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Book ; Online: Numerical simulation and evaluation of global ultrafine particle concentrations at the Earth's surface

Kohl, Matthias / Lelieveld, Jos / Chowdhury, Sourangsu / Ehrhart, Sebastian / Sharma, Disha / Cheng, Yafang / Tripathi, Sachchida Nand / Sebastian, Mathew / Pandithurai, Govindan / Wang, Hongli / Pozzer, Andrea

eISSN: 1680-7324

2023

Abstract: A new global dataset of annually averaged ultrafine particle (UFP) concentrations at the Earth's surface for the years 2015–2017 has been developed through numerical simulations using the ECHAM/MESSy Atmospheric Chemistry model (EMAC). We present total ... ...

Abstract	A new global dataset of annually averaged ultrafine particle (UFP) concentrations at the Earth's surface for the years 2015–2017 has been developed through numerical simulations using the ECHAM/MESSy Atmospheric Chemistry model (EMAC). We present total and size-resolved concentrations along with their interannual variability. Size distributions of emitted particles from the contributing source sectors have been derived based on literature reports. The model results of UFP concentrations are evaluated using particle size distribution and particle number concentration measurements from available datasets and the literature. While we obtain reasonable agreement between the model results and observations (logarithmic-scale correlation of r =0.76 for non-remote, polluted regions), the highest values of observed, street-level UFP concentrations are systematically underestimated, whereas in rural environments close to urban areas the model generally overestimates observed UFP concentrations. As the relatively coarse global model does not resolve concentration gradients in urban centres and industrial UFP hotspots, high-resolution data of anthropogenic emissions are used to account for such differences in each model grid box, obtaining UFP concentrations with unprecedented 0.1 ∘ × 0.1 ∘ <svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="52pt" height="11pt" class="svg-formula" dspmath="mathimg" md5hash="0c30464444980c5c328fe69989ce4832"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-13191-2023-ie00001.svg" width="52pt" height="11pt" src="acp-23-13191-2023-ie00001.png"/></svg:svg> horizontal resolution at the Earth's surface. This observation-guided downscaling further improves the agreement with observations, leading to an increase in the logarithmic-scale correlation between observed and simulated UFP concentrations to r =0.84 in polluted environments (and 0.95 in all regions), a decrease in the root mean squared logarithmic error (from 0.57 to 0.43), and removal of ...
Subject code	910
Language	English
Publishing date	2023-10-19
Publishing country	de
Document type	Book ; Online
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Book ; Online: Numerical simulation and evaluation of global ultrafine particle concentrations at the Earth's surface

eISSN:

2023

Abstract	A new global dataset of annually averaged ultrafine particle (UFP) concentrations at the Earth's surface for the years 2015–2017 has been developed through numerical simulations using the ECHAM/MESSy Atmospheric Chemistry model (EMAC). We present total and size-resolved concentrations along with their interannual variability. Size distributions of emitted particles from the contributing source sectors have been derived based on literature reports. The model results of UFP concentrations are evaluated using particle size distribution and particle number concentration measurements from available datasets and the literature. While we obtain reasonable agreement between the model results and observations (logarithmic-scale correlation of r =0.76 for non-remote, polluted regions), the highest values of observed, street-level UFP concentrations are systematically underestimated, whereas in rural environments close to urban areas the model generally overestimates observed UFP concentrations. As the relatively coarse global model does not resolve concentration gradients in urban centres and industrial UFP hotspots, high-resolution data of anthropogenic emissions are used to account for such differences in each model grid box, obtaining UFP concentrations with unprecedented 0.1 ∘ × 0.1 ∘ <svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="52pt" height="11pt" class="svg-formula" dspmath="mathimg" md5hash="0c30464444980c5c328fe69989ce4832"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-13191-2023-ie00001.svg" width="52pt" height="11pt" src="acp-23-13191-2023-ie00001.png"/></svg:svg> horizontal resolution at the Earth's surface. This observation-guided downscaling further improves the agreement with observations, leading to an increase in the logarithmic-scale correlation between observed and simulated UFP concentrations to r =0.84 in polluted environments (and 0.95 in all regions), a decrease in the root mean squared logarithmic error (from 0.57 to 0.43), and removal of ...
Subject code	910
Language	English
Publishing date	2023-10-19
Publishing country	de
Document type	Book ; Online
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Article ; Online: Calibration of a chemical ionization mass spectrometer for the measurement of gaseous sulfuric acid.

