skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Applications and limitations of constrained high-resolution peak fitting on low resolving power mass spectra from the ToF-ACSM

Abstract

The applicability, methods and limitations of constrained peak fitting on mass spectra of low mass resolving power ( mm 50~500) recorded with a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) are explored. Calibration measurements as well as ambient data are used to exemplify the methods that should be applied to maximise data quality and assess confidence in peak-fitting results. Sensitivity analyses and basic peak fit metrics such as normalised ion separation are employed to demonstrate which peak-fitting analyses commonly performed in high-resolution aerosol mass spectrometry are appropriate to perform on spectra of this resolving power. Information on aerosol sulfate, nitrate, sodium chloride, methanesulfonic acid as well as semi-volatile metal species retrieved from these methods is evaluated. The constants in a commonly used formula for the estimation of the mass concentration of hydrocarbon-like organic aerosol may be refined based on peak-fitting results. Lastly, application of a recently published parameterisation for the estimation of carbon oxidation state to ToF-ACSM spectra is validated for a range of organic standards and its use demonstrated for ambient urban data.

Authors:
 [1];  [2];  [1];  [1];  [1];  [1];  [3];  [4];  [3];  [3];  [1]
  1. Finnish Meteorological Institute, Helsinki (Finland)
  2. TOFWERK AG, Thun (Switzerland)
  3. Aerodyne Research, Inc., Billerica, MA (United States)
  4. Helmholtz Centre for Polar and Marine Research, Bremerhaven (Germany)
Publication Date:
Research Org.:
Aerodyne Research, Inc., Billerica, MA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1434905
Grant/Contract Number:  
SC0001673
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Measurement Techniques (Online)
Additional Journal Information:
Journal Name: Atmospheric Measurement Techniques (Online); Journal Volume: 9; Journal Issue: 7; Journal ID: ISSN 1867-8548
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
47 OTHER INSTRUMENTATION

Citation Formats

Timonen, Hilkka, Cubison, Mike, Aurela, Minna, Brus, David, Lihavainen, Heikki, Hillamo, Risto, Canagaratna, Manjula, Nekat, Bettina, Weller, Rolf, Worsnop, Douglas, and Saarikoski, Sanna. Applications and limitations of constrained high-resolution peak fitting on low resolving power mass spectra from the ToF-ACSM. United States: N. p., 2016. Web. doi:10.5194/amt-9-3263-2016.
Timonen, Hilkka, Cubison, Mike, Aurela, Minna, Brus, David, Lihavainen, Heikki, Hillamo, Risto, Canagaratna, Manjula, Nekat, Bettina, Weller, Rolf, Worsnop, Douglas, & Saarikoski, Sanna. Applications and limitations of constrained high-resolution peak fitting on low resolving power mass spectra from the ToF-ACSM. United States. doi:10.5194/amt-9-3263-2016.
Timonen, Hilkka, Cubison, Mike, Aurela, Minna, Brus, David, Lihavainen, Heikki, Hillamo, Risto, Canagaratna, Manjula, Nekat, Bettina, Weller, Rolf, Worsnop, Douglas, and Saarikoski, Sanna. Mon . "Applications and limitations of constrained high-resolution peak fitting on low resolving power mass spectra from the ToF-ACSM". United States. doi:10.5194/amt-9-3263-2016. https://www.osti.gov/servlets/purl/1434905.
@article{osti_1434905,
title = {Applications and limitations of constrained high-resolution peak fitting on low resolving power mass spectra from the ToF-ACSM},
author = {Timonen, Hilkka and Cubison, Mike and Aurela, Minna and Brus, David and Lihavainen, Heikki and Hillamo, Risto and Canagaratna, Manjula and Nekat, Bettina and Weller, Rolf and Worsnop, Douglas and Saarikoski, Sanna},
abstractNote = {The applicability, methods and limitations of constrained peak fitting on mass spectra of low mass resolving power (m/Δm50~500) recorded with a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) are explored. Calibration measurements as well as ambient data are used to exemplify the methods that should be applied to maximise data quality and assess confidence in peak-fitting results. Sensitivity analyses and basic peak fit metrics such as normalised ion separation are employed to demonstrate which peak-fitting analyses commonly performed in high-resolution aerosol mass spectrometry are appropriate to perform on spectra of this resolving power. Information on aerosol sulfate, nitrate, sodium chloride, methanesulfonic acid as well as semi-volatile metal species retrieved from these methods is evaluated. The constants in a commonly used formula for the estimation of the mass concentration of hydrocarbon-like organic aerosol may be refined based on peak-fitting results. Lastly, application of a recently published parameterisation for the estimation of carbon oxidation state to ToF-ACSM spectra is validated for a range of organic standards and its use demonstrated for ambient urban data.},
doi = {10.5194/amt-9-3263-2016},
journal = {Atmospheric Measurement Techniques (Online)},
number = 7,
volume = 9,
place = {United States},
year = {2016},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 4 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Elemental Analysis of Organic Species with Electron Ionization High-Resolution Mass Spectrometry
journal, November 2007

