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\thispagestyle{mainbody}
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\section{Monoterpenes in the atmosphere}
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The biosphere of Earth emits large quantities of \glspl{VOCa}. The natural flux of \glspl{VOCa} to the atmosphere exceeds the anthropogenic one, and accounts for \qtyrange{75}{90}{\percent} of the total \gls{VOCa} flux \citep{messina_global_2016}. Due to their biogenic origin, these latter \glspl{VOCa} are often referred to as \glspl{BVOCa}.
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\section{Iodine in the atmosphere}
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\section{Relevant instrumentation}
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Iodine is the heaviest stable halogen element with atomic number \qty{53}{}. It has an average atomic weight of \qty{126.904}{\amu} and forms a semi-lustrous solid under standard conditions (here \qty{273.15}{\kelvin} and \qty{1}{\bar}, see \citet{calvert_glossary_1990}) \citep{kaiho_physical_2015}. Its melting and boiling points are \qty{114}{\degreeCelsius} and \qty{184}{\degreeCelsius}, respectively, and its vapour pressure is \qty{0.031}{\kilo\pascal} and \qty{9.17}{\kilo\pascal} at \qty{25}{\degreeCelsius} and \qty{113.6}{\degreeCelsius}, respectively \citep{kaiho_physical_2015}. The atomic radius of iodine is \qty{140}{\pico\meter} and its first ionisation energy is \qty{1015}{\kilo\joule\per\mol} \citep{kaiho_physical_2015}. Iodine is important in the enviornment: in the atmosphere, it influences the chemistry of ozone and important radical species, and it may be cause the formation of particles that may act as nuclei for aerosol or clouds \citep{saiz-lopez_atmospheric_2012}. The former is important for the capability of the atmophere to oxidise and remove species emitted to it, while the latter is important because of its effect on radiative equilibrium of Earth.
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\section{Iodine in the environment}
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Iodine is litophilic and incompatible in Earth's astenosphere, and therefore concentrated in oceans and surface sediments \citep{kendrick_halogen_2024}. Marine sediments constitute the largest iodine reservoir \citep{kendrick_halogen_2024} with much higher concentrations of \qtyrange{20}{600}{\milli\gram\per\kilogram} compared to soil- (\qtyrange{0.5}{20}{\milli\gram\per\kilogram}) or rock (\qtyrange{0.08}{0.5}{\milli\gram\per\kilogram}) concentrations \citep{whitehead_distribution_1984}. Sedimented iodine may be recycled into the oceans through sedimentary brines \citep{muramatsu_recycling_2001, muramatsu_studies_2004} around techtonically active subduction zones \citep{carrano_influence_2020} through diagenesis processes involving thermal decompostion or microbiological reduction of buried organic matter \citep{kendrick_halogen_2024, muramatsu_recycling_2001}. Consequently, iodine concentrations in the oceans are approximately \qtyrange{45}{60}{\micro\gram\per\liter} \citep{whitehead_distribution_1984}, mostly in the form of \gls{IO3-f}, the thermodynamically most stable state of iodine in aqueous solution \citep{fuge_iodine_2015}. However, \gls{IO3-f} exhibits a nutrient-like profile \citep{carrano_influence_2020} being depleted at the surface, whereas \gls{I-f} is enriched in the surface \citep{elderfield_biophilic_1980}. Similarly, organic matter is enriched in the surface, so that the existence of some iodinated organics may be presumed \citep{saiz-lopez_atmospheric_2012}. Within the oceans, iodine is incorporated preferrentially in organic matter \citep{kendrick_halogen_2024} by micro- and macroalgae, and aerobic bacteria \citep{carpenter_biogeochemical_2015}: through faciliated diffusion (see detailed descriptions in \citet{kupper_iodide_2008, winter_exploring_2009, amachi_microbial_2008}), cells store iodine as \ce{\glssymbol{I-f}(aq)} or associated to organic molecules \citep{kupper_iodide_2008, amachi_microbial_2008}.
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\Gls{I-f} within the cell interior may act as an antioxidant \citep{kupper_iodide_2008}: upon oxidative stress, the \gls{I-f} reservoir is mobilised and cells emit \ce{\glssymbol{I-f}(aq)} and a range of \glspl{VOICa} \citep{kupper_iodide_2008, carpenter_biogeochemical_2015} that may volatilise to the atmosphere. Analogously, when oxidative stress occurs during air exposure at low tide, the hetergeneous surface reaction of \gls{I-f} and \gls{O3f} at the sea-water interface produces \gls{HOIf}, \gls{I2f} and \glspl{IO.f} directly emitted to the atmosphere \citep{carpenter_biogeochemical_2015, palmer_iodine_2005, liu_kinetics_2001, sakamoto_direct_2009, hayase_heterogeneous_2010, he_role_2021}. It is currently thought that the biggest source of inorganic iodine to the atmosphere is \gls{HOIf} produced via the same pathway, exceeding the emissions of \gls{I2f} by one order of magnitude \citep{carpenter_atmospheric_2013}.
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Nevertheless, the atmospheric iodine budget is currently not well-constrained \citep{saiz-lopez_atmospheric_2012}. \glspl{VOICa} (notably \ce{\glssymbol{CH3If}}) and inorganic iodine species (\ce{\glssymbol{HOIf}}, \ce{\glssymbol{I2f}}, \ce{\glssymbol{IO.f}}) emitted from the oceans constitute the biggest source of iodine to the atmosphere \citep{carpenter_biogeochemical_2015, carpenter_atmospheric_2013}, with estimated input $\approx\qty{550}{\giga\gram\per\year}$ \citep{saiz-lopez_atmospheric_2012}. Most \glspl{VOICa} are photolabile with lifetimes on the order of minutes to days \citep{bloss_kinetics_2001}. Other natural sources of iodine to the amtosphere include soils and plants \citep{whitehead_distribution_1984, carpenter_biogeochemical_2015, fuge_iodine_2015}, terrestrial water systems \citep{whitehead_distribution_1984}, and volcanoes or salt lakes \citep{carpenter_biogeochemical_2015}. The additional input from terrestrial sources into the atmosphere is $\approx\qtyrange{80}{110}{\giga\gram\per\year}$ \citep{saiz-lopez_atmospheric_2012}. Anthropogenic sources include direct emissions from fossil fuel burning \citep{fuge_iodine_2015} and pesticide use \citep{zheng_accelerated_2003, whitehead_distribution_1984}. There are indirect anthropogenic effects as well: ice core data indicates that the sea-air flux of iodine has tripled between 1950 and 2010 as a consequence of increased anthropogenic ozone pollution of the troposphere \citep{cuevas_rapid_2018}. Sinks of atmospheric iodine include wet- and dry deposition \citep{fuge_iodine_2015}, and direct uptake through plants \citep{fuge_iodine_2015}. Overall, this leads to boundary layer mixing ratios of $\chi_{\ce{\glssymbol{I2f}(g)}}\leq\qty{93}{\pptv}$ \citep{carpenter_biogeochemical_2015}, $\chi_{\ce{\glssymbol{IO.f}(g)}}\leq\qtyrange{3}{20}{\pptv}$ \citep{carpenter_biogeochemical_2015}, $\chi_{\ce{\glssymbol{HOIf}(g)}}\leq\qty{1}{\pptv}$ \citep{he_role_2021} and $\chi_{\ce{\glssymbol{I.f}(g)}}\leq\qtyrange{0.1}{22}{\pptv}$ \citep{carpenter_biogeochemical_2015, he_role_2021}.
