A dense region of a gaseous and dusty cloud collapses to form a protostar surrounded by a disk and an envelope. This thesis uses both observations and models to study physical and chemical... Show moreA dense region of a gaseous and dusty cloud collapses to form a protostar surrounded by a disk and an envelope. This thesis uses both observations and models to study physical and chemical conditions of these protostellar systems which are likely where planets start to form. From the observational side, ALMA is used to quantify abundance ratios of complex organic molecules (COMs) in the gas around young protostars. These ratios are found to be remarkably constant for various nitrogen-bearing COMs which points to formation of these molecules under similar conditions, likely in ices of the prestellar phase. Moreover, observations of JWST are used to tentatively detect molecules such as methyl cyanide and ethyl cyanide in interstellar ices for the first time. In addition, high angular resolution ALMA observations of a protostellar system are analyzed to report the first detection of a disk wind candidate in methanol and hydrogen cyanide. From the modeling side, radiative transfer models are used to investigate how physical conditions such as source structure can change the molecular emission and molecular abundances. These models show that disk and optically thick dust can decrease the emission from COMs and change the correlations among their column densities. Show less
Complex Organic Molecules (COMs) have been detected in objects across different stages of stellar evolution. Many of these COMs are expected to form on interstellar ice and transfer later to the... Show moreComplex Organic Molecules (COMs) have been detected in objects across different stages of stellar evolution. Many of these COMs are expected to form on interstellar ice and transfer later to the gas phase. However, due to the challenge of detecting and assigning molecules in interstellar ice observations, the only frozen COM that has been unambiguously identified is methanol. This scenario is about to change, as the exceptional capabilities of the James Webb Space Telescope (JWST) enable the observation of weak signatures of molecules in interstellar ice.This thesis has a main focus on laboratory studies to support interstellar ice observation with the JWST. The results of the spectroscopic characterization of three COMs, acetone, methylamine, and methyl cyanide mixed in interstellar ice analogs are presented in Chapters 3, 4, and 5, respectively. The potential of their absorption features to trace these species in JWST observations is also discussed. Chapter 6 presents a new experimental approach to studying morphological changes in frozen CO, which is important to understand its morphology in space. Chapter 7 presents a computational study that simulates the infrared spectra of small fullerenes (between 44-70 C atoms) and provides insights for future JWST searches for these molecules Show less
Stars like the sun are born in large molecular clouds existing from gas and dust. During the formation process, the chemical composition of the material can be altered drastically by the changing... Show moreStars like the sun are born in large molecular clouds existing from gas and dust. During the formation process, the chemical composition of the material can be altered drastically by the changing physical conditions. This thesis focuses on how molecules in young protostellar systems are inherited from molecular clouds. The emphasis lies on so-called complex organic molecules and accretion shocks.Based on observations of complex organic molecules, it can be suggested that the molecular composition of a protostellar disk is (partially) inherited from the molecular cloud. The abundance ratio between various molecules is remarkably constant in various protostellar systems, implying that they form under similar conditions in molecular clouds. Furthermore, absence of complex molecules in observations does not directly mean that they are absent in the protostellar system but rather that they are hidden from us.This thesis also focuses on accretion shocks at the boundary between infalling cloud and protostellar disk. Based on a comparison between detailed numerical simulations and observations it can be suggested that strong accretions are not always present in protostellar systems. In turn, this suggests that the chemical composition in protostellar disks can be directly inherited from the molecular cloud. Show less
This Thesis shows discoveries in non-linear astrochemical kinetics as well as a deeper analysis of dark clouds chemistry. It is concluded that autocatalysis in interstellar gas-phase chemistry... Show moreThis Thesis shows discoveries in non-linear astrochemical kinetics as well as a deeper analysis of dark clouds chemistry. It is concluded that autocatalysis in interstellar gas-phase chemistry leads to bistability but when coupled with the gas-grain exchange of key species, the system can show Hopf bifurcation and lead to the appearance of complex chemical oscillations. The results and discussion of the five chapters allow further understanding of the chemical evolution in a gas phase system and in a gas-grain environment, providing better predictions to compare with future observations. Show less
