Os compostos de fósforo apresentam várias implicações em processos atmosféricos e interestelares. Nesta tese, será realizado um estudo ab initio em três diferentes sistemas. (i) Um destes sistemas é o radical PCO. No capítulo três, foi analisado os aspectos conformacionais do radical PCO, sendo avaliado as propriedades moleculares e termodinâmicas da espécie cíclica e das espécies lineares. Entre os isômeros do radical PCO, a espécie i3 (C∞V, 2π) é a mais estável delas, com uma entalpia de formação a 0K de 22.33±2.10 kcal mol-1. Considerando as barreiras de energia, que convergem em direção a espécie i3, elas apresentam valores próximos de 10 kcal mol-1, ao passo que a energia necessária para a isomerização da molécula i3 para outros isômeros é acima de 60 kcal mol-1. Estes valores de energia explicam o fato que, em condições experimentais, foi detectado apenas a espécie i3 (C∞V, 2π). (ii) No capítulo quatro, foi elucidado o mecanismo da reação PH3 +F, assim como foi também caracterizado as propriedades eletrônicas dos intermediários observados nesta reação. Na reação PH3 +F, pode ser observado que, diferente da literatura, dois caminhos são possíveis para esta reação: (a) a reação de abstração de hidrogênio, com a formação dos produtos PH2 e HF, e a reação de adição-eliminação, com a formação das espécies PH2F e H. Analisando a energia eletrônica, é possível observar que a reação de adição-eliminação apresenta uma barreira de energia de 23 kcal mol-1 abaixo da mesma observada para a reação de abstração de hidrogênio. Considerando os intermediários formados na reação PH3 + F, são observados dois tipos de simetria: uma C1 e duas Cs. Além disso, a entalpia de formação em 298K dos intermediários variou de -22.99 to -29.74 kcal mol-1. (iii) No capítulo cinco, foi avaliada a interação da fosfina com diferentes aglomerados de água. Neste capítulo, foi realizada uma análise nos aglomerados PH3-(H2O)n (n=1-8,12,20) e avaliado a estabilidade dos potenciais isômeros, assim como as propriedades moleculares e espectroscópicas dos diferentes isômeros. Nas estruturas PH3-(H2O)n (n=1-8) foi possível observar que os modos vibracionais δ(PH3) e δsym(PH3) apresentaram um deslocamento para o vermelho, ao passo que as freqüências de estiramento simétrico e assimétrico da fosfina apresentaram um deslocamento para o azul. No caso da estrutura PH3(H2O)20, as variações nos modos vibracionais foram similares embora que mais intensas, sendo o mesmo também observado para as respectivas intensidades. Além disso, a energia necessária para o confinamento da fosfina no interior de um aglomerado de água dodecaedro hexagonal variou de -1.81 to -6.38 kcal mol-1. / The phosphorus compounds show several implications to atmospheric and interstellar processes. In this thesis, was performed an ab initio study on three different systems. (i) One of these systems is the PCO radical. In chapter three, was studied the conformation aspects of PCO radicals, which was assessed the molecular and thermodynamic properties of the cyclic and linear species. In PCO species, it was observed that the linear specie i3 (C∞V, 2π) is the most stable one, with the enthalpy formation at 0K of 22.33±2.10 kcal mol-1. Considering the barrier heights, which converge into the direction of i3, they are close to 10 kcal mol-1, while the energy necessary to the isomerization of i3 to other conformations are high than 60 kcal mol-1. These energy values explain the fact that, in experimental conditions, was detected only the i3 (C∞V, 2π) specie. (ii) In chapter four, it was elucidated the mechanism of the PH3 + F reaction, and it was also described the electronic properties of the intermediates observed in this reaction. In the PH3 + F reaction can be seen that, different from the literature, two possible pathways can be observed: (a) the hydrogen abstraction, with the formation of PH2 and HF products, (b) and the addition-elimination route, with the formation of PH2F and H species. Analyzing the electronic energy, can be observed that the barrier energy of the addition-elimination process is 23 kcal mol-1 bellow the hydrogen abstraction route. Considering the intermediates, two different point groups were detected: a C1 and two Cs. In addition, the enthalpy formation at 298K of the intermediates, in the PH3 + F reaction, range from -22.99 to -29.74 kcal mol-1. (iii) In chapter five, it was studied the interaction of phosphine with different water clusters. In this chapter was performed an analysis of the PH3-(H2O)n (n=1-8,12,20) clusters, and evaluated the stability of the potential isomers as also the molecular and spectroscopy aspects of the different species. In the PH3(H2O)n (n=1-8) structures are seen a redshift in the δ(PH3) and δsym(PH3) vibrational modes, while is observed a blueshift from the asymmetric and symmetric stretching frequencies of phosphine. In the case of PH3(H2O)20 structure, the variations in the vibrational modes were similar however more intense, as also in their respective intensities. In addition, the necessary energy to trap phosphine in the interior of an hexagonal dodecahedron water clusters range from -1.81 to -6.38 kcal mol-1.

