Evaporation of sulfate aerosols at low relative humidity

Tsagkogeorgas, Georgios; Roldin, Pontus; Duplissy, Jonathan; Rondo, Linda; Tröstl, Jasmin; Slowik, Jay G.; Ehrhart, Sebastian; Franchin, Alessandro; Kürten, Andreas; Amorim, A.; Bianchi, Federico; Kirkby, J.; Petäj̈ä, Tuukka; Baltensperger, Urs; Boy, Michael; Curtius, Joachim; Flagan, Richard C.; Kulmala, Markku; Donahue, Neil M.; Stratmann, Frank

doi:10.5194/acp-17-8923-2017

Cited by 16 publications

(11 citation statements)

References 83 publications

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“…The saturation vapour pressures of HOMs were calculated using SIM-POL (Pankow and Asher, 2008) as the method of Nanoolal et al (2008) produces unrealistic estimates of vapour pressures for multifunctional HOMs containing hydroperoxide or a peroxy acid group (Kurteìn et al, 2016). H 2 SO 4 was treated as a non-volatile condensing vapour, which generally is a reasonable assumption at typical atmospheric relative humidity and NH 3 levels (Tsagkogeorgas et al, 2017). The coagulation process, dry deposition process, and the dilution of aerosol number concentration caused by boundary layer evolution were estimated in the model as well.…”

Section: Model Descriptionsmentioning

confidence: 99%

Modelling studies of HOMs and their contributions to new particle formation and growth: comparison of boreal forest in Finland and a polluted environment in China

Ding

Roldin

et al. 2018

Atmos. Chem. Phys.

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Abstract. Highly oxygenated multifunctional compounds (HOMs) play a key role in new particle formation (NPF), but their quantitative roles in different environments of the globe have not been well studied yet. Frequent NPF events were observed at two "flagship" stations under different environmental conditions, i.e. a remote boreal forest site (SMEAR II) in Finland and a suburban site (SORPES) in polluted eastern China. The averaged formation rate of 6 nm particles and the growth rate of 6-30 nm particles were 0.3 cm −3 s −1 and 4.5 nm h −1 at SMEAR II compared to 2.3 cm −3 s −1 and 8.7 nm h −1 at SORPES, respectively. To explore the differences of NPF at the two stations, the HOM concentrations and NPF events at two sites were simulated with the MALTE-BOX model, and their roles in NPF and particle growth in the two distinctly different environments are discussed. The model provides an acceptable agreement between the simulated and measured concentrations of sulfuric acid and HOMs at SMEAR II. The sulfuric acid and HOM organonitrate concentrations are significantly higher but other HOM monomers and dimers from monoterpene oxidation are lower at SORPES compared to SMEAR II. The model simulates the NPF events at SMEAR II with a good agreement but underestimates the growth of new particles at SORPES, indicating a dominant role of anthropogenic processes in the polluted environment. HOMs from monoterpene oxidation dominate the growth of ultrafine particles at SMEAR II while sulfuric acid and HOMs from aromatics oxidation play a more important role in particle growth. This study highlights the distinct roles of sulfuric acid and HOMs in NPF and particle growth in different environmental conditions and suggests the need for molecular-scale measurements in improving the understanding of NPF mechanisms in polluted areas like eastern China.

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Section: Model Descriptionsmentioning

confidence: 99%

Modelling studies of HOMs and their contributions to new particle formation and growth: comparison of boreal forest in Finland and a polluted environment in China

Ding

Roldin

et al. 2018

Atmos. Chem. Phys.

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“…Furthermore, NPF was found to be an important process inside the convective outflows (e.g. Twohy et al, 2002;Waddicor et al, 2012). From measurements in the upper troposphere it is commonly assumed that the occurrence of NPF is directly connected to deep-convective cloud systems (e.g.…”

Section: Introductionmentioning

confidence: 99%

In situ observation of new particle formation (NPF) in the tropical tropopause layer of the 2017 Asian monsoon anticyclone – Part 2: NPF inside ice clouds