Kürten, Andreas / Rondo, Linda / Ehrhart, Sebastian / Curtius, Joachim

The journal of physical chemistry. A

2012 Volume 116, Issue 24, Page(s) 6375–6386

Abstract: The accurate measurement of the gaseous sulfuric acid concentration is crucial within many fields of atmospheric science. Instruments utilizing chemical ionization mass spectrometry (CIMS) measuring H(2)SO(4), therefore, require a careful calibration. We ...

Abstract	The accurate measurement of the gaseous sulfuric acid concentration is crucial within many fields of atmospheric science. Instruments utilizing chemical ionization mass spectrometry (CIMS) measuring H(2)SO(4), therefore, require a careful calibration. We have set up a calibration source that can provide a stable and adjustable concentration of H(2)SO(4). The calibration system initiates the production of sulfuric acid through the oxidation of SO(2) by OH. The hydroxyl radical is produced by UV photolysis of water vapor. A numerical model calculates the H(2)SO(4) concentration provided at the outlet of the calibration source. From comparison of this concentration and the signals measured by CIMS, a calibration factor is derived. This factor is evaluated to be 1.1 × 10(10) cm(-3), which is in good agreement with values found in the literature for other CIMS instruments measuring H(2)SO(4). The calibration system is described in detail and the results are discussed. Because the setup is external to the CIMS instrument, it offers the possibility for future CIMS intercomparison measurements by providing defined and stable concentrations of sulfuric acid.
Language	English
Publishing date	2012-06-21
Publishing country	United States
Document type	Journal Article
ISSN	1520-5215
ISSN (online)	1520-5215
DOI	10.1021/jp212123n
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Article ; Online: The SAMPL5 challenge for embedded-cluster integral equation theory: solvation free energies, aqueous pK

Tielker, Nicolas / Tomazic, Daniel / Heil, Jochen / Kloss, Thomas / Ehrhart, Sebastian / Güssregen, Stefan / Schmidt, K Friedemann / Kast, Stefan M

Journal of computer-aided molecular design

2016 Volume 30, Issue 11, Page(s) 1035–1044

Abstract: We predict cyclohexane-water distribution coefficients (log ... ...

Abstract	We predict cyclohexane-water distribution coefficients (log D
MeSH term(s)	Computer Simulation ; Cyclohexanes/chemistry ; Models, Chemical ; Molecular Structure ; Pharmaceutical Preparations/chemistry ; Quantum Theory ; Solubility ; Solvents/chemistry ; Thermodynamics ; Water/chemistry
Chemical Substances	Cyclohexanes ; Pharmaceutical Preparations ; Solvents ; Water (059QF0KO0R) ; Cyclohexane (48K5MKG32S)
Language	English
Publishing date	2016-08-23
Publishing country	Netherlands
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	808166-9
ISSN	1573-4951 ; 0920-654X
ISSN (online)	1573-4951
ISSN	0920-654X
DOI	10.1007/s10822-016-9939-7
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Book ; Online: Modelling the gas–particle partitioning and water uptake of isoprene-derived secondary organic aerosol at high and low relative humidity

eISSN: 1680-7324

2022

Abstract: This study presents a characterization of the hygroscopic growth behaviour and effects of different inorganic seed particles on the formation of secondary organic aerosols (SOAs) from the dark ozone-initiated oxidation of isoprene at low NO x conditions. ...

