This thesis examines the preparation of thin layers of material for photovoltaic applications with focused on perovskites and determining their optical properties. Basic information about the photovoltaic panels, especially about the perovskites, and the preparation of thin layers is supplied in the theoretical section. This section includes description of optical properties and the main method of study of optical properties, spectroscopic ellipsometry. Experimental section is focused on the preparation of thin layers of perovskites FAPbBr3 and its precursors by spin-coating. Optical properties are evaluated using profilometry, UV VIS spectrometry and spectroscopic ellipsometry. The conclusion summarizes the results of this experiment with focused on comparison of ellipsometric spectrums of perovskites and its precursors.

Tato studie je zaměřena na základní výzkum tenkých vrstev plazmových polymerů a vliv depozičních podmínek na strukturu a vlastnosti jednotlivých vrstev a multivrstev připravených pomocí metody PE CVD. Jednotlivé vrstvy a multivrstvy a-SiC:H byly deponovány na křemíkové substráty z monomeru tetravinylsilanu (TVS) při různých výkonech v kontinuálním a pulzním režimu. Vrstvy byly rozsáhle zkoumány pomocí spektroskopické elipsometrie, nanoindentace, mikroskopie atomárních sil (AFM), rentgenové fotoelektronové spektroskopie (XPS), spektroskopie Rutherfordova zpětného rozptylu (RBS), rentgenové reflektivity, Fourierovy transformační infračervené spektroskopie (FTIR) a měření kontaktního úhlu, pro zjištění jejich optických, mechanických a chemických vlastností. Byl zkoumán a prokázán vliv depozičních podmínek na fyzikálně-chemické vlastnosti pp-TVS vrstev. Jednotlivé vrstvy byly v rámci po-depoziční úpravy vystaveny UV záření a byl zkoumán účinek stárnutí a vliv UV záření na jejich fyzikální a chemické vlastnosti. Multivrstevnaté struktury (plazmaticky polymerizované 2-vrstvy a 10-ti-vrstvy) s tloušťkou jednotlivých vrstev od 0,5 µm do 25 nm byly úspěšně deponovány a charakterizovány pomocí elipsometrické spektroskopie. Na základě získaných poznatků je možné připravit materiály s vlastnostmi upravenými podle požadavků pro využití v nanokompozitních aplikacích a optických zařízeních.

abstract: The emergence of perovskite and practical efficiency limit to silicon solar cells has opened door for perovskite and silicon based tandems with the possibility to achieve >30% efficiency. However, there are material and optical challenges that have to be overcome for the success of these tandems. In this work the aim is to understand and improve the light management issues in silicon and perovskite based tandems through comprehensive optical modeling and simulation of current state of the art tandems and by characterizing the optical properties of new top and bottom cell materials. Moreover, to propose practical solutions to mitigate some of the optical losses. Highest efficiency single-junction silicon and bottom silicon sub-cell in silicon based tandems employ monocrystalline silicon wafer textured with random pyramids. Therefore, the light trapping performance of random pyramids in silicon solar cells is established. An accurate three-dimensional height map of random pyramids is captured and ray-traced to record the angular distribution of light inside the wafer which shows random pyramids trap light as well as Lambertian scatterer. Second, the problem of front-surface reflectance common to all modules, planar solar cells and to silicon and perovskite based tandems is dealt. A nano-imprint lithography procedure is developed to fabricate polydimethylsiloxane (PDMS) scattering layer carrying random pyramids that effectively reduces the reflectance. Results show it increased the efficiency of planar semi-transparent perovskite solar cell by 10.6% relative. Next a detailed assessment of light-management in practical two-terminal perovskite/silicon and perovskite/perovskite tandems is performed to quantify reflectance, parasitic and light-trapping losses. For this first a methodology based on spectroscopic ellipsometry is developed to characterize new absorber materials employed in tandems. Characterized materials include wide-bandgap (CH3NH3I3, CsyFA1-yPb(BrxI1-x)3) and low-bandgap (Cs0.05FA0.5MA0.45(Pb0.5Sn0.5)I3) perovskites and wide-bandgap CdTe alloys (CdZnSeTe). Using this information rigorous optical modeling of two-terminal perovskite/silicon and perovskite/perovskite tandems with varying light management schemes is performed. Thus providing a guideline for further development. / Dissertation/Thesis / Doctoral Dissertation Electrical Engineering 2019