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\section{Iodine Chemistry in the Atmosphere}
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The importance of the marine iodine source is likely also reflected in aerosol composition: above marine areas, aerosol is enriched in iodine relative to seawater content by a factor of \qtyrange{100}{1000}{} \citep{carpenter_biogeochemical_2015}. Iodine may be transported into the aerosol phase through bubble-bursting of iodine-rich surface ocean waters \citep{saiz-lopez_atmospheric_2012}, or through the formation of aerosol via \glspl{IOPa} \citep{odowd_marine_2002}. Likely, low-volatility iodinated organics may also condense into the aerosol phase. Overall, various iodinated species may be present in aerosol including \gls{I-f}, \gls{IO3-f}, \gls{HOIf} and \gls{SOIa} \citep{saiz-lopez_atmospheric_2012}. \Citet{saiz-lopez_atmospheric_2012, gilfedder_iodine_2008} report that \gls{SOIa} is very frequent in aerosol and may constitute the largest reservoir of iodine in aerosol. There appear to be two principal pathways of \gls{SOIa} accomodation: direct accumulation from sea spray enriched in iodinated organics, and the reaction of \gls{HOIf} with aerosol organics. \Gls{HOIf} may also be highly reactive towards other species, likely due to its affinity for nucelophilic attacks on susceptible species. In general however, \gls{HOIf} or other likewise reduced iodine species such as \gls{I-f} should be oxidised to \gls{IO3-f} \citep{gilfedder_iodine_2008}, the thermodynamically most stable form of iodine in aqueous solution. Consequently, the accumulated form of iodine in condensed aerosol phases is often thought to be \gls{IO3-f} \citep{gilfedder_iodine_2008, saiz-lopez_atmospheric_2012}. However, observations in the troposphere indicate higher aerosol contents of \gls{I-f} than \gls{IO3-f} \citep{gilfedder_iodine_2008}, or high variability in the \gls{I-f}/\gls{IO3-f} ratio \citep{saiz-lopez_atmospheric_2012}. This indicates the presence of a mechanism reducing \gls{IO3-f} in the troposphere.
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Hetergeneous aerosol chemistry of iodine is closely linked to homogeneous chemistry of iodine through many iodine species. Generally, atmospheric iodine chemistry is initiated mostly through \gls{RISa} such as \glspl{I.f} or \glspl{IO.f}. Briefly, homogeneous iodine chemistry involves catalytic destruction of troposheric ozone via various pathways involving \glspl{HOxf} and \glspl{NOxf} as well as other halogen atoms in the atmosphere \citep{saiz-lopez_reactive_2012}. This process is photochemically driven and initiated with \glssymbol{IO.f} and \glssymbol{I.f}. \citet{saiz-lopez_reactive_2012} have outlined the mechanism: the intial step is the production of \glspl{I.f} from \glspl{RInf} or \gls{I2f}. The \glspl{I.f} react with \gls{O3f} to produce \glspl{IO.f} that in turn recombine to again produce \glspl{I.f}:
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\begin{reactions}
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\RI{}(g) + ${h\nu}$ &-> R^{\bullet}(g) + \glssymbol{I.f}(g)\\
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\glssymbol{I2f}(g) + ${h\nu}$ &-> 2 \glssymbol{I.f}(g)\\
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\glssymbol{I.f}(g) + \glssymbol{O3f}(g) &-> \glssymbol{IO.f}(g) + \glssymbol{O2f}(g) \label{reac: intro: iodine radical ozone loss}\\
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2\glssymbol{IO.f} &-> 2\glssymbol{I.f}(g) + \glssymbol{O2f}(g)\label{reac: intro: 2IO to 2I and O2}
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\end{reactions}
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The net outcome is ozone destruction with \ce{2\glssymbol{O3f}(g) -> 3\glssymbol{O2f}(g)}, although reaction \ref{reac: intro: 2IO to 2I and O2} has other channels that may involve \glssymbol{HOxf} and \glssymbol{NOxf} cycles. Importantly, the \gls{IO.f} has a lifetime against photolysis in the boundary layer on the order of seconds \citep{bloss_kinetics_2001}. Likewise, the effective lifetime of \gls{Ix.f} against uptake in aerosol is on the order of hours \citep{dix_detection_2013}: sustained presence of \glspl{IO.f} in the atmosphere therefore requires an effective recycling mechanism for \ce{\glssymbol{IO.f}}.
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Additionally, iodine may be involved in the oxidation of atmospheric organic molecules or mercury, allowing the latter to enter the food chain as highly poisonous methylmercury \citep{steffen_synthesis_2008, saiz-lopez_reactive_2012, saiz-lopez_atmospheric_2012}, and likely leading to enhanced condensation of organics into the aerosol phase through the former. Further, through formation of \glspl{IOPa}, iodine oxides may lead to the production of \glspl{UFAPa} \citep{carpenter_biogeochemical_2015}. Volatile species may condense on \glspl{UFAPa} that can grow up to the point of becoming \glspl{CCNa} \citep{saiz-lopez_atmospheric_2012}. Recent evidence shows that nucleation via iodine oxoacids to produce \glspl{IOPa} is highly efficient and sometimes competitive with sulfuric acid-ammonium driven nucleation \citep{he_role_2021}. Moreover, heterogeneous iodine chemistry on pre-existing frozen or liquid salt particles may lead to sudden increases in gas phase iodine species \citep{saiz-lopez_reactive_2012}. Importantly, the reaction of \gls{Br-f} with \gls{O3f} on frozen salt solutions occurs in the brine pertaining to the bulk ice phase, rather than \emph{within} the bulk ice phase \citep{oldridge_formation_2011}: such brines are formed when freezing solutions exclude solutes --- the heterogeneous reaction of \gls{O3f} with \gls{I-f} on frozen aerosol is here assumed to behave similarly. In other words, the heterogeneous reaction of \gls{O3f} with aerosol surfaces is assumed to be similar for frozen and liquid aerosol particles.
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Other heterogeneous effects may lead to substantial iodine emissions through the reaction of ozone with dissolved \gls{I-f} in ocean and aerosols \citep{palmer_iodine_2005, liu_kinetics_2001, sakamoto_direct_2009, hayase_heterogeneous_2010}. In the upper troposphere and lower stratosphere, heterogeneous recycling of iodine species is highly important: Model calculations by \citet{saiz-lopez_injection_2015} show that from the lower troposphere, convection may transport inorganic- and organic iodine species to the lower stratosphere, causing a \gls{Iyf} injection of \qtyrange{0.25}{0.7}{\pptv} \citep{saiz-lopez_injection_2015}. Measurements by \citet{koenig_quantitative_2020} are in agreement with this, indicating an injection of \qty{0.77\pm0.10}{\pptv} of \glssymbol{Iyf} into the lower stratosphere. Associated therewith is a mixing ratio of $\chi_{\ce{\glssymbol{IO.f}(g)}}=\qty{0.06\pm0.03}{\pptv}$ even for aged stratospheric air. \Citet{koenig_quantitative_2020} also observed that increases in altitude across the troposphere are associated with (1) an increase in particulate iodine and a decrease in gas phase iodine; and (2) a shift of \gls{I-f}-\gls{IO3-f} speciation in the condensed phase towards \gls{IO3-f}. Simulations could reproduce observed $\chi_{\ce{\glssymbol{IO.f}(g)}}$ only when a recycling scheme for iodine on ice particles was applied, and when the proper partioning between condensed- and gas phase was applied. This indicates that, as for the troposphere, a recycling mechanism producing gas phase \glspl{IO.f} must exist. There is also evidence that \gls{IO3-f} should be reduced to \gls{I-f}: \citet{pillar-little_conversion_2013} have established a pathway through which \gls{I-f} and \gls{O3f} cause volatilization of \ce{\glssymbol{I2f}(g)} and \ce{\glssymbol{HOIf}(g)} from watery microdroplets. However, it is still unclear \emph{how} the necessary \gls{I-f} is formed, given that most iodine should be present as \gls{IO3-f}. Consequently, an important question to answer is: how is \glssymbol{IO3-f} reduced to species --- most likely \glssymbol{I-f} --- that may, directly of after reacting, volatilise to the gas phase?
