Measurement of ammonia, amines and iodine compounds using protonated water cluster chemical ionization mass spectrometry

Pfeifer, Joschka; Simon, Mario; Heinritzi, Martin; Piel, Felix; Weitz, Lena; Wang, Dongyu; Granzin, Manuel; Müller, Tatjana; Bräkling, Steffen; Kirkby, J.; Curtius, Joachim; Kürten, Andreas

doi:10.5194/amt-13-2501-2020

Cited by 28 publications

(24 citation statements)

References 75 publications

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“…4b. In addition, we show the growth rates using the time-and sizeresolving growth rate analysis method INSIDE (Pichelstorfer et al, 2018), which agrees with the appearance time method, demonstrating a minor systematic bias in our growth rate determination. All approaches reproduce the size dependence at an acceptable level (R 2 larger than 0.87).…”

Section: Size Dependence and Hydration Effectssupporting

confidence: 77%

“…S1b). In the second method, we applied the size-and time-resolving growth rate analysis method "IN-SIDE" (INterpreting the change rate of the Size-Integrated general Dynamic Equation; Pichelstorfer et al, 2018) to cross-check our results. The INSIDE method uses the measured particle size distribution at a time t 1 and simulates the expected aerosol dynamics (coagulation, wall losses and dilution) until time t 2 .…”

Section: Experimental Approachmentioning

confidence: 99%

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Enhanced growth rate of atmospheric particles from sulfuric acid

et al. 2020

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Abstract. In the present-day atmosphere, sulfuric acid is the most important vapour for aerosol particle formation and initial growth. However, the growth rates of nanoparticles (<10 nm) from sulfuric acid remain poorly measured. Therefore, the effect of stabilizing bases, the contribution of ions and the impact of attractive forces on molecular collisions are under debate. Here, we present precise growth rate measurements of uncharged sulfuric acid particles from 1.8 to 10 nm, performed under atmospheric conditions in the CERN (European Organization for Nuclear Research) CLOUD chamber. Our results show that the evaporation of sulfuric acid particles above 2 nm is negligible, and growth proceeds kinetically even at low ammonia concentrations. The experimental growth rates exceed the hard-sphere kinetic limit for the condensation of sulfuric acid. We demonstrate that this results from van der Waals forces between the vapour molecules and particles and disentangle it from charge–dipole interactions. The magnitude of the enhancement depends on the assumed particle hydration and collision kinetics but is increasingly important at smaller sizes, resulting in a steep rise in the observed growth rates with decreasing size. Including the experimental results in a global model, we find that the enhanced growth rate of sulfuric acid particles increases the predicted particle number concentrations in the upper free troposphere by more than 50 %.

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Section: Size Dependence and Hydration Effectssupporting

confidence: 77%

Section: Experimental Approachmentioning

confidence: 99%

Enhanced growth rate of atmospheric particles from sulfuric acid

et al. 2020

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“…Reactive iodine species are released into the atmosphere mainly by biological processes in marine environments (i.e., from macro-and micro-algae) (McFiggans et al, 2004), O 3 deposition on the sea surface (Carpenter et al, 2013), and from the sea ice (Spolaor et al, 2013) and snowpack in the polar region (Raso et al, 2017). Once emitted, iodine species can modify atmospheric oxidative capacity via a chain of catalytic reactions with O 3 that form iodine oxides, leading to about 20 %-28 % of O 3 loss in the marine boundary layer (Prados-Roman et al, 2015;Sherwen et al, 2016). Through convection, reactive iodine species can be transported from the lower troposphere to the upper troposphere-lower stratosphere, causing one third of the iodine-induced ozone loss in the upper troposphere-lower stratosphere (Koenig et al, 2020).…”

Section: Introductionmentioning

confidence: 99%

Measurement of iodine species and sulfuric acid using bromide chemical ionization mass spectrometers

Wang

Finkenzeller

et al. 2021

Atmos. Meas. Tech.

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Abstract. Iodine species are important in the marine atmosphere for oxidation and new-particle formation. Understanding iodine chemistry and iodine new-particle formation requires high time resolution, high sensitivity, and simultaneous measurements of many iodine species. Here, we describe the application of a bromide chemical ionization mass spectrometer (Br-CIMS) to this task. During the iodine oxidation experiments in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber, we have measured gas-phase iodine species and sulfuric acid using two Br-CIMS, one coupled to a Multi-scheme chemical IONization inlet (Br-MION-CIMS) and the other to a Filter Inlet for Gasses and AEROsols inlet (Br-FIGAERO-CIMS). From offline calibrations and intercomparisons with other instruments, we have quantified the sensitivities of the Br-MION-CIMS to HOI, I2, and H2SO4 and obtained detection limits of 5.8 × 106, 3.8 × 105, and 2.0 × 105 molec. cm−3, respectively, for a 2 min integration time. From binding energy calculations, we estimate the detection limit for HIO3 to be 1.2 × 105 molec. cm−3, based on an assumption of maximum sensitivity. Detection limits in the Br-FIGAERO-CIMS are around 1 order of magnitude higher than those in the Br-MION-CIMS; for example, the detection limits for HOI and HIO3 are 3.3 × 107 and 5.1 × 106 molec. cm−3, respectively. Our comparisons of the performance of the MION inlet and the FIGAERO inlet show that bromide chemical ionization mass spectrometers using either atmospheric pressure or reduced pressure interfaces are well-matched to measuring iodine species and sulfuric acid in marine environments.

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“…Extremely high NPF rates are frequently observed in the polluted boundary layer, although current understanding suggests that newly formed particles should be rapidly scavenged by the high concentration of preexisting aerosols (Kulmala et al, 2017). Different vapours have been postulated to participate in NPF, including sulfuric acid, ammonia (Kirkby et al, 2011;, amines (Almeida et al, 2013) and organics (Kirkby et al, 2016;Lehtipalo et al, 2018;Riccobono et al, 2014).…”

Section: Introductionmentioning

confidence: 99%

The driving factors of new particle formation and growth in the polluted boundary layer

et al. 2021

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Abstract. New particle formation (NPF) is a significant source of atmospheric particles, affecting climate and air quality. Understanding the mechanisms involved in urban aerosols is important to develop effective mitigation strategies. However, NPF rates reported in the polluted boundary layer span more than 4 orders of magnitude, and the reasons behind this variability are the subject of intense scientific debate. Multiple atmospheric vapours have been postulated to participate in NPF, including sulfuric acid, ammonia, amines and organics, but their relative roles remain unclear. We investigated NPF in the CLOUD chamber using mixtures of anthropogenic vapours that simulate polluted boundary layer conditions. We demonstrate that NPF in polluted environments is largely driven by the formation of sulfuric acid–base clusters, stabilized by the presence of amines, high ammonia concentrations and lower temperatures. Aromatic oxidation products, despite their extremely low volatility, play a minor role in NPF in the chosen urban environment but can be important for particle growth and hence for the survival of newly formed particles. Our measurements quantitatively account for NPF in highly diverse urban environments and explain its large observed variability. Such quantitative information obtained under controlled laboratory conditions will help the interpretation of future ambient observations of NPF rates in polluted atmospheres.

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Measurement of ammonia, amines and iodine compounds using protonated water cluster chemical ionization mass spectrometry

Cited by 28 publications

References 75 publications

Enhanced growth rate of atmospheric particles from sulfuric acid

Enhanced growth rate of atmospheric particles from sulfuric acid

Measurement of iodine species and sulfuric acid using bromide chemical ionization mass spectrometers

The driving factors of new particle formation and growth in the polluted boundary layer

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