Publications by authors named "Markus Leiminger"

Article Synopsis
  • New particle formation (NPF) in the tropical free troposphere is crucial for creating cloud condensation nuclei, influencing cloud properties and climate.
  • Researchers conducted molecular-level measurements of oxidized organic molecules (OOMs) at a high-altitude site in Bolivia, uncovering their presence in both gas and particle phases, with a focus on short-chain carbon compounds.
  • The study links these OOMs to isoprene emissions from distant rainforests and suggests they play a role in the growth of newly formed nanoparticles, advancing our understanding of aerosol formation in this region.
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Proton-transfer-reaction mass spectrometry (PTR-MS) is widely used for measuring organic trace gases in air. In traditional PTR-MS, both nonpolar and polar analytes are ionized with unit efficiency, as predicted from ion-molecule collision theories. This well-defined ion chemistry allows for direct quantification of analytes without prior calibration and therefore is an important characteristic of PTR-MS.

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Article Synopsis
  • - Iodic acid (HIO) can rapidly form aerosol particles in coastal areas, with nucleation rates surpassing those of sulfuric acid-ammonia under similar conditions.
  • - Ion-induced nucleation involves the initial formation of IO followed by the addition of HIO, occurring efficiently at temperatures below +10°C, while neutral nucleation relies on a different process involving iodous acid.
  • - Freshly formed HIO particles significantly contribute to fast particle growth and can effectively compete with sulfuric acid particle formation in unpolluted atmospheric regions.
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In most organisms, the concentration of free Zn is controlled by metallothioneins (MTs). In contrast, no significant proportions of Zn are bound to MTs in the slug, Arion vulgaris. Instead, this species possesses cytoplasmic low-molecular-weight Zn (LMW Zn) binding compound that divert these metal ions into pathways uncoupled from MT metabolism.

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We use a real-time temperature-programmed desorption chemical-ionization mass spectrometer (FIGAERO-CIMS) to measure particle-phase composition and volatility of nucleated particles, studying pure α-pinene oxidation over a wide temperature range (-50 °C to +25 °C) in the CLOUD chamber at CERN. Highly oxygenated organic molecules are much more abundant in particles formed at higher temperatures, shifting the compounds toward higher O/C and lower intrinsic (300 K) volatility. We find that pure biogenic nucleation and growth depends only weakly on temperature.

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Article Synopsis
  • Nucleation and growth of aerosol particles from atmospheric vapors are important for forming cloud condensation nuclei (CCN), particularly for particles smaller than 10 nm that face significant losses from coagulation.
  • Recent findings indicate that oxidation products from biogenic volatile organic compounds are key to particle formation and initial growth; however, the role of these oxidized organics in particle growth across various temperatures remains uncertain.
  • Experiments conducted in the CLOUD chamber at CERN reveal that organic particle growth occurs across a broad temperature range, with growth rates influenced by particle curvature and supported by a gas-phase model of oxidized organic molecules.
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About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles, thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across.

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The growth of freshly formed aerosol particles can be the bottleneck in their survival to cloud condensation nuclei. It is therefore crucial to understand how particles grow in the atmosphere. Insufficient experimental data has impeded a profound understanding of nano-particle growth under atmospheric conditions.

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We investigated the nucleation of sulfuric acid together with two bases (ammonia and dimethylamine), at the CLOUD chamber at CERN. The chemical composition of positive, negative, and neutral clusters was studied using three Atmospheric Pressure interface-Time Of Flight (APi-TOF) mass spectrometers: two were operated in positive and negative mode to detect the chamber ions, while the third was equipped with a nitrate ion chemical ionization source allowing detection of neutral clusters. Taking into account the possible fragmentation that can happen during the charging of the ions or within the first stage of the mass spectrometer, the cluster formation proceeded via essentially one-to-one acid-base addition for all of the clusters, independent of the type of the base.

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For atmospheric sulfuric acid (SA) concentrations the presence of dimethylamine (DMA) at mixing ratios of several parts per trillion by volume can explain observed boundary layer new particle formation rates. However, the concentration and molecular composition of the neutral (uncharged) clusters have not been reported so far due to the lack of suitable instrumentation. Here we report on experiments from the Cosmics Leaving Outdoor Droplets chamber at the European Organization for Nuclear Research revealing the formation of neutral particles containing up to 14 SA and 16 DMA molecules, corresponding to a mobility diameter of about 2 nm, under atmospherically relevant conditions.

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Article Synopsis
  • Nucleation of aerosol particles from trace atmospheric vapors contributes significantly to cloud condensation nuclei, potentially cooling the climate by enhancing cloud properties.
  • Recent studies indicate that traditional explanations, like sulfuric acid and ammonia, are insufficient to explain observed particle formation rates, prompting exploration of amines.
  • Using the CLOUD chamber at CERN, researchers found that dimethylamine vastly improves particle formation rates through a stabilization mechanism, suggesting a need to reevaluate how human activities affect aerosol formation in the atmosphere.
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