Search results for "ATMOSPHERIC CHEMISTRY"

2015

Abstract. Atmospheric concentrations of nitrous acid (HONO), one of the major precursors of the hydroxyl radical (OH) in the troposphere, significantly exceed the values predicted by the assumption of a photostationary state (PSS) during daytime. Therefore, additional sources of HONO were intensively investigated in the last decades. This study presents budget calculations of HONO based on simultaneous measurements of all relevant species, including HONO and OH at two different measurement heights, i.e. 1 m above the ground and about 2 to 3 m above the canopy (24 m above the ground), conducted in a boreal forest environment. We observed mean HONO concentrations of about 6.5 × 108 molecules …

2017

Abstract. We analysed the extensive dataset from the HUMPPA-COPEC 2010 and the HOPE 2012 field campaigns in the boreal forest and rural environments of Finland and Germany, respectively, and estimated the abundance of stabilised Criegee intermediates (SCIs) in the lower troposphere. Based on laboratory tests, we propose that the background OH signal observed in our IPI-LIF-FAGE instrument during the aforementioned campaigns is caused at least partially by SCIs. This hypothesis is based on observed correlations with temperature and with concentrations of unsaturated volatile organic compounds and ozone. Just like SCIs, the background OH concentration can be removed through the addition of su…

2015

Abstract. The aerosol optical depth (AOD) trend between 2001 and 2010 is estimated globally and regionally from observations and results from simulations with the EMAC (ECHAM5/MESSy Atmospheric Chemistry) model. Although interannual variability is applied only to anthropogenic and biomass-burning emissions, the model is able to quantitatively reproduce the AOD trends as observed by the MODIS (Moderate Resolution Imaging Spectroradiometer) satellite sensor, while some discrepancies are found when compared to MISR (Multi-angle Imaging SpectroRadiometer) and SeaWIFS (Sea-viewing Wide Field-of-view Sensor) observations. Thanks to an additional simulation without any change in emissions, it is s…

Diurnal and seasonal variation of monoterpene and sesquiterpene emissions from Scots pine (Pinus sylvestris L.)

2006

Abstract Recent research pointed out the question of missing OH reactivity in a forest system and the question for unknown highly reactive biogenic emissions. In this study we show that coniferous forests are an important source of highly reactive hydrocarbons, the sesquiterpenes. We investigated the seasonality of terpene emissions from Scots pine to work out influences on atmospheric chemistry in different seasons for both mono- and sesquiterpenes. Especially sesquiterpenes (C15) change dramatically in their contribution to the terpene emissions of Scots pine. Fourteen sesquiterpenes and oxygenated compounds were found in the emissions. In spring, the pattern was most complex with all 14 …

2018

Abstract. Volcanoes are a natural source of several reactive gases (e.g., sulfur and halogen containing species) and nonreactive gases (e.g., carbon dioxide) to the atmosphere. The relative abundance of carbon and sulfur in volcanic gas as well as the total sulfur dioxide emission rate from a volcanic vent are established parameters in current volcano-monitoring strategies, and they oftentimes allow insights into subsurface processes. However, chemical reactions involving halogens are thought to have local to regional impact on the atmospheric chemistry around passively degassing volcanoes. In this study we demonstrate the successful deployment of a multirotor UAV (quadcopter) system with c…

The primary volcanic aerosol emission from Mt Etna: Size-resolved particles with SO2 and role in plume reactive halogen chemistry

2018

International audience; Volcanoes are an important source of aerosols to the troposphere. Within minutes after emission, volcanic plume aerosol catalyses conversion of co-emitted HBr, HCl into highly reactive halogens (e.g. BrO, OClO) through chemical cycles that cause substantial ozone depletion in the dispersing downwind plume.This study quantifies the sub-to-supramicron primary volcanic aerosol emission (0.2-5 μm diameter) and its role in this process. An in-situ ground-based study at Mt Etna (Italy) during passive degassing co-deployed an optical particle counter and Multi-Gas SO2 sensors at high time resolution (0.1 Hz) enabling to characterize the aerosol number, size-distribution and…

Implementation of the Community Earth System Model (CESM) version 1.2.1 as a new base model into version 2.50 of the MESSy framework

2016

Abstract. The Community Earth System Model (CESM1), maintained by the United States National Centre for Atmospheric Research (NCAR) is connected with the Modular Earth Submodel System (MESSy). For the MESSy user community, this offers many new possibilities. The option to use the Community Atmosphere Model (CAM) atmospheric dynamical cores, especially the state-of-the-art spectral element (SE) core, as an alternative to the ECHAM5 spectral transform dynamical core will provide scientific and computational advances for atmospheric chemistry and climate modelling with MESSy. The well-established finite volume core from CESM1(CAM) is also made available. This offers the possibility to compare …

A denuder-impinger system with in situ derivatization followed by gas chromatography-mass spectrometry for the determination of gaseous iodine-contai…

2008

Reactive iodine species have been suggested to play an important role in the atmosphere (e.g. tropospheric ozone depletion, coastal new particle formation). However, there still exist major uncertainties about their atmospheric chemistry, mostly due to the lack of analytical approaches for the accurate speciation of certain key compounds. In this study, 1,3,5-trimethoxybenzene (1,3,5-TMB)-coated denuder proved to be suitable for the differentiation between gaseous interhalogens (iodine monochloride (ICl), iodine monobromide (IBr)) and molecular iodine (I2) based on a selective collection/derivatization method. The results of the denuder sampling were compared with the results of impinger sa…

Determinación de las propiedades físicas y radiativas de aerosoles atmosféricos a partir de medidas de extinción de la radiación solar a nivel del su…

2001

Quantum dynamical study of the O(1D) + CH4→ CH3+ OH atmospheric reaction

2014

Time independent quantum mechanical (TIQM) scattering calculations have been carried out for the O((1)D) + CH4(X(1)A1) → CH3(X(2)A2″) + OH(X(2)Π) atmospheric reaction, using an ab initio ground potential energy surface where the CH3 group is described as a pseudo-atom. Total and state-to-state reaction probabilities for a total angular momentum J = 0 have been determined for collision energies up to 0.5 eV. The vibrational and rotational state OH product distributions show no specific behavior. The rate coefficient has been calculated by means of the J-shifting approach in the 10-500 K temperature range and slightly depends on T at ordinary temperatures (as expected for a barrierless reacti…