Les étoiles sont de très mauvaises voisines: elles perturbent souvent leur environnement. Parfois, elles se déplacent à grande vitesse dans le milieu interstellaire (MIS). Souvent, elles subissent des soubresauts violents qui laissent une empreinte dans leur voisinage (jets, vents, supernovae). Ces flots supersoniques génèrent des chocs à la fois dans le matériau éjecté par l'étoile et dans l'environnement stellaire. L'étude de ces chocs constituent le sujet de cette thèse, et nous les modélisons avec le code de chocs stationnaires plan parallèle Paris-Durham, qui incorpore une riche panoplie de processus microphysiques et chimiques adaptés au MIS magnétisé.Tout d'abord, nous utilisons ce code pour modéliser des chocs magnétisés 3D pour des formes arbitraires à symétrie axiale, grâce à un formalisme qui lie mathématiquement la forme des chocs à une fonction de distribution de chocs 1D équivalente. Pour la première fois, nous examinons systématiquement l'effet de la géométrie, de l'âge, et de quelques autres paramètres sur le diagramme d'excitation de H2 résultant et la forme des profils raies d'émission de H2. Par exemple, nous dévoilons un effet géométrique qui montre que l'ajustement par des modèles 1D de l'émission de H2 observée sur un choc 3D est sujette à un biais vers les basses vitesses. Nous appliquons aussi nos modèles à l'observation de H2 spatialement intégrée de chocs d'étrave dans Orion BN-KL et BHR71 où nous obtenons un bien meilleur ajustement des observations avec un nombre à peine plus grand de paramètres comparé aux modèles précédents. Nous illustrons sur l'objet de Herbig-Haro HH54 la grande richesse d'information dynamique que renferme le profil des raies d'émission résolues de H2. Ensuite, nous incluons dans le code de Paris-Durham un ensemble minimal de processus nécessaires pour décrire les modèles de vents d'étoiles de la branche asymptotique des géantes (AGB): la dilution géométrique, l'éclairage UV externe, la pression de radiation sur les grains, la gravité, le chauffage dû au pompage radiatif par l'étoile, les réactions à trois corps et le passage du point sonique. Avec cet outil, nous commençons à examiner la cinétique chimique de l'hydrogène dans les vents d'étoiles AGB chaudes et froides. Nous suggérons que la faible abondance de HI déduite des observations s'explique par la forme principalement moléculaire que prend l'hydrogène. Nous générons le choc terminal dans le vent et nous essayons avec nos modèles de reproduire les observations de la raie HI dans une AGB chaude (Y CVn).Bien que nous ayons principalement concentré notre attention sur l'hydrogène (atomique ou bien moléculaire) dans cette étude, l'extension de ce travail à des transitions optiquement minces d'autres molécules est assez directe. Ces modèles simplifiés pour modéliser la chimie dans des géométries et dynamiques néanmoins complexes se révèlent très utiles au moment où de nouveaux instruments comme ALMA dévoilent une grande richesse spectrale et spatiale pour une multitude de traceurs chimiques. Ceci alors que le JWST est sur le point d'apporter dans l'infra-rouge de l'information complémentaire sur les raies de H2 et les raies ioniques avec une résolution et une sensibilité inégalées. / Stars are bad neighbors: they often disturb their surroundings. They sometimes travel very fast through the interstellar medium (ISM). They frequently undergo violent ejection events which leave an imprint on their neighborhood (jets, winds, supernovae). These supersonic flows generate shocks both in the ejected material and in the stellar environment. The study of these shocks constitute the subject of this thesis, and we model them with the Paris-Durham planar shock code, which incorporates a wealth of micro-physics and chemical processes relevant to the magnetized ISM.First, we use this code to model 3D magnetized axisymmetric shocks with arbitrary shapes, thanks to a formalism which links mathematically the shape