Abstract	This study presents a characterization of the hygroscopic growth behaviour and effects of different inorganic seed particles on the formation of secondary organic aerosols (SOAs) from the dark ozone-initiated oxidation of isoprene at low NO x conditions. We performed simulations of isoprene oxidation using a gas-phase chemical reaction mechanism based on the Master Chemical Mechanism (MCM) in combination with an equilibrium gas–particle partitioning model to predict the SOA concentration. The equilibrium model accounts for non-ideal mixing in liquid phases, including liquid–liquid phase separation (LLPS), and is based on the AIOMFAC (Aerosol Inorganic–Organic Mixtures Functional groups Activity Coefficients) model for mixture non-ideality and the EVAPORATION (Estimation of VApour Pressure of ORganics, Accounting for Temperature, Intramolecular, and Non-additivity effects) model for pure compound vapour pressures. Measurements from the Cosmics Leaving Outdoor Droplets (CLOUD) chamber experiments, conducted at the European Organization for Nuclear Research (CERN) for isoprene ozonolysis cases, were used to aid in parameterizing the SOA yields at different atmospherically relevant temperatures, relative humidity (RH), and reacted isoprene concentrations. To represent the isoprene-ozonolysis-derived SOA, a selection of organic surrogate species is introduced in the coupled modelling system. The model predicts a single, homogeneously mixed particle phase at all relative humidity levels for SOA formation in the absence of any inorganic seed particles. In the presence of aqueous sulfuric acid or ammonium bisulfate seed particles, the model predicts LLPS to occur below ∼ 80 % RH, where the particles consist of an inorganic-rich liquid phase and an organic-rich liquid phase; however, this includes significant amounts of bisulfate and water partitioned to the organic-rich phase. The measurements show an enhancement in the SOA amounts at 85 % RH, compared to 35 % RH, for both the seed-free and seeded cases. The model predictions of RH-dependent SOA yield enhancements at 85 % RH vs. 35 % RH are 1.80 for a seed-free case, 1.52 for the case with ammonium bisulfate seed, and 1.06 for the case with sulfuric acid seed. Predicted SOA yields are enhanced in the presence of an aqueous inorganic seed, regardless of the seed type (ammonium sulfate, ammonium bisulfate, or sulfuric acid) in comparison with seed-free conditions at the same RH level. We discuss the comparison of model-predicted SOA yields with a selection of other laboratory studies on isoprene SOA formation conducted at different temperatures and for a variety of reacted isoprene concentrations. Those studies were conducted at RH levels at or below 40 % with reported SOA mass yields ranging from 0.3 % up to 9.0 %, indicating considerable variations. A robust feature of our associated gas–particle partitioning calculations covering the whole RH range is the predicted enhancement of SOA yield at high RH ( > 80 %) compared to low RH (dry) conditions, which is explained by the effect of particle water uptake and its impact on the equilibrium partitioning of all components.
Subject code	660
Language	English
Publishing date	2022-01-07
Publishing country	de
Document type	Book ; Online
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Book ; Online: Temperature uniformity in the CERN CLOUD chamber

Dias, Antonio / Ehrhart, Sebastian / Vogel, Alexander / Williamson, Christina / Almeida, Joao / Kirkby, Jasper / Mathot, Serge / Mumford, Samuel / Onnela, Antti

eISSN: 1867-8548

2017

Abstract: The CLOUD (Cosmics Leaving OUtdoor Droplets) experiment at CERN is studying the nucleation and growth of aerosol particles under atmospheric conditions, and their activation into cloud droplets. A key feature of the CLOUD experiment is precise control of ...

Abstract	The CLOUD (Cosmics Leaving OUtdoor Droplets) experiment at CERN is studying the nucleation and growth of aerosol particles under atmospheric conditions, and their activation into cloud droplets. A key feature of the CLOUD experiment is precise control of the experimental parameters. Temperature uniformity and stability in the chamber are important since many of the processes under study are sensitive to temperature and also to contaminants that can be released from the stainless steel walls by upward temperature fluctuations. The air enclosed within the 3 m CLOUD chamber is equipped with several arrays (<q>strings</q>) of high precision, fast-response thermometers to measure its temperature. Here we present a study of the air temperature uniformity inside the CLOUD chamber under various experimental conditions. Measurements were performed under calibration conditions and run conditions, which are distinguished by the flow rate of fresh air and trace gases entering the chamber: 20 l/min and up to 210 l/min, respectively. During steady-state calibration runs between −70 °C and +20 °C, the air temperature uniformity is better than +/−0.06 °C in the radial direction and +/−0.1 °C in the vertical direction. Larger non-uniformities are present during experimental runs, depending on the temperature control of the make-up air and trace gases (since some trace gases require elevated temperatures until injection into the chamber). The temperature stability is a few times 0.01 °C over periods of several hours during either calibration or steady-state run conditions. During rapid adiabatic expansions to activate cloud droplets and ice particles, the chamber walls are up to 10 °C warmer than the enclosed air. This results in larger non-uniformities while the air returns to its equilibrium temperature with time constant of about 200 s.
Subject code	660
Language	English
Publishing date	2017-05-16
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: Modelling the gas–particle partitioning and water uptake of isoprene-derived secondary organic aerosol at high and low relative humidity

eISSN: 1680-7324

2021

Abstract: This study presents a characterization of the hygroscopic growth behaviour and effects of different inorganic seed particles on the formation of secondary organic aerosols (SOA) from the dark ozone-initiated oxidation of isoprene at low NOx conditions. ... ...

