Accurate Measurement of the Optical Properties of Single Aerosol Particles Using Cavity Ring-Down Spectroscopy

Michael I Cotterell; Jamie W Knight; Jonathan P Reid; Andrew J Orr-Ewing

doi:10.1021/acs.jpca.2c01246

Accurate Measurement of the Optical Properties of Single Aerosol Particles Using Cavity Ring-Down Spectroscopy

Michael I Cotterell^*, Jamie W Knight, Jonathan P Reid, Andrew J Orr-Ewing^*

^*Corresponding author for this work

Research output: Contribution to journal › Article (Academic Journal) › peer-review

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Abstract

New approaches for the sensitive and accurate quantification of aerosol optical properties are needed to improve the current understanding of the unique physical chemistry of airborne particles and to explore their roles in fields as diverse as chemical manufacturing, healthcare, and atmospheric science. We have pioneered the use of cavity ring-down spectroscopy (CRDS), with concurrent angularly resolved elastic light scattering measurements, to interrogate the optical properties of single aerosol particles levitated in optical and electrodynamic traps. This approach enables the robust quantification of optical properties such as extinction cross sections for individual particles of known size. Our measurements can now distinguish the scattering and absorption contributions to the overall light extinction, from which the real and imaginary components of the complex refractive indices can be retrieved and linked to chemical composition. In this Feature Article, we show that this innovative measurement platform enables accurate and precise optical measurements for spherical and nonspherical particles, whether nonabsorbing or absorbing at the CRDS probe wavelength. We discuss the current limitations of our approach and the key challenges in physical and atmospheric chemistry that can now be addressed by CRDS measurements for single aerosol particles levitated in controlled environments.

Original language	English
Pages (from-to)	2619 - 2631
Number of pages	13
Journal	Journal of Physical Chemistry A
Volume	126
Issue number	17
Early online date	25 Apr 2022
DOIs	https://doi.org/10.1021/acs.jpca.2c01246
Publication status	Published - 5 May 2022

Bibliographical note

Funding Information:
We are grateful to many former and current colleagues, and to visitors to the University of Bristol’s Aerosol Research Centre for their contributions to the development of single-particle CRDS methods. These include Timothy Butler, Johanna Miller, Thomas Preston, Rui Wang, Joanna Egan, Rose Willoughby, Jim Walker, Antonia Carruthers, Bernard Mason, Hongze Lin, Fenghong Chu, Antonio Valenzuela, Rachael Miles, Svemir Rudić, Allen Haddrell, and Bryan Bzdek. We thank NERC (NE/C512537/1, NE/H001972/1) for funding the development and application of this research and for the award of an Independent Research Fellowship to MIC (NE/S014314/1). The EPSRC Centre for Doctoral Training in Aerosol Science (EP/S023593/1) provided studentship funding for J.W.K.

Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.

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Accurate and Direct Measurements of Brown Carbon Aerosol Optical Properties During Formation and Atmospherically-Relevant Ageing Processes
Cotterell, M. I.
4/11/19 → 3/11/24
Project: Research
EPSRC Centre for Doctoral Training in Aerosol Science
Reid, J. P.
1/04/19 → 30/09/27
Project: Research
A Novel Instrument for Characterising the Properties and Processes of Single Accumulation Mode Aerosol Particles
Reid, J. P. & Orr-Ewing, A. J.
1/03/10 → 1/03/12
Project: Research

Cite this

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title = "Accurate Measurement of the Optical Properties of Single Aerosol Particles Using Cavity Ring-Down Spectroscopy",

abstract = "New approaches for the sensitive and accurate quantification of aerosol optical properties are needed to improve the current understanding of the unique physical chemistry of airborne particles and to explore their roles in fields as diverse as chemical manufacturing, healthcare, and atmospheric science. We have pioneered the use of cavity ring-down spectroscopy (CRDS), with concurrent angularly resolved elastic light scattering measurements, to interrogate the optical properties of single aerosol particles levitated in optical and electrodynamic traps. This approach enables the robust quantification of optical properties such as extinction cross sections for individual particles of known size. Our measurements can now distinguish the scattering and absorption contributions to the overall light extinction, from which the real and imaginary components of the complex refractive indices can be retrieved and linked to chemical composition. In this Feature Article, we show that this innovative measurement platform enables accurate and precise optical measurements for spherical and nonspherical particles, whether nonabsorbing or absorbing at the CRDS probe wavelength. We discuss the current limitations of our approach and the key challenges in physical and atmospheric chemistry that can now be addressed by CRDS measurements for single aerosol particles levitated in controlled environments.",