of shocks to an equivalent statistical distribution of 1D shocks. For the first time, we examine systematically the effect of the geometry, age, and various other parameters on the H2 excitation diagram and emission line profiles. For example, we unveil a geometrical effect which shows that 1D planar shocks emission fits to 3D bow shocks are biased towards small velocities. We also apply our models to spatially integrated H2 observations of bow-shocks in Orion BN-KL and BHR71 where a much better match is obtained with only a limited number of additional parameters compared to former planar models. We illustrate on the Herbig-Haro object HH54 how spectrally resolved H2 line emission profiles can be used to extract a wealth of dynamical information.Second, we include in the Paris-Durham shock code a minimum set of processes necessary to describe asymptotic giant branch (AGB) wind models: geometrical dilution, external UV radiation, radiative pressure on grains, gravity, heating from stellar radiation pumping, three-body reactions, and sonic-point crossing. With this tool, we started to examine the time-dependent chemistry of hydrogen in winds of hot and cool AGB stars. We suggest that the low abundance of HI inferred from observations is due to hydrogen locked in its molecular form, and we use our model to try and reproduce HI line observations lines in a hot AGB (Y CVn).Although we have mainly focused on atomic or molecular hydrogen in this study it would be straightforward to extend it to other molecules with optically thin transitions. These simplified tools to model chemistry for complex geometries and dynamics are proving very useful at a time when new instruments such as ALMA discover a wealth of spectral and spatial information for a multitude of chemical tracers, and also when the JWST will soon provide complementary data in the infrared H$_2$ and ionic lines with unprecedented resolution and sensitivity.

A B S T R A C T Presented work focuses on experimental study of anion interaction with neutral particles at temperatures relevant for astrophysics. Anion H− , important for molecular hydrogen creation, and O− as a possible source of water are investigated. The temperature dependence of reac- tion rate coefficients from 10 to 150 K for reactions H− + H → H2 + e− and O− + H2 → H2O + e− has been determined. The energy distri- bution of electrons produced in the latter reaction at 300 K has also been acquired. These studies have been performed on two experimen- tal setups, which are presented together with the theory of operation, construction details, calibration, and supporting test measurements.

Origin of life is a still-enduring gap in human knowledge. This work is focused on revealing of several pieces of this puzzle. State of the art scenarios of biomolecules synthesis under prebiotic conditions are presented and discussed. This thesis presents our recent experiments suggesting a novel idea that neutral planetary atmosphere containing a mixture of neutral volcanic-type gasses (CO2, N2, H2O) can be converted over acidic mineral catalysts upon irradiation by a soft UV-radiation into a relatively reactive mixture of reducing gases (CH4, CO), which can be further reprocessed by high-energy chemistry. The resulting mixture (CH4, CO + N2) represents a common reducing atmosphere related e.g. to the chemistry of Titan, the largest moon of Saturn, as well as a possible representation of the secondary atmosphere of our planet. Also, photocatalytic reduction of CO2-rich atmosphere can explain the abiotic origin of methane on current Mars or other terrestrial planets. In our subsequent experiments, corresponding equimolar model mixture of CH4 : CO : N2 in presence of water vapour was subjected to reprocessing by high-power laser plasma simulating an asteroid impact - one of a series of impact events which the young Earth experienced during the first 600 million years of her history. Upon delivery...