Abstract	This study presents a characterization of the hygroscopic growth behaviour and effects of different inorganic seed particles on the formation of secondary organic aerosols (SOA) from the dark ozone-initiated oxidation of isoprene at low NOx conditions. We performed simulations of isoprene oxidation using a gas-phase chemical reaction mechanism based on the Master Chemical Mechanism (MCM) in combination with an equilibrium gas–particle partitioning model to predict the SOA concentration. The equilibrium model accounts for non-ideal mixing in liquid phases, including liquid–liquid phase separation (LLPS), and is based on the AIOMFAC model for mixture non-ideality and the EVAPORATION model for pure compound vapour pressures. Measurements from the Cosmics Leaving Outdoor Droplets (CLOUD) chamber experiments conducted at the European Organization for Nuclear Research (CERN) for isoprene ozonolysis cases, were used to aid in parameterizing the SOA yields at different atmospherically relevant temperatures, relative humidity (RH) and reacted isoprene concentrations. To represent the isoprene ozonolysis-derived SOA, a selection of organic surrogate species is introduced in the coupled modelling system. The model predicts a single, homogeneously mixed particle phase at all relative humidity levels for SOA formation in the absence of any inorganic seed particles. In the presence of aqueous sulfuric acid or ammonium bisulfate seed particles, the model predicts LLPS to occur below ~80 % RH, where the particles consist of an inorganic-rich liquid phase and an organic-rich liquid phase; however, with significant amounts of bisulfate and water partitioned to the organic-rich phase. The measurements show an enhancement in the SOA amounts at 85 % RH compared to 35 % RH for both the seed-free and seeded cases. The model predictions of RH-dependent SOA yield enhancements at 85 % RH vs. 35 % RH are 1.80 for a seed-free case, 1.52 for the case with ammonium bisulfate seed and 1.06 for the case with sulfuric acid seed. Predicted SOA yields are enhanced in the presence of an aqueous inorganic seed, regardless of the seed type (ammonium sulfate, ammonium bisulfate or sulfuric acid) in comparison with seed-free conditions at the same RH level. We discuss the comparison of model-predicted SOA yields with a selection of other laboratory studies on isoprene SOA formation conducted at different temperatures and for a variety of reacted isoprene concentrations.
Subject code	660
Language	English
Publishing date	2021-04-06
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Article: Comparison of the SAWNUC model with CLOUD measurements of sulphuric acid-water nucleation.

Ehrhart, Sebastian / Ickes, Luisa / Almeida, Joao / Amorim, Antonio / Barmet, Peter / Bianchi, Federico / Dommen, Josef / Dunne, Eimear M / Duplissy, Jonathan / Franchin, Alessandro / Kangasluoma, Juha / Kirkby, Jasper / Kürten, Andreas / Kupc, Agnieszka / Lehtipalo, Katrianne / Nieminen, Tuomo / Riccobono, Francesco / Rondo, Linda / Schobesberger, Siegfried /

Steiner, Gerhard / Tomé, António / Wimmer, Daniela / Baltensperger, Urs / Wagner, Paul E / Curtius, Joachim

Journal of geophysical research. Atmospheres : JGR

2017 Volume 121, Issue 20, Page(s) 12401–12414

Abstract: Binary nucleation of sulphuric acid-water particles is expected to be an important process in the free troposphere at low temperatures. SAWNUC (Sulphuric Acid Water Nucleation) is a model of binary nucleation that is based on laboratory measurements of ... ...

Abstract	Binary nucleation of sulphuric acid-water particles is expected to be an important process in the free troposphere at low temperatures. SAWNUC (Sulphuric Acid Water Nucleation) is a model of binary nucleation that is based on laboratory measurements of the binding energies of sulphuric acid and water in charged and neutral clusters. Predictions of SAWNUC are compared for the first time comprehensively with experimental binary nucleation data from the CLOUD chamber at European Organization for Nuclear Research. The experimental measurements span a temperature range of 208-292 K, sulphuric acid concentrations from 1·10
Language	English
Publishing date	2017-01-30
Publishing country	United States
Document type	Journal Article
ZDB-ID	710256-2
ISSN	2169-8996 ; 2169-897X ; 0148-0227
ISSN (online)	2169-8996
ISSN	2169-897X ; 0148-0227
DOI	10.1002/2015JD023723
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Book ; Online: Evaporation of sulfate aerosols at low relative humidity

eISSN: 1680-7324

2017

Abstract: Evaporation of sulfuric acid from particles can be important in the atmospheres of Earth and Venus. However, the equilibrium constant for the dissociation of H 2 SO 4 to bisulfate ions, which is the one of the fundamental parameters controlling the ... ...

