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35
SootParticle-AMS or LaserVaporizer-AMS Aerodyne Research, Inc. et al.

Transcript of or L V -AMS - CIREScires.colorado.edu › ... › 2014_SP_AMS_update_presentation_short.pdf · 9...

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SootParticle-AMSor

LaserVaporizer-AMS

Aerodyne Research, Inc.

et al.

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SP-AMS Instruments in the Field

# Research Group Instrument Status

1 Aerodyne Research, Inc. SP module Delivered

2 Aerodyne Research, Inc. SP module Delivered

3 University of Manchester SP module Delivered

4 University of Toronto SP-AMS Delivered

5 Lund University, Sweden SP module Delivered

6 ETH, Switzerland SP module Delivered

7 FMI Helsinki SP module Delivered

8 NASA Langley SP-AMS Delivered

9 Drexel University SP-AMS Delivered

10 Aarhus University/Denmark SP-AMS Delivered

11 Environment Canada SP-AMS Delivered

12 Masschusetts Institute of Technology SP module Delivered

13 University of Eastern Finland, Kuopio SP module Delivered

14 Carnegie Mellon University SP module (HR-AMS upgrade) Delivered

15 NIUST/Handix SP-AMS Delivered

16 Environment Canada SP-AMS Ordered

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SP-AMS Papers# SP-AMS papers

1

Buffaloe, G. M., Lack, D. a., Williams, E. J., Coffman, D., Hayden, K. L., Lerner, B. M., Li, S.-M., Nuaaman,

I., Massoli, P., Onasch, T. B., Quinn, P. K. and Cappa, C. D.: Black carbon emissions from in-use ships: a

California regional assessment, Atmos. Chem. Phys., 14(4), 1881–1896, doi:10.5194/acp-14-1881-2014,

2014.

2

Cappa, C. D., Onasch, T. B., Massoli, P., Worsnop, D. R., Jobson, B. T., Kolesar, K. R., Lack, D. a., Lerner,

B. M., Li, S.-M. S., Bates, T. S., Cross, E. S., Davidovits, P., Hakala, J., Hayden, K. L., Mellon, D., Nuaaman,

I., Olfert, J. S., Petäjä, T., Quinn, P. K., Song, C., Subramanian, R., Williams, E. J., Zaveri, R. a. and Petaja,

T.: Radiative Absorption Enhancements Due to the Mixing State of Atmospheric Black Carbon, Science

(80-. )., 337(6098), 1078–81, doi:10.1126/science.1223447, 2012.

3

Cappa, C. D., Williams, E. J., Lack, D. a., Buffaloe, G. M., Coffman, D., Hayden, K. L., Herndon, S. C.,

Lerner, B. M., Li, S.-M., Massoli, P., McLaren, R., Nuaaman, I., Onasch, T. B. and Quinn, P. K.: A case

study into the measurement of ship emissions from plume intercepts of the NOAA ship Miller

Freeman , Atmos. Chem. Phys., 14(3), 1337–1352, doi:10.5194/acp-14-1337-2014, 2014.

4

Corbin, J. C., Sierau, B., Gysel, M., Laborde, M., Keller, A., Kim, J., Petzold, A., Onasch, T. B., Lohmann,

U. and Mensah, a. a.: Mass spectrometry of refractory black carbon particles from six sources: carbon-

cluster and oxygenated ions, Atmos. Chem. Phys., 14(5), 2591–2603, doi:10.5194/acp-14-2591-2014,

2014.

5

Cross, E. S., Onasch, T. B., Ahern, A., Wrobel, W., Slowik, J. G., Olfert, J., Lack, D. a., Massoli, P., Cappa,

C. D., Schwarz, J. P., Spackman, J. R., Fahey, D. W., Sedlacek, A., Trimborn, A., Jayne, J. T., Freedman,

A., Williams, L. R., Ng, N. L., Mazzoleni, C., Dubey, M., Brem, B., Kok, G., Subramanian, R., Freitag, S.,

Clarke, A., Thornhill, D., Marr, L. C., Kolb, C. E., Worsnop, D. R. and Davidovits, P.: Soot Particle

Studies—Instrument Inter-Comparison—Project Overview, Aerosol Sci. Technol., 44(8), 592–611,

doi:10.1080/02786826.2010.482113, 2010.

