Cette thèse traite principalement des théorèmes limites pour les processus empiriques de fonctionnelles de clusters d'extrêmes de séquences et champs aléatoires faiblement dépendants. Des théorèmes limites pour les processus empiriques de fonctionnelles de clusters d'extrême de séries temporelles stationnaires sont donnés par Drees & Rootzén [2010] sous des conditions de régularité absolue (ou "ß-mélange"). Cependant, ces conditions de dépendance de type mélange sont très restrictives : elles sont particulièrement adaptées aux modèles dans la finance et dans l'histoire, et elles sont de plus compliquées à vérifier. Généralement, pour d'autres modèles fréquemment rencontré dans les domaines applicatifs, les conditions de mélange ne sont pas satisfaites. En revanche, les conditions de dépendance faible, selon Doukhan and Louhichi [1999] et Dedecker & Prieur [2004a], sont des conditions qui généralisent les notions de mélange et d'association. Elles sont plus simple à vérifier et peuvent être satisfaites pour de nombreux modèles. Plus précisément, sous des conditions faibles, tous les processus causals ou non causals sont faiblement dépendants: les processus Gaussien, associés, linéaires, ARCH(∞), bilinéaires et notamment Volterra entrent dans cette liste. À partir de ces conditions favorables, nous étendons certains des théorèmes limites de Drees & Rootzén [2010] à processus faiblement dépendants. En outre, comme application des théorèmes précédents, nous montrons la convergence en loi de l'estimateur de l'extremogramme de Davis & Mikosch [2009] et l'estimateur fonctionnel de l'indice extrémal de Drees [2011] sous dépendance faible. Nous démontrons un théorème de la valeur extrême pour les champs aléatoires stationnaires faiblement dépendants et nous proposons, sous les mêmes conditions, un critère du domaine d'attraction d'une loi d'extrêmes. Le document se conclue sur des théorèmes limites pour les processus empiriques de fonctionnelles de clusters d’extrêmes de champs aléatoires stationnaires faiblement dépendants, et met en évidence la convergence en loi de l'estimateur d'un extremogramme de processus spatio-temporels stationnaires faiblement dépendants en tant qu'application. / This thesis deals mainly with limit theorems for empirical processes of extreme cluster functionals of weakly dependent random fields and sequences. Limit theorems for empirical processes of extreme cluster functionals of stationnary time series are given by Drees & Rootzén [2010] under absolute regularity (or "ß-mixing") conditions. However, these dependence conditions of mixing type are very restrictive: on the one hand, they are best suited for models in finance and history, and on the other hand, they are difficult to verify. Generally, for other models common in applications, the mixing conditions are not satisfied. In contrast, weak dependence conditions, as defined by Doukhan & Louhichi [1999] and Dedecker & Prieur [2004a], are dependence conditions which generalises the notions of mixing and association. These are easier to verify and applicable to a wide list of models. More precisely, under weak conditions, all the causal or non-causal processes are weakly dependent: Gaussian, associated, linear, ARCH(∞), bilinear and Volterra processes are some included in this list. Under these conveniences, we expand some of the limit theorems of Drees & Rootzén [2010] to weakly dependent processes. These latter results are used in order to show the convergence in distribution of the extremogram estimator of Davis & Mikosch [2009] and the functional estimator of the extremal index introduced by Drees [2011] under weak dependence. We prove an extreme value theorem for weakly dependent stationary random fields and we propose, under the same conditions, a domain of attraction criteria of a law of extremes. The document ends with limit theorems for the empirical process of extreme cluster functionals of stationary weakly dependent random fields, deriving also the convergence in distribution of the estimator of an extremogram for stationary weakly dependent space-time processes.