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\section{Reduction of Iodate}
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\Citet{saunders_insights_2012} have shown that \gls{IO3-f} may be reduced when solutions of \gls{IO3-f} and \gls{HAa} are irradiated with \gls{UV-Aa} and \gls{VISa} light between $\gls{LAMBDAs}\geq\qty{310}{\nano\meter}$ and $\gls{LAMBDAs}\approx\qty{780}{\nano\meter}$. The light source was filtered to exclude \gls{IRa} light and lamp output below $\gls{LAMBDAs}=\qty{310}{\nano\meter}$ to simulate the \gls{UV-Aa}-\gls{VISa} solar spectrum in the lower troposphere. They found that the major product of this photochemically induced process was \gls{SOIa} and that the proportion of \gls{I-f} in the reactant solution remained constant at approximately \qty{20}{\percent}. Since \gls{HAa} is a \gls{CHROMOPHOREg}, the suggested mechanism involves photogeneration of solvated electrons \ce{e-(aq)} that, in dependence of \gls{pHs}, yield \gls{HOIf}: \ce{\glssymbol{IO3-f}(aq) + 4e-(aq) + 5\glssymbol{H+f}(aq) ->\glssymbol{HOIf}(aq) + 2\glssymbol{H2Of}(aq)}. From there, \gls{SOIa} may be created through the nucleophilic attack of \gls{HOIf} on diphenolic functional groups \citep{saunders_insights_2012}. Alternatively, \gls{I2f} may be produced through reaction \ref{reac: intro: HOI to I2}, as described by \citet{pillar-little_conversion_2013}:
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\begin{reaction}
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\glssymbol{HOIf}(aq) + \glssymbol{I-f} + \glssymbol{H+f}(aq) -> \glssymbol{I2f}(aq) + \glssymbol{H2Of}(l) \label{reac: intro: HOI to I2}
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\end{reaction}
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Since \gls{I2f} is insoluble \citep{saiz-lopez_atmospheric_2012}, there will be volatilisation of \gls{I2f} to the gas phase. Overall, the mechanism suggested by \citet{saunders_insights_2012} produces primarily \gls{HOIf} \gls{I2f} --- the production pathway of \gls{I-f} has not been elucidated. The presence of \gls{I-f}, however, appears necessary for the production of \ce{\glssymbol{I2f}(g)}. It is hypothetised that \gls{I-f} may be regenerated from \gls{SOIa} \citep{saunders_insights_2012, baker_marine_2005}. Finally, \citet{saunders_insights_2012} have reported oscillations in the release of \ce{\glssymbol{I2f}(g)}. This is likely associated with formation of \gls{H2O2f} as a byproduct of \gls{HAa} photolysis \citep{saunders_insights_2012}. Indeed, \citet{cooper_photochemical_1988} have shown that \gls{H2O2f} is a common product when irradiating aqueous solutions of \glspl{CHROMOPHOREg}. Given \gls{H2O2f}, oscillations in \ce{\glssymbol{I2f}}-\ce{\glssymbol{IO3-f}} are known as the \gls{BRAY-LIEBHAFSKY-MECHANISMa}, first described by \citet{bray_periodic_1921, bray_reactions_1931}: \gls{H2O2f} interacts with \gls{I2f} and \gls{IO3-f} via
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\begin{reactions}
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&2\glssymbol{IO3-f}(aq) + 2\glssymbol{H+f}(aq) + 5\glssymbol{H2O2f}(aq) <=> \glssymbol{I2f}(aq) + 5\glssymbol{O2f}(g) + 6\glssymbol{H2Of}(l) \label{reac: oxidation of iodine through hydrogen peroxide}\\
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&\glssymbol{I2f}(aq) + 5\glssymbol{H2O2f}(aq) <=> 2\glssymbol{IO3-f}(aq) + 2\glssymbol{H+f}(aq) + 4\glssymbol{H2Of}(l) \label{reac: reduction of iodate through hydrogen peroxide}
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\end{reactions}
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to yield a net catalytic decomposition of \gls{H2O2f} via
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\begin{reaction}
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2\glssymbol{H2O2f}(aq) -> 2\glssymbol{H2Of}(l) + \glssymbol{O2f}(g) \label{reac: net catalytic destruction of hydrogen peroxide through iodine-iodate system}
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\end{reaction}
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The oscillation reaction has a \emph{stable} regime --- here, all species reach steady state except \glssymbol{H2O2f}: likely, \glssymbol{O2f}\ce{(g)} volatilises and \gls{LE-CHATELIER-PRINCIPLEa} dictates that \gls{H2O2f} consequently depletes. The \emph{unstable} regime where either reaction \ref{reac: oxidation of iodine through hydrogen peroxide} or \ref{reac: reduction of iodate through hydrogen peroxide} occur preferrentially, leads to oscillations in \gls{I2f} and \gls{IO3-f}. These oscillations are modulated by initial \gls{pHs} \citep{bray_periodic_1921} and temperature. Including an organic reducing agent and a metal-ion catalyst results in the \gls{BRIGGS-RAUSCHER-MECHANISMa} after \citet{briggs_oscillating_1973}, elucidated by \citet{schmitz_kinetics_2012}: Briefly, in addition to reaction \ref{reac: reduction of iodate through hydrogen peroxide}, the presence of some organic species \ce{R-H2} will induce the following reactions:
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\begin{reactions}
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\glssymbol{H+f}(aq) + \glssymbol{IO3-f}(aq) + 2\glssymbol{I2f}(aq) + 5 R-H2(aq) &-> 5 R-HI + 3\glssymbol{H2Of}\\
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\glssymbol{H+f}(aq) + \glssymbol{IO3-f}(aq) + 2\glssymbol{I2f}(aq) + 5 R-HI(aq) &-> 5 R-I2 + 3\glssymbol{H2Of}\\
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R-I2 + R-H2 &<=> 2 R-HI
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\end{reactions}
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The backward reaction likely proceeds via the metal ion catalyst, although \citet{schmitz_kinetics_2012} reported the possibility of non-catalysed pathways.
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A lot has been learned so far: organic substances may lead to the reduction of \gls{IO3-f}, via \gls{CHROMOPHOREg} activity. Furthermore, observed oscillations in gas phase \ce{\glssymbol{I2f}} may be explained through \gls{BRAY-LIEBHAFSKY-MECHANISMa}-\gls{BRIGGS-RAUSCHER-MECHANISMa} mechanisms. However, the suitability of \glspl{HAa} to represent organic aerosol has been questioned: \citet{graber_atmospheric_2006} suggested that humic-like substances found in aerosol particles may differ substantially from humic substances found in soil. More specifically, \citet{graber_atmospheric_2006} argue that terrestrial sources --- from which the \gls{HAa} used by \citet{saunders_insights_2012} likely originate --- may not be the origin of the majority of humic-like substances in aerosol. Differences may be found in terms of molecular weight, aromatic moiety content, surface properties and other properties \citep{graber_atmospheric_2006}. Although \glspl{HAa} as organics have profen useful to elucidate the mechanisms of \glssymbol{I2f} recycling, quantitatively constraining this recycling better requires more realistic organics. Another important question to answer, therefore, is: are there proxies that represent organics in aerosol more accurately, and to which the same \gls{CHROMOPHOREg}-dependent pathway of iodine recycling applies?
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\section{Reduction of Iodate: Proxies for Secondary Organic Aerosol}
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\Citet{guenther_global_1995} modelled global natural \gls{VOCa} emissions in 1990. They found a total flux of $\qty{1150}{\tera\gramCarbon\per\year}$, of which \qty{44}{\percent} (\qty{503}{\tera\gramCarbon\per\year}) was \gls{ISOPRENEf} and \qty{11}{\percent} (\qty{127}{\tera\gramCarbon\per\year}) were monoterpenes such as \gls{A-PINENEf}. Thereof, approximately \qty{75}{\percent} orginated from forests. In 2006, The annual atmospheric \gls{VOCa} injection was further specified in 2012 when \citet{guenther_model_2012} reported the following emissions of \glspl{VOCa} for the year 2000: total emissions were \qty{1089}{\tera\gramCarbon\per\year}, of which \gls{ISOPRENEf} emissions were \qty{49.1}{\percent} (\qty{535}{\tera\gramCarbon\per\year}) and the monoterpenes \gls{A-PINENEf}, \gls{B-PINENEf} and \gls{LIMONENEf} contributed \qty{6.7}{\percent} (\qty{66.1}{\tera\gramCarbon\per\year}), \qty{1.7}{\percent} (\qty{18.9}{\tera\gramCarbon\per\year}) and \qty{1.0}{\percent} (\qty{11.4}{\tera\gramCarbon\per\year}), respectively. \gls{ISOPRENEf} and monoterpene emissions are biogenic and mostly linked to vegetation --- overall they contributed approximately \qty{65}{\percent} to global \gls{VOCa} emissions in 2000 \citep{guenther_model_2012}, rendering them a major source of atmospheric \glspl{VOCa}.