6

Cross, E. S., Sappok, A., Fortner, E. C., Hunter, J. F., Jayne, J. T., Brooks, W. a., Onasch, T. B., Wong, V.

W., Trimborn, A., Worsnop, D. R. and Kroll, J. H.: Real-Time Measurements of Engine-Out Trace

Elements: Application of a Novel Soot Particle Aerosol Mass Spectrometer for Emissions

Characterization, J. Eng. Gas Turbines Power, 134(7), 072801, doi:10.1115/1.4005992, 2012.

7Dallmann, T. R., Demartini, S. J., Kirchstetter, T. W., Herndon, S. C., Onasch, T. B., Wood, E. C. and

Harley, R. a: On-road measurement of gas and particle phase pollutant emission factors for individual

heavy-duty diesel trucks., Environ. Sci. Technol., 46(15), 8511–8, doi:10.1021/es301936c, 2012.

8

Dallmann, T. R., Onasch, T. B., Kirchstetter, T. W., Worton, D. R., Fortner, E. C., Herndon, S. C., Wood, E.

C., Franklin, J. P., Worsnop, D. R., Goldstein, a. H. and Harley, R. a.: Characterization of particulate

matter emissions from on-road gasoline and diesel vehicles using a soot particle aerosol mass

spectrometer, Atmos. Chem. Phys. Discuss., 14(3), 4007–4049, doi:10.5194/acpd-14-4007-2014, 2014.

9Decesari, S., Allan, J., Plass-Duelmer, C., Williams, B. J., Paglione, M., Facchini, M. C., ... & Dall'Osto, M.

(2014). Measurements of the aerosol chemical composition and mixing state in the Po Valley using

multiple spectroscopic techniques. Atmospheric Chemistry and Physics Discussions, 14(7), 9275-9343.

10

Fortner, E. C., Brooks, W. a., Onasch, T. B., Canagaratna, M. R., Massoli, P., Jayne, J. T., Franklin, J. P.,

Knighton, W. B., Wormhoudt, J., Worsnop, D. R., Kolb, C. E. and Herndon, S. C.: Particulate Emissions

Measured During the TCEQ Comprehensive Flare Emission Study, Ind. Eng. Chem. Res., 51(39),

12586–12592, doi:10.1021/ie202692y, 2012.

11

Gilardoni, S., Massoli, P., Giulianelli, L., Rinaldi, M., Paglione, M., Pollini, F., ... & Fuzzi, S. (2014). Fog

scavenging of organic and inorganic aerosol in the Po Valley. Atmospheric Chemistry and Physics

Discussions, 14(4), 4787-4826.

12

Happonen, M., Mylläri, F., Karjalainen, P., Frey, A., Saarikoski, S., Carbone, S., Hillamo, R., Pirjola, L.,

Häyrinen, A., Kytömäki, J., Niemi, J. V, Keskinen, J. and Rönkkö, T.: Size distribution, chemical

composition, and hygroscopicity of fine particles emitted from an oil-fired heating plant., Environ. Sci.

Technol., 47(24), 14468–75, doi:10.1021/es4028056, 2013.

13Lee, A. K. Y., Willis, M. D., Healy, R. M., Onasch, T. B. and Abbatt, J. P. D.: Single particle

characterization using the soot particle aerosol mass spectrometer (SP-AMS), ACPD, 2014.

14

Liu, D., Allan, J., Whitehead, J., Young, D., Flynn, M., Coe, H., McFiggans, G., Fleming, Z. L. and Bandy,

B.: Ambient black carbon particle hygroscopic properties controlled by mixing state and composition,

Atmos. Chem. Phys., 13(4), 2015–2029, doi:10.5194/acp-13-2015-2013, 2013.

15

Massoli, P., Fortner, E. C., Canagaratna, M. R., Williams, L. R., Zhang, Q., Sun, Y., Schwab, J. J., Trimborn,

A., Onasch, T. B., Demerjian, K. L., Kolb, C. E., Worsnop, D. R. and Jayne, J. T.: Pollution Gradients and

Chemical Characterization of Particulate Matter from Vehicular Traffic near Major Roadways: Results

from the 2009 Queens College Air Quality Study in NYC, Aerosol Sci. Technol., 46(11), 1201–1218,

doi:10.1080/02786826.2012.701784, 2012.

