Final Report
Cooperative Research Agreement
CX 825834
Carbonaceous Aerosol and Smoke over the Eastern US
Prepared by:
Rudolf B. Husar
Center for Air Pollution Impact and Trend Analysis CAPITA,
Washington University
Saint Louis, Missouri 63130-4899
Submitted to Project Officer:
Kenneth Shere
U.S. Environmental Protection Agency
Office of Research and Development
Research Triangle Park, NC 27711
May 30, 2001
Contents
Aerosol Types: ‘Dust’, ‘Smoke’ and ‘Haze’
Objectives and Approach to the Analysis
Smoke Physical, Chemical and Optical
Properties
Chemical Properties: Detection of Organics is
Problematic
Spatio-Temporal Pattern of Carbonaceous
Aerosol
Organic and Absorbing Carbon – IMPROVE
Carbonaceous Aerosol Components
Cumulative Seasonal PM2.5 Composition
New England: Chemical Mass Balance
Mid-Atlantic: Chemical Mass Balance
Central EUS: Chemical Mass Balance
Peripheral Sites: Chemical Mass Balance
New England: Carbonaceous Mass Balance
Mid-Atlantic: Carbonaceous Mass Balance
Central EUS:
Carbonaceous Mass Balance
Peripheral Sites: Carbonaceous Mass Balance
Semi-Quantitative Satellite and other
Observations
Fire Locations and TOMS Smoke Pattern
Satellite Images if Smoke Plumes over the
Southeast
Smoke Plumes over the Southeast
Smoke Aerosol and Ozone During the Smoke
Episode – Inverse Relationship.
Hourly PM10 During the Smoke Event
Smoke Composition at Big Bend, TX
Central American Smoke Pattern, April, 2000
·
Aerosol are composed of multiple types including
urban-industrial sulfates, nitrates and organics (industrial haze), biomass
smoke and windblown dust.
· Each type may be considered a different pollutant since it has its own class of sources, aerosol properties and associated with different effects.
· In this sense dust, smoke and haze are aerosol equivalents of the gaseous pollutants, SO2, NOx and CO but under the current regulations they are lumped under PM2.5 and PM10.
This section focuses on the ‘smoke’ portion of the North American aerosol. It will also include discussion of the carbonaceous aerosol in general.
·
There is considerable evidence that smoke from
biomass fires constitutes a significant component of the aerosol over North
America, particularly in the PM2.5 size range.
· However, both the recent and previous research results on smoke are fragmented, and uneven in spatial, temporal and compositional coverage.
An integrated assessment of the North American smoke using the rich literature and the most recent data would be most desirable.
·
Explore qualitatively the spatio-temporal and chemical
pattern of smoke over North America
Characterize spatio-temporal features of smoke dust from the different sources
·
Integrate data from surface and satellite
observations
·
Combine spatial, temporal and compositional analysis
Invite the community to actively particulate in conducting this open, integrative analysis
·
Recent data from several satellite and surface sensors
were analyzed and presented graphically
· The data and knowledge from the literature has not yet been incorporated
An open discussion and interaction with the community is to begin in June 2001
·
NARSTO-PM Assessment.
NARSTO is conducting a PM Assessment for North America. This work supports
the NARSTO PM Assessment process.
· Monitoring Network Design/Evaluation. EPA is implementing an extensive monitoring network for speciated PM sampling. This work supports the design and performance-evaluation of the new network.
· MODELS-3 Evaluation. EPA’s MODELS-3/CMAQ is a sophisticated high resolution, regional-scale modeling system designed to simulate and investigate gaseous and fine pattern over the US. This work supports the evaluation and further development of the model.
Regional Haze Management. In response to the new haze regulations, Regional Planning Organizations (RPOs, Central States, Northeast OTC, Western States ) have been set up for haze management. This work is to provide background information to be used by the RPOs.
·
Physical - size distribution and shape
o
Determines the
atmospheric residence time, optical properties
· Chemical – elemental and molecular composition
o
Influences
optical properties and other effects on health
Serves as source fingerprint
·
Optical –
refractive index
o
Influences
effects on visibility and climate
o
Allows detection
by remote sensing

Hegg and Hobbs, as part of the TARFOX project conducted airborne organics
measurements. They found that the organics fraction
of fine mass increases with elevation and the total fine carbon correlates well
with the light absorption. Hence, they
reason that the carbonations aerosol originated from combustion sources. Smoke from biomass smoke is a plausible
source.


Source: IMPROVE, Sisler & Malm
Organics and light absorbing carbon are most abundant in the Southeast

Carbonaceous aerosols (Organics + Light Absorbing Carbon) are most abundant
over the East and West Coasts.
PM2.5 chemical components were calculated based on the CIRA methodology
.
· In addition, the the organics were (tentatively) further separated as Primary Smoke Organics (red) and Remainder organics (purple)
o PSO = 20*(K - 0.15*Si – 0.02* Na)
o Remainder Org = Organics - PSO
· Also, the ‘Unknown’ mass (white area) is the difference between the gravimetrically measured and the chemically reconstructed PM2.5.

