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Fine Particle Composition Measured During ICARTT, Exams of Inorganic Chemistry

Georgia Institute of Technology School of Earth and Atmospheric Sciences. Roadmap. A. Measurement overview. Statistics, altitude profile, charge balance.

Typology: Exams

2022/2023

Uploaded on 05/11/2023

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The School of Earth and
Atmospheric Sciences
Fine Particle Composition
Measured During ICARTT _ An
Overview Of Inorganic Ions And
Water Soluble Organic Carbon
Rick Peltier
Amy Sullivan
Chris Hennigan
Rodney Weber
Charles A. Brock
Joost de Gouw
John Holloway
Additional Acknowledgements:
Ann Middlebrook, Brendan Matthews, Adam Wollny, Carsten Warneke,
Donna Sueper, and the rest of the NOAA AL team.
Support: NOAA
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The School of Earth and

Atmospheric Sciences

Fine Particle Composition

Measured During ICARTT _ An

Overview Of Inorganic Ions And

Water Soluble Organic Carbon

Rick Peltier

Amy Sullivan

Chris Hennigan

Rodney Weber

Charles A. Brock

Joost de Gouw

John Holloway

Additional Acknowledgements:

Ann Middlebrook, Brendan Matthews, Adam Wollny, Carsten Warneke,

Donna Sueper, and the rest of the NOAA AL team.

Support: NOAA

Roadmap

A. Measurement overview

Statistics, altitude profile, charge balance

B. Case Study 1: Aerosol source variability

C. Case Study 2: Urban aerosols that are

subjected to power plant influence.

D. Summary

Observed Plume Types

l Relatively pure biomass

– High WSOC and

Acetonitrile concs.

– Well-correlated WSOC &

Acetonitrile

– Little sulfate

l Mixed Biomass/Regional

(Flt 040722)

– High WSOC, acetonitrile,

sulfate.

l Urban/Regional

– High sulfate, lower WSOC

(~<4 mgC m

WSOC (

m

gC m

Acetonitrile (pptv)

Biomass

Slope: 0.

R

2

Mixed Plume

Urban/Regional

Biomass (smoke)

Observation Overview

l Sulfate, WSOC, Ammonium often

observed. Occasional nitrate (usually

biomass).

l Sulfate well correlated with volume in

urban/regional and mixed plumes,

while WSOC correlated with volume in

all plumes (strongest in biomass)

l Significant variability in aerosol

concentrations.

WSOC (

m^ gC m

Fine Volume ( mm^3 cm -3) Biomass Slope: 0.184 ± 0. Int: 0.236 ± 0. R^2 = 0. Mixed Slope: 0.103 ± 0. Int: 3.544 ± 0. R^2 = 0. Urban/Regional Slope: 0.092 ± 0. Int: 0.726 ± 0. R^2 = 0. 30 25 20 15 10 5 0 Sulfate ( m^ g m

Fine Volume ( mm^3 cm-3) Mixed Slope: 0.371 ± 0. Int: -5.457 ± 0. R^2 = 0. Urban/Regional Slope: 0.411 ± 0. Int: -0.522 ± 0. R^2 = 0. Biomass Slope: -0.008 ± 0. Int: 2.220 ± 1. R^2 = 0.

Additional Analysis of Altitude Profile l Species/fine volume median of 500m bins. l Little change in fraction for sulfate and biomass- derived WSOC. l Increase in WSOC/fine volume fraction with altitude.

Altitude (meters - bin centroid)

(Species/Fine Particle Volume)

Sulfate

Biomass WSOC

Urban/Regional WSOC

Charge Balance Along Altitude l Measured aerosol ionic components generally in charge balance (especially at high alt) l Many events where net charge is negative – driven by sulfate, and most frequently at low alt. (i.e. excess sulfate not balanced by ammonium) l Transient events of positive net charge during biomass events – suggest unmeasured organic acid as anion pair (to NH 4

?). 6000 5000 4000 3000 2000 1000 0 Altitude (m) -0.3 -0.2 -0.1 0.0 0. Net Charge (meq m

)

Sulfate/Fine Particle Volume^ Biomass Mixed Urban/Regional Biomass

Case Study 2: Flight 040815 Plumes over Atlanta, GA.

Latitude -85.5 -85.0 -84.5 -84.0 -83.5 -83. Longitude Georgia Alabama 80100120140160180 CO (ppbv) Wind Direction and Speed SO 2 Source (scaled by '99 emissions)

X
B A
C

D E 5 4 3 2 1 WSOC (μgC m

  • ) 18: 8/15/ 18:30 19:00 19:30 20: UTC 200 180 160 140 120 100 80 CO (ppbv) 50 40 30 20 10 0 Fine Volume (μm3 cm
  • ) 5 4 3 2 1 0 Altitude (km) 30 25 20 15 10 5 0 SO (^2) (ppbv) 15 10 5 0 Sulfate (μg m
  • ) A B C D E X Molar Ratio 1.56 1.21 2.12 1. (ammonium/sulfate) 1 2 3 3-sec WSOC (^) WSOC-CO: R^2 = 0. SO 2 and SO 4 = spikes from local power plants

Case Study 2: Flight 040815 Plumes over Atlanta, GA. 5 4 3 2 1 WSOC (μgC m

  • ) 18: 8/15/ 18:30 19:00 19:30 20: UTC 200 180 160 140 120 100 80 CO (ppbv) 50 40 30 20 10 0 Fine Volume (μm3 cm
  • ) 5 4 3 2 1 0 Altitude (km) 30 25 20 15 10 5 0 SO (^2) (ppbv) 15 10 5 0 Sulfate (μg m
  • ) A B C D E X Molar Ratio 1.56 1.21 2.12 1. (ammonium/sulfate) 1 2 3 Little WSOC enhancement in Power Plant Plumes

Latitude -85.5 -85.0 -84.5 -84.0 -83.5 -83. Longitude Georgia Alabama 80100120140160180 CO (ppbv) Wind Direction and Speed SO 2 Source (scaled by '99 emissions)

X
B A
C
D
E

Summary (2/2)

l Case Study 1: example of aerosol source

variability.

– Higher [sulfate/fine volume] in power generation

regions, higher [WSOC/fine volume] in urban outflow

l has implications on O 3 chemistry, Brown et al., Science,

submitted.

l Case Study 2: urban SO

and WSOC w/ local

power plant plumes.

– Sulfate composed of background (NH 4

/SO 4

2-

~ 2) that

is enhanced (~x2) by distinct high-concentration

sulfate plumes (NH 4

/SO 4

2-

– WSOC correlated with CO, little enhancement in fresh

PP plumes.