16

Nordin, E. Z., Eriksson, a. C., Roldin, P., Nilsson, P. T., Carlsson, J. E., Kajos, M. K., Hellén, H., Wittbom,

C., Rissler, J., Löndahl, J., Swietlicki, E., Svenningsson, B., Bohgard, M., Kulmala, M., Hallquist, M. and

Pagels, J. H.: Secondary organic aerosol formation from idling gasoline passenger vehicle emissions

investigated in a smog chamber, Atmos. Chem. Phys., 13(12), 6101–6116, doi:10.5194/acp-13-6101-

2013, 2013.

17

Onasch, T. B., Trimborn, A., Fortner, E. C., Jayne, J. T., Kok, G. L., Williams, L. R., Davidovits, P. and

Worsnop, D. R.: Soot Particle Aerosol Mass Spectrometer: Development, Validation, and Initial

Application, Aerosol Sci. Technol., 46(7), 804–817, doi:10.1080/02786826.2012.663948, 2012.

18

Saarikoski, S., Carbone, S., Cubison, M. J., Hillamo, R., Keronen, P., Sioutas, C., ... & Jimenez, J. L.

(2014). Evaluation of the performance of a particle concentrator for online instrumentation.

Atmospheric Measurement Techniques, 7(7), 2121-2135.

19

Taylor, J. W., Allan, J. D., Liu, D., Flynn, M., Weber, R., Zhang, X., ... & Coe, H. (2014). Assessment of the

sensitivity of core/shell parameters derived using the single-particle soot photometer to density and

refractive index.

20

Willis, M. D., Lee, A. K. Y., Onasch, T. B., Fortner, E. C., Williams, L. R., Lambe, A. T., Worsnop, D. R. and

Abbatt, J. P. D.: Collection efficiency of the Soot-Particle Aerosol Mass Spectrometer (SP-AMS) for

internally mixed particulate black carbon, Atmos. Meas. Tech. Discuss., 7(5), 5223–5249,

doi:10.5194/amtd-7-5223-2014, 2014.

20+… more submitted and many more in preparation/planning…

# SP-AMS papers

1

Buffaloe, G. M., Lack, D. a., Williams, E. J., Coffman, D., Hayden, K. L., Lerner, B. M., Li, S.-M., Nuaaman,

I., Massoli, P., Onasch, T. B., Quinn, P. K. and Cappa, C. D.: Black carbon emissions from in-use ships: a

California regional assessment, Atmos. Chem. Phys., 14(4), 1881–1896, doi:10.5194/acp-14-1881-2014,

2014.

2

Cappa, C. D., Onasch, T. B., Massoli, P., Worsnop, D. R., Jobson, B. T., Kolesar, K. R., Lack, D. a., Lerner,

B. M., Li, S.-M. S., Bates, T. S., Cross, E. S., Davidovits, P., Hakala, J., Hayden, K. L., Mellon, D., Nuaaman,

I., Olfert, J. S., Petäjä, T., Quinn, P. K., Song, C., Subramanian, R., Williams, E. J., Zaveri, R. a. and Petaja,

T.: Radiative Absorption Enhancements Due to the Mixing State of Atmospheric Black Carbon, Science

(80-. )., 337(6098), 1078–81, doi:10.1126/science.1223447, 2012.

3

Cappa, C. D., Williams, E. J., Lack, D. a., Buffaloe, G. M., Coffman, D., Hayden, K. L., Herndon, S. C.,

Lerner, B. M., Li, S.-M., Massoli, P., McLaren, R., Nuaaman, I., Onasch, T. B. and Quinn, P. K.: A case

study into the measurement of ship emissions from plume intercepts of the NOAA ship Miller

Freeman , Atmos. Chem. Phys., 14(3), 1337–1352, doi:10.5194/acp-14-1337-2014, 2014.

4

Corbin, J. C., Sierau, B., Gysel, M., Laborde, M., Keller, A., Kim, J., Petzold, A., Onasch, T. B., Lohmann,

U. and Mensah, a. a.: Mass spectrometry of refractory black carbon particles from six sources: carbon-

cluster and oxygenated ions, Atmos. Chem. Phys., 14(5), 2591–2603, doi:10.5194/acp-14-2591-2014,

2014.

