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Characterization of a bipolar near-infrared laser desorption/ionization aerosol mass spectrometer

Kenseth, Christopher M. and Petrucci, Giuseppe A. (2016) Characterization of a bipolar near-infrared laser desorption/ionization aerosol mass spectrometer. Aerosol Science and Technology, 50 (8). pp. 790-801. ISSN 0278-6826. http://resolver.caltech.edu/CaltechAUTHORS:20160811-152001424

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Abstract

A novel method of soft ionization aerosol mass spectrometry (AMS), bipolar near-infrared laser desorption/ionization AMS (BP-NIR-LDI-AMS), has been developed for the on-line, real-time analysis of organic aerosols. Use of a single NIR laser pulse to desorb/ionize aerosols deposited onto an aluminum probe results in minimal analyte fragmentation to produce exclusively intact pseudomolecular ions at [M–H]^− for acidic organic analytes and [M+H]^+ for basic organic analytes. Incorporation of a bipolar mass spectrometer with the NIR-LDI source enables simultaneous detection of acidic and basic species in organic particles. Limits of detection (total particulate mass sampled) for amino acids common to the organic fraction of atmospheric aerosols ranged from 69.1 pg for ornithine to 197 pg for serine on the positive channel, and from 17.0 pg for glycine to 100 pg for ornithine on the negative channel. From studies of the laser energy dependence of the NIR-LDI mechanism, it was found that [M–H]^− formation for oleic acid proceeds through simultaneous action of two 1064 nm photons, suggesting a surface-assisted process rather than direct photoionization, for which photon energy is insufficient. For acidic aerosol species, sensitivity was found to increase as a function of analyte acidity, while for basic species, [M+H]^+ ion signals were detected only in the presence of a labile proton source, with the intensity of the ion signals scaling with the acidity of the proton source. The sensitivity of BP-NIR-LDI-AMS to the amino acids was rationalized in terms of their acidic/basic character, as measured by isoelectric point (pI), with the cationic sensitivity scaling proportionally with pI and the anionic sensitivity scaling inversely with pI.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1080/02786826.2016.1189074DOIArticle
http://www.tandfonline.com/doi/full/10.1080/02786826.2016.1189074PublisherArticle
Additional Information:© 2016 American Association for Aerosol Research. Received 23 January 2016. Accepted 26 April 2016. EDITOR: Paul J. Ziemann. The authors thank Shashank Jain for useful discussion. Financial support for this work was provided by the National Science Foundation (Grants NSF-1101194 and NSF-1213632).
Funders:
Funding AgencyGrant Number
NSFNSF-1101194
NSFNSF-1213632
Record Number:CaltechAUTHORS:20160811-152001424
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20160811-152001424
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:69573
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:11 Aug 2016 23:24
Last Modified:11 Aug 2016 23:24

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