  • Aiken, Allison C.; DeCarlo, Peter F.; Jimenez, Jose L.
  • Analytical Chemistry, Vol. 79, Issue 21
  • DOI: 10.1021/ac071150w

O/C and OM/OC Ratios of Primary, Secondary, and Ambient Organic Aerosols with High-Resolution Time-of-Flight Aerosol Mass Spectrometry
journal, June 2008

  • Aiken, Allison C.; DeCarlo, Peter F.; Kroll, Jesse H.
  • Environmental Science & Technology, Vol. 42, Issue 12
  • DOI: 10.1021/es703009q

A generalised method for the extraction of chemically resolved mass spectra from Aerodyne aerosol mass spectrometer data
journal, July 2004


Chemical and Source Characterization of Submicron Particles at Residential and Traffic Sites in the Helsinki Metropolitan Area, Finland
journal, January 2015

  • Aurela, Minna; Saarikoski, Sanna; Niemi, Jarkko V.
  • Aerosol and Air Quality Research, Vol. 15, Issue 4
  • DOI: 10.4209/aaqr.2014.11.0279

Elemental ratio measurements of organic compounds using aerosol mass spectrometry: characterization, improved calibration, and implications
journal, January 2015

  • Canagaratna, M. R.; Jimenez, J. L.; Kroll, J. H.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 1
  • DOI: 10.5194/acp-15-253-2015

On data analysis in PTR-TOF-MS: From raw spectra to data mining
journal, July 2011

  • Cappellin, Luca; Biasioli, Franco; Granitto, Pablo M.
  • Sensors and Actuators B: Chemical, Vol. 155, Issue 1
  • DOI: 10.1016/j.snb.2010.11.044

Oceanic phytoplankton, atmospheric sulphur, cloud albedo and climate
journal, April 1987

  • Charlson, Robert J.; Lovelock, James E.; Andreae, Meinrat O.
  • Nature, Vol. 326, Issue 6114
  • DOI: 10.1038/326655a0

Peak-fitting and integration imprecision in the Aerodyne aerosol mass spectrometer: effects of mass accuracy on location-constrained fits
journal, January 2015

  • C. Corbin, J.; Othman, A.; D. Allan, J.
  • Atmospheric Measurement Techniques, Vol. 8, Issue 11
  • DOI: 10.5194/amt-8-4615-2015

A review on the importance of metals and metalloids in atmospheric dust and aerosol from mining operations
journal, September 2012


Statistical precision of the intensities retrieved from constrained fitting of overlapping peaks in high-resolution mass spectra
journal, January 2015


Field-Deployable, High-Resolution, Time-of-Flight Aerosol Mass Spectrometer
journal, December 2006

  • DeCarlo, Peter F.; Kimmel, Joel R.; Trimborn, Achim
  • Analytical Chemistry, Vol. 78, Issue 24
  • DOI: 10.1021/ac061249n

A New Time-of-Flight Aerosol Mass Spectrometer (TOF-AMS)—Instrument Description and First Field Deployment
journal, July 2005

  • Drewnick, Frank; Hings, Silke S.; DeCarlo, Peter
  • Aerosol Science and Technology, Vol. 39, Issue 7
  • DOI: 10.1080/02786820500182040

Aerosol mass spectrometry: particle–vaporizer interactions and their consequences for the measurements
journal, January 2015

  • Drewnick, F.; Diesch, J. -M.; Faber, P.
  • Atmospheric Measurement Techniques, Vol. 8, Issue 9
  • DOI: 10.5194/amt-8-3811-2015

The ToF-ACSM: a portable aerosol chemical speciation monitor with TOFMS detection
journal, January 2013

  • Fröhlich, R.; Cubison, M. J.; Slowik, J. G.
  • Atmospheric Measurement Techniques, Vol. 6, Issue 11
  • DOI: 10.5194/amt-6-3225-2013

The contribution of ocean-leaving DMS to the global atmospheric burdens of DMS, MSA, SO 2 , and NSS SO 4 = : DMS, MSA, SO
journal, May 2003

  • Gondwe, M.; Krol, M.; Gieskes, W.
  • Global Biogeochemical Cycles, Vol. 17, Issue 2
  • DOI: 10.1029/2002GB001937

Development of an Aerosol Mass Spectrometer for Size and Composition Analysis of Submicron Particles
journal, July 2000

