s p -ams l v -ams - welcome | cirescires1.colorado.edu › jimenez-group › usrmtgs › usersmtg17...
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SootParticle-AMSor
LaserVaporizer-AMS
Aerodyne Research, Inc.
et al.
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Outline
• SP-AMS technique and hardware• Reference material
• SP-AMS applications• Quick highlight a few applications
• SP-AMS quantification• Challenges and summary
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SP-AMS hardwareSP Module
Second vaporizer in AMSDifferent ionization chamber configurationThree potential vaporizer configurations
ADQ, ePTOF, BWP (ebox) upgrades
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Laser Vaporizer Module
Onasch et al. (AS&T 2012)
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Ionizer Configurations
HR-AMS (Tungsten vaporizer)
• Filaments on sides of ion chamber
• Filament position is mechanically set
• Filament wire is typically well positioned with respect to well formed slits in ion chamber walls
• Narrow or Wide chamber widths
SP-AMS (Laser Vaporizer)
• Filament is on bottom of ion chamber
• Filament position is moveable (vert& horz)
• Filament slit width and breadth may vary due to custom procedure
• Large holes in sides to accommodate laser beam
• Narrow or Wide chamber widths
Need to optimize vertical position
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Vaporizer Configurations
1. Tungsten Vaporizer (HR-AMS)2. Laser Vaporizer 3. Laser + Tungsten Vaporizers
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SP-AMS Orthogonal Detection Axes
Sampled Particles
Ion Extraction and MS detection
• Characterization of particle-laser interaction region:• Vertical Particle Beam Walk• Horizontal/Vertical Beam Width Probe• Laser Beam Walk
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Laser Vaporizer Detection Scheme
The laser is not the vaporizer, the absorbing particles are the vaporizer!!
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Ambient Mass Spectrum
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Nomenclature
Corbin et al., 2014 - ETH
4000 oC
PM = Particulate MatterNR = Non-RefractoryR = RefractoryL = Light Absorbing (1064 nm)
LR-PM:1. Refractory Black Carbon (rBC)2. Metals
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SP-AMS applicationsAmbient rBC measurements (Massoli et al., 2015)
Source characterization of laboratory metal nanoparticles (Nilsson et al., 2015)
Dual vaporizer measurements including single particle detection (Lee et al., 2015)
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CalNex 2010 – Massoli et al., 2014 JGR
Separate instruments operated side-by-side:• SP-AMS laser vaporizer• HR-AMS tungsten vaporizer
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rBC particle chemical composition and size
• Increasing Photochemical aging• Observations of secondary
condensation• Observations of compaction
and growth of rBC particles
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Direct comparison between rBC subset of particles and total aerosol loading
Chemical information Mass information
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Source characterization of metal nanoparticles –Nilsson et al., 2015 Nano Research
• Chemical information, including metal composition, oxide formation, and contaminants
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Source characterization of metal nanoparticles –Nilsson et al., 2015 Nano Research
• Size and effective density information
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Dual vaporizer measurements of ambient rBC particles – Lee et al., 2015 ACP
• Single particle detection allows for the measurement of rBC particles even with dual vaporizer configurations
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Average MS comparisons
• Apparent increased sensitivity to NR-PM vaporized in laser vaporizer!
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SP-AMS QuantificationSensitivities
Refractory black carbon (rBC) [Laser]
Non-Refractory PM [Laser and Tungsten]
Collection EfficienciesTungsten Vaporizer
Laser Vaporizer
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mIE calibrations
300 nm AN
NR-PM using tungsten vaporizer rBC using laser vaporizer
• We need to include a third calibration: NR-PM for laser vaporizer!
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mIE NR-PM calibrations using laser vaporizer
• Difficult, but not impossible
• Two approaches attempted to date:1. Coat Regal black with DOS (Willis et al., 2014 AMT)
2. Atomize ammonium nitrate with Regal black (Carbone et al., 2015 AMTD)
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• Coated Regal black particles with DOS to make spherical
• With thicker coatings, RIE_rBCincreased as the particle beam narrowed down closer to laser beam width
• Dual laser/tungsten vaporizer setup• Both rBC and Org ion signals
increased• NR-PM mIE for DOS appears to be
~2x larger from laser vaporizer than from tungsten vaporizer!