Magnetic ordering of dopants in diamond holds the prospect of exploiting diamond’s unique properties in the emerging field of spintronics. Several transition metal defects have been reported to order ferromagnetically in various semiconductors, however, low Curie temperatures and lack of other fundamental material properties have hindered practical implementation in room temperature spintronic applications. In this Thesis, we consider the energetic stability of 3d transition metal doped-diamond and its magnetic ordering properties at various lattice sites and charge states using ab initio Density Functional Theory methods. We find the majority of 3d transition metal impurities in diamond at any charge state to be energetically most stable at the divacancy site compared to substitutional or interstitial lattice sites, with the interstitial site being highly unstable (by ~8 - 10 eV compared to the divacancy site). At each lattice site and charge state, we find the formation energies of transition metals in the middle of the 3d series (Cr, Mn, Fe, Co, Ni) to be considerably lower compared to those early or late in the series. The energetic stability of transition metal impurities across the 3d series is shown to be strongly dependent on the position of the Fermi level in the diamond band gap, with the formation energies at any lattice site being lower in p-type or ntype diamond compared to intrinsic diamond. Further, we show that incorporation of isolated transition metal impurities into diamond introduces spin polarised impurity bands into the diamond band gap, while maintaining its semiconducting nature, with band gaps in both the spin-up and spin-down channels. These impurity bands are shown to originate mainly from s, p-d hybridization between carbon sp 3 orbitals with the 3d orbitals of the transition metal. In addition, the 4p orbitals contribute significantly to hybridization for transition metal atoms at the substitutional site, but not at the divacancy site. In both cases, the spin polarisation and magnetic stabilization energies are critically dependent on the lattice site and charge state of the transition metal impurity. By allowing magnetic interactions between transition metal atoms, we find that ferromagnetic ordering is likely to be achieved in divacancy Cr+2, Mn+2, Mn+1 and Co0 as well as in substitutional Fe+2 and Fe+1, indicating that transition metal-doped diamond is likely to form a diluted magnetic semiconductor which may successfully be considered for room temperature spintronic applications. In addition, these charge states correspond to p-type diamond, except for divacancy Co0, suggesting that co-doping with shallow acceptors such as B ( will result in an increase of charge concentration, which is likely to enhance mediation of ferromagnetic spin coupling. The highest magnetic stabilization energy occurs in substitutional Fe+1 (33.3 meV), which, also exhibits half metallic ferromagnetic ordering at the Fermi level, with an induced magnetic moment of 1.0 μB per ion, thus suggesting that 100 % spin polarisation may be achieved in Fe-doped diamond. / Physics / D. Litt. et Phil. (Physics)

La présente thèse couvre deux principaux thèmes de recherche qui seront présentés dans deux parties et précédés par un prolegomenon commun. Dans ce dernier nous introduisons les concepts essentiels et nous exploitons aussi le lien entre les deux parties.<p><p>Dans la première partie, le principal objet d’intérêt est la soi-disant fonctionnelle exponentielle de processus de Lévy. La loi de cette variable aléatoire joue un rôle primordial dans de nombreux domaines divers tant sur le plan théorique que dans des domaines appliqués. Doney dérive une factorisation de la loi arc-sinus en termes de suprema de processus stables indépendants et de même index. Une factorisation similaire de la loi arc-sinus en termes de derniers temps de passage au niveau 1 de processus de Bessel peut aussi être établie en utilisant un résultat dû à Getoor. Des factorisations semblables d’une variable de Pareto en termes des mêmes objets peut également être obtenue. Le but de cette partie est de donner une preuve unifiée et une généralisation de ces factorisations qui semblent n’avoir aucun lien à première vue. Même s’il semble n’y avoir aucune connexion entre le supremum d’un processus stable et le dernier temps de passage d’un processus de Bessel, il peut être montré que ces variables aleatoires sont liées à des fonctionnelles exponentielles de processus de Lévy spécifiques. Notre contribution principale dans cette partie et aussi au niveau de caractérisations de la loi de la fonctionnelle exponentielle sont des factorisations de la loi arc-sinus et de variables de Pareto généralisées. Notre preuve s’appuie sur une factorisation de Wiener-Hopf récente de Patie et Savov.