Spatially resolved chemical imaging of individual atmospheric particles using nanoscale imaging mass spectrometry: insight into particle origin and chemistry
Abstract
Knowledge of the spatially resolved composition of atmospheric particles is essential for differentiating between their surface versus bulk chemistry and understanding particle reactivity and the potential environmental impact. Here, we demonstrate the application of nanometer-scale secondary ion mass spectrometry (CAMECA NanoSIMS 50 ion probe) for 3D chemical imaging of individual atmospheric particles without any sample pre-treatment, such as sectioning of particles. Use of NanoSIMS depth profile analysis enables elemental mapping of particles with nanometer spatial resolution over a broad range of particle sizes. We have used this technique to probe the spatially resolved composition of ambient particles collected during a field campaign in Mexico City. Particles collected during this campaign have been extensively characterized in the past using other particle analysis techniques and hence offer a unique opportunity for exploring the utility of depth-resolved chemical imaging in ambient particle research. The particles that we examined in our study include those collected during a pollution episode related to urban waste incineration as well as background particles from the same location before the episode. Particles from the pollution episode show substantial intra-particle compositional variability typical of particles resulting from multiple emission sources. In contrast, the background particles have relatively homogeneous compositions withmore »
- Authors:
-
- California Dept. of Public Health, Richmond, CA (United States)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1321443
- Report Number(s):
- LLNL-JRNL-650135
Journal ID: ISSN 1759-9660; AMNECT
- Grant/Contract Number:
- AC52-07NA27344
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Analytical Methods
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 8; Journal ID: ISSN 1759-9660
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; particle analysis; NanoSIMS; internally mixed particles
Citation Formats
Ghosal, Sutapa, Weber, Peter K., and Laskin, Alexander. Spatially resolved chemical imaging of individual atmospheric particles using nanoscale imaging mass spectrometry: insight into particle origin and chemistry. United States: N. p., 2014.
Web. doi:10.1039/C3AY42012D.
Ghosal, Sutapa, Weber, Peter K., & Laskin, Alexander. Spatially resolved chemical imaging of individual atmospheric particles using nanoscale imaging mass spectrometry: insight into particle origin and chemistry. United States. https://doi.org/10.1039/C3AY42012D
Ghosal, Sutapa, Weber, Peter K., and Laskin, Alexander. Tue .
"Spatially resolved chemical imaging of individual atmospheric particles using nanoscale imaging mass spectrometry: insight into particle origin and chemistry". United States. https://doi.org/10.1039/C3AY42012D. https://www.osti.gov/servlets/purl/1321443.
@article{osti_1321443,
title = {Spatially resolved chemical imaging of individual atmospheric particles using nanoscale imaging mass spectrometry: insight into particle origin and chemistry},
author = {Ghosal, Sutapa and Weber, Peter K. and Laskin, Alexander},
abstractNote = {Knowledge of the spatially resolved composition of atmospheric particles is essential for differentiating between their surface versus bulk chemistry and understanding particle reactivity and the potential environmental impact. Here, we demonstrate the application of nanometer-scale secondary ion mass spectrometry (CAMECA NanoSIMS 50 ion probe) for 3D chemical imaging of individual atmospheric particles without any sample pre-treatment, such as sectioning of particles. Use of NanoSIMS depth profile analysis enables elemental mapping of particles with nanometer spatial resolution over a broad range of particle sizes. We have used this technique to probe the spatially resolved composition of ambient particles collected during a field campaign in Mexico City. Particles collected during this campaign have been extensively characterized in the past using other particle analysis techniques and hence offer a unique opportunity for exploring the utility of depth-resolved chemical imaging in ambient particle research. The particles that we examined in our study include those collected during a pollution episode related to urban waste incineration as well as background particles from the same location before the episode. Particles from the pollution episode show substantial intra-particle compositional variability typical of particles resulting from multiple emission sources. In contrast, the background particles have relatively homogeneous compositions with enhanced presence of nitrogen, oxygen, and chlorine at the particle surface. We also observed the surface enhancement of nitrogen and oxygen species is consistent with the presence of surface nitrates resulting from gas–particle heterogeneous interactions and is indicative of atmospheric ageing of the particles. The results presented here illustrate 3D characterization of ambient particles for insight into their chemical history.},
doi = {10.1039/C3AY42012D},
journal = {Analytical Methods},
number = 8,
volume = 6,
place = {United States},
year = {Tue Jan 14 00:00:00 EST 2014},
month = {Tue Jan 14 00:00:00 EST 2014}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 20 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Analysis of Atmospheric Aerosols
journal, July 2008
- Prather, Kimberly A.; Hatch, Courtney D.; Grassian, Vicki H.
