30 May 2024
 | 30 May 2024
Status: this preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).

Viscosity of aqueous ammonium nitrate–organic particles: Equilibrium partitioning may be a reasonable assumption for most tropospheric conditions

Liviana K. Klein, Allan K. Bertram, Andreas Zuend, Florence Gregson, and Ulrich K. Krieger

Abstract. The viscosity of aerosol particles determines the critical mixing time of gas–particle partitioning of volatile compounds in the atmosphere. The partitioning of the semi-volatile ammonium nitrate (NH4NO3) might alter the viscosity of highly viscous secondary organic aerosol particles during their lifetime. In contrast to the viscosity of organic particles, data on the viscosity of internally mixed inorganic–organic aerosol particles are scarce. We determined the viscosity of an aqueous ternary inorganic–organic system consisting of NH4NO3 and a proxy compound for a highly viscous organic, sucrose. Three techniques were applied to cover the atmospherically relevant humidity range: viscometry, fluorescence recovery after photobleaching, and the poke-flow technique. We show that the viscosities of NH4NO3–sucrose–H2O with an organic to inorganic dry mass ratio of 4:1 are four orders of magnitude lower than those of the aqueous sucrose under low humidity conditions (30 % relative humidity (RH), 293 K). By comparing viscosity predictions of mixing rules with those of the AIOMFAC-VISC model, we found that a mixing rule based on mole fractions performs similarly when data from corresponding binary aqueous subsystems are available. Applying this mixing rule, we estimated the characteristic internal mixing time of aerosol particles, indicating significantly faster mixing for inorganic—organic mixtures compared to electrolyte-free particles, especially at lower RH’s. Hence, the assumption in global atmospheric chemistry models of quasi-instantaneous equilibrium gas–particle partitioning is reasonable for internally mixed single-phase particles containing dissolved electrolytes (but not necessarily for phase-separated particles), for most conditions in the planetary boundary layer. This assumption may even hold for the entire troposphere at mid-latitudes and RH > 35 %.

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Liviana K. Klein, Allan K. Bertram, Andreas Zuend, Florence Gregson, and Ulrich K. Krieger

Status: open (until 11 Jul 2024)

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  • RC1: 'Comment on egusphere-2024-1459', Anonymous Referee #1, 06 Jun 2024 reply
Liviana K. Klein, Allan K. Bertram, Andreas Zuend, Florence Gregson, and Ulrich K. Krieger
Liviana K. Klein, Allan K. Bertram, Andreas Zuend, Florence Gregson, and Ulrich K. Krieger


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Short summary
The viscosity of ammonium nitrate–sucrose–H2O was quantified with three methods ranging from liquid to solid state depending on the relative humidity. Moreover, the corresponding estimated internal aerosol mixing times remain below an hour for most tropospheric conditions, making equilibrium partitioning a reasonable assumption.