Natural marine aerosols : A study on atmospheric chemistry, new particle formation and particle growth
(2024)- Abstract
- The role of natural marine aerosols in the global climate system remains understudied and uncertain. This is true for the emissions of natural volatile compounds over the ocean, the oxidation of said compounds and their impact on particle formation and particle growth. In this thesis, the emission, chemistry and aerosol particle processes relating to these compounds were studied using different process-based modelling techniques. This included the box model ADCHAM, and the chemistry transport model ADCHEM. The aim was to understand the role of naturally emitted volatile compounds over the oceans and over land, through their ability to form aerosols and thereby impact both clouds and climate. One of these compounds, namely dimethyl sulfide... (More)
- The role of natural marine aerosols in the global climate system remains understudied and uncertain. This is true for the emissions of natural volatile compounds over the ocean, the oxidation of said compounds and their impact on particle formation and particle growth. In this thesis, the emission, chemistry and aerosol particle processes relating to these compounds were studied using different process-based modelling techniques. This included the box model ADCHAM, and the chemistry transport model ADCHEM. The aim was to understand the role of naturally emitted volatile compounds over the oceans and over land, through their ability to form aerosols and thereby impact both clouds and climate. One of these compounds, namely dimethyl sulfide (DMS), was studied under controlled laboratory experiments in the AURA smog chamber. Simulations using the ADCHAM model indicated that the mechanisms on DMS oxidation in the literature (e.g. MCMv3.3.1) had a tendency to underestimate the DMS-derived particle mass production in the chamber. By revising and extending said mechanisms with more recent and alternative studies on DMS oxidation, the model representation of the particle mass production was improved. The revised mechanism was also tested on experiments performed in the CLOUD smog chamber, where it was found to improve the model representation of the gas-phase concentration of sulfuric acid (SA) and methane sulfonic acid (MSA). The role of DMS was later studied at various field stations around the world. At the Zeppelin research station on Svalbard, DMS was shown to form and grow particles in combination with natural emissions of ammonia (NH3). The particles formed around Svalbard and in the rest of the north Atlantic Ocean were also shown to impact measurements over land, namely those at the Pallas, Hyytiälä and Hyltemossa research stations located in the Nordic boreal forest. The particles formed over the ocean were transported towards the forest by the movement of air-masses, and grown into the cloud condensation nuclei (CCN) size range by the condensation of low volatile oxidation products from emissions of biogenic volatile organic compounds (BVOCs). In the Arctic and Antarctic regions, DMS also dominated the formation and growth of particles (both over land and over the open ocean). The measurements in these regions could nevertheless not be explained without the emission of iodine compounds of both organic and inorganic origin. These proved to be important through the formation of iodic acid (IA), which impacted the formation and growth of aerosol particles in the region. (Less)
Please use this url to cite or link to this publication:
https://lup.lub.lu.se/record/f54be643-508b-4bf4-bdf8-f008a1c892f7
- author
- de Jonge, Robin Wollesen LU
- supervisor
- opponent
-
- Prof. Archibald, Alexander T., University of Cambridge, United Kingdom.
- organization
- publishing date
- 2024
- type
- Thesis
- publication status
- published
- subject
- keywords
- Fysicumarkivet A:2024:De Jonge
- pages
- 251 pages
- publisher
- Division of Combustion Physics, Department of Physics, Lund University
- defense location
- Lecture Hall Rydbergsalen, Department of Physics, Professorsgatan 1, Faculty of Engineering LTH, Lund University, Lund.
- defense date
- 2024-12-13 13:15:00
- ISBN
- 9789181042696
- 9789181042689
- language
- English
- LU publication?
- yes
- id
- f54be643-508b-4bf4-bdf8-f008a1c892f7
- date added to LUP
- 2024-11-19 10:42:59
- date last changed
- 2025-05-28 12:36:50
@phdthesis{f54be643-508b-4bf4-bdf8-f008a1c892f7,
abstract = {{The role of natural marine aerosols in the global climate system remains understudied and uncertain. This is true for the emissions of natural volatile compounds over the ocean, the oxidation of said compounds and their impact on particle formation and particle growth. In this thesis, the emission, chemistry and aerosol particle processes relating to these compounds were studied using different process-based modelling techniques. This included the box model ADCHAM, and the chemistry transport model ADCHEM. The aim was to understand the role of naturally emitted volatile compounds over the oceans and over land, through their ability to form aerosols and thereby impact both clouds and climate. One of these compounds, namely dimethyl sulfide (DMS), was studied under controlled laboratory experiments in the AURA smog chamber. Simulations using the ADCHAM model indicated that the mechanisms on DMS oxidation in the literature (e.g. MCMv3.3.1) had a tendency to underestimate the DMS-derived particle mass production in the chamber. By revising and extending said mechanisms with more recent and alternative studies on DMS oxidation, the model representation of the particle mass production was improved. The revised mechanism was also tested on experiments performed in the CLOUD smog chamber, where it was found to improve the model representation of the gas-phase concentration of sulfuric acid (SA) and methane sulfonic acid (MSA). The role of DMS was later studied at various field stations around the world. At the Zeppelin research station on Svalbard, DMS was shown to form and grow particles in combination with natural emissions of ammonia (NH3). The particles formed around Svalbard and in the rest of the north Atlantic Ocean were also shown to impact measurements over land, namely those at the Pallas, Hyytiälä and Hyltemossa research stations located in the Nordic boreal forest. The particles formed over the ocean were transported towards the forest by the movement of air-masses, and grown into the cloud condensation nuclei (CCN) size range by the condensation of low volatile oxidation products from emissions of biogenic volatile organic compounds (BVOCs). In the Arctic and Antarctic regions, DMS also dominated the formation and growth of particles (both over land and over the open ocean). The measurements in these regions could nevertheless not be explained without the emission of iodine compounds of both organic and inorganic origin. These proved to be important through the formation of iodic acid (IA), which impacted the formation and growth of aerosol particles in the region.}},
author = {{de Jonge, Robin Wollesen}},
isbn = {{9789181042696}},
keywords = {{Fysicumarkivet A:2024:De Jonge}},
language = {{eng}},
publisher = {{Division of Combustion Physics, Department of Physics, Lund University}},
school = {{Lund University}},
title = {{Natural marine aerosols : A study on atmospheric chemistry, new particle formation and particle growth}},
year = {{2024}},
}