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Organic matter in aerosol is present either as \gls{POAa} or \gls{SOAa}. \gls{POAa} and \gls{SOAa} comprise the largest share of \emph{fine} particles with diameters $d\leq\qty{2.5}{\micro\meter}$. On the other hand, large particles with diameters $d>\qty{2.5}{\micro\meter}$ are mostly comprised of particles formed mechanically, including soil and mineral dust, sea salt particles and plant particles \citep{jziemann_kinetics_2012}. \gls{POAa} requires no chemical reactions to condense to the aerosol phase. Conversely, \gls{SOAa} is created when volatile precursor species are chemically altered to lower volatilities, and consequently condense to the aerosol phase. Likely, \gls{SOAa} constitues a large fraction of organic aerosol \cite{bianchi_highly_2019, hallquist_formation_2009}. As a general rule of thumb, higher oxygen content of a molecule indicates \emph{lower} volatility. Therefore, oxidation reactions are highly important in \gls{SOAa} formation because oxidation effectively \emph{decreases} volatility. Recent work summarised by \citet{bianchi_highly_2019} suggests that there exists class of of low-volatile species referred to as \glspl{HOMa} with low volatility. Such \glspl{HOMa} are formed through \emph{autooxidation} reactions involving peroxy radicals: this process is detailed by \citet{bianchi_highly_2019}, and the subtle but important difference between \glspl{HOMa} and molecules with high oxygen content is laid out. Briefly, \glspl{HOMa} are species of very low vapour pressure so that condensation onto existing particles is very probable and almost irreversible \citep{bianchi_highly_2019}. High yields of \glspl{HOMa} have been observed for \gls{ISOPRENEf} and the monoterpenes \gls{A-PINENEf} and especially \gls{LIMONENEf} \citep{bianchi_highly_2019}, with total yields of \qty{4}{\percent} (\gls{ISOPRENEf}), \qtyrange{7.0\pm3.5}{3.4\pm1.0}{\percent} (\gls{A-PINENEf}) and \qty{17.0\pm8.5}{\percent} (\gls{LIMONENEf}), respectively \citep{bianchi_highly_2019, jokinen_production_2015, ng_secondary_2008, ehn_large_2014, kirkby_ion-induced_2016}. It may therefore be assumed that derivatives --- or more precisely oxidation products --- of monoterpenes or \gls{ISOPRENEf} are common in \gls{SOAa}. Building on the work of \citet{saunders_insights_2012}, chosing an oxidation product of \gls{ISOPRENEf} or monoterpenes as the investigated organics may constitute a more realistc proxy for aerosol organics.
|
||||
|
||||
Recently, \citet{reza_iodine_2024} have performed similar experiments as \citet{saunders_insights_2012}, but using organic species better representing \gls{VOCa} oxidation. Recent observations have shown elevated concentrations of \ce{\glssymbol{IO.f}(g)} in dust layers above the Atacama and Sechura deserts: \citet{koenig_ozone_2021} measured a ten-fold enhancement of \gls{IO.f} concentrations compared to the regional background signal of \qtyrange{0.10}{0.25}{\pptv}. Because iron is hypothetised to catalyse photochemistry in dust particles, and since it is the most abundant transition metal in dust minerals \citep{aal-abadleh_perspective_2023}, iron may serve as a proxy for dust when investigating the reduction of \gls{IO3-f}. In a series of \gls{CWFTRa} experiments, \citet{reza_iodine_2024} used a \gls{CE-DOASa} to detect \glssymbol{I2f}\ce{(g)} and a \gls{ToF I-CIMSa} to detect \glspl{OVOCa} associated with \gls{IO3-f} reduction in thin aqueous films. The films were inserted into the \gls{CWFTRa} and consisted of an organic or inorganic matrix and \gls{IO3-f}.
|
||||
The organic matrices included \gls{IRON-3-CITRATEa}, \gls{CAa} and \gls{BTCAa}. \gls{CAa} was found in aerosol \citep{lienhard_measurements_2012} and is a proxy for oxygenated organic species. \gls{IRON-3-CITRATEa}, as a known photoactive compound, is considered a suitable proxy for \ce{Fe}(\toRoman{3}) carboxylate complexes found in the atmosphere \citep{reza_iodine_2024}. Importantly, \gls{CAa} has well-characterised hygroscopic properties \citep{reza_iodine_2024} so that this matrix can be used to control against \glspl{MATRIX-EFFECT-(CHEM)g} of organics that are due to iron when using \gls{IRON-3-CITRATEa}. These matrices were mixed with a solution of \gls{NaIO3f} to introduce \gls{IO3-f} at a concentration of $\approx\qty{30}{\milli\Molar}$. The results show that irradiation with \gls{VISa} for films containing \gls{IRON-3-CITRATEa} led to the reduction of $\approx\qty{40}{\percent}$ of the initially present \gls{IO3-f}. Likely, \gls{IRON-3-CITRATEa} undergoes a \gls{LMCTa} induced through irradiance with a photon at $\lambda<\qty{500}{\nano\meter}$ to yield \gls{CITRATEa} radicals and solvated electrons \ce{e-(aq)}, as described by \citet{saunders_insights_2012}. Likely, reduction of \gls{IO3-f} is driven through these solvated electrons. Furthermore, \citet{reza_iodine_2024} report that the speciation of the \glspl{CHROMOPHOREg} may include iodine-containing compounds.
|
||||
|
||||
\end{document}
|
||||
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|
||||
% makeindex style file created by the glossaries package
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|
||||
\textbf{Data Analysis}. In this step, the data from the \gls{BTOF-CIMSa} are analysed using \emph{IGOR Pro} and \emph{Python}. Details are available in section \ref{methods: section: data analysis}.}
|
||||
\end{enumerate}
|
||||
|
||||
\section{\glsname{SOAa} filter production in \gls{OFRa}}\label{methods: section: SOA filter production in OFR}
|
||||
\section{SOA filter production in OFR}\label{methods: section: SOA filter production in OFR}
|
||||
|
||||
An overview over the setup for filter production is displayed in figure \ref{methods: fig: overview over OFR setup}. \Gls{O2f} and \gls{N2f} from the in-house gas connection at \gls{PSIa} are first mixed at controlled ratios and guided inton the flow tube of the \gls{OFRa}. Usually, $\gls{VFLOWs}_{\ce{N2}}=\qty{3.95}{\liter\per\minute}$ and $\gls{VFLOWs}_{\ce{O2}}^{(3)}=\qty{1.05}{\liter\per\minute}$ was set, giving a relative fraction of $\glssymbol{N2f}:\glssymbol{O2f}\approx0.79:0.21$, which is close to atmospheric comoposition. This was achieved through the \glspl{MFCa} 2 (for \gls{N2f}) and 3 (for \gls{O2f}), respectively (see also figure \ref{methods: fig: overview over OFR setup}). \Gls{MFCa} 1 was used to control the flow of \gls{N2f} through a glass bottle containing \gls{VOCa}, with a value set at $\gls{VFLOWs}_{\textnormal{VOC}}=\qty{0.04}{\liter\per\minute}$. In order to inhibit diffusion of \gls{VOCa} into the \gls{OFRa}, a plug valve (PV1) was installed on the \gls{VOCa} input line just before the \gls{OFRa}. Finally, \gls{MFCa} 4 was used to control the flow of \gls{O2f} into the \glstext{O3f} generator, where \glstext{O2f} reacted with \gls{UVa} light to produce \glstext{O3f}, as in reaction below:
|
||||
|
||||
@@ -131,20 +131,35 @@
|
||||
\bottomrule
|
||||
\end{longtblr}
|
||||
|
||||
\section{Filter extraction and \gls{TOCa}-analysis}\label{methods: section: filter extraction and TOC analysis}
|
||||
\section{Filter extraction and TOC-analysis}\label{methods: section: filter extraction and TOC analysis}
|
||||
|
||||
In order to quantify the exact (organic) carbon content used in \gls{CWFTRa} samples, the organic carbon content on filters needs to be known. While an estimate is provided via the \gls{SMPSa} measurements, the exact quantity of organic carbon on the filters is determined using \gls{TOCa} analysis. For this, \gls{NPOCa} and \gls{TOCa} of filter samples are measured. While the pertaining instrument, Shimazdu TOC Analyser 200, directly provides measurements of \gls{NPOCa}, the value of \gls{TOCa} has to be computed via measurements of \gls{TCa} and \gls{ICa}, respectively:
|
||||
|
||||
\begin{equation}
|
||||
\gls{TOCs}\coloneqq\gls{TCs}-\gls{ICs}
|
||||
\end{equation}
|
||||
|
||||
The values of \gls{TOCa} and \gls{NPOCa} are measured in \unit{\milli\gramCarbon\per\liter}.