<p>Dans la deuxième partie, motivée par le fait que la dérivée fractionnaire de Caputo et d’autres opérateurs fractionnaires classiques coïncident avec le générateur de processus de Markov auto-similaires positifs particuliers, nous introduisons des opérateurs généralisés de Caputo et nous étudions certaines propriétés. Nous nous intéressons particulièrement aux conditions sous lesquelles ces opérateurs coïncident avec les générateurs infinitésimaux de processus de Markov auto-similaires positifs généraux. Dans ce cas, nous étudions les fonctions invariantes de ces opérateurs qui admettent une représentation en termes de séries entières. Nous précisons que cette classe de fonctions contient les fonctions de Bessel modifiées, les fonctions de Mittag-Leffler ainsi que plusieurs fonctions hypergéométriques. Nous proposons une étude unifiant et en profondeur de cette classe de fonctions. / Doctorat en Sciences / info:eu-repo/semantics/nonPublished

The Kohn-Sham density functional theory (KS-DFT) finds an approximate solution for the many-electron problem for the ground state energy and density by solving the self-consistent one-electron Schr\"{o}dinger equations. KS-DFT would be an exact theory if we could find the precise form of exchange-correlation energy $(E_{xc})$. However, this would not be computationally feasible. The density functional approximations (DFAs) are designed to be exact in the limit of uniform densities. They require a parametrization of the correlation energy per electron $(\varepsilon_c)$ of the uniform electron gas (UEG). These DFAs take the parametrizations of correlation energy as their input since the exact analytical form of $\varepsilon_c$ is still unknown. Almost all the DFAs of higher rungs of Jacob's ladder employ an additional function on top of $\varepsilon_c$ for approximating their correlation energy. Exchange energies in these DFAs are also approximated by applying an enhancement factor to the exchange energy per electron of the UEG. Exchange-correlation energy is the glue that holds the atoms and molecules together. The correlation energy is an important part of ``nature's glue" that binds one atom to another, and it changes significantly when the bonding of the molecule changes. It is a measure of the effect of Coulomb repulsion due to electronic mutual avoidance and is necessarily negative. We compared three parametrizations of the correlation energy per electron of the uniform electron gas to the original and the corrected density parameter interpolation (DPI), which is almost independent of QMC input, and with the recent QMC of Spink \textit{et al.}, which extends the Ceperley-Alder results to fractional spin polarization and higher densities or smaller Seitz radius $r_s$. These three parametrizations are Perdew-Zunger or PZ 1981, Vosko-Wilk-Nusair or VWN 1980, and Perdew-Wang or PW 1992. The three parametrizations (especially the sophisticated PW92) are closer to the constraint satisfying DPI and are very close to the high-density limit rather than the QMC results of Spink \textit{et al.}. These DFAs suffer from self-interaction error (SIE) which arises due to an imperfect cancellation of self-Hartree energy by self-exchange-correlation energy of a single fully occupied orbital. The self-interaction correction (SIC) method introduced by Perdew and Zunger (PZ) in 1981 to remove the SIE encounters a size-extensivity problem when applied to the Kohn-Sham (KS) orbitals. Hence, we make use of Fermi L\"owdin orbitals (FLO) for applying the PZ-SIC to the density functional approximations (DFAs). FLOs are the unitary transformation of the KS orbitals localized at the Fermi orbital descriptor (FOD) positions and then orthonormalized using L\"owdin's symmetric method. The PZ-SIC makes any approximation exact only in the region of one-electron density and no correction if applied to the exact functional. But it spoils the slowly varying (in space) limits of the uncorrected approximate functionals, where those functionals are right by construction. Hence, scaling of PZ-SIC is required such that it remains intact in the region of one-electron density and scales down in the region of many-electron densities. The PZ-SIC improves the performance of DFAs for the properties that involve significant SIE, as in stretched bond situations, but overcorrects for equilibrium properties where SIE is insignificant. This overcorrection is often