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Atmos. Meas. Tech., 11, 195-213, 2018
https://doi.org/10.5194/amt-11-195-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 3.0 License.
Research article
11 Jan 2018
Online differentiation of mineral phase in aerosol particles by ion formation mechanism using a LAAP-TOF single-particle mass spectrometer
Nicholas A. Marsden1, Michael J. Flynn1, James D. Allan1,2, and Hugh Coe1 1School of Earth and Environmental Science, University of Manchester, Manchester, M13 9PL, UK
2National Centre for Atmospheric Science, Manchester, M13 9PL, UK
Abstract. Mineralogy of silicate mineral dust has a strong influence on climate and ecosystems due to variation in physiochemical properties that result from differences in composition and crystal structure (mineral phase). Traditional offline methods of analysing mineral phase are labour intensive and the temporal resolution of the data is much longer than many atmospheric processes. Single-particle mass spectrometry (SPMS) is an established technique for the online size-resolved measurement of particle composition by laser desorption ionisation (LDI) followed by time-of-flight mass spectrometry (TOF-MS). Although non-quantitative, the technique is able to identify the presence of silicate minerals in airborne dust particles from markers of alkali metals and silicate molecular ions in the mass spectra. However, the differentiation of mineral phase in silicate particles by traditional mass spectral peak area measurements is not possible. This is because instrument function and matrix effects in the ionisation process result in variations in instrument response that are greater than the differences in composition between common mineral phases.

In this study, we introduce a novel technique that enables the differentiation of mineral phase in silicate mineral particles by ion formation mechanism measured from subtle changes in ion arrival times at the TOF-MS detector. Using a combination of peak area and peak centroid measurements, we show that the arrangement of the interstitial alkali metals in the crystal structure, an important property in silicate mineralogy, influences the ion arrival times of elemental and molecular ion species in the negative ion mass spectra. A classification scheme is presented that allowed for the differentiation of illite–smectite, kaolinite and feldspar minerals on a single-particle basis. Online analysis of mineral dust aerosol generated from clay mineral standards produced mineral fractions that are in agreement with bulk measurements reported by traditional XRD (X-ray diffraction) analysis.


Citation: Marsden, N. A., Flynn, M. J., Allan, J. D., and Coe, H.: Online differentiation of mineral phase in aerosol particles by ion formation mechanism using a LAAP-TOF single-particle mass spectrometer, Atmos. Meas. Tech., 11, 195-213, https://doi.org/10.5194/amt-11-195-2018, 2018.
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Short summary
Mineralogy of silicate mineral dust has a strong influence on climate and ecosystems due to variation in physiochemical properties that result from differences in composition and crystal structure (mineral phase). Traditional offline methods of analysing mineral phase are labour intensive and the temporal resolution of the data is lost. We introduce a novel technique that enables the online differentiation of mineral phase in silicate particles by single-particle mass spectrometry.
Mineralogy of silicate mineral dust has a strong influence on climate and ecosystems due to...
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