|
||||
|
||||
\subsection{Preparation}
|
||||
|
||||
Preparation for \gls{TOCa} measurements essentially consists in cleaning glassware required for analysis and extraction. This is rather not straightforward, and two procedures need to be distinguished: a special procedure before the campaign to obtain a standard of cleanliness, and a procedure during the campaign to retain the obtained standard.
|
||||
|
||||
\subsubsection{Intial Cleaning}
|
||||
\subsubsection{Intial Glassware Cleaning}
|
||||
|
||||
During initial cleaning, \gls{NPOCa} of glassware is tested. Glassware is considered clean if $\gls{NPOCs}<\qty{0.1}{\milli\gram\per\liter}$.
|
||||
|
||||
\subsubsection{Subsequent cleaning steps}
|
||||
\subsubsection{Subsequent Glassware cleaning}
|
||||
|
||||
\subsection{Extraction}
|
||||
|
||||
\subsection{Calibration}
|
||||
|
||||
Calibration for \gls{TOCa} and \gls{NPOCa} measurements require that the instrument be calibrated prior to measurements. For this, stock solutions of known quantites are related to the instrument response, i.e. area under the voltage curve. For \gls{TOCa} measurements, two stock solutions are required, one containing a known quantity of \gls{TCa}, and one where the exact amount of \gls{ICa} is known. In practice, \gls{TCa} calibration can be performed using a \gls{TOCa} stock solution. This is possible because the used standard of \gls{TOCa} is practically free of any \gls{ICa} --- for the used \gls{TOCa} standard, it therefore holds that $\gls{TCs}\approx\gls{TOCs}$.
|
||||
|
||||
A \gls{TOCa} solution of \qty{1000}{\milli\gramCarbon\per\liter} is used to create a \gls{TOCa} calibrant stock solution of \qty{4}{\milli\gramCarbon\per\liter}. For this, exactly \qty{1}{\milli\liter} of \qty{1000}{\milli\gramCarbon\per\liter} solution is mixed with \qty{244}{\milli\liter} MQ. Similarly, an \gls{ICa} stock solution of \qty{1000}{\milli\gram\per\liter} is used to mix an \gls{ICa} calibrant stock of \qty{4}{\milli\gramCarbon\per\liter} by mixing \qty{1}{\milli\liter} of stock solution with \qty{244}{\milli\liter} MQ.
|
||||
|
||||
|
||||
\subsection{Measurements}
|
||||
|
||||
\begin{figure}
|
||||
|
||||
+11
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@@ -193,6 +193,14 @@
|
||||
description={oxygenated volatile organic compound}
|
||||
}
|
||||
|
||||
\newglossaryentry{BVOCa}{
|
||||
type=\acronymtype,
|
||||
first={biogenic volatile organic compound (BVOC)},
|
||||
firstplural={biogenic volatile organic compounds (BVOCs)},
|
||||
name={BVOC},
|
||||
description={biogenic volatile organic compound}
|
||||
}
|
||||
|
||||
\newglossaryentry{LVOCa}{
|
||||
type=\acronymtype,
|
||||
first={low-volatity organic compound (LVOC)},
|
||||
@@ -333,7 +341,7 @@
|
||||
|
||||
\newglossaryentry{TOCa}{
|
||||
type=\acronymtype,
|
||||
first={total organic carbon (TOC)},
|
||||
first={total organic carbon (TOC)\glsadd{TOCs}},
|
||||
name={TOC},
|
||||
description={Total organic carbon}
|
||||
}
|
||||
@@ -347,14 +355,14 @@
|
||||
|
||||
\newglossaryentry{ICa}{
|
||||
type=\acronymtype,
|
||||
first={inorganic carbon (IC)},
|
||||
first={inorganic carbon (IC)\glsadd{ICs}},
|
||||
name={IC},
|
||||
description={inorganic carbon}
|
||||
}
|
||||
|
||||
\newglossaryentry{TCa}{
|
||||
type=\acronymtype,
|
||||
first={total carbon (TC)},
|
||||
first={total carbon (TC)\glsadd{TCs}},
|
||||
name={TC},
|
||||
description={Total carbon}
|
||||
}
|
||||
|
||||
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-94
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@@ -67,6 +67,24 @@
|
||||
description={Mass flow rate}
|
||||
}
|
||||
|
||||
@symbol{TOCs,
|
||||
unit={\qty{}{\milli\gram\per\liter}},
|
||||
name={\ensuremath{\textnormal{TOC}}},
|
||||
description={Total organic carbon}
|
||||
}
|
||||
|
||||
@symbol{ICs,
|
||||
unit={\qty{}{\milli\gram\per\liter}},
|
||||
name={\ensuremath{\textnormal{IC}}},
|
||||
description={Inorganic carbon}
|
||||
}
|
||||
|
||||
@symbol{TCs,
|
||||
unit={\qty{}{\milli\gram\per\liter}},
|
||||
name={\ensuremath{\textnormal{TC}}},
|
||||
description={Total carbon}
|
||||
}
|
||||
|
||||
@symbol{NPOCs,
|
||||
unit={\qty{}{\milli\gram\per\liter}},
|
||||
name={\ensuremath{\textnormal{NPOC}}},
|
||||
|
||||
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\subfile{../chapters/06_acknowledgements.tex}
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|
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\appendix
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|
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|
||||
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|
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|
||||
\graphicspath{{../../graphics/charts/}{../../config/logos/}{../../config/titlepage/}}
|
||||
|
||||
%% ------------------------------------------------------------------%
|
||||
%% PACKAGES
|
||||
|
||||
%\usepackage{amsfonts}
|
||||
%\usepackage{amsmath}
|
||||
%\usepackage{amssymb}
|
||||
\usepackage{amsthm}
|
||||
%\usepackage{alphalph}
|
||||
%\usepackage[toc,page]{appendix}
|
||||
%\usepackage[affil-it]{authblk}
|
||||
\usepackage[backend=biber,
|
||||
style=authoryear,
|
||||
citestyle=authoryear,
|
||||
natbib,
|
||||
maxcitenames=1,
|
||||
maxbibnames=99,
|
||||
doi=false,
|
||||
isbn=false,
|
||||
url=false,
|
||||
eprint=false,
|
||||
giveninits=true]{biblatex}
|
||||
%\usepackage{blindtext}
|
||||
%\usepackage{commath}
|
||||
%\usepackage{dblfnote}
|
||||
%\usepackage{dirtree}
|
||||
%\usepackage{dirtytalk}
|
||||
style=science,
|
||||
citestyle=science,
|
||||
natbib,
|
||||
maxcitenames=1,
|
||||
maxbibnames=99,
|
||||
doi=false,
|
||||
isbn=false,
|
||||
url=false,
|
||||
eprint=false,
|
||||
giveninits=true]{biblatex}
|
||||
\addbibresource{../../config/literature.bib}
|
||||
|
||||
%\usepackage{eso-pic}
|
||||
%\usepackage{epstopdf}
|
||||
%\epstopdfsetup{outdir=../graphics/}
|
||||
|
||||
%\usepackage{etoolbox}
|
||||
\usepackage{pdfpages}
|
||||
\usepackage{fancyhdr}
|
||||
%\usepackage{float}
|
||||
%\usepackage[record=hybrid, acronym, symbols, automake, indexcrossrefs=true, autoseeindex=true, stylemods={longextra}]{glossaries-extra}
|
||||
\usepackage{graphbox}
|
||||
%\usepackage[colorlinks=true, linktoc=true, allcolors=black]{hyperref} % allcolors=black
|
||||
%\usepackage{imakeidx}
|
||||
%\usepackage{kantlipsum}
|
||||
%\usepackage{lastpage}
|
||||
%\usepackage[switch*, modulo]{lineno}
|
||||
%\usepackage{mathtools}
|
||||
\usepackage[arrows=pgf-filled, version=4]{mhchem}
|
||||
%\usepackage{multicol}
|
||||
%\usepackage{nameref}
|
||||
%\usepackage{setspace}
|
||||
\usepackage[free-standing-units=true]{siunitx}
|
||||
\usepackage{subcaption}
|
||||
%\usepackage{scrwfile}
|
||||
%\usepackage{tabularray}
|
||||
%\usepackage{tikz}
|
||||
%\usepackage{tikz-3dplot}