5

Cross, E. S., Onasch, T. B., Ahern, A., Wrobel, W., Slowik, J. G., Olfert, J., Lack, D. a., Massoli, P., Cappa,

C. D., Schwarz, J. P., Spackman, J. R., Fahey, D. W., Sedlacek, A., Trimborn, A., Jayne, J. T., Freedman,

A., Williams, L. R., Ng, N. L., Mazzoleni, C., Dubey, M., Brem, B., Kok, G., Subramanian, R., Freitag, S.,

Clarke, A., Thornhill, D., Marr, L. C., Kolb, C. E., Worsnop, D. R. and Davidovits, P.: Soot Particle

Studies—Instrument Inter-Comparison—Project Overview, Aerosol Sci. Technol., 44(8), 592–611,

doi:10.1080/02786826.2010.482113, 2010.

6

Cross, E. S., Sappok, A., Fortner, E. C., Hunter, J. F., Jayne, J. T., Brooks, W. a., Onasch, T. B., Wong, V.

W., Trimborn, A., Worsnop, D. R. and Kroll, J. H.: Real-Time Measurements of Engine-Out Trace

Elements: Application of a Novel Soot Particle Aerosol Mass Spectrometer for Emissions

Characterization, J. Eng. Gas Turbines Power, 134(7), 072801, doi:10.1115/1.4005992, 2012.

7Dallmann, T. R., Demartini, S. J., Kirchstetter, T. W., Herndon, S. C., Onasch, T. B., Wood, E. C. and

Harley, R. a: On-road measurement of gas and particle phase pollutant emission factors for individual

heavy-duty diesel trucks., Environ. Sci. Technol., 46(15), 8511–8, doi:10.1021/es301936c, 2012.

8

Dallmann, T. R., Onasch, T. B., Kirchstetter, T. W., Worton, D. R., Fortner, E. C., Herndon, S. C., Wood, E.

C., Franklin, J. P., Worsnop, D. R., Goldstein, a. H. and Harley, R. a.: Characterization of particulate

matter emissions from on-road gasoline and diesel vehicles using a soot particle aerosol mass

spectrometer, Atmos. Chem. Phys. Discuss., 14(3), 4007–4049, doi:10.5194/acpd-14-4007-2014, 2014.

9Decesari, S., Allan, J., Plass-Duelmer, C., Williams, B. J., Paglione, M., Facchini, M. C., ... & Dall'Osto, M.

(2014). Measurements of the aerosol chemical composition and mixing state in the Po Valley using

multiple spectroscopic techniques. Atmospheric Chemistry and Physics Discussions, 14(7), 9275-9343.

10

Fortner, E. C., Brooks, W. a., Onasch, T. B., Canagaratna, M. R., Massoli, P., Jayne, J. T., Franklin, J. P.,

Knighton, W. B., Wormhoudt, J., Worsnop, D. R., Kolb, C. E. and Herndon, S. C.: Particulate Emissions

Measured During the TCEQ Comprehensive Flare Emission Study, Ind. Eng. Chem. Res., 51(39),

12586–12592, doi:10.1021/ie202692y, 2012.

11

Gilardoni, S., Massoli, P., Giulianelli, L., Rinaldi, M., Paglione, M., Pollini, F., ... & Fuzzi, S. (2014). Fog

scavenging of organic and inorganic aerosol in the Po Valley. Atmospheric Chemistry and Physics

Discussions, 14(4), 4787-4826.

12

Happonen, M., Mylläri, F., Karjalainen, P., Frey, A., Saarikoski, S., Carbone, S., Hillamo, R., Pirjola, L.,

Häyrinen, A., Kytömäki, J., Niemi, J. V, Keskinen, J. and Rönkkö, T.: Size distribution, chemical

composition, and hygroscopicity of fine particles emitted from an oil-fired heating plant., Environ. Sci.

Technol., 47(24), 14468–75, doi:10.1021/es4028056, 2013.

13Lee, A. K. Y., Willis, M. D., Healy, R. M., Onasch, T. B. and Abbatt, J. P. D.: Single particle

characterization using the soot particle aerosol mass spectrometer (SP-AMS), ACPD, 2014.

14

Liu, D., Allan, J., Whitehead, J., Young, D., Flynn, M., Coe, H., McFiggans, G., Fleming, Z. L. and Bandy,

B.: Ambient black carbon particle hygroscopic properties controlled by mixing state and composition,

Atmos. Chem. Phys., 13(4), 2015–2029, doi:10.5194/acp-13-2015-2013, 2013.