L’origine de la matière de la Terre primitive est un important sujet de recherche en planétologie. Cette thèse présente une étude expérimentale de la formation de composés organiques dans l’atmosphère de la Terre primitive en étudiant la réactivité de mélanges gazeux majoritairement composé de N2 et CO2. Ils présentent une importante réactivité se traduisant par la formation de produits gazeux et solides, appelés tholins. La formation de ces produits met en avant l’efficacité de CO2 comme source de carbone pour la croissance organique atmosphérique. L’identification des produits gazeux et l’analyse élémentaire des tholins ont montré qu’ils étaient constitués de C, N, H et O, soulignant un couplage efficace entre la chimie de ces éléments nécessaire à la formation de composés d’intérêts prébiotiques. Ce type d’étude a été appliqué ensuite à Titan qui a une atmophère plus réduite,faite de N2 et CH4, mais contient des traces d’espèces oxygénées, majoriatirement CO. L’ajout de CO au mélange réactif induit également un couplage entre la chimie de l’O et la chimie C, N, H considérée habituellement pour Titan. Enfin je propose et étudie expériemntalement deux phénomènes suseptibles de modifier la composition des aérosols de Titan durant leur sédimentation vers la surface. Premièrement une exposition de tholins aux photons VUV caractéristique de la thermosphère de Titan et qui induit une diminution sélective des fonctions amines en faveurs des fonctions aliphatiques. Deuxièmement une irradiation par des photons UV d’espèces condensées à la surface de tholins et qui induit une réactivité de l’espèce en interaction avec les tholins, modifiant sa composition chimique. / The origin of the organic matter on the early Earth is an important subject of research in planetology. This thesis presents an experimental study of the formation of organic compounds in the atmosphere of the early Earth investigating the reactivity of gaseous mixtures majority made of N2 and CO2. They present an important reactivity highlighted by the formation of gaseous products and solid products called tholins. The formation of these products points out CO2 as an efficiency source of carbon for the organic atmospheric growth. The identification of the gaseous products and the elemental analysis of the tholins showed a composition by C, N, H and O highlighting an efficiency coupling between the chemistry of these elements necessary for the formation of prebiotic compounds. This type of study have been applied then toTitan, which have a more reduced atmosphere, made of N2 and CH4, but, which contained also oxygenated trace species: principally CO. The addition of CO in the reactive medium involves also a coupling between the chemistry of O and the C, N, H chemistry currently considered for Titan. Finally I propose and investigate experimentally two phenomena, which may involve a chemical evolution of the aerosols of Titan during their sedimentation to the surface. First, an exposition of tholins to VUV photons, characteristic of the thermosphere of Titan, involves a selective depletion of amines function in favor of aliphatic functions. Second, an irradiation by UV photons of condensed species at the surface of tholins involves a reactivity of the solid species in interaction with the tholins, changing their chemical composition.

No description available.

In the search for molecular species in the interstellar medium and extraterrestrial planetary atmospheres, theoretical methods continue to be an invaluable tool to astronomically minded chemists. Using state-of-the art methods, this doctoral work characterizes the electronically excited states of interstellar radicals, cations, and even rare anions and also predicts the gas phase fundamental vibrational frequencies of the cis and trans-HOCO radicals, as well as the cis-HOCO anion. First, open-shell coupled cluster methods of singles and doubles (CCSD) and singles and doubles with triples-inclusion (CC3) are tested on the C₂H and C₄H radicals. The significant double-excitation character, as well as the quartet multiplicity of some states yields inaccurate excitation energies and large spin contamination with CCSD. CC3 somewhat improves this for select states, but discrepancies between CC and multireference results for certain states exist and likely arise from the lack of spin adaptation in conventional spin-orbital CC. Next, coupled-cluster methods predict the presence of an excited state of the closed-shell allyl cation and its related H₂CCCHCH₂⁺ cousin at 443 nm near an unidentified laboratory peak at 442.9 nm which is also close to one of the largest unattributed interstellar absorption features. Additionally, the dipole moments, electron binding energies, and excited states of neutral radicals and corresponding closed-shell anions of interstellar interest are also computed. These are calibrated against experimental data for CH₂CN⁻ and CH₂CHO⁻. Since coupled cluster theory closely reproduces the known experimental data, dipole-bound excited states for eight previously unknown anions are predicted: CH2SiN⁻ , SiH₂CN⁻, CH₂SiHO⁻, SiN⁻, CCOH⁻, HCCO⁻, SiCCN⁻, and SiNC⁻. In addition, we predict the existence of one rare valence-bound excited state of CH₂SiN⁻ and also SiCCN⁻ as well as even rarer two valence-bound states of CCSiN⁻. Lastly, the reaction of CO + OH and its transient potential intermediate, the HOCO radical, may be responsible for the regeneration of CO₂ in the Martian atmosphere, but past spectroscopic observations have not produced a full gas-phase set of the fundamental vibrational frequencies of the HOCO radical. Using established, highly-accurate quantum chemical coupled cluster tech- niques and quartic force fields, all six fundamental vibrational frequencies for 1 ²A′ cis and trans-HOCO and 1 ¹A′ cis-HOCO⁻ are computed in the gas phase. / Ph. D.

