Estimation of hygroscopic growth for ambient single particles · 2 10 3 10 4 10 5 or 150-191 nm...

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Estimation of hygroscopic growth for ambient single particles IAC Busan 30 Aug 2014 Robert Healy , Greg Evans, Michael Murphy, Zsofia Juranyi, Torsten Tritscher, Ernest Weingartner, Martin Gysel, Laurent Poulain, Katharina Kamilli, Alfred Wiedensohler , Ian O’Connor, Eoin McGillicuddy, John Sodeau, John Wenger

Transcript of Estimation of hygroscopic growth for ambient single particles · 2 10 3 10 4 10 5 or 150-191 nm...

Page 1: Estimation of hygroscopic growth for ambient single particles · 2 10 3 10 4 10 5 or 150-191 nm 191-244 nm 244-312 nm 312-399 nm 399-511 nm 511-653 nm 653-835 nm 835-1067 nm Box-plot

Estimation of hygroscopic growth for ambient

single particles

IAC Busan 30 Aug 2014

Robert Healy, Greg Evans, Michael Murphy, Zsofia Juranyi, Torsten Tritscher,

Ernest Weingartner, Martin Gysel, Laurent Poulain, Katharina Kamilli, Alfred

Wiedensohler, Ian O’Connor, Eoin McGillicuddy, John Sodeau, John Wenger

Page 2: Estimation of hygroscopic growth for ambient single particles · 2 10 3 10 4 10 5 or 150-191 nm 191-244 nm 244-312 nm 312-399 nm 399-511 nm 511-653 nm 653-835 nm 835-1067 nm Box-plot

2

Overview

- Background on particle composition and hygroscopicity

- The Aerosol Time-of-Flight Mass Spectrometer

- Predicting hygroscopic growth for single particles

- Conclusions and future directions

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Background – hygroscopicity (single component)

Organic aerosol (OA)

Black carbon (BC)

(NH4)2SO4

90 % RH

Growth factor (GF) for BC ~1, for OA ~1.2 and for (NH4)2SO4 ~1.66 at 90% RH

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Background – hygroscopicity (mixture)

Organic aerosol (OA)

Black carbon (BC) 90 % RH

???

(NH4)2SO4

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Traditional growth factor predictions based on the ZSR

mixing rule

The Zdanovskii–Stokes–Robinson (ZSR) mixing rule is often used to

predict hygroscopic growth for bulk aerosol mixtures (gmix)*:

𝑔𝑚𝑖𝑥 ≈

𝑖

𝑁

𝜀𝑖𝑔𝑖3

13

where N is the number of species, εi is the volume fraction of species i and

gi is the growth factor of species i

*Zdanovskii, 1948 / Stokes & Robinson 1966

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• Bulk aerosol ZSR mixing rule example for RH = 90%:

• Mass fractions of OA, BC and (NH4)2SO4 can be converted to volume

fractions using densities of separate components

• The GF and volume fraction of each component species can be used to

predict the GF of the bulk mixture:

𝑔𝑚𝑖𝑥 ≈

𝑖

𝑁

𝜀𝑖𝑔𝑖3

13

*e.g. Gysel et al. 2004, 2007

GFmix = 1.41

*GF = 1.66

*GF = 1 *GF = 1.20

Bulk aerosol ZSR mixing rule example

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Single particle hygroscopicity?

• What about ambient particle populations like this:

• Internally/externally mixed species

• Different particle compositions will lead to different growth behaviours at a

given RH

• Using bulk aerosol composition is not representative

?????RH = 90%

Page 8: Estimation of hygroscopic growth for ambient single particles · 2 10 3 10 4 10 5 or 150-191 nm 191-244 nm 244-312 nm 312-399 nm 399-511 nm 511-653 nm 653-835 nm 835-1067 nm Box-plot

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Overview

- Background on particle composition and hygroscopicity

- The Aerosol Time-of-Flight Mass Spectrometer

- Predicting hygroscopic growth for single particles

- Conclusions and future directions

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Single particle sampling- online:

Aerosol Time-of-Flight Mass Spectrometer (ATOFMS)

- Detection of organic aerosol, inorganics, metals and rBC

- High time resolution (1 s)

- Size resolved data (150-3000 nm)

*

*TSI Inc. (Model 3800)

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Single particle sampling- online:

ATOFMS

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Single particle sampling- online:

ATOFMS

- Single particle information retained

- Enables source identification and investigation of chemical processing

- Data typically qualitative only

Data output:Single particlemixing state(qualitative)

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Quantitative approach

- Derived ATOFMS mass spectral relative sensitivity factors (RSF) for OA, BC,

NH4, NO3 and SO4 constrained using support AMS and MAAP data

- Calculated quantitative chemical composition estimates for each single particle

*Healy et al. Atmos. Chem. Phys. 2013

RSF

*

quantitative

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Overview

- Background on particle composition and hygroscopicity

- The Aerosol Time-of-Flight Mass Spectrometer

- Predicting hygroscopic growth for single particles

- Conclusions and future directions

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• Particles assumed to be composed of only BC, OA NH4, SO4 and NO3

• Inorganics combined and assigned hygroscopic properties of (NH4)2SO4

• The GF and volume fraction of BC, OA and inorganic aerosol (IA) are used

to predict the GF of each single particle at 90% RH:

𝑔𝑚𝑖𝑥 ≈

𝑖

𝑁

𝜀𝑖𝑔𝑖3

13

*e.g. Gysel et al. 2004, 2007

GFmix = 1.41

*GF = 1.66

*GF = 1 *GF = 1.20

Single particle ZSR mixing rule approach

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Single particle GF vs size for Paris, France

*Healy et al. J. Geophys. Res. 2014

*

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Single particle GF vs size for Paris, France