reduced by LSIC, local scaling of the PZ-SIC to the local spin density approximation (LSDA). We propose a new scaling factor to use in an LSIC-like approach that satisfies an additional important constraint: the correct coefficient of Z in the asymptotic expansion of the $E_{xc}$ for atoms of atomic number Z, which is neglected by LSIC. LSIC and LSIC+ are scaled by functions of the iso-orbital indicator $z_{\sigma}$ that distinguishes one-electron regions from many-electron regions. LSIC+ applied to LSDA works better than LSDA-LSIC and the Perdew, Burke, and Ernzerhof (PBE) generalized gradient approximation (GGA) and gives comparable results to the strongly constrained and appropriately normed (SCAN) meta-GGA in predicting the total energies of atoms, atomization energies, barrier heights, ionization potentials, electron affinities, and bond-length of molecules. LSDA-LSIC and LSDA-LSIC+ both fail to predict interaction energies involving weaker bonds, in sharp contrast to their earlier successes. It is found that more than one set of localized SIC orbitals can yield a nearly degenerate energetic description of the same multiple covalent bonds, suggesting that a consistent chemical interpretation of the localized orbitals requires a new way to choose their Fermi orbital descriptors. A spurious correction to the exact functional would be found unless the self-Hartree and exact self-exchange-correlation terms of the PZ-SIC energy density were expressed in the same gauge. Therefore, LSIC and LSIC+ are applied only to LSDA since only LSDA has the exchange-correlation (xc) energy density in the gauge of the Hartree energy density. The transformation of energy density that achieves the Hartree gauge for the exact xc functional can be applied to approximate functionals. The use of this compliance function guarantees that scaled-down self-interaction correction (sdSIC) will make no spurious non-zero correction to the exact functional and transforms the xc energy density into the Hartree gauge. We start from the interior scaling of PZ-SIC and end at exterior scaling after the gauge transformation. SCAN-sdSIC evaluated on SCAN-SIC total and localized orbital densities is applied to the highly accurate SCAN functional, which is already much better than LSDA. Hence, the predictive power of SCAN-sdSIC is much better, even though it is scaled by $z_\sigma$ too. It provides good results for several ground state properties discussed here, including the interaction energy of weakly bonded systems. SCAN-sdSIC leads to an acceptable description of many equilibrium properties, including the dissociation energies of weak bonds. However, sdSIC fails to produce the correct asymptotic behavior $-\frac{1}{r}$ of xc potential. The xc potential as seen by the outermost electron will be $\frac{-X_{HO}^{sd}}{r}$ where HO labels the highest occupied orbital and hence doesn't guarantee a good description of charge transfer. The optimal SIC that remains to be developed might be PZ-SIC evaluated on complex Fermi-L\"owdin orbitals (with nodeless orbital densities) and Fermi orbital descriptors chosen to minimize a measure of the inhomogeneity of the orbital densities. / Physics

Organic π-conjugated solids are promising candidates for new optoelectronic materials. The large body of evidence points at their advantageous properties such as high charge-carrier mobility, large nonlinear polarizability, mechanical flexibility, simple and low cost fabrication and superior luminescence. They can be used as nonlinear optical (NLO) materials with large two-photon absorption (2PA) and as electronic components capable of generating nonlinear neutral (excitonic) and charged (polaronic) excitations. In this work, we investigate the appropriate theoretical methods used for the (a) prediction of 2PA properties for rational design of organic materials with improved NLO properties, and (b) understanding of the essential electronic excitations controlling the energy-transfer and charge-transport properties in organic optoelectronics. Accurate prediction of these electro-optical properties is helpful for structureactivity relationships useful for technological innovations. In Chapter 1 we emphasize on the potential use of the organic materials for these two applications. The 2PA process is advantageous over one-photon absorption for deep-tissue fluorescence microscopy, photodynamic therapy, microfabrication and optical data storage owing to the three-dimensional spatial selectivity and improved penetration depth in the absorbing or scattering media. The design of the NLO materials with large 2PA cross-sections