- Annual Review of Analytical Chemistry, Vol. 1, Issue 1
Heterogeneous and Multiphase Chemistry in the Troposphere
journal, May 1997
- Ravishankara, A. R.
- Science, Vol. 276, Issue 5315
Experiments and Simulations of Ion-Enhanced Interfacial Chemistry on Aqueous NaCl Aerosols
journal, April 2000
- Knipping, E. M.
- Science, Vol. 288, Issue 5464
Tropospheric Air Pollution: Ozone, Airborne Toxics, Polycyclic Aromatic Hydrocarbons, and Particles
journal, May 1997
- Finlayson-Pitts, B. J.
- Science, Vol. 276, Issue 5315
Mass spectrometry of atmospheric aerosols-Recent developments and applications. Part I: Off-line mass spectrometry techniques
journal, March 2011
- Pratt, Kerri A.; Prather, Kimberly A.
- Mass Spectrometry Reviews, Vol. 31, Issue 1
Mass spectrometry of atmospheric aerosols-Recent developments and applications. Part II: On-line mass spectrometry techniques
journal, March 2011
- Pratt, Kerri A.; Prather, Kimberly A.
- Mass Spectrometry Reviews, Vol. 31, Issue 1
Mass spectrometric approaches for chemical characterisation of atmospheric aerosols: critical review of the most recent advances
journal, January 2012
- Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A.
- Environmental Chemistry, Vol. 9, Issue 3
New mass spectrometry techniques for studying physical chemistry of atmospheric heterogeneous processes
journal, March 2013
- Laskin, Julia; Laskin, Alexander; Nizkorodov, Sergey A.
- International Reviews in Physical Chemistry, Vol. 32, Issue 1
Nature and Climate Effects of Individual Tropospheric Aerosol Particles
journal, April 2010
- Pósfai, Mihály; Buseck, Peter R.
- Annual Review of Earth and Planetary Sciences, Vol. 38, Issue 1
Ambient measurements of metal-containing PM2.5 in an urban environment using laser-induced breakdown spectroscopy
journal, June 2004
- Lithgow, G. A.; Robinson, A. L.; Buckley, S. G.
- Atmospheric Environment, Vol. 38, Issue 20
Scanning Electron Microanalysis and Analytical Challenges of Mapping Elements in Urban Atmospheric Particles
journal, September 2011
- Conny, Joseph M.; Norris, Gary A.
- Environmental Science & Technology, Vol. 45, Issue 17
Chemical imaging analysis of environmental particles using the focused ion beam/scanning electron microscopy technique: microanalysis insights into atmospheric chemistry of fly ash
journal, January 2013
- Chen, Haihan; Grassian, Vicki H.; Saraf, Laxmikant V.
- The Analyst, Vol. 138, Issue 2
Depth-resolved chemical analysis of environmental microparticles by secondary mass spectrometry
journal, June 1993
- Goschnick, J.; Fichtner, M.; Lipp, M.
- Applied Surface Science, Vol. 70-71
Recent advances in the analysis of individual environmental particles. A review
journal, January 1995
- Jambers, Wendy; De Bock, Lieve; Van Grieken, Ren�
- The Analyst, Vol. 120, Issue 3
Imaging and 3D Elemental Characterization of Intact Bacterial Spores by High-Resolution Secondary Ion Mass Spectrometry
journal, August 2008
- Ghosal, Sutapa; Fallon, Stewart J.; Leighton, Terrance J.
- Analytical Chemistry, Vol. 80, Issue 15
Why ozonolysis may not increase the hydrophilicity of particles
journal, March 2010
- McIntire, T. M.; Ryder, O. S.; Gassman, P. L.
- Atmospheric Environment, Vol. 44, Issue 7
Sulfur isotope fractionation during heterogeneous oxidation of SO2 on mineral dust
journal, January 2012
- Harris, E.; Sinha, B.; Foley, S.
