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Institute
The fact that photovoltaics is a key technology for climate-neutral energy production can be taken as a given. The question to what extent perovskite will be used for photovoltaic technologies has not yet been fully answered. From a photophysical point of view, however, it has the potential to make a useful contribution to the energy sector. However, it remains to be seen whether perovskite-based modules will be able to compete with established technologies in terms of durability and cost efficiency. The additional aspect of ionic migration poses an additional challenge. In the present work, primarily the interaction between ionic redistribution, capacitive properties and recombination dynamics was investigated. This was done using impedance spectroscopy, OCVD and IV characteristics as well as extensive numerical drift-diffusion simulations. The combination of experimental and numerical methods proved to be very fruitful. A suitable model for the description of solar cells with respect to mobile ions was introduced in chapter 4.4. The formal mathematical description of the model was transferred by a non-dimensionalization and suitable numerically solvable form. The implementation took place in the Julia language. By intelligent use of structural properties of the sparse systems of equations, automatic differentiation and the use of efficient integration methods, the simulation tool is not only remarkably fast in finding the solution, but also scales quasi-linearly with the grid resolution. The software package was released under an open source license. In conventional semiconductor diodes, capacitance measurements are often used to determine the space charge density. In the first experimental chapter 5, it is shown that although this is also possible for the ionic migration present in perovskites, it cannot be directly understood as doping related, since the space charge distribution strongly depends on the preconditions and can be manipulated by an externally applied voltage. The exact form of this behavior depends on the perovskite composition. This shows, among other things, that experimental results can only be interpreted within the framework of conventional semiconductors to a very limited extent. Nevertheless, the built-in 99 potential of the solar cell can be determined if the experiments are carried out properly. A statement concerning the type and charge of the mobile ions is not possible without further effort, while their number can be determined. The simulations were applied to experimental data in chapter 6. Thus, it could be shown that mobile ions make a significant contribution to the OCVD of perovskite solar cells. j-V characteristics and OCVD transients measured as a function of temperature and illumination intensities could be quantitatively modeled simultaneously using a single global set of parameters. By the simulations it was further possible to derive a simple experimental procedure to determine the concentration and the diffusivity of the mobile ions. The possibility of describing different experiments in a uniform temperaturedependent manner strongly supports the model of mobile ions in perovskites. In summary, this work has made an important contribution to the elucidation of ionic contributions to the (photo)electrical properties of perovskite solar cells. Established experimental techniques for conventional semiconductors have been reinterpreted with respect to ionic mass transport and new methods have been proposed to draw conclusions on the properties for ionic transport. As a result, the published simulation tools can be used for a number of further studies.
Explaining the baryon asymmetry of the Universe has been a long-standing problem of particle physics, with the consensus being that new physics is required as the Standard Model (SM) cannot resolve this issue. Beyond the Standard Model (BSM) scenarios would need to incorporate new sources of \(CP\) violation and either introduce new departures from thermal equilibrium or modify the existing electroweak phase transition. In this thesis, we explore two approaches to baryogenesis, i.e. the generation of this asymmetry.
In the first approach, we study the two-particle irreducible (2PI) formalism as a means to investigate non-equilibrium phenomena. After arriving at the renormalised equations of motions (EOMs) to describe the dynamics of a phase transition, we discuss the techniques required to obtain the various counterterms in an on-shell scheme. To this end, we consider three truncations up to two-loop order of the 2PI effective action: the Hartree approximation, the scalar sunset approximation and the fermionic sunset approximation. We then reconsider the renormalisation procedure in an \(\overline{\text{MS}}\) scheme to evaluate the 2PI effective potential for the aforementioned truncations. In the Hartree and the scalar sunset approximations, we obtain analytic expressions for the various counterterms and subsequently calculate the effective potential by piecing together the finite contributions. For the fermionic sunset approximation, we obtain similar equations for the counterterms in terms of divergent parts of loop integrals. However, these integrals cannot be expressed in an analytic form, making it impossible to evaluate the 2PI effective potential with the fermionic contribution. Our main results are thus related to the renormalisation programme in the 2PI formalism: \( (i) \)the procedure to obtain the renormalised EOMs, now including fermions, which serve as the starting point for the transport equations for electroweak baryogenesis and \( (ii) \) the method to obtain the 2PI effective potential in a transparent manner.
In the second approach, we study baryogenesis via leptogenesis. Here, an asymmetry in the lepton sector is generated, which is then converted into the baryon asymmetry via the sphaleron process in the SM. We proceed to consider an extension of the SM along the lines of a scotogenic framework. The newly introduced particles are charged odd under a \(\mathbb{Z}_2\) symmetry, and masses for the SM neutrinos are generated radiatively. The \(\mathbb{Z}_2\) symmetry results in the lightest BSM particle being stable, allowing for a suitable dark matter (DM) candidate. Furthermore, the newly introduced heavy Majorana fermionic singlets provide the necessary sources of \(CP\) violation through their Yukawa interactions and their out-of-equilibrium decays produce a lepton asymmetry. This model is constrained from a wide range of observables, such as consistency with neutrino oscillation data, limits on branching ratios of charged lepton flavour violating decays, electroweak observables and obtaining the observed DM relic density. We study leptogenesis in this model in light of the results of a Markov chain Monte Carlo scan, implemented in consideration of the aforementioned constraints. Successful leptogenesis in this model, to account for the baryon asymmetry, then severely constrains the available parameter space.