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

  • Karl D. Froyd (Corresponding author)
  • , Daniel M. Murphy
  • , Charles Brock
  • , Pedro Campuzano-Jost
  • , Jack Dibb
  • , Jose-Luis Jimenez
  • , Agnieszka Kupc
  • , Ann M. Middlebrook
  • , Gregory P. Schill
  • , Kenneth L. Thornhill
  • , Christina J. Williamson
  • , James C. Wilson
  • , Luke D. Ziemba

Publications: Contribution to journalArticlePeer Reviewed

Abstract

Single-particle mass spectrometry (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 similar to 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 mu m for accumulation-mode studies and D > 2 mu m for coarse-mode analysis. 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.

Original languageEnglish
Pages (from-to)6209–6239
Number of pages31
JournalAtmospheric Measurement Techniques
Volume12
Issue number11
DOIs
Publication statusPublished - 27 Nov 2019

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

  1. SDG 13 - Climate Action
    SDG 13 Climate Action

Austrian Fields of Science 2012

  • 104026 Spectroscopy
  • 103039 Aerosol physics

Keywords

  • ATMOSPHERIC AEROSOL
  • CHEMICAL-COMPOSITION
  • COMPLEX REFRACTIVE-INDEX
  • DYNAMIC SHAPE FACTORS
  • EFFECTIVE DENSITY
  • MIXING STATE
  • OPTICAL-PROPERTIES
  • REAL-TIME ANALYSIS
  • SECONDARY ORGANIC AEROSOL
  • SIZE DISTRIBUTION

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