· The daily chemical composition was aggregated over the available IMPROVE data range (1988-99) to retain the seasonal structure.
In order to reduce the noise, the daily data were smoothed by a 15-day moving average filter.
·
For this work the IMPROVE sites were grouped as
follows:
o
New England
o
Mid-Atlantic
o
Central EUS
o
Peripheral
· For each region, the seasonality is displayed for:
o
Chemical Mass
Balance
o
Carbonaceous
Mass Balance
“Smoke Organics” Percentiles


The concentration of organics and ‘smoke organics’ is low over the Northeast
·
At the Mid-Atlantic region, carbonations aerosol are
25-40% of the fine mass
· The seasonality of organics and ‘smoke organics’ is pronounced
· In Washington DC, there is a winter peak that is largely contributed by organics organics and ‘smoke organics’

·
The pattern of the Central EUS is similar to the
Mid-Atlantic region
· However, several stations show multiple peaks

·
Eastern N. America is surrounded by aerosol source
regions such as Sahara and Central America.
As a consequence, the PM concentration at the ‘edges’ ranges between 4-15 ug/m3; much of it originating outside.
The chemical composition of the inflow varies by location and season.
· At the Everglades, organics, ‘smoke organics’ and LAC dominate over sulfate and fine dust
·

Sahara dust, and smoke from Central America and W. US/Canada are the main
contributions to Everglades, FL, and Big Bend, TX.
·
Carbonaceous aerosols peak in the summer at 2-3 mg/m3.
· At Moosehorn, ‘smoke organics’ exceeds organics.

·
The seasonality of carbonaceous aerosol vary
· Shenandoah is strongly summer peaked
· Washington DC and Jefferson have summer and winter peaks
· Dolly Sods and Brigantine are mildly seasonal

Except for Jefferson, the ‘smoke organics’ are a small fraction of the total
organics
·
Throughout the Central EUS, the carbonaceous aerosol
contributes 4-6 mg/m3
· There is a 50% seasonal variation with a summer peak
‘Smoke Organics’ constitute 20-30% of the total organics

At the northern peripheral sites, Badlands, Voyageurs and Acadia, the organics range from 1.5 to 4 mg/m3
· At Big Bend the organics show a spring peak, with a majority of ‘smoke organics’. This indicates biomass smoke origin.

At the Everglades, the fall peak is due to organics, while ‘smoke organics’
light absorption is present throughout the year.
·
Infrared satellite sensors on NOAA polar satellites
detect the location of fires under cloud-free conditions
· The daily fire location data are routinely processed by ESA
· In 1998, the highest fire density was over Central America in April-May.
In July, fires were observed throughout the and particularly in N. Canada.
·

For April and May 1998, the TOMS satellite data show major
plumes of absorbing aerosol (smoke) dispersing from the Central American fires.


During the fall season, fires and biomass smoke can be
observed throughout the southeastern US.
During a St. Louis – Atlanta flight, December 1998 over a dozen biomass smoke plumes were photographed.

Satellites now allow detection of fire locations through out the world.
For example, in December 1998, the fires recorded by the ESA IONIA
Program are indicated below.

On a single day, an astronaut photo of North Carolina reveals over a dozen
individual smoke plumes. These are presumed to be biomass fires.

Color SeaWiFS image of the smoke plumes originating from Kentucky, Nov 15, 1999.

Enhanced smoke image
Smoke from the major Idaho Fires in August 2000 was tracked through the Absorbing Aerosol Index product from the TOMS ozone sensor.

Satellite detection yields the origin, location, and shape of smoke plumes.

·
The influence of
smoke is to increase the reflectance at short wavelength (0.4 mm)

·
At longer wavelength, the aerosol reflectance is
insignificant.
During a ten-day period, May 7-17, 1998, smoke from numerous widespread fires in Central America drifted northward and caused severe perturbation of the atmospheric environment over parts of Eastern North America. A draft paper describes the impact of the Central American smoke on the on the atmospheric environment of Eastern North America.

·
Fire locations detected by the Defense
Meteorological Satellite Program (DMSP) sensor.
The sensor detects low levels of visible night at night.
·
Satellite image of color SeaWiFS data, contours of TOMS satellite data (green) and surface extinction coefficient, Bext. The smoke plume extends from Guatemala to Hudson Bay in Canada. The Bext values indicate that the smoke is present at the surface


Extinction Coefficient (visibility)

Surface Ozone
The surface ozone is generally depressed under the smoke cloud.

Hourly PM10 concentration pattern at six eastern US locations during May 1998.

Daily average light scattering coefficient and chemically speciated fine mass
concentration for the IMPROVE monitoring site at Big Bend, TX, May 1998.

The May major 1998 Central American smoke event was not a unique phenomenon. On
April 25, 2000, the intense smoke plume was similar to the ’98 event. The plume covers part of Florida.