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Nucleation and growth of aerosol particles from atmospheric vapors constitutes a major source of global cloud condensation nuclei (CCN). The fraction of newly formed particles that reaches CCN sizes is highly sensitive to particle growth rates, especially for particle sizes <10 nm, where coagulation losses to larger aerosol particles are greatest. Recent results show that some oxidation products from biogenic volatile organic compounds are major contributors to particle formation and initial growth. However, whether oxidized organics contribute to particle growth over the broad span of tropospheric temperatures remains an open question, and quantitative mass balance for organic growth has yet to be demonstrated at any temperature. Here, in experiments performed under atmospheric conditions in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN), we show that rapid growth of organic particles occurs over the range from −25 ∘C to 25 ∘C. The lower extent of autoxidation at reduced temperatures is compensated by the decreased volatility of all oxidized molecules. This is confirmed by particle-phase composition measurements, showing enhanced uptake of relatively less oxygenated products at cold temperatures. We can reproduce the measured growth rates using an aerosol growth model based entirely on the experimentally measured gas-phase spectra of oxidized organic molecules obtained from two complementary mass spectrometers. We show that the growth rates are sensitive to particle curvature, explaining widespread atmospheric observations that particle growth rates increase in the single-digit-nanometer size range. Our results demonstrate that organic vapors can contribute to particle growth over a wide range of tropospheric temperatures from molecular cluster sizes onward.
Strain localization in the lithosphere and the formation, evolution, and maintenance of resulting plate boundaries play a crucial role in plate tectonics and thermo‐chemical mantle convection. Previously activated lithospheric deformation zones often appear to maintain a “memory” of weakening, leading to tectonic inheritance within plate reorganizations including the Wilson cycle. Different mechanisms have been proposed to explain such strain localization, but it remains unclear which operates on what spatio‐temporal scales, and how to best incorporate them in large‐scale mantle convection models. Here, we analyze two candidates, (1), grain‐size sensitive rheology and, (2), damage‐style parameterizations of yield, stress which are sometimes used to approximate the former. Grain‐size reduction due to dynamic recrystallization can drive localization in the ductile domain, and grain growth provides a time‐dependent rheological hardening component potentially enabling the preservation of rheological heterogeneities. We compare the dynamic weakening and hardening effects as well as the timescales of strength evolution for a composite rheology including grain‐size dynamics with a pseudo‐plastic rheology including damage‐ (or “strain”‐) dependent weakening. We explore the implications of different proposed grain‐size evolution laws, and test to which extent strain‐dependent rheologies can mimic the weakening and hardening effects of the more complex micro‐physical behavior. Such an analysis helps to better understand the parallels and differences between various strain‐localization modeling approaches used in different tectonics and geodynamics communities. More importantly, our results contribute to efforts to identify the key ingredients of strain‐localization and damage hysteresis within plate tectonics and how to represent those in planetary‐scale modeling.
The formation of secondary particles in the atmosphere accounts for more than half of global cloud condensation nuclei. Experiments at the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber have underlined the importance of ions for new particle formation, but quantifying their effect in the atmosphere remains challenging. By using a novel instrument setup consisting of two nano-particle counters, one of them equipped with an ion filter, we were able to further investigate the ion-related mechanisms of new particle formation. In autumn 2015, we carried out experiments at CLOUD on four systems of different chemical compositions involving monoterpenes, sulfuric acid, nitrogen oxides, and ammonia. We measured the influence of ions on the nucleation rates under precisely controlled and atmospherically relevant conditions. Our results indicate that ions enhance the nucleation process when the charge is necessary to stabilize newly formed clusters, i.e. in conditions where neutral clusters are unstable. For charged clusters that were formed by ion-induced nucleation, we were able to measure, for the first time, their progressive neutralization due to recombination with oppositely charged ions. A large fraction of the clusters carried a charge at 1.2 nm diameter. However, depending on particle growth rates and ion concentrations, charged clusters were largely neutralized by ion–ion recombination before they grew to 2.2 nm. At this size, more than 90 % of particles were neutral. In other words, particles may originate from ion-induced nucleation, although they are neutral upon detection at diameters larger than 2.2 nm. Observations at Hyytiälä, Finland, showed lower ion concentrations and a lower contribution of ion-induced nucleation than measured at CLOUD under similar conditions. Although this can be partly explained by the observation that ion-induced fractions decrease towards lower ion concentrations, further investigations are needed to resolve the origin of the discrepancy.