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Title: Morphology of diesel soot residuals from supercooled water droplets and ice crystals: implications for optical properties

Abstract

Freshly emitted soot particles are fractal-like aggregates, but atmospheric processing often transforms their morphology. Morphology of soot particles plays an important role in determining their optical properties, life cycle and hence their effect on Earth’s radiative balance. However, little is known about the morphology of soot particles that participated in cold cloud processes. Here we report results from laboratory experiments that simulate cold cloud processing of diesel soot particles by allowing them to form supercooled droplets and ice crystals at -20 and -40°C, respectively. Electron microscopy revealed that soot residuals from ice crystals were more compact (roundness~0.55) than those from supercooled droplets (roundness ~0.45), while nascent soot particles were the least compact (roundness~0.41). Optical simulations using the discrete dipole approximation showed that the more compact structure enhances soot single scattering albedo by a factor up to 1.4, thereby reducing the top-of-the-atmosphere direct radiative forcing by ~63%. Lastly, these results underscore that climate models should consider the morphological evolution of soot particles due to cold cloud processing to improve the estimate of direct radiative forcing of soot.

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1239042
Alternate Identifier(s):
OSTI ID: 1226403; OSTI ID: 1239045
Report Number(s):
PNNL-SA-112661
Journal ID: ISSN 1748-9326
Grant/Contract Number:  
SC0010019; AC05-76RL01830
Resource Type:
Published Article
Journal Name:
Environmental Research Letters
Additional Journal Information:
Journal Name: Environmental Research Letters Journal Volume: 10 Journal Issue: 11; Journal ID: ISSN 1748-9326
Publisher:
IOP Publishing
Country of Publication:
United Kingdom
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; soot; morphology; ice cloud processing; optical properties; radiative forcing

Citation Formats

China, Swarup, Kulkarni, Gourihar, Scarnato, Barbara V., Sharma, Noopur, Pekour, Mikhail, Shilling, John E., Wilson, Jacqueline, Zelenyuk, Alla, Chand, Duli, Liu, Shang, Aiken, Allison C., Dubey, Manvendra, Laskin, Alexander, Zaveri, Rahul A., and Mazzoleni, Claudio. Morphology of diesel soot residuals from supercooled water droplets and ice crystals: implications for optical properties. United Kingdom: N. p., 2015. Web. doi:10.1088/1748-9326/10/11/114010.
China, Swarup, Kulkarni, Gourihar, Scarnato, Barbara V., Sharma, Noopur, Pekour, Mikhail, Shilling, John E., Wilson, Jacqueline, Zelenyuk, Alla, Chand, Duli, Liu, Shang, Aiken, Allison C., Dubey, Manvendra, Laskin, Alexander, Zaveri, Rahul A., & Mazzoleni, Claudio. Morphology of diesel soot residuals from supercooled water droplets and ice crystals: implications for optical properties. United Kingdom. doi:10.1088/1748-9326/10/11/114010.
China, Swarup, Kulkarni, Gourihar, Scarnato, Barbara V., Sharma, Noopur, Pekour, Mikhail, Shilling, John E., Wilson, Jacqueline, Zelenyuk, Alla, Chand, Duli, Liu, Shang, Aiken, Allison C., Dubey, Manvendra, Laskin, Alexander, Zaveri, Rahul A., and Mazzoleni, Claudio. Wed . "Morphology of diesel soot residuals from supercooled water droplets and ice crystals: implications for optical properties". United Kingdom. doi:10.1088/1748-9326/10/11/114010.
@article{osti_1239042,
title = {Morphology of diesel soot residuals from supercooled water droplets and ice crystals: implications for optical properties},
author = {China, Swarup and Kulkarni, Gourihar and Scarnato, Barbara V. and Sharma, Noopur and Pekour, Mikhail and Shilling, John E. and Wilson, Jacqueline and Zelenyuk, Alla and Chand, Duli and Liu, Shang and Aiken, Allison C. and Dubey, Manvendra and Laskin, Alexander and Zaveri, Rahul A. and Mazzoleni, Claudio},
abstractNote = {Freshly emitted soot particles are fractal-like aggregates, but atmospheric processing often transforms their morphology. Morphology of soot particles plays an important role in determining their optical properties, life cycle and hence their effect on Earth’s radiative balance. However, little is known about the morphology of soot particles that participated in cold cloud processes. Here we report results from laboratory experiments that simulate cold cloud processing of diesel soot particles by allowing them to form supercooled droplets and ice crystals at -20 and -40°C, respectively. Electron microscopy revealed that soot residuals from ice crystals were more compact (roundness~0.55) than those from supercooled droplets (roundness ~0.45), while nascent soot particles were the least compact (roundness~0.41). Optical simulations using the discrete dipole approximation showed that the more compact structure enhances soot single scattering albedo by a factor up to 1.4, thereby reducing the top-of-the-atmosphere direct radiative forcing by ~63%. Lastly, these results underscore that climate models should consider the morphological evolution of soot particles due to cold cloud processing to improve the estimate of direct radiative forcing of soot.},
doi = {10.1088/1748-9326/10/11/114010},
journal = {Environmental Research Letters},
number = 11,
volume = 10,
place = {United Kingdom},
year = {2015},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1088/1748-9326/10/11/114010

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Cited by: 9 works
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    Works referencing / citing this record:

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