  • Jayne, John T.; Leard, Danna C.; Zhang, Xuefeng
  • Aerosol Science and Technology, Vol. 33, Issue 1-2
  • DOI: 10.1080/027868200410840

Ambient aerosol sampling using the Aerodyne Aerosol Mass Spectrometer
journal, January 2003


A high-resolution mass spectrometer to measure atmospheric ion composition
journal, January 2010

  • Junninen, H.; Ehn, M.; Petäjä, T.
  • Atmospheric Measurement Techniques, Vol. 3, Issue 4
  • DOI: 10.5194/amt-3-1039-2010

Real-time aerosol mass spectrometry with millisecond resolution
journal, May 2011

  • Kimmel, Joel R.; Farmer, Delphine K.; Cubison, Michael J.
  • International Journal of Mass Spectrometry, Vol. 303, Issue 1
  • DOI: 10.1016/j.ijms.2010.12.004

Influence of oceanic dimethyl sulfide emissions on cloud condensation nuclei concentrations and seasonality over the remote Southern Hemisphere oceans: A global model study
journal, January 2008

  • Korhonen, Hannele; Carslaw, Kenneth S.; Spracklen, Dominick V.
  • Journal of Geophysical Research, Vol. 113, Issue D15
  • DOI: 10.1029/2007JD009718

Deconvolution of isobaric interferences in mass spectra
journal, May 2004

  • Meija, Juris; Caruso, Joseph A.
  • Journal of the American Society for Mass Spectrometry, Vol. 15, Issue 5
  • DOI: 10.1016/j.jasms.2003.12.016

A new software tool for the analysis of high resolution PTR-TOF mass spectra
journal, August 2013


Real-Time Methods for Estimating Organic Component Mass Concentrations from Aerosol Mass Spectrometer Data
journal, February 2011

  • Ng, N. L.; Canagaratna, M. R.; Jimenez, J. L.
  • Environmental Science & Technology, Vol. 45, Issue 3
  • DOI: 10.1021/es102951k

An Aerosol Chemical Speciation Monitor (ACSM) for Routine Monitoring of the Composition and Mass Concentrations of Ambient Aerosol
journal, July 2011


Secondary organic aerosol formation and primary organic aerosol oxidation from biomass burning smoke in a flow reactor during FLAME-3
journal, January 2013

  • Ortega, A. M.; Day, D. A.; Cubison, M. J.
  • Atmospheric Chemistry and Physics Discussions, Vol. 13, Issue 5
  • DOI: 10.5194/acpd-13-13799-2013

Characterization of the aerosol over the sub-arctic north east Pacific Ocean
journal, October 2006

  • Phinney, Lisa; Richard Leaitch, W.; Lohmann, Ulrike
  • Deep Sea Research Part II: Topical Studies in Oceanography, Vol. 53, Issue 20-22
  • DOI: 10.1016/j.dsr2.2006.05.044

Health Effects of Fine Particulate Air Pollution: Lines that Connect
journal, June 2006


Feasibility of the Detection of Trace Elements in Particulate Matter Using Online High-Resolution Aerosol Mass Spectrometry
journal, November 2012


Sub-Antarctic marine aerosol: dominant contributions from biogenic sources
journal, January 2013

  • Schmale, J.; Schneider, J.; Nemitz, E.
  • Atmospheric Chemistry and Physics, Vol. 13, Issue 17
  • DOI: 10.5194/acp-13-8669-2013

Methods to extract molecular and bulk chemical information from series of complex mass spectra with limited mass resolution
journal, October 2015

  • Stark, Harald; Yatavelli, Reddy L. N.; Thompson, Samantha L.
  • International Journal of Mass Spectrometry, Vol. 389
  • DOI: 10.1016/j.ijms.2015.08.011

Characterization of the inter-annual, seasonal, and diurnal variations of condensation particle concentrations at Neumayer, Antarctica
journal, January 2011


Natural new particle formation at the coastal Antarctic site Neumayer
journal, January 2015


Photooxidation of dimethyl sulfide and dimethyl disulfide. II: Mechanism evaluation
journal, November 1990

  • Yin, Fangdon; Grosjean, Daniel; Flagan, Richard C.
  • Journal of Atmospheric Chemistry, Vol. 11, Issue 4
  • DOI: 10.1007/BF00053781

Fast Analytical Design Algorithms for FIR Notch Filters
journal, March 2004

  • Zahradnik, P.; Vlcek, M.
  • IEEE Transactions on Circuits and Systems I: Regular Papers, Vol. 51, Issue 3
  • DOI: 10.1109/TCSI.2003.822404

    Works referencing / citing this record:

    Particulate matter characteristics, dynamics, and sources in an underground mine
    journal, September 2017