This diploma thesis is devoted to systematic study of structural trans- formations of Heusler alloys by means of spectroscopic ellipsometry and magneto-optical spectroscopy. Structural transformations in these alloys are induced by different microscopic mechanisms. Obtained experimental results were confronted with theoretical calculations. This allowed the discussion of obtained results and suggestion of their interpretation. In the case of Co- Fe-Si alloys, changes in optical and magneto-optical properties with change of Co-Fe ratio were observer. This was explained by lowering of the gap for minority spins with increasing Fe concentrations. Temperature dependent optical and magneto-optical properties of Ni-Mn-Ga alloy showed the pres- ence of so-called Martensitic transformation from cubic to tetragonal phase. A study of Mn-Rh-Co-Sn alloys did not show a clear dependence of physical properties upon the concentration of Rh and Mn. This was explained by strong strain inside the samples, which distorted obtained results. 1

Cílem této práce bylo studium Heuslrových sloučenin pomocí optických a magneto-optických (MO) metod. V případě první sloučeniny, Co2FeGa0.5Ge0.5, jsme studovali výskyt strukturálního disorderu za pomoci spektroskopické elipsometrie, MO spektroskopie a MO Kerrovy magnetome- trie. Experimentální výsledky jsme poté porovnali s teoretickými modely. Doplnili jsme také výsledky našich spolupracovník·, a to včetně X-ray difrakce, atomic-force mikroskopie a ab initio výpočt·, abych potvrdili naši interpretaci naměřených výsledk·. Bylo zjištěno, že strukturální disorder je vskutku pozorovatelný pomocí metod, kterých jsme využili. Jeho výskyt se projevil změnou elektronové struktury vzork·. V případě druhé sloučeniny, Fe2MnGa, jsme vyšetřovali vliv obsahu Fe složky na optické a MO vlastnosti tohoto materiálu. Zjistili jsme, že atomy Fe ovlivňují koncentraci volných elektron·, čímž dodávají sloučenině kovový charakter (v porovnání s Ni2MnGa). Zároveň zvyšují optickou a MO odezvu v blízké infra-červené oblasti spektra. Dále bylo zjištěno, že vzorek s nejvyšším obsahem Fe má nulovou magnetizaci. 1

The developement of a femtosecond-time-resolved spectroscopic ellipsometry setup based on a pump-probe technique is described. The characterization of the setup is presented as well as first results of experiments on a c-plane oriented ZnO thin film are shown. Indications for the study of fast charge-carrier dynamics are given.:Introduction 1 1 Theoretical framework 3 1.1 Zinc oxide . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3 1.1.1 Crystal and band structure . . . . . . . . . . . . . . . . . . . . . 3 1.1.2 Excitons . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4 1.2 Dielectric function and electronic transitions . . . . . . . . . . . . . . . . 5 1.2.1 Electronic transitions . . . . . . . . . . . . . . . . . . . . . . . . . 5 1.2.2 Dielectric function . . . . . . . . . . . . . . . . . . . . . . . . . . 5 1.3 Charge carrier dynamics . . . . . . . . . . . . . . . . . . . . . . . . . . . 7 1.3.1 High excitation effects . . . . . . . . . . . . . . . . . . . . . . . . 8 1.3.2 Charge carrier density-dependent dielectric function model . . . . 9 1.4 Light polarization . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11 2 Preliminary experiments 14 2.1 Methods and instrumentation . . . . . . . . . . . . . . . . . . . . . . . . 14 2.2 Setup . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19 2.3 Experimental challenges . . . . . . . . . . . . . . . . . . . . . . . . . . . 24 2.4 Results . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28 2.4.1 Time-integrated micro-ellipsometry . . . . . . . . . . . . . . . . . 28 2.4.2 Time-resolved ellipsometry . . . . . . . . . . . . . . . . . . . . . . 31 2.4.3 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33 3 Conclusive experiments at ELI Beamlines 35 3.1 Setup . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 36 3.2 Samples . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 48 3.3 Demonstration of functionality . . . . . . . . . . . . . . . . . . . . . . . . 49 3.3.1 Time-resolved reflectometry . . . . . . . . . . . . . . . . . . . . . 49 3.3.2 Time-resolved ellipsometry . . . . . . . . . . . . . . . . . . . . . . 51 4 Results and discussion 55 4.1 Time-resolved reflectometry . . . . . . . . . . . . . . . . . . . . . . . . . 55 4.2 Time-resolved ellipsometry . . . . . . . . . . . . . . . . . . . . . . . . . . 60 5 Summary and outlook 63

