A dual-droplet approach for measuring the hygroscopicity of aqueous aerosol

Accurate characterization of the water activity and hygroscopicity of aqueous aerosol material allows us to predict the chemical and physical state of aerosol particles exposed to humid conditions in the environment. The hygroscopicity of aerosol determines the size, phase morphology, viscosity, chemical reactivity, and optical properties of constituent particles and directly impacts their ability to form clouds in the atmosphere. In this work, we describe measurements of hygroscopicity using a linear quadrupole electrodynamic balance (LQ-EDB). We levitate two droplets, one droplet that acts as a relative humidity (RH) probe and one sample droplet, and expose them to controlled environmental conditions. We describe the development of an RH measurement using probe droplets of aqueous NaCl or LiCl, allowing for precise in situ measurements of RH in the LQ-EDB chamber. We demonstrate that the RH may be determined with an accuracy of 0.5 % at 50 % RH and better than 0.1 % at 90 % RH using NaCl, and we show that LiCl is effective at characterizing the RH from ∼ 10 % RH up to ∼ 90 %. We simultaneously measure the response of sample droplets containing aqueous material (including ammonium sulfate, citric acid, 1,2,6-hexanetriol, and tetra-ethylene glycol) and report hygroscopic growth via their radial growth factors. We use established thermodynamic models to validate the accuracy of the RH probe and to compare with the measured hygroscopicity of the samples. This approach shows significant advantages over other methods for accurately characterizing the hygroscopicity of samples with a range of characteristics, such as high viscosity and vapor pressure.

A Dual-Droplet Approach for Measuring the Hygroscopicity of Aqueous Aerosol

Accurate characterization of the water activity and hygroscopicity of aqueous aerosol material allows us to predict the chemical and physical state of aerosol particles exposed to humid conditions in the environment. The hygroscopicity of aerosol determines the size, phase morphology, viscosity, chemical reactivity, and optical properties of constituent particles, and directly impacts their ability to form clouds in the atmosphere. In this work, we describe measurements of hygroscopicity using a linear quadrupole electrodynamic balance (LQ-EDB). We levitate two droplets, one droplet that acts as a relative humidity (RH) probe and one sample droplet, and expose them to controlled environmental conditions. We describe the development of a RH measurement using probe droplets of aqueous NaCl or LiCl, allowing for precise in-situ measurements of RH in the LQ-EDB chamber. We demonstrate that the RH may be determined with an accuracy of 0.5 % at 50 % RH and better than 0.1 % at 90 % RH using NaCl, and show that LiCl is effective at characterizing the RH from ~10 % RH up to ~90 %. We simultaneously measure the response of sample droplets containing aqueous material (including ammonium sulfate, citric acid, 1,2,6-hexanetriol, and tetraethylene glycol) and report hygroscopic growth via their radial growth factors. We use established thermodynamic models to validate the accuracy of the RH probe and to compare with the measured hygroscopicity of the samples. This approach shows significant advantages over other methods for accurately characterizing the hygroscopicity of samples with a range of characteristics, such as high viscosity and vapor pressure.

Multicomponent diffusion in atmospheric aerosol particles

Condensed phase mass transport in single aerosol particles is investigated using a linear quadrupole electrodynamic balance (LQ-EDB) and the Maxwell–Stefan (MS) framework.

Effect of ammonium salts on the photochemical degradation of iron containing organic aerosol

<p>Formation of organic aerosol by oxidation of gas phase compounds has been intensely studied, and is much better understood than the aerosol ageing transformations during the lifetime of organic aerosol. Aerosol ageing influences how those aerosol particles affect climate and human health and is still not well constrained in current models.</p><p>Photochemistry in the condensed phase is an important mechanism responsible for ageing of organic aerosol. In the lower troposphere, where UV light intensity with sufficiently low wavelength to directly photolyze aerosol components is low, indirect photochemistry (catalyzing redox processes of non-absorbing molecules) is especially relevant. Recently we studied transition metal complex photochemistry in single particles levitated in an electrodynamic balance. In particular, we investigated the aqueous iron(III)-citrate/citric acid system and found that irradiation at 473 nm led to rapid and significant degradation of the citric acid. Up to 80% of the initial particle mass was partitioned to the gas phase with the degradation rate depending on kinetic transport limitations of oxygen. These kinetic limitations arise are influenced strongly by the relative humidity dependence of particle viscosity where water acts as a plasticizer.</p><p>Here we will report on photochemical degradation experiments adding various salts in different (ammonium sulfate, ammonium bisulfate, etc.) to the reference system iron(III)-citrate/citric acid. Preliminary experiments suggest that pH of the aerosol particle influences the degradation rate in this system significantly.</p>

Water diffusion measurements of single charged aerosols using H2O/D2O isotope exchange and Raman spectroscopy in an electrodynamic balance

We report water diffusion measurements on single charged aerosols using isotope exchange in an electrodynamic balance.