Les études astrochimiques de la formation stellaire sont particulièrement importantes pour la compréhension de l'évolution de l'Univers, du milieu interstellaire diffus à la formation des systèmes stellaires. Les récentes avancées en matière de modélisation chimique permettent d'apporter de nouveaux résultats sur le processus de formation stellaire et les structures mises en jeu. L'objectif de ma thèse était donc d'apporter un regard neuf sur la chimie de la formation stellaire en utilisant les récentes avancées sur le modèle chimique Nautilus. J'ai pour cela étudié l'évolution de la chimie du soufre durant la formation stellaire pour tenter d'apporter de nouvelles réponses au problème de déplétion du soufre. J'ai d'abord effectué une révision du réseau chimique soufré et étudié son effet sur la modélisation du soufre dans les nuages denses. En comparant aux observations, j'ai montré que le modèle textsc{Nautilus} était capable de reproduire les abondances des espèces soufrées dans les nuages denses en utilisant comme abondance élémentaire de soufre son abondance cosmique. Ce résultat m'a permis d'apporter de nouveaux indices sur les reservoirs de soufre dans ces objets. Puis j'ai effectué une étude complète de la chimie du souffre dans les coeurs chauds en me concentrant sur les effets sur la chimie de la composition pre-effondrement. J'ai également étudié les conséquences des différentes simplifications couramment faites pour la modélisation des coeurs chauds. Mes résultats montrent que la composition pre-effondrement est un paramètre majeur de l'évolution chimique des coeurs chauds, fournissant de nouveaux indices pour expliquer la variété de compositions en espèces soufrées observée dans ces objets. De plus, ma recherche a mis en évidence la nécessité d'uniformiser les modèles de chimie utilisés pour les coeurs chauds. Enfin, j'ai développé une méthode efficace pour inverser les paramètres initiaux d'effondrement de nuages denses en me basant sur une base de données de modèles physico-chimiques d'effondrement, ainsi que sur l'observation d'enveloppes de protoétoiles de Classe 0. A partir d'un échantillon de 12 sources, j'ai pu en déduire des probabilités concernant les possibles paramètres initiaux d'effondrement de la formation d'étoiles de faible masse. / Astrochemical studies of star formation are of particular interest because they provide a better understanding of how the chemical composition of the Universe has evolved, from the diffuse interstellar medium to the formation of stellar systems and the life they can shelter. Recent advances in chemical modeling, and particularly a better understanding of grains chemistry, now allow to bring new hints on the chemistry of the star formation process, as well as the structures it involves. In that context, the objective of my thesis was to give a new look at the chemistry of star formation using the recent enhancements of the Nautilus chemical model. To that aim, I focused on the sulphur chemistry throughout star formation, from its evolution in dark clouds to hot cores and corinos, attempting to tackle the sulphur depletion problem. I first carried out a review of the sulphur chemical network before studying its effects on the modeling of sulphur in dark clouds. By comparison with observations, I showed that the textsc{Nautilus} chemical model was the first able to reproduce the abundances of S-bearing species in dark clouds using as elemental abundance of sulphur its cosmic one. This result allowed me to bring new insights on the reservoirs of sulphur in dark clouds. I then conducted an extensive study of sulphur chemistry in hot cores and corinos, focusing on the effects of their pre-collapse compositions on the evolution of their chemistries. I also studied the consequences of the use of the common simplifications made on hot core models. My results show that the pre-collapse composition is a key parameter for the evolution of hot cores which could explain the variety of sulphur composition observed in such objects. Moreover, I highlighted the importance of standardizing the chemical modeling of hot cores in astrochemical studies. For my last study, I developed an efficient method for the derivation of the initial parameters of collapse of dark clouds via the use of a physico-chemical database of collapse models, and comparison with observations of Class 0 protostars. From this method, and based on a sample of 12 sources, I was able to derive probabilities on the possible initial parameters of collapse of low-mass star formation.