may reduce the optical damage due to the use of the high intensity laser beams for excitation. The organic molecules also possess self-localized excited states which can decay radiatively or nonradiatively to form excitonic states. This suggests the use of these materials in the electroluminescent devices such as light-emitting diodes and photovoltaic cells through the processes of exciton formation or dissociation, respectively. It is therefore necessary to understand ultrafast relaxation processes required in understanding the interplay between the iv efficient radiative transfer between the excited states and exciton dissociation into polarons for improving the efficiency of these devices. In Chapter 2, we provide the detailed description of the various theoretical methods applied for the prediction as well as the interpretation of the optical properties of a special class of substituted PPV [poly (p-phenylene vinylene)] oligomers. In Chapter 3, we report the accuracy of different second and third order time dependent density functional theory (TD-DFT) formalisms in prediction of the 2PA spectra compared to the experimental measurements for donor-acceptor PPV derivatives. We recommend a posteriori Tamm-Dancoff approximation method for both qualitative and quantitative analysis of 2PA properties. Whereas, Agren's quadratic response methods lack the double excitations and are not suitable for the qualitative analysis of the state-specific contributions distorting the overall quality of the 2PA predictions. We trace the reasons to the artifactual excited states above the ionization threshold. We also study the effect of the basis set, geometrical constraints and the orbital exchange fraction on the 2PA excitation energies and cross-sections. Higher exchange (BMK and M05-2X) and range-separated (CAM-B3LYP) hybrid functionals are found to yield inaccurate predictions both quantitatively and qualitatively. The failure of the exchangecorrelation (XC) functionals with correct asymptotic is traced to the inaccurate transition dipoles between the valence states, where functionals with low HF exchange succeed. In Chapter 4, we test the performance of different semiempirical wavefunction theory methods for the prediction of 2PA properties compared to the DFT results for the same set of molecules. The spectroscopic parameterized (ZINDO/S) method is relatively better than the general purpose parameterized (PM6) method but the accuracy is trailing behind the DFT methods. The poor performances of PM6 and ZINDO/S methods are attributed to the incorrect description of excited-to-excited state transition and 2PA energies, respectively. The different v semiempirical parameterizations can at best be used for quantitative analysis of the 2PA properties. The ZINDO/S method combined with different orders of multi-reference configuration interactions provide an improved description of 2PA properties. However, the results are observed to be highly dependent on the specific choice for the active space, order of excitation and reference configurations. In Chapter 5, we present a linear response TD-DFT study to benchmark the ability of existing functional models to describe the extent of self-trapped neutral and charged excitations in PPV and its derivative MEH-PPV considered in their trans-isomeric forms. The electronic excitations in question include the lowest singlet (S1) and triplet (T1 † ) excitons, positive (P+ ) and negative (P- ) polarons and the lowest triplet (T1) states. Use of the long-range-corrected DFT functional, such as LC-wPBE, is found to be crucial in order to predict the physically correct spatial localization of all the electronic excitations in agreement with experiment. The inclusion of polarizable dielectric environment play an important role for the charged states. The particlehole symmetry is preserved for both the polymers in trans geometries. These studies indicate two distinct origins leading to self-localization of electronic excitations. Firstly, distortion of molecular geometry may create a spatially localized potential energy well where the state wavefunction self-traps. Secondly, even in the absence of geometric and vibrational dynamics, the excitation may become spatially confined due to energy stabilization caused by polarization effects from surrounding dielectric medium. In Chapter 6, we aim to separate these two fundamental sources of spatial localization. We observe the electronic localization of P + and Pis determined by the polarization effects of the surrounding media and the character of the DFT functional. In contrast, the