|
||||
\usepackage[breakable, many]{tcolorbox}
|
||||
\usepackage{tikz}
|
||||
%\usepackage[titles]{tocloft}
|
||||
%\usepackage{verbatim}
|
||||
%\usepackage{xcolor}
|
||||
|
||||
% Chemical equations and according setup: Needs to be loaded after \usepackage{mhchem}
|
||||
\usepackage{chemmacros}
|
||||
@@ -102,18 +80,24 @@ reactions/tag-close=]
|
||||
%\usetheme{Darmstadt}
|
||||
\usecolortheme{seagull}
|
||||
|
||||
\setbeamersize{sidebar width left= 0pt}
|
||||
\setbeamersize{text margin left = 0.3cm}
|
||||
\setbeamersize{text margin right = 0.3cm}
|
||||
|
||||
% Fonts
|
||||
\setbeamerfont{frametitle}{size=\large, series=\itshape\bfseries}
|
||||
\setbeamerfont{frametitle}{size=\large, series=\itshape\bfseries}
|
||||
|
||||
% Logo
|
||||
\addtobeamertemplate{frametitle}{}{
|
||||
\addtobeamertemplate{background}{}{
|
||||
\begin{tikzpicture}[remember picture, overlay]
|
||||
\node[anchor=north east, yshift=2pt] at (current page.north east) {\includegraphics[height=0.4cm, align=c]{PSI_Logo.pdf}\hspace*{0.15cm}
|
||||
\includegraphics[height=0.3cm, align=c]{iac_logo.pdf}\hspace*{0.15cm}
|
||||
\includegraphics[height=0.4cm, align=c]{ETH_Logo.pdf}};
|
||||
\end{tikzpicture}}
|
||||
\node[anchor=south east, yshift=0.85em] at (current page.south east) {
|
||||
\includegraphics[height=0.3cm, align=c]{PSI_Logo.pdf}\hspace*{0.15cm}
|
||||
\includegraphics[height=0.25cm, align=c]{iac_logo.pdf}\hspace*{0.15cm}
|
||||
\includegraphics[height=0.3cm, align=c]{ETH_Logo.pdf}
|
||||
};
|
||||
\end{tikzpicture}
|
||||
}
|
||||
|
||||
% Title Format
|
||||
\makeatletter
|
||||
@@ -125,35 +109,48 @@ reactions/tag-close=]
|
||||
\makeatletter
|
||||
\def\beamer@andinst{\\[0.25em]}
|
||||
\makeatother
|
||||
|
||||
\makeatletter
|
||||
\let\leftmarginone\beamer@leftmargin
|
||||
\let\leftmargintwo\beamer@leftsidebar
|
||||
\makeatother
|
||||
|
||||
\setbeamertemplate{title page}{
|
||||
\setlength\parindent{0pt}
|
||||
|
||||
|
||||
\vfill
|
||||
\usebeamerfont{date}\insertdate{:}\par
|
||||
\usebeamerfont{subtitle}\insertsubtitle\par
|
||||
\vspace*{0.5em}
|
||||
\usebeamerfont{title}\inserttitle\par
|
||||
\vspace*{1em}
|
||||
\usebeamerfont{author}\insertauthor\par
|
||||
\vfill
|
||||
\vspace{2em}
|
||||
\insertinstitute
|
||||
\vspace*{0.5em}
|
||||
}
|
||||
\addtobeamertemplate{title page}{
|
||||
\begin{tikzpicture}[remember picture, overlay]
|
||||
\node[anchor=north east, yshift=2pt] at (current page.north east){
|
||||
\includegraphics[height=0.4cm, align=c]{PSI_Logo.pdf}\hspace*{0.15cm}
|
||||
\includegraphics[height=0.3cm, align=c]{iac_logo.pdf}\hspace*{0.15cm}
|
||||
\includegraphics[height=0.4cm, align=c]{ETH_Logo.pdf}
|
||||
};
|
||||
\end{tikzpicture}
|
||||
\begin{center}
|
||||
\begin{tikzpicture}[remember picture, overlay]
|
||||
\node [anchor=center] at (current page.center){
|
||||
\node[anchor=center] at (current page.center){
|
||||
\includegraphics[width=\paperwidth]{title_page.png}
|
||||
};
|
||||
\end{tikzpicture}
|
||||
\end{center}}{}
|
||||
\makeatother
|
||||
\end{center}
|
||||
\begin{tikzpicture}[remember picture, overlay]
|
||||
\node[below right, yshift=-2pt, xshift=\leftmarginone - 2pt] at (current page.north west){
|
||||
\includegraphics[height=0.5cm, align=c]{PSI_Logo.pdf}
|
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\hspace*{2em}
|
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\includegraphics[height=0.4cm, align=c]{iac_logo.pdf}
|
||||
\hspace*{2em}
|
||||
\includegraphics[height=0.5cm, align=c]{ETH_Logo.pdf}
|
||||
\hspace*{\fill}
|
||||
};
|
||||
\end{tikzpicture}
|
||||
}{}
|
||||
|
||||
% Page numbers
|
||||
\setbeamertemplate{page number in head/foot}[totalframenumber]
|
||||
|
||||
% Title
|
||||
\author[D. Tschan]{
|
||||
@@ -173,6 +170,65 @@ reactions/tag-close=]
|
||||
\inst{2} Laboratory for Atmospheric Chemistry, Paul-Scherrer Institute (PSI)}
|
||||
\date{28.09.2026}
|
||||
|
||||
% Bibliography size
|
||||
\AtBeginBibliography{\footnotesize}
|
||||
|
||||
|
||||
%% GLOSSARY
|
||||
|
||||
% Create new glossary type
|
||||
\newglossary*{species}{species}
|
||||
\makeglossaries
|
||||
|
||||
% Prevents character escaping
|
||||
\renewcommand*{\glsxtrautoindexesc}{}
|
||||
|
||||
|
||||
%% SYMBOLS
|
||||
% Add glossary key 'unit' and 'formula'
|
||||
\glsaddkey{unit}{}{\glsentryunit}{\Glsentryunit}{\glsunit}{\Glsunit}{\GLSunit}
|
||||
\glsxtrprovidestoragekey{formula}{}{\Formula}
|
||||
|
||||
\GlsXtrLoadResources[
|
||||
src={../../config/symbols}, % data in symbols.bib
|
||||
sort-field={desc}, % sort by name field
|
||||
sort={letter-nocase}, % case-insensitive letter sort
|
||||
type=symbols, % put these terms in the symbols list
|
||||
field-aliases={unit=symbol}, % convert unit key to symbol
|
||||
save-locations=false % don't save location lists
|
||||
]
|
||||
|
||||
%% CHEMICAL SPECIES
|
||||
\GlsXtrLoadResources[
|
||||
src={../../config/species}, % data in symbols.bib
|
||||
sort-field={desc}, % sort by name field
|
||||
sort={letter-nocase}, % case-insensitive letter sort
|
||||
type=species, % put these terms in the symbols list
|
||||
field-aliases={formula=symbol}, % convert unit key to symbol
|
||||
save-locations=false % don't save location lists
|
||||
]
|
||||
|
||||
% Enable hyperlinks for glossary
|
||||
\glsenablehyper
|
||||
\input{../../config/glossary}
|
||||
|
||||
% SISETUP
|
||||
\DeclareSIUnit\amu{u}
|
||||
\DeclareSIUnit\bar{bar}
|
||||
\DeclareSIUnit\year{yr}
|
||||
\DeclareSIUnit\month{m}
|
||||
\DeclareSIUnit\week{w}
|
||||
\DeclareSIUnit\day{d}
|
||||
\DeclareSIUnit\ppm{ppm}
|
||||
\DeclareSIUnit\ppb{ppb}
|
||||
\DeclareSIUnit\ppt{ppt}
|
||||
\DeclareSIUnit\pptv{pptv}
|
||||
\DeclareSIUnit\atm{atm}
|
||||
\DeclareSIUnit\Molar{M}
|
||||
\DeclareSIUnit\gramCarbon{g\ce{C}}
|
||||
\DeclareSIUnit\permille{\text{\textperthousand}}
|
||||
\sisetup{separate-uncertainty, multi-part-units=single, range-units=single, range-phrase=\ensuremath{\ldots}}
|
||||
|
||||
|
||||
\begin{document}
|
||||
|
||||
@@ -181,21 +237,236 @@ reactions/tag-close=]
|
||||
\titlepage
|
||||
\end{frame}
|
||||
|
||||
\frame{
|
||||
\frametitle{some title}
|
||||
\framesubtitle{something}
|
||||
}
|
||||
\begin{frame}[plain]
|
||||
\small
|
||||
Literature cited in this presentation and the information contained therein is drawn from my Master's Thesis proposal entitled «Photochemical reduction of iodate through iron-containing complexes in secondary organic aerosol from monoterpene oxidation», handed in on 21.12.2025, for the course \emph{701-1211-01 Master Seminar: Atmosphere and Climate}. This proposal is declared here to be an official reference, but it is not stated within the reference section. No information has been copied in verbatim, and all information is paraphrased if it has been used.