This thesis is an experimental study of the UV irradiation of the interstellar ice analogues, relevant for the different stages of the star and planet formation sequence. It describes in detail... Show moreThis thesis is an experimental study of the UV irradiation of the interstellar ice analogues, relevant for the different stages of the star and planet formation sequence. It describes in detail photodesorption and photoconversion processes, and as such, contributes to worldwide efforts that aim at understanding how chemistry in space could have contributed to the origin of life on Earth and possibly planets around other stars. Show less
Organic molecules in interstellar space are important as they influence the structure of galaxies and star formations. Studying catalytic processes in space allows us to understand how molecular... Show moreOrganic molecules in interstellar space are important as they influence the structure of galaxies and star formations. Studying catalytic processes in space allows us to understand how molecular species are formed and chemically evolved in the interstellar medium and solar system objects. Quantum chemical methods, such as “Density Functional Theory” (DFT), can be employed to study the chemical pathways for the formation of molecular species, which is challenging with only observations and experiments. This thesis studies, with DFT methods, how polycyclic aromatic hydrocarbons (PAHs), the most abundant organic species in space, catalyze the formation of molecular hydrogen in the interstellar medium. Specifically, how linear PAHs become superhydrogenated and how the presence of Stone Wales defect in PAHs contributes to their catalytic activity for molecular hydrogen formation. In addition, this thesis reports the study of the catalytic activity of forsterite, a silicate mineral abundant in grains, asteroids, and meteorites. Specifically, the presence of Schottky MgO vacancy in forsterite can catalyze the C-H activation of PAHs as the first step to study the breakdown reaction of PAHs in asteroidal settings. The latter is indispensable to understand the formation of the so-called organic inventory of solar system objects. Show less
This thesis is largely an experimental study on the formation of solid-state simple and complex organic molecules in the H2O-rich and CO-rich ice phases of dense interstellar clouds and dark cores.... Show moreThis thesis is largely an experimental study on the formation of solid-state simple and complex organic molecules in the H2O-rich and CO-rich ice phases of dense interstellar clouds and dark cores. Astronomical ice observations are also presented and are strongly linked to the experimental work. For decades, it has been realized that particularly complex organic molecules can be formed at extremely low temperatures with the aid of 'energetic' particles, such as UV photons. In this thesis, it is clearly shown that complex organic molecules can also be formed without 'energetic' particles. The experimental laboratory work is supported by computational calculations to constrain which molecules are more or less likely to form under the extreme conditions of interstellar clouds. Show less
This thesis discusses the physical and chemical processes than influence the composition of forming planets. The focus is on the effect of these processes on the abundance and distribution of... Show moreThis thesis discusses the physical and chemical processes than influence the composition of forming planets. The focus is on the effect of these processes on the abundance and distribution of moleculus in the birth places of planets, proto-planetary disks. The thesis further discusses how current and future observations can be used to quantify the effects of these processes. A good grasp of these processes will enable researchers to link the composition of (exo)planets to their formation origin. Specifically this thesis studies the the most abundant carbon and oxygen carrying molecules, CO, CO2 and H2O. Chemical modelling of CO indicates that conversion of CO into other molecules needs to be fast to explain the current observations. Study of the transport and distribution of CO2 indicate that the measured the CO2 abundance in the surface layers of disks is not bulk CO2 abundance. The power of spectroscopic CO observations in the infrared to find physical structures in disks, possibly created by planets is also discussed. Finally, a combination of infrared observations is used to show that the closest proto-planetary disk is poor in molecules that contain carbon and oxygen, indicating that a process is removing these molecules from the gas phase. Show less