author = "Cotterell, {Michael I} and Knight, {Jamie W} and Reid, {Jonathan P} and Orr-Ewing, {Andrew J}",

note = "Funding Information: We are grateful to many former and current colleagues, and to visitors to the University of Bristol{\textquoteright}s Aerosol Research Centre for their contributions to the development of single-particle CRDS methods. These include Timothy Butler, Johanna Miller, Thomas Preston, Rui Wang, Joanna Egan, Rose Willoughby, Jim Walker, Antonia Carruthers, Bernard Mason, Hongze Lin, Fenghong Chu, Antonio Valenzuela, Rachael Miles, Svemir Rudi{\'c}, Allen Haddrell, and Bryan Bzdek. We thank NERC (NE/C512537/1, NE/H001972/1) for funding the development and application of this research and for the award of an Independent Research Fellowship to MIC (NE/S014314/1). The EPSRC Centre for Doctoral Training in Aerosol Science (EP/S023593/1) provided studentship funding for J.W.K. Publisher Copyright: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

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N1 - Funding Information: We are grateful to many former and current colleagues, and to visitors to the University of Bristol’s Aerosol Research Centre for their contributions to the development of single-particle CRDS methods. These include Timothy Butler, Johanna Miller, Thomas Preston, Rui Wang, Joanna Egan, Rose Willoughby, Jim Walker, Antonia Carruthers, Bernard Mason, Hongze Lin, Fenghong Chu, Antonio Valenzuela, Rachael Miles, Svemir Rudić, Allen Haddrell, and Bryan Bzdek. We thank NERC (NE/C512537/1, NE/H001972/1) for funding the development and application of this research and for the award of an Independent Research Fellowship to MIC (NE/S014314/1). The EPSRC Centre for Doctoral Training in Aerosol Science (EP/S023593/1) provided studentship funding for J.W.K. Publisher Copyright: © 2022 American Chemical Society. All rights reserved.

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N2 - New approaches for the sensitive and accurate quantification of aerosol optical properties are needed to improve the current understanding of the unique physical chemistry of airborne particles and to explore their roles in fields as diverse as chemical manufacturing, healthcare, and atmospheric science. We have pioneered the use of cavity ring-down spectroscopy (CRDS), with concurrent angularly resolved elastic light scattering measurements, to interrogate the optical properties of single aerosol particles levitated in optical and electrodynamic traps. This approach enables the robust quantification of optical properties such as extinction cross sections for individual particles of known size. Our measurements can now distinguish the scattering and absorption contributions to the overall light extinction, from which the real and imaginary components of the complex refractive indices can be retrieved and linked to chemical composition. In this Feature Article, we show that this innovative measurement platform enables accurate and precise optical measurements for spherical and nonspherical particles, whether nonabsorbing or absorbing at the CRDS probe wavelength. We discuss the current limitations of our approach and the key challenges in physical and atmospheric chemistry that can now be addressed by CRDS measurements for single aerosol particles levitated in controlled environments.

AB - New approaches for the sensitive and accurate quantification of aerosol optical properties are needed to improve the current understanding of the unique physical chemistry of airborne particles and to explore their roles in fields as diverse as chemical manufacturing, healthcare, and atmospheric science. We have pioneered the use of cavity ring-down spectroscopy (CRDS), with concurrent angularly resolved elastic light scattering measurements, to interrogate the optical properties of single aerosol particles levitated in optical and electrodynamic traps. This approach enables the robust quantification of optical properties such as extinction cross sections for individual particles of known size. Our measurements can now distinguish the scattering and absorption contributions to the overall light extinction, from which the real and imaginary components of the complex refractive indices can be retrieved and linked to chemical composition. In this Feature Article, we show that this innovative measurement platform enables accurate and precise optical measurements for spherical and nonspherical particles, whether nonabsorbing or absorbing at the CRDS probe wavelength. We discuss the current limitations of our approach and the key challenges in physical and atmospheric chemistry that can now be addressed by CRDS measurements for single aerosol particles levitated in controlled environments.

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Accurate Measurement of the Optical Properties of Single Aerosol Particles Using Cavity Ring-Down Spectroscopy

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Projects

Accurate and Direct Measurements of Brown Carbon Aerosol Optical Properties During Formation and Atmospherically-Relevant Ageing Processes

EPSRC Centre for Doctoral Training in Aerosol Science

A Novel Instrument for Characterising the Properties and Processes of Single Accumulation Mode Aerosol Particles

Cite this