Abstract	Evaporation of sulfuric acid from particles can be important in the atmospheres of Earth and Venus. However, the equilibrium constant for the dissociation of H 2 SO 4 to bisulfate ions, which is the one of the fundamental parameters controlling the evaporation of sulfur particles, is not well constrained. In this study we explore the volatility of sulfate particles at very low relative humidity. We measured the evaporation of sulfur particles versus temperature and relative humidity in the CLOUD chamber at CERN. We modelled the observed sulfur particle shrinkage with the ADCHAM model. Based on our model results, we conclude that the sulfur particle shrinkage is mainly governed by H 2 SO 4 and potentially to some extent by SO 3 evaporation. We found that the equilibrium constants for the dissociation of H 2 SO 4 to HSO 4 − (K H 2 SO 4 ) and the dehydration of H 2 SO 4 to SO 3 ( x K SO 3 ) are K H 2 SO 4 = 2–4 × 10 9 mol kg −1 and x K SO 3 ≥ 1.4 × 10 10 at 288.8 ± 5 K.
Subject code	290 ; 333
Language	English
Publishing date	2017-07-25
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: Measurement-model comparison of stabilized Criegee Intermediate and Highly Oxygenated Molecule production in the CLOUD chamber

Sarnela, Nina / Jokinen, Tuija / Duplissy, Jonathan / Yan, Chao / Nieminen, Tuomo / Ehn, Mikael / Schobesberger, Siegfried / Heinritzi, Martin / Ehrhart, Sebastian / Lehtipalo, Katrianne / Tröstl, Jasmin / Simon, Mario / Kürten, Andreas / Leiminger, Markus / Lawler, Michael Joseph / Rissanen, Matti P. / Bianchi, Federico / Praplan, Arnaud P. / Hakala, Jani /

Amorim, Antonio / Gonin, Marc / Hansel, Armin / Kirkby, Jasper / Dommen, Josef / Curtius, Joachim / Smith, James / Petäjä, Tuukka / Worsnop, Douglas R. / Kulmala, Markku / Donahue, Neil M. / Sipilä, Mikko

eISSN: 1680-7324

2017

Abstract: Atmospheric oxidation is an important phenomenon, which produces large quantities of low-volatile compounds such as sulphuric acid and oxidised organic compounds. Such species may be involved in nucleation of particles and enhance their subsequent growth ...

Abstract	Atmospheric oxidation is an important phenomenon, which produces large quantities of low-volatile compounds such as sulphuric acid and oxidised organic compounds. Such species may be involved in nucleation of particles and enhance their subsequent growth to reach the size of cloud condensation nuclei (CCN). In this study, we investigate α -pinene, the most abundant monoterpene globally, and its oxidation products formed through the ozonolysis in the Cosmic Leaving OUtdoors Droplets (CLOUD) chamber at CERN (the European Organization for Nuclear Research). By scavenging hydroxyl radicals (OH) with hydrogen (H 2 ), we were able to investigate the formation of Highly Oxygenated Molecules (HOM) purely driven by ozonolysis, and study the oxidation of sulphur dioxide (SO 2 ) driven by stabilized Criegee Intermediates (sCI). We measured the concentrations of HOM and sulphuric acid with a chemical ionization atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometer and compared the measured concentrations with simulated concentrations calculated with a dynamic model. We found molar yields in the range of 3.5–6.5 % for the HOM formation and 22–32 % for the formation of stabilized Criegee Intermediates by fitting our model to the measured concentrations. The simulated time evolution of the ozonolysis products was in good agreement with measured concentrations except that in some of the experiments sulphuric acid formation was faster than simulated. The results shown here are consistent with the recently published yields for HOM formation from different laboratory experiments. Together with the sCI yields, these results help to understand atmospheric oxidation processes better and make the reaction parameters more comprehensive for broader use.
Subject code	660
Language	English
Publishing date	2017-09-13
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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