- Atmospheric Chemistry and Physics, Vol. 12, Issue 11
Sulfur isotope fractionation during oxidation of sulfur dioxide: gas-phase oxidation by OH radicals and aqueous oxidation by H2O2, O3 and iron catalysis
journal, January 2012
- Harris, E.; Sinha, B.; Hoppe, P.
- Atmospheric Chemistry and Physics, Vol. 12, Issue 1
Sulfur isotope ratio measurements of individual sulfate particles by NanoSIMS
journal, April 2008
- Winterholler, Baerbel; Hoppe, Peter; Foley, Stephen
- International Journal of Mass Spectrometry, Vol. 272, Issue 1
Enhanced Role of Transition Metal Ion Catalysis During In-Cloud Oxidation of SO2
journal, May 2013
- Harris, E.; Sinha, B.; van Pinxteren, D.
- Science, Vol. 340, Issue 6133
An overview of the MILAGRO 2006 Campaign: Mexico City emissions and their transport and transformation
journal, January 2010
- Molina, L. T.; Madronich, S.; Gaffney, J. S.
- Atmospheric Chemistry and Physics, Vol. 10, Issue 18
Microscopic characterization of carbonaceous aerosol particle aging in the outflow from Mexico City
journal, January 2010
- Moffet, R. C.; Henn, T. R.; Tivanski, A. V.
- Atmospheric Chemistry and Physics, Vol. 10, Issue 3
Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) – Part 1: Fine particle composition and organic source apportionment
journal, January 2009
- Aiken, A. C.; Salcedo, D.; Cubison, M. J.
- Atmospheric Chemistry and Physics, Vol. 9, Issue 17
Time-Resolved Aerosol Collector for CCSEM/EDX Single-Particle Analysis
journal, March 2003
- Laskin, Alexander; Iedema, Martin J.; Cowin, James P.
- Aerosol Science and Technology, Vol. 37, Issue 3
Analysis of individual environmental particles using modern methods of electron microscopy and X-ray microanalysis
journal, February 2006
- Laskin, A.; Cowin, J. P.; Iedema, M. J.
- Journal of Electron Spectroscopy and Related Phenomena, Vol. 150, Issue 2-3
Water-Induced Reorganization of Ultrathin Nitrate Films on NaCl: Implications for the Tropospheric Chemistry of Sea Salt Particles
journal, January 1996
- Allen, Heather C.; Laux, J. M.; Vogt, Rainer
- The Journal of Physical Chemistry, Vol. 100, Issue 16
Mineral dust is a sink for chlorine in the marine boundary layer
journal, November 2007
- Sullivan, Ryan C.; Guazzotti, Sergio A.; Sodeman, David A.
- Atmospheric Environment, Vol. 41, Issue 34
Works referencing / citing this record:
Rapid, 3D Chemical Profiling of Individual Atmospheric Aerosols with Stimulated Raman Scattering Microscopy
journal, December 2019
- Ao, Jianpeng; Feng, Yiqing; Wu, Simin
- Small Methods, Vol. 4, Issue 2
Air pollution–aerosol interactions produce more bioavailable iron for ocean ecosystems
journal, March 2017
- Li, Weijun; Xu, Liang; Liu, Xiaohuan
- Science Advances, Vol. 3, Issue 3
Physicochemical Characteristics of Individual Aerosol Particles during the 2015 China Victory Day Parade in Beijing
journal, January 2018
- Wang, Wenhua; Shao, Longyi; Xing, Jiaoping
- Atmosphere, Vol. 9, Issue 2
Direct observations of organic aerosols in common wintertime hazes in North China: insights into direct emissions from Chinese residential stoves
journal, January 2017
- Chen, Shurui; Xu, Liang; Zhang, Yinxiao
- Atmospheric Chemistry and Physics, Vol. 17, Issue 2
Organic coating on sulfate and soot particles during late summer in the Svalbard Archipelago
journal, January 2019
- Yu, Hua; Li, Weijun; Zhang, Yangmei
- Atmospheric Chemistry and Physics, Vol. 19, Issue 15
Quantitative capabilities of STXM to measure spatially resolved organic volume fractions of mixed organic ∕ inorganic particles
journal, January 2019
- Fraund, Matthew; Park, Tim; Yao, Lin
- Atmospheric Measurement Techniques, Vol. 12, Issue 3