|
||||
\end{frame}
|
||||
|
||||
\section{Introduction}
|
||||
|
||||
\begin{frame}
|
||||
\frametitle{Hello world}
|
||||
This is some text
|
||||
\frametitle{Motivation}
|
||||
\framesubtitle{Relevance --- why should be care about Iodine?}
|
||||
|
||||
In the atmosphere, iodine is important in several ways:
|
||||
|
||||
\begin{enumerate}
|
||||
\item<2-> It may contibute to (stratospheric) \glssymbol{O3f} depletion \citep{saiz-lopez_atmospheric_2012, carpenter_biogeochemical_2015, saiz-lopez_reactive_2012} (planetary health);
|
||||
\item<3-> It could form particles when reacting with oxygen that could grow into cloud-condensation nuclei \cite{saiz-lopez_atmospheric_2012} (direct- and indirect radiative forcing);
|
||||
\item<4-> \ldots
|
||||
\end{enumerate}
|
||||
|
||||
\end{frame}
|
||||
|
||||
\begin{frame}
|
||||
\frametitle{Some title}
|
||||
Some words
|
||||
\frametitle{Motivation}
|
||||
\framesubtitle{Monoterpenes and Iodine in the Atmosphere}
|
||||
|
||||
\begin{minipage}[b]{0.65\textwidth}
|
||||
\centering
|
||||
\only<1>{\includegraphics[width=\textwidth]{14_Introduction_Overview_01.pdf}}%
|
||||
\only<2>{\includegraphics[width=\textwidth]{14_Introduction_Overview_02.pdf}}%
|
||||
\only<3>{\includegraphics[width=\textwidth]{14_Introduction_Overview_03.pdf}}%
|
||||
\only<4>{\includegraphics[width=\textwidth]{14_Introduction_Overview_04.pdf}}%
|
||||
\only<5>{\includegraphics[width=\textwidth]{14_Introduction_Overview_05.pdf}}%
|
||||
\only<6>{\includegraphics[width=\textwidth]{14_Introduction_Overview_06.pdf}}%
|
||||
\only<7>{\includegraphics[width=\textwidth]{14_Introduction_Overview_07.pdf}}%
|
||||
\only<8>{\includegraphics[width=\textwidth]{14_Introduction_Overview_08.pdf}}%
|
||||
\only<9>{\includegraphics[width=\textwidth]{14_Introduction_Overview_09.pdf}}%
|
||||
\only<10>{\includegraphics[width=\textwidth]{14_Introduction_Overview_10.pdf}}%
|
||||
\only<11>{\includegraphics[width=\textwidth]{14_Introduction_Overview_11.pdf}}%
|
||||
\only<12>{\includegraphics[width=\textwidth]{14_Introduction_Overview_12.pdf}}%
|
||||
\only<13>{\includegraphics[width=\textwidth]{14_Introduction_Overview_13.pdf}}%
|
||||
\end{minipage}%
|
||||
\hfill
|
||||
\begin{minipage}[b]{0.33\textwidth}
|
||||
|
||||
\small
|
||||
\only<3>{Atmospheric mixing ratios:\\
|
||||
$\gls{CHIs}_{\ce{I2}}\approx\qty{93}{\pptv}$ \citep{carpenter_biogeochemical_2015},\\
|
||||
$\gls{CHIs}_{\glssymbol{IO.f}}\approx\qtyrange{3}{20}{\pptv}$ \citep{carpenter_biogeochemical_2015},\\
|
||||
$\gls{CHIs}_{\ce{HOI}}\approx\qty{1}{\pptv}$ \citep{he_role_2021},\\ $\gls{CHIs}_{\glssymbol{I.f}}\approx\qtyrange{0.1}{22}{\pptv}$ \citep{carpenter_biogeochemical_2015, he_role_2021}.}
|
||||
|
||||
\small
|
||||
\begin{itemize}
|
||||
\item<4> \glsname{VOCa}: \glsdesc{VOCa}\glsadd{VOCa}.
|
||||
\item<4> \glsname{LVOCa}: \glsdesc{LVOCa}
|
||||
\item<5> \glsname{SOAa}: \glsdesc{SOAa}
|
||||
\end{itemize}
|
||||
|
||||
\hfill
|
||||
|
||||
Relevant literature:
|
||||
\only<1>{\citep{kendrick_halogen_2024, whitehead_distribution_1984, muramatsu_recycling_2001, muramatsu_studies_2004, carrano_influence_2020}}
|
||||
\only<2>{\citep{carrano_influence_2020, elderfield_biophilic_1980, kupper_iodide_2008, amachi_microbial_2008, winter_exploring_2009, carpenter_biogeochemical_2015}}
|
||||
\only<3>{\citep{kupper_iodide_2008, carpenter_biogeochemical_2015, palmer_iodine_2005, liu_kinetics_2001, sakamoto_direct_2009, hayase_heterogeneous_2010, he_role_2021, carpenter_atmospheric_2013}}
|
||||
\only<4>{\citep{guenther_global_1995, guenther_model_2012, bianchi_highly_2019, hallquist_formation_2009, messina_global_2016, malik_environmental_2023}}
|
||||
\only<5>{\citep{bianchi_highly_2019, jokinen_production_2015, ng_secondary_2008, ehn_large_2014, kirkby_ion-induced_2016}}
|
||||
\only<6>{\citep{aal-abadleh_perspective_2023}}
|
||||
\only<7>{\citep{koenig_quantitative_2020}}
|
||||
\only<8>{\citep{saiz-lopez_atmospheric_2012}}
|
||||
\only<9>{\citep{saiz-lopez_reactive_2012}}
|
||||
\only<10>{\citep{koenig_ozone_2021}}
|
||||
\only<11>{\citep{koenig_quantitative_2020}}
|
||||
\only<13>{\citep{pillar-little_conversion_2013}}
|
||||
|
||||
|
||||
\end{minipage}
|
||||
|
||||
\hfill
|
||||
|
||||
\only<4>{
|
||||
\hbox{\emph{Monoterpenes are second-most important biogenic \glsname{VOCa} source after isoprenes (\qty{107.5}{\tera\gramCarbon\per\year} vs. \qty{465}{\tera\gramCarbon\per\year}) \cite{messina_global_2016, malik_environmental_2023}}}
|
||||
}
|
||||
\only<5>{
|
||||
\hbox{\emph{Oxidation products of monoterpenes (and isoprenes) may be common in \glsname{SOAa} as they have (very) low volatility \cite{bianchi_highly_2019}.}}
|
||||
}
|
||||
\only<6>{
|
||||
\hbox{\emph{Iron is most abundant transition mineral in dust. It may catalyse dust particle photochemistry \citep{aal-abadleh_perspective_2023}}}
|
||||
}
|
||||
\only<9>{
|
||||
\hbox{\emph{Recent tropospheric obeservations: more \gls{I-f} in aerosol than \gls{IO3-f} \citep{saiz-lopez_reactive_2012}. Thermodynamics?}}}
|
||||
\only<10>{
|
||||
\hbox{\emph{Free troposphere dust layers (\qtyrange{1.5}{7}{\kilo\meter}): $10\times\glssymbol{IO.f}$ than atmospheric background \citep{koenig_ozone_2021}.}}}
|
||||
\only<11>{
|
||||
\hbox{\emph{Without recycling scheme, sustained concentrations of \glssymbol{IO.f} in upper tropopshere / lower stratosphere cannot be explained \cite{koenig_quantitative_2020}.}}}
|
||||
\only<13>{
|
||||
\hbox{\emph{Presence of gas-phase \gls{IO.f} requires recycling mechanism. But how\ldots? Some ideas are here \citep{pillar-little_conversion_2013}}}}
|
||||
|
||||
\end{frame}
|
||||
|
||||
\begin{frame}
|
||||
\frametitle{Objectives}
|
||||
\framesubtitle{Open Questions}
|
||||
|
||||
Open \emph{scientific} questions include:
|
||||
\begin{itemize}
|
||||
\item<2-> By what mechanism is iodate reduced?