A new cluster tool for in situ real-time processing and depth-resolved compositional, structural and optical characterization of thin films at temperatures from -100 to 800 °C is described. The implemented techniques comprise magnetron sputtering, ion irradiation, Rutherford backscattering spectrometry, Raman spectroscopy and spectroscopic ellipsometry. The capability of the cluster tool is demonstrated for a layer stack MgO/ amorphous Si (~60 nm)/ Ag (~30 nm), deposited at room temperature and crystallized with partial layer exchange by heating up to 650°C. Its initial and final composition, stacking order and structure were monitored in situ in real time and a reaction progress was defined as a function of time and temperature.

We report an influence of disorder on structural and magnetic properties of ZnFe2O4 thin films grown at temperatures ranging from 400°C to 600°C by pulsed laser deposition in O2 atmosphere on SrTiO3 (100) substrates evidenced by properties of electronic transitions observed in the dielectric function. Inversion of the normal spinel structure was found to be one of the main mechanisms responsible for the increase in the magnetic response for the lowest growth temperature. The enhanced feature in the dielectric function located at ~3.5 eV, related to the transition involving tetrahedrally coordinated Fe3+ cations, corresponds to the dominating magnetic coupling between the octahedral and tetrahedral lattice sites, responsible for the overall ferrimagnetic behaviour of the film grown at the lowest temperature.

Thin films are a prerequisite for application of the emergent exotic ground states in iridates that result from the interplay of strong spin-orbit coupling and electronic correlations. We report on pulsed laser deposition of Li2IrO3 films on ZrO2:Y (001) single crystalline substrates. X-ray diffraction confirms preferential (001) and (10-1) out-of-plane crystalline orientations with well defined in-plane orientation. Resistivity between 35 and 300K is dominated by a three-dimensional variable range hopping mechanism. The dielectric function is determined by means of spectroscopic ellipsometry and, complemented by Fourier transform infrared transmission spectroscopy, reveals a small optical gap of ≈300 meV, a splitting of the 5d-t2g manifold, and several in-gap excitations attributed to phonons and possibly magnons.

The dielectric function of heteroepitaxial YBiO3 grown on a-Al2O3 single crystals via pulsed laser deposition is determined in the spectral range from 0.03 eV to 4.5 eV by a simultaneous modeling of the spectroscopic ellipsometry and optical transmission data of YBiO3 films of different thicknesses. The (111)-oriented YBiO3 films are nominally unstrained and crystallize in a defective fluorite-type structure with a Fm3⎯⎯m space group. From the calculated absorption spectrum, a direct electronic bandgap energy of 3.6(1) eV and the signature of an indirect electronic transition around 0.5 eV are obtained. These values provide necessary experimental feedback to previous conflicting electronic band structure calculations predicting either a topologically trivial or a non-trivial insulating ground state in YBiO3.