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Organic aerosol composition using Thermal Desorption Aerosol Gas Chromatograph (TAG) combined with
High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS)Spectrometer (HR ToF AMS)
TAG-AMS
Thorsten Hohaus1, Andrew Lambe1, Brent Williams4, John Jayne1, Douglas Worsnop1, Leah Williams1, Joel Kimmel1, Donna Sueper1, Nathan Kreisberg2, Susan Herring2,
Gabriel Isaacman3, David Worton3, Allen Goldstein3Gabriel Isaacman , David Worton , Allen Goldstein
1Aerodyne Research Inc, Billerica, MA2Aerosol Dynamics Inc., Berkeley, CA
3Dept of Environmental Science, Policy, & Management, UC-Berkeley, Berkeley, CA4Department of Energy, Environmental, and Chemical Engineering, Washington University in St.
Louis
Outline
MotivationInstrument descriptionTAG-AMS projectStandard measurementsField deployment at CalNex 2010
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Field deployment at CalNex 2010Summary
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“Towards the perfect instrument”
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Hallequist et al, ACP, 2009
Combined AMS and TAG instrument: TAG-AMS
Thermal desorption aerosol GC/MS (TAG) (Williams et al, AS&T, 2006)Automated sample collection on CTD cellMolecular speciation, Marker compoundsHourly time resolution
Aerosol Mass Spectrometer (AMS) (Jayne et al, AS&T, 2000)
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PM1.0 organic and inorganic mass concentrations and size distributionsHR-ToF-MS: H:C, O:C, N:C ratios
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TAG-AMS design
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courtesy of Brent WilliamsAutomated data acquisition switchingChopper blocks particle beam during TAG analysis
TAG-AMS design
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TAG-AMS design
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TAG-AMS design
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TAG-AMS design
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TAG-AMS design
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TAG-AMS project overviewCollaboration between
Aerosol Dymanics, Inc. (Nathan Kreisberg, Susan Herring)
University of California at Berkeley (Allen Goldstein, David Worton, Gabriel Isaacman)
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Aerodyne Research, Inc.
TAG-AMS project overviewCollaboration between
Aerosol Dymanics, Inc. (Nathan Kreisberg, Susan Herring)CTD cell (filter based cell → reduced aerosol bounce)Automated standard injections on the CTD cellAutomated standard injections on the CTD cell
University of California at Berkeley (Allen Goldstein, David Worton, Gabriel Isaacman)
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Aerodyne Research, Inc.
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TAG-AMS project overviewCollaboration between
Aerosol Dymanics, Inc. (Nathan Kreisberg, Susan Herring)CTD cell (filter based cell → reduced aerosol bounce)Automated standard injections on the CTD cellAutomated standard injections on the CTD cell
University of California at Berkeley (Allen Goldstein, David Worton, Gabriel Isaacman)Custom made small GC oven (approx. 30 cm x 30 cm)GC as a modular AMS equipment
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Aerodyne Research, Inc.
TAG-AMS project overviewCollaboration between
Aerosol Dymanics, Inc. (Nathan Kreisberg, Susan Herring)CTD cell (filter based cell → reduced aerosol bounce)Automated standard injections on the CTD cellAutomated standard injections on the CTD cell
University of California at Berkeley (Allen Goldstein, David Worton, Gabriel Isaacman)Custom made small GC oven (approx. 30 cm x 30 cm)GC as a modular AMS equipment
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Aerodyne Research, Inc.TAG-AMS interfaceacquisition and analysis methods for TAG-AMS datacommercialize the TAG collector as a module
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TAG-AMS project overview
Goal → 3 commercially available TAG systems
Standalone TAG collectorWilliams et al., AS&T 2006, Williams et al., JGR, 2007
TAG collector with new HR-ToF-MSPo Valley campaign, Summer 2009
TAG-AMS → TAG module for existing AMS
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TAG AMS TAG module for existing AMSCalNex 2010 campaign
TAG Igor analysis tool
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TAG-AMS standard chromatogram
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TAG-AMS standard chromatogram
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TAG-AMS PAH standard chromatogram
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First TAG-AMS field deployment• May 15th - June 15th 2010 CalNex ground site (Pasadena,
CA)
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5 weeks’ operation over 2 weeks of continuous measurements
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TAG-AMS CalNex design
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courtesy of Brent Williams
TAG-AMS CalNex design
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courtesy of Brent Williams
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Measurement Cycles
Simultaneous AMS measurement and sample collection with TAGSubsequent analysis of desorbed and GC separated aerosol constituentsaerosol constituents Measurement cycle (120 min)
60 min AMS measurements (V-mode) + 60 min TAG sampling60 min TAG analysis
Internal standard (deuterated compounds) External standard (compound mixture of alkanes, acids, PAH steranes hopanes etc )
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PAH, steranes, hopanes etc.)Blank measurementExternal and internal standard measurements with syringe and auto-injector
TAG-AMS CalNex design
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CalNex data sample overview I
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CalNex data sample overview II
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CalNex chromatogram
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Ambient Pyrene
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Unresolved Complex Mixture (UCM)
UCM on 27th May 2010 11:00 AM
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Undenuded vs. Denuded
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Undenuded vs. Denuded
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Petroleum Source Fingerprinting
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Summary & OutlookStandalone automated TAG-AMS measurements
Analysis tool exits and will be further developed/improved
Demonstrated proof-of-concept: TAG-AMS field deploymentp p p yBulk NR-PM1.0 speciation and sizing Molecular speciation of organic tracer compounds
Technical improvementsGC oven, control unit, TAG-AMS interface
PMF analysis of TAG-AMS measurements
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PMF analysis for TAG data
Correlate changes in average AMS mass spectra to changes in abundances in molecular marker compounds
V-mode → W-mode
Thank you!
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TAG-AMS design
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TAG-AMS bulk diurnal trends
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Organics afternoon peak ⌫ SOA
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TAG-AMS study-average size distribution
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TAG-AMS alkane mass spectrum
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