15

Massoli, P., Fortner, E. C., Canagaratna, M. R., Williams, L. R., Zhang, Q., Sun, Y., Schwab, J. J., Trimborn,

A., Onasch, T. B., Demerjian, K. L., Kolb, C. E., Worsnop, D. R. and Jayne, J. T.: Pollution Gradients and

Chemical Characterization of Particulate Matter from Vehicular Traffic near Major Roadways: Results

from the 2009 Queens College Air Quality Study in NYC, Aerosol Sci. Technol., 46(11), 1201–1218,

doi:10.1080/02786826.2012.701784, 2012.

16

Nordin, E. Z., Eriksson, a. C., Roldin, P., Nilsson, P. T., Carlsson, J. E., Kajos, M. K., Hellén, H., Wittbom,

C., Rissler, J., Löndahl, J., Swietlicki, E., Svenningsson, B., Bohgard, M., Kulmala, M., Hallquist, M. and

Pagels, J. H.: Secondary organic aerosol formation from idling gasoline passenger vehicle emissions

investigated in a smog chamber, Atmos. Chem. Phys., 13(12), 6101–6116, doi:10.5194/acp-13-6101-

2013, 2013.

17

Onasch, T. B., Trimborn, A., Fortner, E. C., Jayne, J. T., Kok, G. L., Williams, L. R., Davidovits, P. and

Worsnop, D. R.: Soot Particle Aerosol Mass Spectrometer: Development, Validation, and Initial

Application, Aerosol Sci. Technol., 46(7), 804–817, doi:10.1080/02786826.2012.663948, 2012.

18

Saarikoski, S., Carbone, S., Cubison, M. J., Hillamo, R., Keronen, P., Sioutas, C., ... & Jimenez, J. L.

(2014). Evaluation of the performance of a particle concentrator for online instrumentation.

Atmospheric Measurement Techniques, 7(7), 2121-2135.

19

Taylor, J. W., Allan, J. D., Liu, D., Flynn, M., Weber, R., Zhang, X., ... & Coe, H. (2014). Assessment of the

sensitivity of core/shell parameters derived using the single-particle soot photometer to density and

refractive index.

20

Willis, M. D., Lee, A. K. Y., Onasch, T. B., Fortner, E. C., Williams, L. R., Lambe, A. T., Worsnop, D. R. and

Abbatt, J. P. D.: Collection efficiency of the Soot-Particle Aerosol Mass Spectrometer (SP-AMS) for

internally mixed particulate black carbon, Atmos. Meas. Tech. Discuss., 7(5), 5223–5249,

doi:10.5194/amtd-7-5223-2014, 2014.

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Outline

• SP-AMS hardware

• Nomenclature

• Quantification

– Collection Efficiencies

– Sensitivities

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SP-AMS hardware

• SP Module

– New vaporizer to AMS

– New ionization chamber configuration

– Three potential vaporizer configurations

• ADQ and ePTOF 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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Suggested Modifications

• Pump and intracavity lasers are class IV lasers. All class IV lasers need to be fully enclosed with interlocks that shut down the lasers when the enclosures are opened.

– Following up with James Allan about how they modified their instrument

• Need computer logged laser diagnostics– Ideally, this might be USB connection to laser electronics box to control laser and obtain pump

and intracavity laser intensities and Nd:YAG crystal temperatures– Access to CCD camera during operations and logging of the CCD camera output

• Currently, can log CCD camera data, but very complicated, too much data is saved, and we have not successfully done this…

• Do all Laser electronics have the laser ON/OFF capabilities?• Need labeling and a description of how this works (Amewu)

• It is not currently clear how useful the photo-diode laser detector is or how it is being used

• Appears to be location sensitive, especially compared with thermal-based laser intensity monitors and even the camera

• Micrometers on laser adjustment knobs: laser tuning adjustment knobs are fine, but without a micrometer like setup, there is no good method for adjusting and returning the same tunings…

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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 Matter

NR = Non-Refractory

R = Refractory

L = Light Absorbing (1064 nm)

LR-PM:

1. Refractory Black Carbon (rBC)

2. Metals

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Quantification

• Collection Efficiencies

– Tungsten Vaporizer

– Laser Vaporizer

• Sensitivities

– Refractory black carbon (rBC) [Laser]

– Non-Refractory PM [Laser and Tungsten]

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Tungsten Vaporizer Collection Efficiency

EL = Aerodynamic Lens transmission

EB = Incomplete vaporization due to particle Bounce

ES = Particle beam divergence due to particle Shape (and size)

