ogren, J. A.; Fiebig, M.
  • Atmospheric Chemistry and Physics, Vol. 13, Issue 16
  • DOI: 10.5194/acp-13-8365-2013

Geochemistry of regional background aerosols in the Western Mediterranean
journal, November 2009


Daily evolution of sulphate aerosols in a rural area, northeastern Spain—elucidation of an atmospheric reservoir effect
journal, June 1999


Variability in regional background aerosols within the Mediterranean
journal, January 2009

  • Querol, X.; Alastuey, A.; Pey, J.
  • Atmospheric Chemistry and Physics, Vol. 9, Issue 14
  • DOI: 10.5194/acp-9-4575-2009

Physicochemical properties and origin of organic groups detected in boreal forest using an aerosol mass spectrometer
journal, January 2010

  • Raatikainen, T.; Vaattovaara, P.; Tiitta, P.
  • Atmospheric Chemistry and Physics, Vol. 10, Issue 4
  • DOI: 10.5194/acp-10-2063-2010

Three years of aerosol mass, black carbon and particle number concentrations at Montsec (southern Pyrenees, 1570 m a.s.l.)
journal, January 2014

  • Ripoll, A.; Pey, J.; Minguillón, M. C.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 8
  • DOI: 10.5194/acp-14-4279-2014

Joint analysis of continental and regional background environments in the western Mediterranean: PM 1 and PM 10 concentrations and composition
journal, January 2015

  • Ripoll, A.; Minguillón, M. C.; Pey, J.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 2
  • DOI: 10.5194/acp-15-1129-2015

Rethinking Organic Aerosols: Semivolatile Emissions and Photochemical Aging
journal, March 2007


Saharan dust contributions to PM10 and TSP levels in Southern and Eastern Spain
journal, May 2001


Origin of high summer PM10 and TSP concentrations at rural sites in Eastern Spain
journal, July 2002


Events Affecting Levels and Seasonal Evolution of Airborne Particulate Matter Concentrations in the Western Mediterranean
journal, January 2003

  • Rodríguez, Sergio; Querol, Xavier; Alastuey, Andrés
  • Environmental Science & Technology, Vol. 37, Issue 2
  • DOI: 10.1021/es020106p

Characterization of ambient aerosols in Mexico City during the MCMA-2003 campaign with Aerosol Mass Spectrometry: results from the CENICA Supersite
journal, January 2006

  • Salcedo, D.; Onasch, T. B.; Dzepina, K.
  • Atmospheric Chemistry and Physics, Vol. 6, Issue 4
  • DOI: 10.5194/acp-6-925-2006

Artefacts in the sampling of nitrate studied in the “INTERCOMP” campaigns of EUROTRAC-AEROSOL
journal, December 2004


Contrasting winter and summer VOC mixing ratios at a forest site in the Western Mediterranean Basin: the effect of local biogenic emissions
journal, January 2011


Seasonal variability of aerosol optical properties observed by means of a Raman lidar at an EARLINET site over Northeastern Spain
journal, January 2011

  • Sicard, M.; Rocadenbosch, F.; Reba, M. N. M.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 1
  • DOI: 10.5194/acp-11-175-2011

Intra- and inter-annual variability of VOC emissions from natural and semi-natural vegetation in Europe and neighbouring countries
journal, March 2009


Organic functional groups in aerosol particles from burning and non-burning forest emissions at a high-elevation mountain site
journal, January 2011

  • Takahama, S.; Schwartz, R. E.; Russell, L. M.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 13
  • DOI: 10.5194/acp-11-6367-2011

Chemical composition, main sources and temporal variability of PM 1 aerosols in southern African grassland
journal, January 2014

  • Tiitta, P.; Vakkari, V.; Croteau, P.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 4
  • DOI: 10.5194/acp-14-1909-2014

Short-term climatology of PM10 at a high altitude background station in southern Europe
journal, February 2013


Secondary organic aerosol formation from anthropogenic air pollution: Rapid and higher than expected
journal, January 2006

  • Volkamer, Rainer; Jimenez, Jose L.; San Martini, Federico
  • Geophysical Research Letters, Vol. 33, Issue 17
  • DOI: 10.1029/2006GL026899

Hydrocarbon-like and oxygenated organic aerosols in Pittsburgh: insights into sources and processes of organic aerosols
journal, January 2005

  • Zhang, Q.; Worsnop, D. R.; Canagaratna, M. R.
  • Atmospheric Chemistry and Physics, Vol. 5, Issue 12
  • DOI: 10.5194/acp-5-3289-2005

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