<p>This thesis presents a first principle approach to model helium diffusionand retention in molybdenum. Results from electron structure calculations within the framework of density functional theory are used to assess parameters in a rate theory model. The model is used to reproduce experimental desorption spectra, which, to a large degree of accuracy, coincide with experimental data in temperature regions relevant for nuclear fuel applications. The models indicate that produced helium will diffuse out into the fuel pin during operation. However, some helium will be trapped in molybdenum vacancies. The amount of trapped helium will largely depend on the fuel operational temperature.</p><p>Data presented in the thesis is a first step towards a self consistent dataset of first principle data on helium diffusion in CERMET fuel, one candidate fuel suggested for transmutation of nuclear waste. To realise the use of CERMET fuel, modelling of fuel performance is essential, and to accomplish this, the understanding of helium diffusion and retention in molybdenum is one important aspect.</p><p> </p>

The synthesis of type-enriched semiconducting or metallic single-walled carbon nanotubes (sc/m-SWCNTs) with high quality by means of catalytic chemical vapor deposition (CCVD) are essential prerequisites for implementing of SWCNTs into nanodevices. In particular, the Fe−Co bimetallic catalysts system is promising due to its ability to grow SWCNTs by CCVD. However, there is still a gap in understanding how to adjust catalyst composition aiming further improvements in SWCNTs properties with respect to the electronic type. In particular, formation of well-defined nanoalloy of bimetallic catalysts during catalyst conditioning as well as its impact on SWCNTs growth are not clearly understood. Here we present a systematic investigation on effects of catalyst composition based on different Molar ratios of Fe:Co catalysts on the properties of CCVD grown SWCNTs using Raman spectroscopy. After CVD growth of SWCNTs on different molar ratios of Fe:Co, We find that by using molar ratio of Fe:Co=1:1.5, growth of SWNTs that are strongly dominated by two types of semiconducting tubes, the (7,5) and (12,1) tubes, can be achieved.

This thesis consists of two distinct parts. The first part, based on the first two accompanied papers, is in the field of topological phases of matter and the second part, based on the third accompanied paper, looks at a problem in the field of quantum graphs, a rapidly growing field of mathematical physics. First, we investigate the entanglement property of the Laughlin state by looking at the rank of the reduced density operator when particles are divided into two groups. We show that the problem of determining this rank translates itself into a  question about symmetric polynomials, namely, one has to determine the lower bound for the degree in each variable of the symmetric polynomials that vanish under a transformation that clusters the particles into groups of equal size and then brings the particles in each group together. Although we were not able to prove this, but we were able to determine the lower bound for the total degree of symmetric polynomials that vanish under the  transformation described. Moreover, we were able to characterize all symmetric polynomials that vanish under this transformation. In the second paper, we introduce a one-dimensional model of interacting su(2)k anyons. The specific feature of this model is that, through pairing terms present in the Hamiltonian,  the number of anyons of the chain can fluctuate. We also take into account the possibility that anyons hop to empty neighboring sites. We investigate the model in five different points of the parameter space. At one of these points, the Hamiltonian of the model becomes a sum of projectors and we determine the explicit form of all the zero-energy ground states for odd values of k. At the other four points, the system is integrable and we determine the behavior of the model at these integrable points. In particular, we show that the system is critical and determine the CFT describing the system at these points. It is known that there are non-Hermitian Hamiltonians whose spectra are entirely real. This property can be understood in terms of a certain symmetry of these Hamiltonians, known as PT-symmetry. It is also known that the spectrum of a non-Hermitian PT-symmetric Hamiltonian has reflection symmetry with respect to the real axis. We then ask the reverse question whether or not the reflection symmetry of a non-Hermitian Hamiltonian necessarily implies that the Hamiltonian is PT-symmetric. In the context of quantum graphs, we introduce a model for which the answer to this question is positive.

Carbon nanostructures have emerged as a key material in nanotechnology and continuously find new areas of applications. Particularly, they are attractive due to their excellent properties as support for catalyst nanostructures leading to highly efficient composite materials for various electrochemical applications. The interest in these structures is further increased by the possibility to alter their electronic and structural properties by various methods. Heteroatom doping of carbon nanostructures is one of the approaches which may induce intrinsic catalytic activity in these materials. In addition, such introduction of guest elements into the hexagonal carbon skeleton provides strong nucleation sites which facilitate the stabilization of nanostructures on their surface. In this thesis we present detailed studies on the nitrogen incorporation into carbon nanostructures, particularly carbon nanotubes and reduced graphene oxide. Due to the high impact of nitrogen configuration on the intrinsic electrocatalytic properties of carbon nanostructures, we investigated the nitrogen functionalities using X-ray photoelectron spectroscopy and Raman spectroscopy. Based on our achievements we could assign the most electrocatalytic active nitrogen site in nitrogen-doped carbon nanotubes (NCNTs) for catalytic oxygen reduction reaction (ORR) which is an important reaction in energy conversion systems such as fuel cells. We then used nitrogen-doped carbon nanostructures as a key component to manufacture hybrid material, where the nitrogen doped nanostructures has a role of both stabilizing the nanostructures and to work as conductive additive to assist the charge transfer from the other constituents suffering from inherently poor conductivity. Our hybrid material comprising transition metal oxides (Fe2O3 and Co3O4) anchored on nitrogen-doped carbon nanostructure were used to both manufacture an exotic type of graphene nanoscrolls, as well as studied and evaluated as an electrocatalyst in various electrochemical reactions. We show that the self-assembled electrodes exhibited better performance and higher stability compared to when the same material was loaded on common current collectors such as fluorine tin oxide (FTO) coated glass and glassy carbon electrode, with both higher current densities, more efficient charge transfer and lower overpotentials for oxygen evolution and hydrogen evolution reactions, the two important processes in a water splitting device. Our NCNTs-based electrodes showed further excellent performance in lithium ion batteries with high cyclability and capacity. The thesis gives insight into processes, materials, and methods that can be utilized to manufacture an efficient water splitting device, based on earth-abundant self-assembled materials. It further represents a significant advancement of the role of nitrogen in heteroatom-doped nanostructures, both regarding their intrinsic catalytic activity, as well as their role for stabilizing nanostructures.