EL ~ 1 for dva = 70-700 nm

EB ~ 0.5 due to solid/refractory particle bounce

ES = 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 Laser Vaporizer

Beam width probe measurement

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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SP-AMS CE’s

Vaporizer-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

wire motion

Particle beam

BWP wire

diameter

Measuring CELaser = ES

Beam Width Probe (BWP)

Huffman et al. 2005 Willis et al., 2014

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Laser and Particle Beam Widths

• Particle beam widths: DOS coated Regal black ~ pure DOS particles• Laser beam width (s) is ~ 0.1 mm• Use BWP for CE determination in future

Typ

ical

Am

bie

nt

Ran

ge

Salcedo et al.,2007

Tungsten vaporizer (3.8 mm)

Willis et al., 2014

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CE vs PBW

• CELaser ~ ES is a strong function of Particle Beam Width

• BWP will help make SP-AMS measurements independent

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BES coating experiments

Willis, Lee et al., 2014

University of Toronto – Abbatt lab

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CELaser as function of RBC

Willis et al., 2014

rBC

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CalNex 2010

• Observe similar RBC-dependent CE for rBC in field

• Not expected to be same, as NR-PM in ambient is

likely significantly different than liquid BESMassoli et al., 2014

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SP-AMS Sensitivities

• rBC

– Refractory carbon ion distribution dependent?

– Black carbon particle type dependent?

• NR-PM

– Vaporizer dependent?

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Refractory Carbon Ion Spectra

• Different rBC particle types

generate different

refractory carbon ion

distributions

• Fullerene ions are

detected where expected

and not otherwise

• All rBC particle types

exhibit low carbon ion

signal (C1+-C5

+)

Onasch et al., 2014

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C1+-C5

+ vs HRBC

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HRBC calibration plot

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C1+-C5

+ Calibration Plot

• Regal black and fullerene soot appear to agree reasonably well

• Aquadag is significantly lower (ES < 1 ?)

• Suggests low carbon (C1+ – C5

+) be used for quantification

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Laser-induced ion generation

• Fullerene ions generated in laser (with electron beam off)

• Larger ions generated more easily

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C1+ – C3

+ Ratios

Corbin et al., 2014

More Graphitic

Less Graphitic

• Need more work to verify quantification of rBC

for various particle types

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• Distinct combustion sources

generate different SP-AMS

refractory carbon ion mass

spectra (both in terms of carbon

ion distributions and C1+/C3

+

ratios)

• Potential to provide insights into

ambient particulate sources

Emissions

Measurements

Caldecott Tunnel Dallmann et al., 2014

FLAME3 McMeeking et al., JGR 2009

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Is the SP-AMS NR-PM

measurement sensitivity

vaporizer dependent?

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CELaser as function of RBC

Willis et al., 2014

rBC

NR-PM

(BES)

• Laser and Tungsten

vaporizers

• Correlated CE’s for

rBC and NR-PM

• NR-PM sensitivity is

rather large

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Laser OFF/ON ambient results

Lee et al., 2014

HOA

OOA

COA

• Increase in signal with laser ON for Org

components related to BC particles

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Effects on relative coat-core

measurements

• SP-AMS measures composition down to at least 5% rBC by mass

(i.e., small core, large coating) once corrected

• Uncorrected relative results appear decent, but more work needs to

be done to verifyWillis et al., 2014 – U Toronto

• fBC measurements up to 50% low

• RBC measurements up to 2X high

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Summary• Hardware: Working to optimize ionization chamber configurations.

• Nomenclature: Corbin et al. have set SP-AMS terminology based on

vaporization temperature (instrument and particle specific) and laser-

light absorbing (particle specific) properties.

• Collection efficiency: Willis et al. have shown that ES dominates SP-

AMS CE, which can be quantified with BWP measurements.

• Sensitivity (rBC): Low carbon (C1+ – C5

+) ion signals are likely best

for quantification. Working on assessing rBC quantification for

different BC particle types (i.e., Sensitivity vs CE). Refractory carbon

ion distributions appear to be related to BC chemical composition (i.e.,

graphitization).

• Sensitivity (NR-PM): NR-PM mIE from laser vaporizer appears to be

greater than NR-PM mIE from tungsten vaporizer; working on

quantifying.

SP-AMS technology is rapidly maturing and opening

new avenues for studying absorbing, refractory particles