Optimized instrument configurations for tandem particle mass analyzer and single particle-soot photometer experiments

2021 ◽  
pp. 105897
Author(s):  
A. Naseri ◽  
T.A. Sipkens ◽  
S.N. Rogak ◽  
J.S. Olfert
2012 ◽  
Vol 5 (5) ◽  
pp. 1031-1043 ◽  
Author(s):  
M. Laborde ◽  
P. Mertes ◽  
P. Zieger ◽  
J. Dommen ◽  
U. Baltensperger ◽  
...  

Abstract. Black carbon (BC) is now mainly of anthropogenic origin. It is the dominant light absorbing component of atmospheric aerosols, playing an important role in the earth's radiative balance and therefore relevant to climate change studies. In addition, BC is known to be harmful to human beings making it relevant to policy makers. Nevertheless, the measurement of BC remains biased by the instrument-based definition of BC. The Single Particle Soot Photometer (SP2), allows the measurement of the refractory BC (rBC) mass of individual particles using laser-induced incandescence. However, the SP2 needs an empirical calibration to retrieve the rBC mass from the incandescence signal and the sensitivity of the SP2 differs between different BC types. Ideally, for atmospheric studies, the SP2 should be calibrated using ambient particles containing a known mass of ambient rBC. However, such "ambient BC" calibration particles cannot easily be obtained and thus commercially available BC particles are commonly used for SP2 calibration instead. In this study we tested the sensitivity of the SP2 to different BC types in order to characterize the potential error introduced by using non-ambient BC for calibration. The sensitivity of the SP2 was determined, using an aerosol particle mass analyzer, for rBC from thermodenuded diesel exhaust, wood burning exhaust and ambient particles as well as for commercially available products: Aquadag® and fullerene soot. Thermodenuded, fresh diesel exhaust has been found to be ideal for SP2 calibration for two reasons. First, the small amount of non-BC matter upon emission reduces the risk of bias due to incomplete removal of non-BC matter and second, it is considered to represent atmospheric rBC in urban locations where diesel exhaust is the main source of BC. The SP2 was found to be up to 16% less sensitive to rBC from thermodenuded ambient particles (≤15 fg) than rBC from diesel exhaust, however, at least part of this difference can be explained by incomplete removal of non-refractory components in the thermodenuder. The amount of remaining non-refractory matter was estimated to be below 30% by mass, according to a comparison of the scattering cross sections of the whole particles with that of the pure BC cores. The SP2 sensitivity to rBC from wood burning exhaust agrees with the SP2 sensitivity to rBC from diesel exhaust within an error of less than 14% (≤40 fg). If, due to experimental restrictions, diesel exhaust cannot be used, untreated fullerene soot was found to give an SP2 calibration curve similar to diesel exhaust and ambient rBC (within ±10% for a rBC mass ≤15 fg) and is therefore recommended although two different batches differed by ~14% between themselves. In addition, the SP2 was found to be up to 40% more sensitive to Aquadag® than to diesel exhaust rBC. Therefore Aquadag® cannot be recommended for atmospheric application without accounting for the sensitivity difference. These findings for fullerene soot and Aquadag® confirm results from previous literature.


2011 ◽  
Vol 102 (1-2) ◽  
pp. 49-56 ◽  
Author(s):  
Elmar Gelhausen ◽  
Klaus-Peter Hinz ◽  
Andres Schmidt ◽  
Bernhard Spengler

2012 ◽  
Vol 12 (4) ◽  
pp. 1681-1700 ◽  
Author(s):  
R. M. Healy ◽  
J. Sciare ◽  
L. Poulain ◽  
K. Kamili ◽  
M. Merkel ◽  
...  

Abstract. An Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed to investigate the size-resolved chemical composition of single particles at an urban background site in Paris, France, as part of the MEGAPOLI winter campaign in January/February 2010. ATOFMS particle counts were scaled to match coincident Twin Differential Mobility Particle Sizer (TDMPS) data in order to generate hourly size-resolved mass concentrations for the single particle classes observed. The total scaled ATOFMS particle mass concentration in the size range 150–1067 nm was found to agree very well with the sum of concurrent High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and Multi-Angle Absorption Photometer (MAAP) mass concentration measurements of organic carbon (OC), inorganic ions and black carbon (BC) (R2 = 0.91). Clustering analysis of the ATOFMS single particle mass spectra allowed the separation of elemental carbon (EC) particles into four classes: (i) EC attributed to biomass burning (ECbiomass), (ii) EC attributed to traffic (ECtraffic), (iii) EC internally mixed with OC and ammonium sulfate (ECOCSOx), and (iv) EC internally mixed with OC and ammonium nitrate (ECOCNOx). Average hourly mass concentrations for EC-containing particles detected by the ATOFMS were found to agree reasonably well with semi-continuous quantitative thermal/optical EC and optical BC measurements (r2 = 0.61 and 0.65–0.68 respectively, n = 552). The EC particle mass assigned to fossil fuel and biomass burning sources also agreed reasonably well with BC mass fractions assigned to the same sources using seven-wavelength aethalometer data (r2 = 0.60 and 0.48, respectively, n = 568). Agreement between the ATOFMS and other instrumentation improved noticeably when a period influenced by significantly aged, internally mixed EC particles was removed from the intercomparison. 88% and 12% of EC particle mass was apportioned to fossil fuel and biomass burning respectively using the ATOFMS data compared with 85% and 15% respectively for BC estimated from the aethalometer model. On average, the mass size distribution for EC particles is bimodal; the smaller mode is attributed to locally emitted, mostly externally mixed EC particles, while the larger mode is dominated by aged, internally mixed ECOCNOx particles associated with continental transport events. Periods of continental influence were identified using the Lagrangian Particle Dispersion Model (LPDM) "FLEXPART". A consistent minimum between the two EC mass size modes was observed at approximately 400 nm for the measurement period. EC particles below this size are attributed to local emissions using chemical mixing state information and contribute 79% of the scaled ATOFMS EC particle mass, while particles above this size are attributed to continental transport events and contribute 21% of the EC particle mass. These results clearly demonstrate the potential benefit of monitoring size-resolved mass concentrations for the separation of local and continental EC emissions. Knowledge of the relative input of these emissions is essential for assessing the effectiveness of local abatement strategies.


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