No description available.

The theoretical studies of several magnetic materials are presented in this thesis. To each of them, it was investigated the electronic structure, by means of density functional theory calculations, and/or magnetization dynamics, in the context of atomistic spin dynamics (ASD).  For bulk properties, we evaluate the magnon spectra of the heavy rare earths (Gd, Tb, Dy, Ho, Er, and Tm), using the exchange parameters and magnetic moments from first-principles calculations in ASD simulations. Additionally, we performed Monte Carlo simulations that nicely reproduced the qualitative trend of lowering of the critical temperatures across the series. Next, we discuss about the microscopic mechanism of the vanishingly low magnetic anisotropy of Permalloy using the concept of the orbital moment anisotropy for Fe and Ni atoms in the alloy.  Turning to surface magnetism, we discuss the use of exchange parameters computed by a noncollinear formalism for 6 monolayers of Fe on the Ir(001) substrate, in order to have a more accurate description of magnons at finite temperature and to obtain good comparison with experimental data. Besides that, we also studied surface magnons on 3 and 9 Ni monolayers on Cu(001) and Cu(111) in order to track the significant surface and/or interface effects and contrast it to properties that are fcc Ni bulk-like. Likewise, we used the Monte Carlo method to estimate the critical temperatures of Ni surfaces and compared with experimental data.  Finally, in the field of low dimensional magnetism, we present the ab-initio calculations for the electronic structure of Cr nanostructures of diverse geometries adsorbed on the Pd(111) surface, with focus on the formation of non-collinear spin configurations, either due to geometric frustration or the spin-orbit coupling provided by the substrate.

Disorder in crystalline materials can take different forms and originate from different sources. In particular, temperature introduces disorder in any kind of material. This can be observed as the appearance of vacant lattice sites in an otherwise perfect crystal, or as a random distribution of different elements on the same lattice in an alloy; at the same time, if the material is magnetic, temperature induces disorder also on the magnetic degrees of freedom. In this thesis, different levels of disorder associated to structure and magnetism are investigated by means of density functional theory and thermodynamic models. I start with diffusion of Ti vacancies in TiN, which is studied by means of nonequilibrium ab initio molecular dynamics using the color diffusion algorithm at different temperatures. The result is an Arrhenius behavior of Ti vacancy jump rates. A method to perform structural relaxations in magnetic materials in their hightemperature paramagnetic phase is then developed based on the disordered local moments approach in order to study vacancies, interstitial atoms, and combinations of defects in paramagnetic bcc Fe and B1 CrN, as well as the mixing enthalpy of bcc Fe1−xCrx random alloys. A correction to the energetics of every system due to the relaxation in the disordered magnetic state is observed in all cases. Not related to temperature and disorder, but very important for an accurate description of magnetic materials, is the choice of the exchange and correlation functional to be employed in the first principles calculations. We have investigated the performance of a recently developed meta-GGA functional, the strongly constrained and appropriately normed (SCAN) functional, in comparison with the more commonly used LDA and PBE on the ferromagnetic elemental solids bcc Fe, fcc Ni, and hcp Co, and SCAN it is found to give negligible improvements, if not a worsening, in the description of these materials. Finally, the coupling between vibrational and magnetic degrees of freedom is discussed by reviewing the literature and proposing an investigation of the influence of vibrations on longitudinal spin fluctuations. These excitations are here studied by means of thermodynamic models based on Landau expansion of the energy in even powers of the magnitude of the local magnetic moments. We find that vibrational and magnetic disorder alter the energy landscapes as a function of moment size also in bcc Fe, which is often considered a Heisenberg system, inducing a more itinerant electron behavior.

In this project a microscopic description of the magnon-phonon coupling is rederived. This theory is then used to simulate the thermalization process between the spin and lattice system in NiO. It is argued that the Kusuya-LeCraw process (1 mg + 1 ph into 1 mg) cannot be the reason that the phononic and magnonic systems reach a thermal equilibrium. As a consequence a quasi-stable equilibrium, different from the thermal solution, is reached in less than 1 ps for NiO. Finally, the effect of applying an external magnetic field to the system, breaking the degeneracy between the magnons of opposite polarization, is studied.

No description available.

In this work, we investigate electronic transport through a double quantum dot junction, where each dot couple to external localized spins. The junction is embedded in between two metallic leads,functioning as continues electron reservoirs. The double quantum dotjunction forms in the junction a bonding and anti-bonding state, muchresembling the electronic structure of a molecule, hence provides in-sight to such systems. Due to the nature of the parallel coupling weexpect a reduced tunneling through the anti-bonding state as a resultof destructive interference as the tunneling is provided multiple path-ways through the molecule. We predict that signature effects arisecorrelating the quantum observable to the effective exchange couplingbetween the localized spin moment and the electronic structure of theDQD. We expect the Fano resonance to disappear entirely when the anti-bonding state is localized and the transmission is carried purely through the bonding state. We further investigate the effects of in-clusion of Rashba Spin-Orbit coupling, allowing decoherence in thetransport. Here, a further degree of freedom is available and morecontrol of the quantum interference and hence the signatures in theexchange is allowed.