Les 50 dernières années ont été caractérisées par le développement rapide de l’astrochimie. Plus de 150 réactions entre espèces neutres ont déjà été étudiées aux basses températures qui sont celles du le milieu interstellaire et des atmosphères planétaires. Néanmoins, les constantes de vitesse, et la nature des produits, restent inconnus pour de nombreuses réactions potentiellement importantes pour caractériser ces milieux. Nous avons effectué des études cinétiques pour des processus réactifs, et non réactifs, entre des atomes dans un état électronique excité [C(1D), O(1D) et N(2D)] et plusieurs molécules stables afin de quantifier leur importance dans la chimie des atmosphères planétaires. Nous avons aussi étudié la réaction entre les atomes de carbone dans leur état électronique fondamental (3P) et l’eau, confirmant l’importance, pour certaines réactions avec barrière, de l’effet tunnel pour la réactivité à basse température. Les constantes de vitesse et les rapports de branchement pour ces processus ont été déterminés dans la gamme de température entre 50 et 296 K en utilisant un appareil CRESU, les atomes étudiés ont été produits par photolyse à l’aide d’un laser pulsé (PLP) et détectés par fluorescence induite dans l’ultraviolet sous vide (VUV LIF). / The last 50 years have been characterized by the fast development of astrochemistry as a science. To date, more than 150 gas-phase neutral-neutral reactions have been investigated at low temperatures relevant to planetary atmospheres and in cold regions of the interstellar medium. However, the rate constants and nature of the products for many potentially important gas-phase processes remain unknown. We performed kinetic studies of reactive and non-reactive removal processes between electronically excited atoms [C(1D), O(1D) and N(2D)] with several molecules in order to quantify their importance in the chemistry of planetary atmospheres. Furthermore, we also investigated the reaction between carbon atoms in their ground electronic state (3P) with water, providing new evidence of a quantum mechanical tunnelling mechanism at low temperatures, which could play an important role in the chemistry of interstellar clouds. Rate constants and branching ratios for these processes were determined over the 50 - 296 K temperature range using a CRESU (Cinétique de Réaction en Ecoulement Supersonique Uniforme) apparatus coupled with pulsed laser photolysis (PLP) and vacuum ultraviolet laser induced fluorescence (VUV LIF).

L’évolution chimique des phases les plus diffuses aux plus denses du milieu interstellaireest un processus continu : la composition chimique du milieu interstellairedans une phase dépend de sa composition dans sa phase antérieure.Les études, qui s’intéressent à la chimie du milieu dense et froid ainsi qu’à l’évolutionde sa composition au cours du temps, font de fortes hypothèses sur son évolutiondepuis le milieu diffus.L’objectif de ma thèse a donc été de suivre l’évolution de la chimie de la matièreinterstellaire du milieu diffus jusqu’à la formation des nuages denses.J’ai pour cela utilisé un modèle de chimie gaz-grain dépendant du temps que j’aisignificativement contribué à améliorer pour la partie chimie de surface. J’ai dansun premier temps suivi une approche "classique" (c.-à-d. : semblable aux études préexistantes)de la modélisation des régions froides. Cela m’a permis d’étudier en détailles processus physiques et chimiques à l’origine de la complexité moléculaire dans lesnuages denses et froids et de comparer les prédictions du modèle avec les études existantes.Dans une deuxième partie, j’ai appliqué ce modèle pour suivre l’évolution de lacomposition chimique du milieu interstellaire au cours du processus de formation desnuages moléculaires à partir du milieu diffus. Pour cette étude, j’ai utilisé les résultatsd’une simulation hydrodynamique à l’échelle galactique. Cela m’a permis de montrerque l’histoire de l’évolution des conditions physiques dans les phases antérieures à laformation des nuages moléculaires peut avoir un impact significatif sur la compositionchimique de ces derniers. / The chemical evolution from the most diffuse parts of the interstellar medium tothe formation of dense clouds is a continuous process : the chemical composition inone phase depends on the chemical composition in the previous one.However, most studies of the time dependent chemistry in the cold and dense interstellarmedium make strong assumptions on the transition between diffuse and densemedium.The goal of my thesis was to study the chemical evolution of the interstellar mediumfrom the most diffuse parts to the formation of dense clouds in a continuousway.To do so, I used a time dependent gas-grain model that I significantly contributedto improve for the treatment of the surface chemistry. In a first part, I followed a "classical"approach (i.e. : similar to most of the pre-existing studies) to model cold denseclouds. This allowed me to study in details the physical and the chemical mechanismsresponsible for the chemical complexity of dense clouds and to compare the modelpredictions with the existing literature. In a second part, I applied this model to followthe evolution of the chemical composition during the formation process of denseclouds from the diffuse medium. I used results from an hydrodynamical simulation ofthe interstellar medium at galactic scales. This study allowed me to show that the pastphysical history of each particles that form the dense clouds have a significant impacton their chemical composition.