Astronomical observations of cold regions in the universe show a rich inventory of ices. Part of these ices may end up on planets like our own, but in that journey they will be exposed to... Show moreAstronomical observations of cold regions in the universe show a rich inventory of ices. Part of these ices may end up on planets like our own, but in that journey they will be exposed to considerable amounts of radiation. As water is the main component of these ices, the optical and photochemical properties of water ice largely determine how the radiation affects the molecules embedded in the ice. In this thesis, water ice is investigated as a host for photochemical reactions. A new laboratory setup is constructed, and two types of molecules are studied: glycine, an amino acid, and triphenylene, a polycyclic aromatic hydrocarbon. The photochemistry upon exposure to ultraviolet radiation is studied using UVvis and infrared spectroscopy. In addition, the optical properties of water ice are constrained in the UV-vis range, resulting in high-resolution optical constants, relevant for all ice-rich environments - from far away in space to our atmosphere. Water itself does not absorb light in this range, but as most organic molecules do, and are destroyed by radiation in this range, this is of high importance for molecules within the ice. Show less
The thesis explores how interstellar chemistry evolves as a function of time and changing physical architectures during the formation of stars. The motivation behind the work is an aspiration to... Show moreThe thesis explores how interstellar chemistry evolves as a function of time and changing physical architectures during the formation of stars. The motivation behind the work is an aspiration to better understand how the Solar System came to be, which processes led to its chemical composition and ultimately, what enabled life to evolve on Earth. Show less
In this thesis, we present new laboratory data of interstellar dust analogues. These measurements, were transformed to interstellar dust models and were used to fit the spectra of low-mass X... Show moreIn this thesis, we present new laboratory data of interstellar dust analogues. These measurements, were transformed to interstellar dust models and were used to fit the spectra of low-mass X-ray binaries located in the Galactic center neighborhood in order to determine the dust properties along those lines of sight. In these spectra, we focus in particular on the Si K-edge. The XAFS features in the Si K-edge offer a range of possibilities to study silicon-bearing dust, such as investigating the crystallinity, abundance and the chemical composition. We also present a study on the prospects of observing carbon, sulfur, and other lower abundance elements (namely Al, Ca, Ti and Ni) present in the interstellar medium using future X-ray instruments. We simulated data of instruments with characteristics of resolution and sensitivity of the Athena, XARM and Arcus concepts. Lastly, we explore the theory of X-ray scattering for a new parameter space where the small angle approach is no longer valid and where the size distribution of the dust includes large (> 1 micron) particles. We apply this theory to the environment of stellar debris disks where such conditions apply. We use as a best test case the debris disk of AU Microscopii. Show less
This thesis addresses the chemical processes that determine the compositions of giant planet atmospheres. Connecting the observed composition of exoplanets to their formation sites often involves... Show moreThis thesis addresses the chemical processes that determine the compositions of giant planet atmospheres. Connecting the observed composition of exoplanets to their formation sites often involves comparing the observed planetary atmospheric carbon-to-oxygen (C/O) ratio to a disk midplane model with a fixed chemical composition. In this scenario chemistry during the planet formation era is not considered, and the C/O ratios of gas and ice in disk midplane are simply defined by volatile icelines in a midplane of fixed chemical composition. However, kinetic chemical evolution during the lifetime of the gaseous disk can change the relative abundances of volatile species, thus altering the C/O ratios of planetary building blocks. In my chemical evolution models I utilize a large network of gas-phase, grain-surface and gas-grain interaction reactions, thus providing a comprehensive treatment of chemistry. In my talk I will show how chemical evolution can modify disk miplane chemistry and how this affects the C/O ratio of giant planet-forming material. I will argue that midplane chemical evolution needs to be addressed when predicting the chemical makeup of planets and their atmospheres. And as an extra, I will propose that chemical evolution can help constrain the formation histories of comets. Show less