~2x CE
~2x mIE
rBC CE determination
NR-PM mIE determination
Willis et al., 2014 AMT
DOS coated BC with vaporizer and laser
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AN coated BC with vaporizer and laser
Carbone et al., 2015 AMTD; Fortner lab experiments
• Dual vaporizers• Atomize solution of Regal
black and ammonium nitrate• Large [AN] likely produce
significant number of particles without Regal black
• Small [AN] likely produce Regal black particles with thin coatings of AN
• Apparent mIE for AN on laser vaporizer is ~2.3x tungsten vaporizer (laser OFF)
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mIE NR-PM calibrations using laser vaporizer
• Need to further refine mIE calibrations for NR-PM on rBC particles
• Need to assess the differences between mIE for laser and tungsten vaporizer PM
• Need to verify whether the standard suite of RIE’s, determined using tungsten vaporizer only, hold for the laser vaporizer
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Tungsten Vaporizer Collection Efficiency
EL = Aerodynamic Lens transmission EB = Incomplete vaporization due to particle BounceES = Particle beam divergence due to particle Shape (and size)
EL ~ 1 for dva = 70-700 nmEB ~ 0.5 due to solid/refractory particle bounceES = 1 as particle beam width < tungsten vaporizer width
Mass concentration of species “s”
EB governs the overall CE for Tungsten Vaporizer
CE = EL · EB · ES
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Laser Vaporizer Collection Efficiency
Mass concentration of species “s”
ES governs the overall CE for rBC and NR-PM (laser only) Beam width probe measurement
EB complicates rBC (RBC) measurements
CELaser = EL · EB · ES
EL = Aerodynamic Lens transmission
EB = Incomplete vaporization **
ES = Particle beam divergence due to particle Shape (and size)
EL ~ 1 for dva = 70-700 nm
EB ≤ 1 due inefficient energy absorption/transfer issues **
ES < 1 as particle beam width < laser vaporizer width
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Beam Width Probe (Huffmann et al./Salcedo et al.)
laser
wire
wire motion
Particle beam
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BWP Results
• Two independent measures of narrowing of particle beam with coating• Decreasing particle beam width increases particle-laser beam overlap
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Incomplete vaporization and laser power
• Laser Power Drop experiments show a stronger particle-laser beam overlap dependence for rBCthan NR-PM
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SP-AMS CE’sVaporizer-dependent
Vaporizer Measured Species
Tungsten NR-PM * E B
Laser (rBC + R-PMǂ + NR-PM
ǂ) * E S
Laser and Tungsten (rBC + R-PMǂ + NR-PM
ǂ) * E S + (NR-PM - NR-PM
ǂ * E S ) * E B
NR-PM = Nonrefractory Particulate Material measured by a standard AMS [Jimenez et al., 2003 ]
R-PM = Refractory Particulate Material measured by the SP-AMS (see text for details)
rBC = Refractory black carbon measured by the SP-AMS (and SP2) [Schwarz et al., 2006 ]ǂ = Particulate Material on rBC particles as mesaured by the SP-AMS (see text for details)
E B = Particle bounce related Collection Efficiency of the AMS
E S = Size and shape related Collection Efficiency of the SP-AMS
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Laser vaporizer only
Flame 3
Fortner et al., 2015
Regal black
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Resistively heated tungsten vaporizer only
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Refractory black carbon (rBC)
Tungsten vaporizer only
Dual vaporizers
Laser vaporizer only
PMF deconvolution
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Laser ON vs OFF
Government Flats fire (8/21/2013). SP-AMS plume transect with dual vaporizers (left) and tungsten only (right)
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Summary of quantification issues:
# Issue Importance Comments
1Differences between vaporizer
sensitivitiesmajor
mIE sensitivity issue likely due to vaporization temperatures of molecules and
subsent velocities in ion formation chamber. Difficult mIE measurements for NR-
PM from laser vaporizer. Laser vaporizer RIE's need verification (or
determination). Not well characterized to date.
2 Incomplete vaporization majorCollection efficiency (CE) issue that has not been characterized very well to date
and causes over-estimates of [NR-PM]/[rBC] ratios.
3 Particle beam - laser beam overlap major
Collection efficiency (CE) issue strongly depenent upon alignment and particle
morphologies. BWP will help with quantification, though difficult (and slow)
measurements.
4 Laser misalignment minorIncludes laser beam hitting tungsten vaporizer or ion formation chamber. Can be
mitigated through careful alignment procedures.
5 Cn+ ion interference from Org minor Problem for dual vaporizer measurements with significant NR-PM Organics. PMF
of rBC ion signals appears to effectively distinguish Cn+ ion sources.
6Large (mid and fullerene) Cn+ ion
formationminor
Apparent laser power issue that has yet to be resolved.
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Summary
• SP-AMS hardware = laser vaporizer inside HR-AMS• Provides refractory PM detection (chemical, mass, and size information)
• Three vaporizer configurations (laser only, tungsten vaporizer only, dual vaporizers)
• Single particle detection
• SP-AMS technique finding applications in ambient measurements, source (combustion) characterization, laboratory measurements, metal nanoparticles, and single particle detection
• SP-AMS quantification is challenging, but we are making progress