et al. 2021

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Abstract. From 27 July to 10 August 2017, the airborne StratoClim mission took place in Kathmandu, Nepal, where eight mission flights were conducted with the M-55 Geophysica up to altitudes of 20 km. New particle formation (NPF) was identified by the abundant presence of nucleation-mode aerosols, with particle diameters dp smaller than 15 nm, which were in-situ-detected by means of condensation nuclei (CN) counter techniques. NPF fields in clear skies as well as in the presence of cloud ice particles (dp > 3 µm) were encountered at upper troposphere–lowermost stratosphere (UTLS) levels and within the Asian monsoon anticyclone (AMA). NPF-generated nucleation-mode particles in elevated concentrations (Nnm) were frequently found together with cloud ice (in number concentrations Nice of up to 3 cm−3) at heights between ∼ 11 and 16 km. From a total measurement time of ∼ 22.5 h above 10 km altitude, in-cloud NPF was in sum detected over ∼ 1.3 h (∼ 50 % of all NPF records throughout StratoClim). Maximum Nnm of up to ∼ 11 000 cm−3 was detected coincidently with intermediate ice particle concentrations Nice of 0.05–0.1 cm−3 at comparatively moderate carbon monoxide (CO) contents of ∼ 90–100 nmol mol−1. Neither under clear-sky nor during in-cloud NPF do the highest Nnm concentrations correlate with the highest CO mixing ratios, suggesting that an elevated pollutant load is not a prerequisite for NPF. Under clear-air conditions, NPF with elevated Nnm (> 8000 cm−3) occurred slightly less often than within clouds. In the presence of cloud ice, NPF with Nnm between 1500–4000 cm−3 was observed about twice as often as under clear-air conditions. NPF was not found when ice water contents exceeded 1000 µmol mol−1 in very cold air (< 195 K) at tropopause levels. This indicates a reduction in NPF once deep convection is prevalent together with the presence of mainly liquid-origin ice particles. Within in situ cirrus near the cold point tropopause, recent NPF or intense events with mixing ration nnm larger than 5000 mg−1 were observed only in about 6 % of the in-cloud NPF data. In determining whether the cloud-internal NPF is attenuated or prevented by the microphysical properties of cloud elements, the integral radius (IR) of the ice cloud population turned out to be indicative. Neither the number of ice particles nor the free distance between the ice particles is clearly related to the NPF rate detected. While the increase in ice particles' mass per time dmdt is proportional to the IR and mainly due to the condensation of water vapour, additional condensation of NPF precursors proceeds at the expense of the NPF rate as the precursor's saturation ratio declines. Numerical simulations show the impact of the IR on the supersaturation of a condensable vapour, such as sulfuric acid, and furthermore illustrate that the IR of the cloud ice determines the effective limitation of NPF rates.

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“…Based on the expression formulated by Tsagkogeorgas et al (2017) with the saturation vapour pressure psat of H2SO4 (above a flat surface) and with an accommodation coefficient of α = 0.65 (Pöschl et al, 1998), the ice particle's change of mass m per time unit is calculated by: In Figure B-1 the variability of two aspects is considered and in the panels (a-c) it is distinguished between three ice particle radii (1 µm, 10 µm, and 100 µm) and two different ice particle number concentrations (0.01 and 0.1 cm -3 ). The study by Ueyama et al (2020) revealed that ice particles (effective radii of about 15 µm) persist over 12 to 20 hours at convective outflow levels between 365 K and 370 K potential temperature in the 2017 AMA.…”

Section: Appendix B: Impact Of Ice Particles On Npf Precursors' Saturmentioning

confidence: 99%

New particle formation inside ice clouds: In-situ observations in the tropical tropopause layer of the 2017 Asian Monsoon Anticyclone

Weigel

Mahnke

Baumgartner

et al. 2021

Preprint

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Abstract. From 27 July to 10 August 2017 the airborne StratoClim mission took place in Kathmandu, Nepal where eight mission flights were conducted with the M-55 Geophysica up to altitudes of 20 km. New Particle Formation (NPF) was identified by the abundant presence of ultrafine aerosols, with particle diameters dp smaller than 15 nm, which were in-situ detected by means of condensation nuclei counting techniques. NPF fields in clear-skies as well as in the presence of cloud ice particles (dp > 3 µm) were encountered at upper troposphere/lowermost stratosphere (UT/LS) levels and within the Asian Monsoon Anticyclone (AMA). NPF-generated ultrafine particles in elevated concentrations (Nuf) were frequently found together with cloud ice (in number concentrations Nice of up to 3 cm−3) at heights between ~ 11 km and 16 km. From a total measurement time of ~ 22.5 hours above 10 km altitude, in-cloud NPF was in sum detected over ~ 1.3 hours (~ 50 % of all NPF records throughout StratoClim). Maximum Nuf of up to ~ 11000 cm−3 were detected coincidently with intermediate ice particle concentrations Nice of 0.05–0.1 cm−3 at comparatively moderate carbon monoxide (CO) contents of ~ 90–100 nmol mol−1. Neither under clear-sky nor during in-cloud NPF do the highest Nuf concentrations correlate with the highest CO mixing ratios, suggesting that an elevated pollutant load is not a prerequisite for NPF. Under clear-air conditions, NPF with elevated Nuf (> 8000 cm−3) occurred slightly less often than within clouds. In the presence of cloud ice, NPF with Nuf between 1500–4000 cm−3 were observed about twice as often as under clear air conditions. When ice water contents exceeded 1000 µmol mol−1 in very cold air ( 5000 mg−1) were rarely observed (~ 6 % of in-cloud NPF data). For specifying the constraining mechanisms for NPF possibly imposed by the microphysical properties of the cloud elements, the integral radius (IR) of the ice cloud population was identified as the most practicable indicator. Neither of both, the number of ice particles or the free distance between the ice particles, is clearly related to the NPF-rate detected. The results of a numerical simulation indicates how the IR affects the supersaturation of a condensable vapour, such as sulphuric acid, and that IR determines the effective limitation of NPF rates due to cloud ice.

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Evaporation of sulfate aerosols at low relative humidity

Cited by 16 publications

References 83 publications

Modelling studies of HOMs and their contributions to new particle formation and growth: comparison of boreal forest in Finland and a polluted environment in China

Modelling studies of HOMs and their contributions to new particle formation and growth: comparison of boreal forest in Finland and a polluted environment in China

In situ observation of new particle formation (NPF) in the tropical tropopause layer of the 2017 Asian monsoon anticyclone – Part 2: NPF inside ice clouds

New particle formation inside ice clouds: In-situ observations in the tropical tropopause layer of the 2017 Asian Monsoon Anticyclone

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