Laboratory, observation and modeling work on the dissociation of polycyclic aromatic hydrocarbons in interstellar environments and the formation of new molecular species through the fragmentation... Show moreLaboratory, observation and modeling work on the dissociation of polycyclic aromatic hydrocarbons in interstellar environments and the formation of new molecular species through the fragmentation process. Show less
This thesis is about the study of hydrocarbons via infrared spectroscopy. Hydrocarbons play an important role in the chemistry of a variety of astronomical environments from the diffuse... Show moreThis thesis is about the study of hydrocarbons via infrared spectroscopy. Hydrocarbons play an important role in the chemistry of a variety of astronomical environments from the diffuse interstellar medium to dense hydrocarbon atmospheres of solar system bodies (e.g., planetary atmospheres of Jupiter and Saturn’s moon Titan) and exoplanets. For most astronomical objects, the determination of chemical abundances, and consequently an understanding of the chemical evolution relies upon the observation of molecular spectra. However, to date astronomical models need to make assumptions, because not all of the molecules expected have been observed. This is due, in part, to a lack of accurate spectral data, which is needed for unambiguous identification. Using a combination of high-resolution infrared experiments and/or high level ab initio calculations of vibration frequencies and ground state spectroscopic constants, the infrared spectral data of HC2H, HC4H, HC6H, HC8H, C3H4, c-C3H3+ and Dn-PAHs (polycyclic aromatic hydrocarbons, PAH) are studied and presented, in order to fill in some of the missing spectral data. Show less
Large areas of space are filled by molecular clouds that consist of gas and dust grains that are the remnants of dead stars. When these clouds start collapsing, the decreasing temperature and... Show moreLarge areas of space are filled by molecular clouds that consist of gas and dust grains that are the remnants of dead stars. When these clouds start collapsing, the decreasing temperature and increasing density cause gas particles to start accreting onto dust grain surfaces. This results in layered geometries of partially mixed ices on top of the grains that act as molecule reservoirs and cryogenic catalysts on which both simple and complex molecules form in surface reactions. These grains form the material from which celestial bodies form. A good understanding of the elementary processes taking place in dark interstellar clouds, therefore, is necessary to understand the chemical inventory of stellar systems, like our own Solar system.This thesis focuses on laboratory studies investigating the surface chemistry of CO-rich ices on dust grains at temperatures as low as 10 K. The formation mechanisms of complex organic molecules (COMs) are investigated by non-energetic processes (e.g., hydrogenation) and energetic processes (e.g., photolysis). Moreover, the net transfer of the newly formed hydrogenated species from grain surfaces into the gas phase through non-thermal desorption is investigated to link the detection of COMs in the gas phase to their formation in the solid state. Show less
In this thesis chemical and physical processes in the ice mantles on interstellar dust grains are studied. With the Atacama Large Millimetre/submillimetre Array molecules of interest to the... Show moreIn this thesis chemical and physical processes in the ice mantles on interstellar dust grains are studied. With the Atacama Large Millimetre/submillimetre Array molecules of interest to the formation of bigger, life-bearing molecules are detected for the first time around the sun-like low-mass protostar IRAS 16293-2422. These detections give clues about the earliest conditions our solar system formed under and potentially how life on earth emerged. Laboratory studies investigate the formation of these complex species in a laboratory set-up mimicking the conditions on interstellar icy dust grains. In this ways formation routes for molecules with a so-called amide functional group are mapped. Show less
Multiple stars, that is two or more stars composing a gravitationally bound system, are common in the universe.They are the cause of many interesting phenomena, from supernovae and planetary... Show moreMultiple stars, that is two or more stars composing a gravitationally bound system, are common in the universe.They are the cause of many interesting phenomena, from supernovae and planetary nebulae, to binary black hole mergers. Observations of main sequence stars, young stars and forming protostars show that multiplicity is common, and that multiple stars are born. This thesis focuses on several of the open questions on the formation and evolution of multiple stars, namely when do rotationally supported disks form, the factors leading to fragmentation of the cloud core and the physico-chemical structure of multiple protostars. For this purpose, radio interferometric observations of dust continuum and molecular line emission, coupled with chemical and physical models are used to study several young, deeply embedded prototstars. The results of this thesis contribute useful pieces to the puzzle of multiple star formation, demonstrating that rotationally supported disks can form early in the star formation process, while temperature and the presence of disks can alter the physico-chemical protostellar structure. Furthermore, the results of this thesis indicate that mass, rather than temperature, could be an important factor in fragmentation of cloud cores, and the formation of multiple stars. Show less
