A fibre-optic UV system for H2SO4 production in aerosol chambers causing minimal thermal effects

Kupc, Agnieszka; Amorim, A.; Curtius, Joachim; Danielczok, Anja; Duplissy, Jonathan; Ehrhart, Sebastian; Walther, H.; Ickes, Luisa; Kirkby, J.; Kürten, Andreas; Lima, Jorge; Mathot, S.; Minginette, P.; Onnela, A.; Rondo, Linda; Wagner, Paul

doi:10.1016/j.jaerosci.2011.05.001

Cited by 48 publications

(63 citation statements)

References 22 publications

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“…Efforts were taken in its construction to make it the cleanest possible chamber used for studying atmospheric particle nucleation Schnitzhofer et al, 2014;Duplissy et al, 2016). It can be precisely temperature controlled, and UV light at 250-400 nm can be provided to the chamber with minimal heating via an array of fiber-optic bundles (Kupc et al, 2011). It is possible to eliminate ions from the chamber using a 20 kV m −1 clearing field and conversely to increase the number of chamber ions by directing a 3.5 GeV pion beam into the chamber.…”

Section: Laboratory Conditionsmentioning

confidence: 99%

Unexpectedly acidic nanoparticles formed in dimethylamine–ammonia–sulfuric-acid nucleation experiments at CLOUD

et al. 2016

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Abstract. New particle formation driven by acid-base chemistry was initiated in the CLOUD chamber at CERN by introducing atmospherically relevant levels of gas-phase sulfuric acid and dimethylamine (DMA). Ammonia was also present in the chamber as a gas-phase contaminant from earlier experiments. The composition of particles with volume median diameters (VMDs) as small as 10 nm was measured by the Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS). Particulate ammonium-to-dimethylaminium ratios were higher than the gas-phase ammonia-to-DMA ratios, suggesting preferential uptake of ammonia over DMA for the collected 10-30 nm VMD particles. This behavior is not consistent with present nanoparticle physicochemical models, which predict a higher dimethylaminium fraction when NH 3 and DMA are present at similar gas-phase concentrations. Despite the presence in the gas phase of at least 100 times higher base concentrations than sulfuric acid, the recently formed particles always had measured base : acid ratios lower than 1 : 1. The lowest base fractions were found in particles below 15 nm VMD, with a strong size-dependent composition gradient. The reasons for the very acidic composition remain uncertain, but a plausible explanation is thatPublished by Copernicus Publications on behalf of the European Geosciences Union. 13602 M. J. Lawler et al.: Acidic nanoparticles at CLOUD the particles did not reach thermodynamic equilibrium with respect to the bases due to rapid heterogeneous conversion of SO 2 to sulfate. These results indicate that sulfuric acid does not require stabilization by ammonium or dimethylaminium as acid-base pairs in particles as small as 10 nm.

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Section: Laboratory Conditionsmentioning

confidence: 99%

Unexpectedly acidic nanoparticles formed in dimethylamine–ammonia–sulfuric-acid nucleation experiments at CLOUD

et al. 2016

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“…The CLOUD aerosol chamber 7 allows the stable in situ production of gaseous H 2 SO 4 from the SO 2 + OH reaction 8 . The H 2 SO 4 concentration is monitored by a wellcalibrated CIMS instrument 3 (THS Instruments) as well as CI-APiTOF mass spectrometry 4 (Tofwerk AG/Aerodyne Research, Inc.).…”

Section: Experimental Methodsmentioning

confidence: 99%

Experimental study on the influence of dimethylamine on the detection of gas phase sulfuric acid using chemical ionization mass spectrometry (CIMS)

Rondo¹,

Leiminger²,

Simon³

et al. 2013

AIP Conference Proceedings

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“…Additional CI-APi-TOF measurements were made during one experiment in November 2012 (CLOUD7). The CLOUD chamber has been described in previous publications (Kirkby et al, 2011;Duplissy et al, 2015). The 26.1 m 3 electropolished stainless-steel chamber provides an ultra-clean environment for studying new particle formation and growth.…”

Section: Cloud Chambermentioning

confidence: 99%

“…The temperature and the dew/frost point inside the chamber are monitored continuously; the RH is calculated using the equations given by Murphy and Koop (2005). A fiber optic system (Kupc et al, 2011) feeds UV light into the chamber, which initiates the photolytic production of sulfuric acid when H 2 O, O 2 , O 3 , and SO 2 are present. Two mixing fans continuously stir the air inside the chamber, assuring its homogeneity (Voigtländer et al, 2012).…”

