A novel inversion method to calculate the mass fraction of coated refractory black carbon using a centrifugal particle mass analyzer and single particle soot photometer
Abstract
Refractory black carbon (rBC) has important atmospheric impacts due to its ability to absorb light, and its interactions with light are partly governed by the acquisition of coatings or other mixing processes. Here, a novel inversion method is presented which derives the mass fraction of coated rBC using a coupled centrifugal particle mass analyzer (CPMA) and single particle soot photometer (SP2). The CPMA selects particles of a known mass-to-charge ratio, and the SP2 detects the mass of rBC in each individual particle. The results of the inversion are the simultaneous number distributions of both rBC mass and total particle mass. Practically, the distribution can be integrated to find properties of the total aerosol population, for example, i) mass fraction of coating and ii) mass of coating on a particle of known total mass. This was demonstrated via smog chamber experiments. Initially, particles in the chamber were pure rBC, produced from a methane burner and passed through a diffusion dryer and thermal denuder. An organic (non-rBC) coating was then grown onto the aerosol over several hours via photooxidation with p-xylene. The CPMA-SP2 coupled system sampled the aerosol over the reaction period as the coating grew. The CPMA was sequentially stepped over a mass range from 0.3 to 28 fg and the SP2 measured the mass of rBC in each individual CPMA-classified particle. The number and mass distributions were constructed using the inversion. As expected, the mass and number distributions of rBC and total mass were equivalent for uncoated particles. As the non-rBC coating thickness increased over time, a shift in the number distribution towards higher total mass was observed. At the end of the experiment, fresh rBC (i.e. uncoated, bare particles) was injected into the chamber, creating an external mixture of coated and uncoated particles. This external mixture was clearly resolved in the number distribution of rBC and total particle mass. It is expected that the CPMA-SP2 methodology and inversion technique would be useful for field measurements where the rBC mass fraction, and mixing state of rBC-containing particles, could be accurately measured continuously. This methodology is not limited to evaluating coating mass—unlike SP2 only methods, it gives an unambiguous measure of any non-rBC material mixed with the particle.
- Publication:
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AGU Fall Meeting Abstracts
- Pub Date:
- December 2016
- Bibcode:
- 2016AGUFM.A51H0160I
- Keywords:
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- 0305 Aerosols and particles;
- ATMOSPHERIC COMPOSITION AND STRUCTUREDE: 3311 Clouds and aerosols;
- ATMOSPHERIC PROCESSESDE: 3337 Global climate models;
- ATMOSPHERIC PROCESSESDE: 3275 Uncertainty quantification;
- MATHEMATICAL GEOPHYSICS