self-trapping of the electronic wavefunctions of S1 and T1(T1 † ) mostly follows their lattice distortions. Geometry vi relaxation plays an important role in the localization of the S1 and T1 † excitons owing to the nonvariational construction of the excited state wavefunction. While, mean-field calculated P + , Pand T1 states are always spatially localized even in ground state S0 geometry. Polaron P+ and Pformation is signified by the presence of the localized states for the hole or the electron deep inside the HOMO-LUMO gap of the oligomer as a result of the orbital stabilization at the LCwPBE level. The broadening of the HOMO-LUMO band gap for the T1 exciton compared to the charged states is associated with the inverted bond length alternation observed at this level. The molecular orbital energetics are investigated to identify the relationships between state localization and the corresponding orbital structure. In Chapter 7, we investigate the effect of various conformational defects of trans and cis nature on the energetics and localization of the charged P + and Pexcitations in PPV and MEHPPV. We observe that the extent of self-trapping for P+ and Ppolarons is highly sensitive on molecular and structural conformations, and distribution of atomic charges within the polymers. The particle-hole symmetry is broken with the introduction of trans defects and inclusion of the polarizable environment in consistent with experiment. The differences in the behavior of PPV and MEH-PPV is rationalized based on their orbital energetics and atomic charge distributions. We show these isomeric defects influence the behavior and drift mobilities of the charge carriers in substituted PPVs.

The first aim of this PhD Thesis is devoted to the study of geodesic distances defined on a subdomain of a Carnot group, which are bounded both from above and from below by fixed multiples of the Carnot–Carathéodory distance. Then one shows that the uniform convergence, on compact sets, of these distances can be equivalently characterized in terms of Gamma-convergence of several kinds of variational problems. Moreover, it investigates the relation between the class of intrinsic distances, their metric derivatives and the sub-Finsler convex metrics defined on the horizontal bundle. The second purpose is to obtain the integral representation of some classes of local functionals, depending on a family of vector fields, that satisfy a weak structure assumption. These functionals are defined on degenerate Sobolev spaces and they are assumed to be not translations-invariant. Then one proves some Gamma-compactness results with respect to both the strong topology of L^p and the strong topology of degenerate Sobolev spaces.

The Electron Localization Function (ELF) measures electron localization within matter and provides insights into the nature of bonds in materials and molecules. This thesis examines the relationship between ELF and binding energy in bimolecular systems, focusing on van der Waals interactions—specifically Keesom forces, Debye forces, and London dispersion forces—which play significant roles in molecular and crystalline materials. This research addresses the challenge of accurately calculating binding energies in crystalline materials by exploring their correlation with ELF. Using Density Functional Theory (DFT) with two exchange-correlation functionals, rev-vdW-DF2 and PBE-D3(BJ), this study proposes a method for calculating binding energies in crystalline materials with promising accuracy. By analysing the ELF and its correlation with binding energies in 75 bimolecular systems, the research demonstrates a strong linear correlation, with a coefficient of determination (R2) reaching up to 0.956. The findings suggest that ELF can effectively differentiate between weak and strong van der Waals interactions, providing a reliable metric for evaluating interaction strengths. The results indicate that ELF is a valuable tool for understanding the strength of molecular interactions, with potential applications in materials science and electronic structure theory. The study highlights the importance of refining the accuracy of the ELF-based method and expanding its scope to include other types of non-covalent interactions, such as halogen bonds. The main contribution of this thesis is the exploration of methodologies for analysing and predicting molecular interaction strengths within crystalline materials, which may improve computational approaches in the field. Deriving binding energies within the unit cell directly from the ELF has the potential to simplify practical calculations.