*Healy et al. J. Geophys. Res. 2014

*

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GF probability density function for different sizes

110 nm

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GF probability density function for different sizes

165 nm

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GF probability density function for different sizes

265 nm

Page 20: Estimation of hygroscopic growth for ambient single particles · 2 10 3 10 4 10 5 or 150-191 nm 191-244 nm 244-312 nm 312-399 nm 399-511 nm 511-653 nm 653-835 nm 835-1067 nm Box-plot

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External mixing of 165 nm particles

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ATOFMS GF predictions vs HTDMA GF measurements

PARIS

SIRTA

LHVP

20km

GOLF

Livry

- ‘MEGAPOLI’ winter campaign site locations

Hygroscopicity tandem differential mobility analyser (HTDMA)

ATOFMS

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ATOFMS predicted GF vs HTDMA measured GF

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ATOFMS vs HTDMA GF temporal correlation

Continental air mass periods only

Total dataset

26. Jan 2010 18:00 to 21:00

-5 0 5 10 15 20 25 3042

44

46

48

50

52

54

56

[ns/kg]0.005 0.01 0.02 0.04 0.08 0.16 0.32 0.64 1.28 2.56

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Conclusions

• ATOFMS data can be used to predict hygroscopic growth

• Single particle information can be used to generate a growth factor

probability density function (GF-PDF) analogous to that measured by

HTDMA

• External mixing can be determined for particles of a given diameter

• Predicted and measured mean GF values agree within 6% for 110 nm, 165

nm particles and 265 nm particles in Paris, France

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Future Directions

• ATOFMS and HTDMA measurements at the same site

• Coupling of ATOFMS and support instrumentation to the outflow of HTDMA

would avoid uncertainty introduced by particle shape and density assumptions

• Use size-resolved relative sensitivity factors for ATOFMS (e.g. use a soot

particle aerosol mass spectrometer)

Page 26: Estimation of hygroscopic growth for ambient single particles · 2 10 3 10 4 10 5 or 150-191 nm 191-244 nm 244-312 nm 312-399 nm 399-511 nm 511-653 nm 653-835 nm 835-1067 nm Box-plot

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Thanks to…

• John Wenger, UCC

• Greg Evans, Michael Murphy, U of T

• Laurent Poulain, Katharina Kamilli, I f T

• Zsofi Juranyi, Marie Laborde, Martin Gysel,

Ernest Weingartner, PSI

QUESTIONS?

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Page 28: Estimation of hygroscopic growth for ambient single particles · 2 10 3 10 4 10 5 or 150-191 nm 191-244 nm 244-312 nm 312-399 nm 399-511 nm 511-653 nm 653-835 nm 835-1067 nm Box-plot

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Assumptions!

• All particles are spherical with a density of 1.5 g cm-3 for aerodynamic

diameter to mobility diameter conversions

• Ammonium, nitrate and sulphate in all forms have equivalent density to

ammonium sulphate

• Density of BC, OA and ‘inorganic aerosol’ is 2.0, 1.4 and 1.77 g cm-3

respectively

• ATOFMS ‘sees’ all particle types with equal efficiency at a given size

Page 29: Estimation of hygroscopic growth for ambient single particles · 2 10 3 10 4 10 5 or 150-191 nm 191-244 nm 244-312 nm 312-399 nm 399-511 nm 511-653 nm 653-835 nm 835-1067 nm Box-plot

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102

103

104

105

Sca

ling

fa

cto

r

150-

191

nm

191-

244

nm

244-

312

nm

312-

399

nm

399-

511

nm

511-

653

nm

653-

835

nm

835-

1067

nm

Box-plot of hourly size-dependent scaling factors for the entire measurement

period (n = 624). Median, 75th percentile and 90th percentile are denoted by

the solid line, box and whisker respectively.

Size-dependent number scaling factors

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Relative sensitivity factors by species

3

4

56

1

2

3

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10

2

3

4R

ela

tive

sen

sitiv

ity facto

r (a

rbitra

ry u

nits)

SO4

OANH4

NO3

BC

Box-plot of hourly mass spectral relative sensitivity factors (n = 610). Median,

75th percentile and 90th percentile are denoted by the solid line, box and

whisker respectively.

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ATOFMS reconstructed mass vs AMS/MAAP

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ATOFMS reconstructed composition vs AMS/MAAP

1.0

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ss f

ractio

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ATOFMS-derived bulk mass fractions

AMS/MAAP bulk mass fractions

OA NH4

NO3

SO4

BC

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ATOFMS reconstructed mass vs AMS

(size resolved)

Page 34: Estimation of hygroscopic growth for ambient single particles · 2 10 3 10 4 10 5 or 150-191 nm 191-244 nm 244-312 nm 312-399 nm 399-511 nm 511-653 nm 653-835 nm 835-1067 nm Box-plot

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Composition comparison between sites

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Composition comparison between sites

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ss c

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g m

-3)

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SIRTA LHVP

Organic aerosol

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Composition comparison between sites

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NH4

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Composition comparison between sites

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NO3

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Composition comparison between sites

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SIRTA LHVP

SO4


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one piece 653

one piece 653

WIND RIVER VxWORKS 653 PLATFORM 2.4 AND 2 · In partitions using the ARINC 653 APEX API, VxWorks 653 Platform supports several WIND RIVER VxWORKS 653 PLATFORM 2.4 AND 2.5.

WIND RIVER VxWORKS 653 PLATFORM 2.4 AND 2 · In partitions using the ARINC 653 APEX API, VxWorks 653 Platform supports several WIND RIVER VxWORKS 653 PLATFORM 2.4 AND 2.5.

Ward / Quartier 1...$K $K $K $ $K!C nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm …

Ward / Quartier 1...$K $K $K $ $K!C nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm nm …