Section: Cloud Chambermentioning

confidence: 99%

“…Moreover, it is generally accepted that the presence of water vapor enhances nucleation in the binary (H 2 SO 4 -H 2 O) system. However, nucleation under typical ground-level conditions cannot be explained by the binary nucleation of sulfuric acid and water vapor (Kulmala et al, 2004;Kerminen et al, 2010), even if the enhancing effect due to ions is taken into account (Kirkby et al, 2011). Therefore, assuming that sulfuric acid is required for nucleation, at least one additional compound is necessary to stabilize the nucleating clusters (Zhang et al, 2012).…”

Section: Introductionmentioning

confidence: 99%

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Thermodynamics of the formation of sulfuric acid dimers in the binary (H2SO4–H2O) and ternary (H2SO4–H2O–NH3) system

Kürten¹,

Münch

Rondo

et al. 2015

Atmos. Chem. Phys.

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Abstract. Sulfuric acid is an important gas influencing atmospheric new particle formation (NPF). Both the binary (H 2 SO 4 -H 2 O) system and the ternary system involving ammonia (H 2 SO 4 -H 2 O-NH 3 ) may be important in the free troposphere. An essential step in the nucleation of aerosol particles from gas-phase precursors is the formation of a dimer, so an understanding of the thermodynamics of dimer formation over a wide range of atmospheric conditions is essential to describe NPF. We have used the CLOUD chamber to conduct nucleation experiments for these systems at temperatures from 208 to 248 K. Neutral monomer and dimer concentrations of sulfuric acid were measured using a chemical ionization mass spectrometer (CIMS). From these measurements, dimer evaporation rates in the binary system were derived for temperatures of 208 and 223 K. We compare these results to literature data from a previous study that was conducted at higher temperatures but is in good agreement with the present study. For the ternary system the formation of Published by Copernicus Publications on behalf of the European Geosciences Union. A. Kürten et al.: Thermodynamics of the formation of sulfuric acid dimersH 2 SO 4 q NH 3 is very likely an essential step in the formation of sulfuric acid dimers, which were measured at 210, 223, and 248 K. We estimate the thermodynamic properties (dH and dS) of the H 2 SO 4 q NH 3 cluster using a simple heuristic model and the measured data. Furthermore, we report the first measurements of large neutral sulfuric acid clusters containing as many as 10 sulfuric acid molecules for the binary system using chemical ionization-atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometry.

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A fibre-optic UV system for H2SO4 production in aerosol chambers causing minimal thermal effects

Cited by 48 publications

References 22 publications

Unexpectedly acidic nanoparticles formed in dimethylamine–ammonia–sulfuric-acid nucleation experiments at CLOUD

Unexpectedly acidic nanoparticles formed in dimethylamine–ammonia–sulfuric-acid nucleation experiments at CLOUD

Experimental study on the influence of dimethylamine on the detection of gas phase sulfuric acid using chemical ionization mass spectrometry (CIMS)

Thermodynamics of the formation of sulfuric acid dimers in the binary (H<sub>2</sub>SO<sub>4</sub>–H<sub>2</sub>O) and ternary (H<sub>2</sub>SO<sub>4</sub>–H<sub>2</sub>O–NH<sub>3</sub>) system

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A fibre-optic UV system for H2SO4 production in aerosol chambers causing minimal thermal effects

Cited by 48 publications

References 22 publications

Unexpectedly acidic nanoparticles formed in dimethylamine–ammonia–sulfuric-acid nucleation experiments at CLOUD

Unexpectedly acidic nanoparticles formed in dimethylamine–ammonia–sulfuric-acid nucleation experiments at CLOUD

Experimental study on the influence of dimethylamine on the detection of gas phase sulfuric acid using chemical ionization mass spectrometry (CIMS)

Thermodynamics of the formation of sulfuric acid dimers in the binary (H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;–H&lt;sub&gt;2&lt;/sub&gt;O) and ternary (H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;–H&lt;sub&gt;2&lt;/sub&gt;O–NH&lt;sub&gt;3&lt;/sub&gt;) system

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Thermodynamics of the formation of sulfuric acid dimers in the binary (H<sub>2</sub>SO<sub>4</sub>–H<sub>2</sub>O) and ternary (H<sub>2</sub>SO<sub>4</sub>–H<sub>2</sub>O–NH<sub>3</sub>) system