Les fonctionnelles de Minkowski définissent des mesures topologiques et géométriques d'ensembles, insuffisantes pour la caractérisation, des ensembles différents pouvant avoir les mêmes fonctionnelles. D'autres fonctionnelles de forme, géométriques et morphométriques, sont donc utilisées. Un diagramme de forme, défini grâce à deux fonctionnelles morphométriques, donne une représentation permettant d'étudier les formes d'ensembles. En analyse d'image, ces fonctionnelles et diagrammes sont souvent limités aux images binaires et déterminés de manière globale et mono-échelle. Les Voisinages Adaptatifs Généraux (VAG) simultanément adaptatifs avec les échelles d'analyse, structures spatiales et intensités des images, permettent de pallier ces limites. Une analyse locale, adaptative et multi-échelle des images à tons de gris est proposée sous forme de cartographies des fonctionnelles de forme à VAG.Les VAG, définis en tout point du support spatial d'une image à tons de gris, sont homogènes par rapport à un critère d'analyse représenté dans un modèle vectoriel, suivant une tolérance d'homogénéité. Les fonctionnelles de forme calculées pour chaque VAG de l'image définissent les cartographies des fonctionnelles de forme à VAG. Les histogrammes et diagrammes de ces cartographies donnent des distributions statistiques des formes des structures locales de l'image contrairement aux histogrammes classiques qui donnent une distribution globale des intensités de l'image. L'impact de la variation des critères axiomatiques des VAG est analysé à travers ces cartographies, histogrammes et diagrammes. Des cartographies multi-échelles sont construites, définissant des fonctions de forme à VAG. / Minkowski functionals define set topological and geometrical measurements, insufficient for the characterization, because different sets may have the same functionals. Thus, other shape functionals, geometrical and morphometrical are used. A shape diagram, defined thanks to two morphometrical functionals, provides a representation allowing the study of set shapes. In quantitative image analysis, these functionals and diagrams are often limited to binary images and achieved in a global and monoscale way. The General Adaptive Neighborhoods (GANs) simultaneously adaptive with the analyzing scales, the spatial structures and the image intensities, enable to overcome these limitations. The GAN-based Minkowski functionals are introduced, which allow a gray-tone image analysis to be realized in a local, adaptive and multiscale way.The GANs, defined around each point of the spatial support of a gray-tone image, are homogeneous with respect to an analyzing criterion function represented in an algebraic model, according to an homogeneity tolerance. The shape functionals computed on the GAN of each point of the spatial support of the image, define the so-called GAN-based shape maps. The map histograms and diagrams provide statistical distributions of the shape of the gray-tone image local structures, contrary to the classical histogram that provides a global distribution of image intensities. The impact of axiomatic criteria variations is analyzed through these maps, histograms and diagrams. Thus, multiscale maps are built, defining GAN-based shape functions.

The long-standing problem of possible formation of metastable states in collisions of the eta-meson with atomic nuclei is revisited. The two-body eta-nucleon interaction is described by a local potential, which is constructed by fitting known low-energy parameters of this interaction. The many-body eta-nucleus potential obtained within the folding model, is used to search for metastable states of the systems formed by the eta-meson with hydrogen and helium isotopes. It is found that all these systems generate strings of overlapping resonances. / Physics / M.Sc. (Physics)

The electronic structure of the zero-gap two-dimensional graphene has a charge neutrality point exactly at the Fermi level that limits the practical application of this material. There are several ways to modify the Fermi-level-region of graphene, e.g. adsorption of graphene on different substrates or different molecules on its surface. In all cases the so-called dispersion or van der Waals interactions can play a crucial role in the mechanism, which describes the modification of electronic structure of graphene. The adsorption of water on graphene is not very accurately reproduced in the standard density functional theory (DFT) calculations and highly-accurate quantum-chemical treatments are required. A possibility to apply wavefunction-based methods to extended systems is the use of local correlation schemes. The adsorption energies obtained in the present work by means of CCSD(T) are much higher in magnitude than the values calculated with standard DFT functional although they agree that physisorption is observed. The obtained results are compared with the values available in the literature for binding of water on the graphene-like substrates. / Dieser Beitrag ist mit Zustimmung des Rechteinhabers aufgrund einer (DFG-geförderten) Allianz- bzw. Nationallizenz frei zugänglich.