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Atmospheric Measurement Techniques An interactive open-access journal of the European Geosciences Union
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© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 25 Apr 2019

Submitted as: research article | 25 Apr 2019

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Measurement Techniques (AMT).

A new method to quantify mineral dust and other aerosol species from aircraft platforms using single particle mass spectrometry

Karl D. Froyd1,2, Daniel M. Murphy1, Charles A. Brock1, Pedro Campuzano-Jost2,3, Jack E. Dibb4, Jose-Luis Jimenez2,3, Agnieszka Kupc1,5, Ann M. Middlebrook1, Gregory P. Schill1,2, Kenneth L. Thornhill6, Christina J. Williamson1,2, James C. Wilson7, and Luke D. Ziemba8 Karl D. Froyd et al.
  • 1NOAA Earth System Research Laboratory Chemical Sciences Division Boulder, CO, 80305, USA
  • 2Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, 80309, USA
  • 3Department of Chemistry, University of Colorado, Boulder, CO, 80309, USA
  • 4Earth Systems Research Center, Institute for the Study of Earth, Oceans, and Space, University of New Hampshire, Durham, NH, 03824, USA
  • 5Faculty of Physics, University of Vienna, 1090 Vienna, Austria
  • 6NASA Langley Research Center, Science Systems and Applications, Inc., Hampton, VA, 23666, USA
  • 7Department of Mechanical and Materials Engineering, University of Denver, Denver, CO, 80210, USA
  • 8NASA Langley Research Center, Hampton, VA, 23681, USA

Abstract. Single-particle mass spectrometer (SPMS) instruments characterize the composition of individual aerosol particles in real time. Their fundamental ability to differentiate the externally mixed particle types that constitute the atmospheric aerosol population enables a unique perspective into sources and transformation. However, quantitative measurements by SPMS systems are inherently problematic. We introduce a new technique that combines collocated measurements of aerosol composition by SPMS and size-resolved absolute particle concentrations on aircraft platforms. Quantitative number, surface area, volume, and mass concentrations are derived for climate-relevant particle types such as mineral dust, sea salt, and biomass burning smoke. Additionally, relative ion signals are calibrated to derive mass concentrations of internally mixed sulfate and organic material that are distributed across multiple particle types.

The NOAA Particle Analysis by Laser Mass Spectrometry (PALMS) instrument measures size-resolved aerosol chemical composition from aircraft. We describe the identification and quantification of nine major atmospheric particle classes, including sulfate/organic/nitrate mixtures, biomass burning, elemental carbon, sea salt, mineral dust, meteoric material, alkali salts, heavy fuel oil combustion, and a remainder class. Classes can be sub-divided as necessary based on chemical heterogeneity, accumulated secondary material during aging, or other atmospheric processing. Concentrations are derived for sizes that encompass the accumulation and coarse size modes. A statistical error analysis indicates that particle class concentrations can be determined within a few minutes for abundances above ~ 10 ng m−3. Rare particle types require longer sampling times.

We explore the instrumentation requirements and the limitations of the method for airborne measurements. Reducing the size resolution of the particle data increases time resolution with only a modest increase in uncertainty. The principal limiting factor to fast time response concentration measurements is statistically relevant sampling across the size range of interest, in particular, sizes D < 0.2 μm for accumulation mode studies and D > 2 μm for coarse mode analysis. We demonstrate the use of a virtual impactor to enhance sampling statistics for the inherently sparse coarse mode. Performance is compared to other airborne and ground-based composition measurements, and examples of atmospheric mineral dust concentrations are given. The wealth of information afforded by composition-resolved size distributions for all major aerosol types represents a new and powerful tool to characterize atmospheric aerosol properties in a quantitative fashion.

Karl D. Froyd et al.
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Karl D. Froyd et al.
Data sets

ATom: Merged Atmospheric Chemistry, Trace Gases, and Aerosols Wofsy, S.C., S. Afshar, H.M. Allen, E. Apel, E.C. Asher, B. Barletta, J. Bent, H. Bian, B.C. Biggs, D.R. Blake, N. Blake, I. Bourgeois, C.A. Brock, W.H. Brune, J.W. Budney, T.P. Bui, A. Butler, P. Campuzano-Jost, C.S. Chang, M. Chin, R. Commane, G. Correa, J.D. Crounse, P. D. Cullis, B.C. Daube, D.A. Day, J.M. Dean-Day, J.E. Dibb, J.P. DiGangi, G.S. Diskin, M. Dollner, J.W. Elkins, F. Erdesz, A.M. Fiore, C.M. Flynn, K. Froyd, D.W. Gesler, S.R. Hall, T.F. Hanisco, R.A. Hannun, A.J. Hills, E.J. Hintsa, A. Hoffman, R.S. Hornbrook, L.G. Huey, S. Hughes, J.L. Jimenez, B.J. Johnson, J.M. Katich, R.F. Keeling, M.J. Kim, A. Kupc, L.R. Lait, J.-F. Lamarque, J. Liu, K. McKain, R.J. Mclaughlin, S. Meinardi, D.O. Miller, S.A. Montzka, F.L. Moore, E.J. Morgan, D.M. Murphy, L.T. Murray, B.A. Nault, J.A. Neuman, P.A. Newman, J.M. Nicely, X. Pan, W. Paplawsky, J. Peischl, M.J. Prather, D.J. Price, E. Ray, J.M. Reeves, M. Richardson, A.W. Rollins, K.H. Rosenlof, T.B. Ryerson, E. Scheuer, G.P. Schill, J.C. Schroder, J.P. Schwarz, J.M. St.Clair, S.D. Steenrod, B.B. Stephens, S.A. Strode, C. Sweeney, D. Tanner, A.P. Teng, A.B. Thames, C.R. Thompson, K. Ullmann, P.R. Veres, N. Vieznor, N.L. Wagner, A. Watt, R. Weber, B. Weinzierl, P. Wennberg, C.J. Williamson, J.C. Wilson, G.M. Wolfe, C.T. Woods, and L.H. Zeng.

Karl D. Froyd et al.
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Short summary
Single-particle mass spectrometer (SPMS) instruments characterize the composition of individual aerosol particles in real time. We present a new method that combines SPMS composition with independently measured particle size distributions to determine absolute number, surface area, volume, and mass concentrations of mineral dust, biomass burning, sea salt, and other climate-relevant atmospheric particle types, with fast time response applicable to aircraft sampling.
Single-particle mass spectrometer (SPMS) instruments characterize the composition of individual...