|
||||
\item<3-> Which organics are important in (photoactive) complex formation? Or in other words: is \gls{SOAa} a good proxy?
|
||||
\item<4-> Is light \emph{required}? What happens in the dark?
|
||||
\end{itemize}
|
||||
\vspace{\baselineskip}
|
||||
|
||||
\only<5->{These questions entail some \emph{methodological} questions, in turn:}
|
||||
\begin{itemize}
|
||||
\item<6-> How can we represent the oxidation process of \glspl{VOCa} to \glspl{LVOCa} in the laboratory?
|
||||
\item<7-> How can we represent the processes within the aerosol in the laboratory?
|
||||
\end{itemize}
|
||||
\vspace{\baselineskip}
|
||||
|
||||
\only<8->{Asking these questions can help us making some (necessary) simplifications:}
|
||||
\begin{enumerate}
|
||||
\item<9-> We will use the following \gls{VOCa} to represent the organics: the monoterpenes \glstext{A-PINENEf}, \glstext{B-PINENEf} and \glstext{LIMONENEf}.
|
||||
\item<10-> The oxidation process of \glstext{A-PINENEf}, \glstext{B-PINENEf} and \glstext{LIMONENEf} to create a pertaining \gls{SOAa} will be done using an \glsfirst{OFRa} (see next slides).
|
||||
\item<11-> The acutual atmospheric process will be represented with a \glsfirst{CWFTRa} (see next slides). The product species will be monitored used a \gls{BTOF-CIMSa}.
|
||||
\end{enumerate}
|
||||
|
||||
\end{frame}
|
||||
|
||||
\begin{frame}
|
||||
\frametitle{Objective}
|
||||
\framesubtitle{Goals of the project}
|
||||
|
||||
\begin{enumerate}
|
||||
\item<1-> Produce \glsname{SOAa} in \glsname{OFRa};
|
||||
\item<2-> With the \glsname{SOAa}, perform \gls{CWFTRa} experiments;
|
||||
\item<3-> Test the response of the three systems \glstext{A-PINENEf}, \glstext{B-PINENEf}, \glstext{LIMONENEf}.
|
||||
\end{enumerate}
|
||||
\vspace*{\baselineskip}
|
||||
|
||||
\only<4->{
|
||||
\hbox{$\textnormal{System}=\ce{Fe}+\glssymbol{IO3-f}+\textnormal{\gls{SOAa}-extract}$}
|
||||
}
|
||||
|
||||
\vspace*{\baselineskip}
|
||||
\begin{center}
|
||||
\only<5->{\includegraphics[width=\textwidth]{05_Method_Overview.pdf}}
|
||||
\end{center}
|
||||
\end{frame}
|
||||
|
||||
\section{Method}
|
||||
|
||||
\begin{frame}
|
||||
\frametitle{Laboratory Representation}
|
||||
\framesubtitle{SOA generation --- Oxidation Flow Reactor}
|
||||
|
||||
\begin{center}
|
||||
\includegraphics[scale=0.65]{03_OFR_Flowchart.pdf}
|
||||
\end{center}
|
||||
\end{frame}
|
||||
|
||||
\begin{frame}
|
||||
\frametitle{Laboratory Representation}
|
||||
\framesubtitle{SOA generation --- Oxidation Flow Reactor --- Important Aspects}
|
||||
|
||||
\begin{itemize}[<+->]
|
||||
\item<1-> \Glsfirst{SMPSa} allows to \emph{estimate} particle density of generated SOA
|
||||
\item<2-> To know it, we measure \glsfirst{TOCa} using a \gls{TOCa} analyser
|
||||
\end{itemize}
|
||||
\end{frame}
|
||||
|
||||
\begin{frame}
|
||||
\frametitle{Laboratory Representation}
|
||||
\framesubtitle{Fe-SOA Complex Reaction with UV --- Coated Wall Flow Tube Reactor}
|
||||
|
||||
\begin{center}
|
||||
\includegraphics[scale=0.65]{01_CWFTR_Flowchart.pdf}
|
||||
\end{center}
|
||||
\end{frame}
|
||||
|
||||
\section{Results}
|
||||
|
||||
\begin{frame}
|
||||
\frametitle{Amount of SOA on filter}
|
||||
\framesubtitle{SMPS estimates: \only<1>{\glsname{A-PINENEf}}\only<2>{\glsname{LIMONENEf}}\only<3>{\glsname{B-PINENEf}}}
|
||||
|
||||
\centering
|
||||
\only<1>{\includegraphics[width=0.65\textwidth]{../../../analysis/OFR_Analysis/20260903_SET02_EXP14/figure.pdf}}%
|
||||
\only<2>{\includegraphics[width=0.65\textwidth]{../../../analysis/OFR_Analysis/20260914_SET02_EXP18/figure.pdf}}%
|
||||
\only<3>{\includegraphics[width=0.65\textwidth]{../../../analysis/OFR_Analysis/20260916_SET02_EXP22/figure.pdf}}%
|
||||
\end{frame}
|
||||
|
||||
\begin{frame}
|
||||
\frametitle{First CWFTR Results}
|
||||
\framesubtitle{\only<1>{Baseline}\only<2>{\ce{Fe(III)} species}\only<3>{\ce{Fe(II)} species}}
|
||||
|
||||
\centering
|
||||
\only<1>{\includegraphics[page=6, width=0.7\textwidth]{20260721_edited_for_Markus_on_20260811.pdf}}%
|
||||
\only<2>{\includegraphics[page=8, width=0.7\textwidth]{20260721_edited_for_Markus_on_20260811.pdf}}%
|
||||
\only<3>{\includegraphics[page=9, width=0.7\textwidth]{20260721_edited_for_Markus_on_20260811.pdf}}%
|
||||
\end{frame}
|
||||
|
||||
\section{Conclusion}
|
||||
\begin{frame}
|
||||
\frametitle{Conclusion}
|
||||
\framesubtitle{Some final words on the process}
|
||||
|
||||
\only<1->{\textbf{Challenges:}}
|
||||
\begin{itemize}
|
||||
\item<2-> There is a \emph{lot} of laboratory work\ldots Time management is \emph{hard}.
|
||||
\item<3-> Many different instruments: \gls{OFRa}, \gls{SMPSa}, \gls{BTOF-CIMSa}, \gls{TOCa}, plus cleaning procedures\ldots There is a large learning overhead here.
|
||||
\item<4-> Commuting...
|
||||
\end{itemize}
|
||||
\vspace*{\baselineskip}
|
||||
|
||||
\only<5->{\textbf{What is going well:}}
|
||||
\begin{itemize}
|
||||
\item<6-> All protocols for all experimental steps are nearly done!
|
||||
\item<7-> I have one more experimental campaign, then I am done with lab!
|
||||
\item<8-> I have learned a \emph{lot} about data handling, lab work, precision,\ldots
|
||||
\end{itemize}
|
||||
|
||||
\end{frame}
|
||||
|
||||
\begin{frame}[allowframebreaks]
|
||||
\frametitle{References}
|
||||
Much of the literature listed hereafter was taken over from the Master's Thesis proposal, without double-checking it again.
|
||||
\vspace{\baselineskip}
|
||||
|
||||
\printbibliography
|
||||
\end{frame}
|
||||
|
||||
|
||||
%\uselengthunit{mm}\printlength{\textwidth}
|
||||
%\uselengthunit{mm}\printlength{\textheight}
|
||||
\end{document}
|
||||
Reference in new issue
Block a user