Conditional Sampling for Source-Oriented Toxicological Studies Using a Single Particle Mass Spectrometer

2009 ◽  
Vol 43 (24) ◽  
pp. 9445-9452 ◽  
Author(s):  
K. J. Bein ◽  
Y. Zhao ◽  
A. S. Wexler
Keyword(s):  
Mass Spectrometer ◽  
Single Particle ◽  
Particle Mass ◽  
Conditional Sampling ◽  
Toxicological Studies

scholarly journals Sources and mixing state of size-resolved elemental carbon particles in a European megacity: Paris

2012 ◽  
Vol 12 (4) ◽  
pp. 1681-1700 ◽  
Author(s):  
R. M. Healy ◽  
J. Sciare ◽  
L. Poulain ◽  
K. Kamili ◽  
M. Merkel ◽  
...  
Keyword(s):  
Mass Spectrometer ◽  
Biomass Burning ◽  
Single Particle ◽  
Mass Concentration ◽  
Elemental Carbon ◽  
Fossil Fuel ◽  
Time Of Flight ◽  
Particle Mass ◽  
Mass Size ◽  
Mass Concentrations

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.

scholarly journals Quantitative single particle analysis with the Aerodyne aerosol mass spectrometer: development of a new classification algorithm and its application to field data

2013 ◽  
Vol 6 (3) ◽  
pp. 5653-5691 ◽  
Author(s):  
F. Freutel ◽  
F. Drewnick ◽  
J. Schneider ◽  
T. Klimach ◽  
S. Borrmann
Keyword(s):  
Mass Spectrometer ◽  
Single Particle ◽  
Field Data ◽  
Classification Algorithm ◽  
Particle Mass ◽  
Submicron Particles ◽  
Particle Analysis ◽  
Mixing State ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass

Abstract. Single particle mass spectrometry has proven a valuable tool for gaining information on the mixing state of aerosol particles. With the Aerodyne aerosol mass spectrometer (AMS) equipped with a light scattering probe, non-refractory components of submicron particles with diameters larger than about 300 nm can even be quantified on a single particle basis. Here, we present a new method for the analysis of AMS single particle mass spectra. The developed algorithm classifies the particles according to their components (e.g., sulphate, nitrate, different types of organics) and simultaneously provides quantitative information about the composition of the single particles. This classification algorithm was validated by applying it to data acquired in laboratory experiments with particles of known composition, and applied to field data acquired during the MEGAPOLI summer campaign (July 2009) in Paris. As shown, it is not only possible to directly measure the mixing state of atmospheric particles, but also to directly observe repartitioning of semi-volatile species between gas and particle phase during the course of the day.

scholarly journals Single particle diversity and mixing state measurements

2014 ◽  
Vol 14 (12) ◽  
pp. 6289-6299 ◽  
Author(s):  
R. M. Healy ◽  
N. Riemer ◽  
J. C. Wenger ◽  
M. Murphy ◽  
M. West ◽  
...  
Keyword(s):  
Species Diversity ◽  
Ammonium Nitrate ◽  
Black Carbon ◽  
Mass Spectrometer ◽  
Single Particle ◽  
Organic Aerosol ◽  
Particle Mass ◽  
Mixing State ◽  
Mass Fractions ◽  
State Index

Abstract. A newly developed framework for quantifying aerosol particle diversity and mixing state based on information-theoretic entropy is applied for the first time to single particle mass spectrometry field data. Single particle mass fraction estimates for black carbon, organic aerosol, ammonium, nitrate and sulfate, derived using single particle mass spectrometer, aerosol mass spectrometer and multi-angle absorption photometer measurements are used to calculate single particle species diversity (Di). The average single particle species diversity (Dα) is then related to the species diversity of the bulk population (Dγ) to derive a mixing state index value (χ) at hourly resolution. The mixing state index is a single parameter representation of how internally/externally mixed a particle population is at a given time. The index describes a continuum, with values of 0 and 100% representing fully external and internal mixing, respectively. This framework was applied to data collected as part of the MEGAPOLI winter campaign in Paris, France, 2010. Di values are low (~ 2) for fresh traffic and wood-burning particles that contain high mass fractions of black carbon and organic aerosol but low mass fractions of inorganic ions. Conversely, Di values are higher (~ 4) for aged carbonaceous particles containing similar mass fractions of black carbon, organic aerosol, ammonium, nitrate and sulfate. Aerosol in Paris is estimated to be 59% internally mixed in the size range 150–1067 nm, and mixing state is dependent both upon time of day and air mass origin. Daytime primary emissions associated with vehicular traffic and wood-burning result in low χ values, while enhanced condensation of ammonium nitrate on existing particles at night leads to higher χ values. Advection of particles from continental Europe containing ammonium, nitrate and sulfate leads to increases in Dα, Dγ and χ. The mixing state index represents a useful metric by which to compare and contrast ambient particle mixing state at other locations globally.

scholarly journals Quantitative single-particle analysis with the Aerodyne aerosol mass spectrometer: development of a new classification algorithm and its application to field data

2013 ◽  
Vol 6 (11) ◽  
pp. 3131-3145 ◽  
Author(s):  
F. Freutel ◽  
F. Drewnick ◽  
J. Schneider ◽  
T. Klimach ◽  
S. Borrmann
Keyword(s):  
Mass Spectrometer ◽  
Single Particle ◽  
Field Data ◽  
Classification Algorithm ◽  
Particle Mass ◽  
Submicron Particles ◽  
Particle Analysis ◽  
Mixing State ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass

Abstract. Single-particle mass spectrometry has proven a valuable tool for gaining information on the mixing state of aerosol particles. With the Aerodyne aerosol mass spectrometer (AMS) equipped with a light-scattering probe, non-refractory components of submicron particles with diameters larger than about 300 nm can even be quantified on a single-particle basis. Here, we present a new method for the analysis of AMS single-particle mass spectra. The developed algorithm classifies the particles according to their components (e.g. sulphate, nitrate, different types of organics) and simultaneously provides quantitative information about the composition of the single particles. This classification algorithm was validated by applying it to data acquired in laboratory experiments with particles of known composition, and applied to field data acquired during the MEGAPOLI summer campaign (July 2009) in Paris. As shown, it is not only possible to directly measure the mixing state of atmospheric particles, but also to directly observe repartitioning of semi-volatile species between gas and particle phase during the course of the day.

Characterization of surgical aerosols by the compact single-particle mass spectrometer LAMPAS 3

2011 ◽  
Vol 401 (10) ◽  
pp. 3165-3172 ◽  
Author(s):  
K.-P. Hinz ◽  
E. Gelhausen ◽  
K.-C. Schäfer ◽  
Z. Takats ◽  
B. Spengler
Keyword(s):  
Mass Spectrometer ◽  
Single Particle ◽  
Particle Mass
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