skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Optical Properties of Individual Tar Balls in the Free Troposphere

Journal Article · · Environmental Science and Technology
ORCiD logo [1];  [2];  [3]; ORCiD logo [4];  [3];  [5];  [4]; ORCiD logo [3];  [6]; ORCiD logo [3]
  1. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Michigan Technological University, Houghton, MI (United States)
  2. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); The Ohio State University, Columbus, OH (United States)
  3. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  4. Michigan Technological University, Houghton, MI (United States)
  5. Italian National Research Council, Bologna (Italy). Institute of Atmospheric Sciences and Climate (ISAC); University of Vienna (Austria)
  6. Italian National Research Council, Bologna (Italy). Institute of Atmospheric Sciences and Climate (ISAC)

Tar balls are brown carbonaceous particles, highly viscous, spherical, amorphous, and light absorbing. They are believed to form in biomass burning smoke plumes during transport in the troposphere. Tar balls are believed to have a significant impact on the Earth’s radiative balance, but due to poorly characterized optical properties, this impact is highly uncertain. Here, we investigate the chemical composition and optical properties of individual tar balls transported in the free troposphere to the Climate Observatory “Ottavio Vittori” on Mt. Cimone, Italy (2165 meters above sea level) using multi-modal micro-spectroscopy. Our results show that tar balls contributed 50% of carbonaceous particles by number in the size range from 0.25 to 1.8 µm. Of those tar balls, 16% were inhomogeneously mixed with other constituents. Using electron energy loss spectroscopy, we retrieved the complex refractive index from 200 to 1200 nm for both inhomogeneously and homogeneously mixed tar balls. We found no significant difference in the average refractive index of inhomogeneously and homogenously mixed tar balls (1.40 - 0.03i, and 1.36 - 0.03i at 550 nm, respectively). Furthermore, we estimated the top of the atmosphere radiative forcing using the Santa Barbara DISORT Atmospheric Radiative Transfer model (SBDART) and found that a layer of only tar balls with an optical depth of 0.1 above vegetation would exert a positive radiative forcing ranging from 2.8 Wm-2 (on a clear sky day) to 9.5 Wm-2 (when clouds are below the aerosol layer). In conclusion, understanding the optical properties of tar balls can help reduce uncertainties associated with the contribution of biomass-burning aerosol in current climate models.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
AC05-76RL01830; AC02-05CH11231
OSTI ID:
2205586
Report Number(s):
PNNL-SA-185434
Journal Information:
Environmental Science and Technology, Vol. 57, Issue 44; ISSN 0013-936X
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (40)

Brown carbon absorption in the red and near-infrared spectral region journal January 2017
Spectrally-invariant behavior of zenith radiance around cloud edges simulated by radiative transfer journal January 2010
Characterization of light-absorbing carbon particles at three altitudes in East Asian outflow by transmission electron microscopy journal January 2013
Brown Carbon Spheres in East Asian Outflow and Their Optical Properties journal August 2008
Atmospheric Ice Nucleating Particle measurements at the high mountain observatory Mt. Cimone (2165 m a.s.l., Italy) journal December 2017
Optical Properties of Secondary Organic Aerosol Produced by Nitrate Radical Oxidation of Biogenic Volatile Organic Compounds journal February 2021
A technology-based global inventory of black and organic carbon emissions from combustion journal January 2004
Brown carbon in tar balls from smoldering biomass combustion journal January 2010
CO2 emissions from C40 cities: citywide emission inventories and comparisons with global gridded emission datasets journal February 2023
Atmospheric tar balls: Particles from biomass and biofuel burning: ATMOSPHERIC TAR BALLS journal March 2004
Optical Properties of Airborne Soil Organic Particles journal September 2017
Morphology, composition and mixing state of individual carbonaceous aerosol in urban Shanghai journal January 2012
Atmospheric tar balls from biomass burning in Mexico journal January 2011
Do atmospheric aerosols form glasses? journal January 2008
Derivation of Optical Properties of Carbonaceous Aerosols by Monochromated Electron Energy-Loss Spectroscopy journal April 2014
Light Absorption by Carbonaceous Particles: An Investigative Review journal January 2006
Measurement report: Optical properties and sources of water-soluble brown carbon in Tianjin, North China – insights from organic molecular compositions journal May 2022
Automated Chemical Analysis of Internally Mixed Aerosol Particles Using X-ray Spectromicroscopy at the Carbon K-Edge journal October 2010
An amorphous solid state of biogenic secondary organic aerosol particles journal October 2010
Chemistry of Atmospheric Brown Carbon journal February 2015
Individual aerosol particles from biomass burning in southern Africa: 1. Compositions and size distributions of carbonaceous particles: SINGLE PARTICLES FROM SAVANNA BURNING journal March 2003
Evidence for Large Amounts of Brown Carbonaceous Tarballs in the Himalayan Atmosphere journal November 2020
Source-receptor matrix calculation with a Lagrangian particle dispersion model in backward mode journal January 2004
Heterogeneous chemistry of individual mineral dust particles with nitric acid: A combined CCSEM/EDX, ESEM, and ICP-MS study journal January 2005
Aerosol Composition, Mixing State, and Phase State of Free Tropospheric Particles and Their Role in Ice Cloud Formation journal November 2021
Oxygenated Interface on Biomass Burn Tar Balls Determined by Single Particle Scanning Transmission X-ray Microscopy journal June 2007
Individual aerosol particles from biomass burning in southern Africa: 2, Compositions and aging of inorganic particles: COMPOSITIONS AND AGING OF INORGANIC PARTICLES journal March 2003
Optical properties and bandgaps from low loss EELS: Pitfalls and solutions journal December 2008
Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume journal January 2015
Electron Energy-Loss Spectroscopy in the Electron Microscope book January 2011
Observations of Ice Nucleating Particles in the Free Troposphere From Western US Wildfires journal January 2021
SBDART: A Research and Teaching Software Tool for Plane-Parallel Radiative Transfer in the Earth's Atmosphere journal October 1998
Light absorption properties of laboratory-generated tar ball particles journal January 2016
Technical note: The Lagrangian particle dispersion model FLEXPART version 6.2 journal January 2005
Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke journal September 2019
Atmospheric tar balls: aged primary droplets from biomass burning? journal January 2014
Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles journal July 2013
Dynamic changes in optical and chemical properties of tar ball aerosols by atmospheric photochemical aging journal January 2019
Brown carbon in the continental troposphere: LIU ET. AL.; BROWN CARBON IN THE TROPOSPHERE journal March 2014
Optical, physical, and chemical properties of tar balls observed during the Yosemite Aerosol Characterization Study journal January 2005