Open Access
Widening the gap between measurement and modelling ofsecondary organic aerosol properties
Nicholas Good,David Topping,Jonathan Duplissy,Martin Gysel,N. K. Meyer,A. Metzger,Samantha J. Turner,Urs Baltensperger,Zoran Ristovski,Ernest Weingartner,Hugh Coe,Gordon McFiggans +11 more
TLDR
In this article, the authors investigated the link between measured sub-saturated hygroscopicity and cloud activation potential of secondary organic particles produced by the chamber photo-oxidation.Abstract:
The link between measured sub-saturated hygroscopicity
and cloud activation potential of secondary organic
aerosol particles produced by the chamber photo-oxidation
of α-pinene in the presence or absence of ammonium sulphate
seed aerosol was investigated using two models of
varying complexity. A simple single hygroscopicity parameter
model and a more complex model (incorporating surface
effects) were used to assess the detail required to predict
the cloud condensation nucleus (CCN) activity from the subsaturated water uptake. Sub-saturated water uptake measured by three hygroscopicity tandem differential mobility analyser (HTDMA) instruments was used to determine the water activity for use in the models. The predicted CCN activity was compared to the measured CCN activation potential using a continuous flow CCN counter.
Reconciliation using the more complex model formulation
with measured cloud activation could be achieved widely
different assumed surface tension behavior of the growing
droplet; this was entirely determined by the instrument used
as the source of water activity data. This unreliable derivation of the water activity as a function of solute concentration from sub-saturated hygroscopicity data indicates a limitation in the use of such data in predicting cloud condensation nucleus behavior of particles with a significant organic fraction. Similarly, the ability of the simpler single parameter model to predict cloud activation behaviour was dependent on the instrument
used to measure sub-saturated hygroscopicity and
the relative humidity used to provide the model input. However, agreement was observed for inorganic salt solution particles, which were measured by all instruments in agreement with theory. The difference in HTDMA data from validated and extensively used instruments means that it cannot be stated with certainty the detail required to predict the CCN activity from sub-saturated hygroscopicity. In order to narrow the gap between measurements of hygroscopic growth and CCN activity the processes involved must be understood and the instrumentation extensively quality assured. It is impossible to say from the results presented here due to the differences in HTDMA data whether: i) Surface tension suppression occurs ii)
Bulk to surface partitioning is important iii) The water activity coefficient changes significantly as a function of the solute concentration.read more
Citations
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Journal ArticleDOI
A single parameter representation of hygroscopic growth and cloud condensation nucleus activity – Part 3: Including surfactant partitioning
TL;DR: In this article, a hybrid model that accounts for partitioning between the bulk and surface phases in the context of single parameter representations of cloud condensation nucleus activity is introduced, which allows users of the single parameter model to account for surfactant partitioning by applying minor modifications to existing code.
Journal ArticleDOI
Relating hygroscopicity and composition of organic aerosol particulate matter
Jonathan Duplissy,Jonathan Duplissy,Peter F. DeCarlo,Peter F. DeCarlo,J. Dommen,M. R. Alfarra,A. Metzger,A. Metzger,I. Barmpadimos,André S. H. Prévôt,Ernest Weingartner,Torsten Tritscher,Martin Gysel,Allison C. Aiken,Allison C. Aiken,Jose L. Jimenez,Manjula R. Canagaratna,D. R. Worsnop,Don R. Collins,Jason Tomlinson,Jason Tomlinson,Urs Baltensperger +21 more
TL;DR: In this article, a hygroscopicity tandem differential mobility analyzer (HTDMA) was used to measure the water uptake (hygroscopy) of secondary organic aerosol (SOA) formed during the chemical and photochemical oxidation of several organic precursors in a smog chamber.
Journal ArticleDOI
Seasonal variation of CCN concentrations and aerosol activation properties in boreal forest
S.-L. Sihto,Jyri Mikkilä,Joonas Vanhanen,Mikael Ehn,Li Liao,Katrianne Lehtipalo,Pasi Aalto,Jonathan Duplissy,Jonathan Duplissy,Tuukka Petäjä,Veli-Matti Kerminen,Veli-Matti Kerminen,Michael Boy,Markku Kulmala +13 more
TL;DR: In this paper, the annual cycle of cloud condensation nuclei (CCN) concentrations and critical diameter for cloud droplet activation as a function of supersaturation were measured using a CCN counter and a HTDMA (hygroscopicity tandem differential mobility analyzer) at SMEAR II station, Hyytiala, Finland.
Journal ArticleDOI
Influences on the fraction of hydrophobic and hydrophilic black carbon in the atmosphere
TL;DR: In this paper, a method for measuring the hygroscopicity of externally and internally mixed BC particles by coupling a single particle soot photometer with a humidified tandem differential mobility analyzer was introduced.
Journal ArticleDOI
Observations and implications of liquid–liquid phase separation at highrelative humidities in secondary organic material produced by α -pinene ozonolysis without inorganic salts
Lindsay Renbaum-Wolff,Lindsay Renbaum-Wolff,Mijung Song,Mijung Song,Claudia Marcolli,Yue Zhang,Yue Zhang,Pengfei Liu,James W. Grayson,Franz M. Geiger,Scot T. Martin,Allan K. Bertram +11 more
TL;DR: In this article, the phase state of secondary organic material (SOM) particles free of inorganic salts produced by the ozonolysis of α-pinene was investigated in the laboratory using optical microscopy and theoretically using a thermodynamic model at 290 K and for relative humidities ranging from
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A single parameter representation of hygroscopic growth and cloud condensation nucleus activity
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