Polycyclic aromatic hydrocarbons (PAHs) are the most abundant class of organic compounds in space. The PAH field evolves from the constant interaction between experimentalists, theorists,... Show morePolycyclic aromatic hydrocarbons (PAHs) are the most abundant class of organic compounds in space. The PAH field evolves from the constant interaction between experimentalists, theorists, modellers and observers. While laboratory research and quantum chemical calculations together set up the molecular properties of PAH species, astronomers on the other hand, retrieve as much information as possible from the space observations. Nowadays, the PAH field is advanced enough to start implementing all these results into astronomical models, in order to study PAHs from a molecular groundwork. In this regard, the research projects presented in this thesis do precisely that. They constitute a first attempt to gather the vast current knowledge available on specific PAH molecules (not using generic properties), and put it in an astrophysical context, and with it, target some of the key subjects of the field such as: the existence of the so-called grandPAHs in space; the role of PAHs in the formation of molecular hydrogen in photodissociation regions; the abundance of superhydrogenated PAHs and their contribution as a carrier of the 3.4 micron band observed in photodissociation regions; and the deuterium fractionation in PAHs, and their consequent role in explaining the observed deuterium abundance in the local interstellar medium. Show less
In recent years it has become clear that the space in between the stars, contains a remarkable amount of highly diverse molecules, ranging from simple diatomics to large complex species.... Show moreIn recent years it has become clear that the space in between the stars, contains a remarkable amount of highly diverse molecules, ranging from simple diatomics to large complex species. Astronomical observations and dedicated laboratory experiments show that icy dust grains play a prominent role in the chemical enrichment of matter in space. Exotic solid state reactions taking place for temperatures as low as -260 degree merge small abundant species to larger and larger compounds until species are formed that are considered to be of relevance for life; sugars, fats and precursors of amino acids. Ultimately this material is embedded in matter from which stars and planets form. So, could it be possible, that the ingredients for life form everywhere, in space, following very similar chemical pathways? In this thesis a dedicated laboratory study is described that studies exactly these processes. With a new experimental setup the physical and chemical processes are characterized that are needed to interpret and guide astronomical observations and that yield parameters needed as input in astrochemical models. It is concluded that the chemical complexity in the solid state reaches out much further than assumed so far. Show less
In this thesis we used numerical simulations to explore the role that chemistry plays in galaxy formation. Simulations of galaxies often assume chemical equilibrium, where the chemical reactions... Show moreIn this thesis we used numerical simulations to explore the role that chemistry plays in galaxy formation. Simulations of galaxies often assume chemical equilibrium, where the chemical reactions between ions and molecules have reached a steady state. However, this assumption may not be valid if the physical conditions of the gas are evolving rapidly. Therefore, we developed a chemical model to follow the non-equilibrium evolution of ions and molecules. We then incorporated this model into hydrodynamic simulations of galaxies. We ran simulations with different metallicities (i.e. different proportions of heavy elements) and UV radiation fields, first using our full non-equilibrium chemical model and then assuming chemical equilibrium. We found that the total star formation rate is higher at higher metallicity and for weaker radiation fields. In contrast, non-equilibrium chemistry does not strongly influence the total star formation rate or outflow properties of the galaxy. However, it does affect the abundances of individual chemical species, for example in molecular outflows. Finally, we explored the properties of molecular clouds in our simulations. At low metallicity, the molecular fraction of young clouds tends to be below equilibrium, as the molecules are still forming. This also affects the observable CO emission from young clouds. Show less
