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Funding Information: The authors acknowledge SOLEIL for the provision of synchrotron radiation (proposal numbers: 20161265, 20171063, 20180483, 20181721, and 20191506) facilities at the GALAXIES beamline. Some measurements were carried out at the CoESCA endstation at the BESSY-II electron storage ring operated by the Helmholtz-Zentrum Berlin für Materialien und Energie. The research leading to this result has been supported by the project CALIPSOplus under the Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. The authors acknowledge research funding from the Swedish Research Council (Grant Nos. VR 2016-04590, VR 2018-04125, VR 2018-04330, VR 2018-06465), Swedish Energy Agency (P50626-1, P43549-1), the Göran Gustafsson foundation, the Swedish Foundation for Strategic Research (project nr. RMA15-0130), and the Carl Tryggers foundation (Grant No. CTS 18:59). | openaire: EC/H2020/730872/EU//CALIPSOplus A heterojunction is the key junction for charge extraction in many thin film solar cell technologies. However, the structure and band alignment of the heterojunction in the operating device are often difficult to predict from calculations and, due to the complexity and narrow thickness of the interface, are difficult to measure directly. In this study, we demonstrate a technique for direct measurement of the band alignment and interfacial electric field variations of a fully functional lead halide perovskite solar cell structure under operating conditions using hard X-ray photoelectron spectroscopy (HAXPES). We describe the design considerations required in both the solar cell devices and the measurement setup and show results for the perovskite, hole transport, and gold layers at the back contact of the solar cell. For the investigated design, the HAXPES measurements suggest that 70% of the photovoltage was generated at this back contact, distributed rather equally between the hole transport material/gold interface and the perovskite/hole transport material interface. In addition, we were also able to reconstruct the band alignment at the back contact at equilibrium in the dark and at open circuit under illumination.

With each and every passing year, weather patterns seem to become less predictable and more chaotic due to changes to worldwide climate patterns. Greenhouse gas-free energy production is a boon to the aim of preventing further rises in global temperature increases. This thesis concerns itself with one major aspect of green energy, namely photovoltaics, and some materials with great potential for application in photovoltaics, namely single-walled carbon nanotubes (SWNT), and perovskites. SWNT have been known for almost thirty years by now, but their intrinsic fondness of bundling up due to their 2pz-orbitals has to date prevented any large scale application of them. Functionalising of SWNT offers a solution to this problem, either by dispersing them with surfactants in water, or by polymer functionalisation. Here, the latter method was applied to the problem, and the efficacy of deposition from solvents more advantageous than water is shown, achieving values of transmission and sheet resistance close to the necessary values for application in solar cells. Next, an inorganic contender for solar cell applications, Cs2AgBiBr6, is characterised by magneto-optical studies. With these, a direct and indirect gap are identified at 2.85 eV and 1.31eV. Moreover, a strongly Stokes shift influenced AgBi anti-site defect colour centre at 2.25 eV is shown to be part of a self-trapped exciton at low temperatures. Thereafter, the optical properties between 1.4 K and 370 K in conjunction with room temperature x-ray diffraction measurements of MAPbI3 single crystals and thin films grown/annealed at different temperatures are used to explain the double emission structure visible in photo- luminescence and reflectance. A dynamic Rashba effect, likely due to spontaneous alignment of the methylammonium-ions, causes a direct and indirect gap, where the former dominates the surface and the latter dominates the bulk of the samples. The remaining chapter is a study of the polaronic influence on the transitions observed for MAPbBr3 and MAPbI3. In comparison between high field, high energy, and low field, low energy, an almost two-fold difference in exciton binding energy, and an increase in effective mass can be observed due to exciton/lattice interactions in comparison to the established high field literature values. Interestingly, for both perovskites studied, single crystals show more favourable values, indicating that device application improvements could be possible by making thin films more single crystal-like.

Anisotropic two-dimensional materials possess intrinsic angle-dependent physical properties that originate from their low crystal symmetry. Yet, how these properties are affected by external impurities or structural defects in the material is still wholly unclear. Here, we address this question by investigating the electrical transport in the anisotropic layered model system germanium arsenide. First, we show that the ratio of conductivities along the armchair and zigzag crystallographic directions exhibits an intriguing dependence with respect to both temperature and carrier density. Then, by using a conceptually simple model, we demonstrate that this unexpected behavior is directly related to the presence of impurity-induced localized states in the band gap that introduce isotropic hopping conduction. The presence of this conduction mechanism in addition to the intrinsic band conduction significantly influences the anisotropic electrical properties of the material, especially at room temperature, i.e., at application-relevant conditions.

A major obstacle in the advancement of quantum computers is the susceptibility of quantum bits (qubits) to decoherence. Decoherence occurs when a system of qubits encounters local noise like gamma radiation and heat due to incomplete isolation from its surroundings. The noise causes the qubits to change their states, thereby losing information. A new type of quantum computer, called a topological quantum computer, will be built with qubits that use inherent properties to protect against decoherence. Excitations in two-dimensional electron systems can act as this type of qubit. Realizing such a system requires confining electrons to two-dimensional planes inside structures of semiconductor and superconductor layers. A variety of low temperature measurements can be taken in order to evaluate the quality and characteristics of structure samples. These measurements can take many hours at the temperatures necessary to evaluate the sample’s properties. To streamline this process, a cryogenic measurement platform was designed that will allow for rapid assessment of new structures before they are measured at lower temperatures. A probe and a 32-pin sample mount were designed and constructed for the system. A 48 switch BNC panel was machined and wired, and magnet cables were made to charge the 5 Tesla magnet inside the cryostat. A 40-pin sample mount will also be constructed, and the system will be cooled to 4K to take measurements. This cryostat is expected to speed up the sample assessment process greatly.

Geometric and electronic surface reconstructions determine the physical and chemical properties of surfaces and, consequently, their functionality in applications. The reconstruction of a surface minimizes its surface free energy in otherwise thermodynamically unstable situations, typically caused by dangling bonds, lattice stress, or a divergent surface potential, and it is achieved by a cooperative modification of the atomic and electronic structure. Here, we combined first-principles calculations and surface techniques (scanning tunneling microscopy, non-contact atomic force microscopy, scanning tunneling spectroscopy) to report that the repulsion between negatively charged polaronic quasiparticles, formed by the interaction between excess electrons and the lattice phonon field, plays a key role in surface reconstructions. As a paradigmatic example, we explain the (1 × 1) to (1 × 2) transition in rutile TiO2ð110Þ.

Microwave cavities have been widely used to investigate the behavior of closed few-level systems. Here, we show that they also represent a powerful probe for the dynamics of charge transfer between a discrete electronic level and fermionic continua. We have combined experiment and theory for a carbon nanotube quantum dot coupled to normal metal and superconducting contacts. In equilibrium conditions, where our device behaves as an effective quantum dot-normal metal junction, we approach a universal photon dissipation regime governed by a quantum charge relaxation effect. We observe how photon dissipation is modified when the dot admittance turns from capacitive to inductive. When the fermionic reservoirs are voltage biased, the dot can even cause photon emission due to inelastic tunneling to/from a Bardeen-Cooper-Schrieffer peak in the density of states of the superconducting contact. We can model these numerous effects quantitatively in terms of the charge susceptibility of the quantum dot circuit. This validates an approach that could be used to study a wide class of mesoscopic QED devices., Comment: 15 pages, 8 figures, minor differences with published version

International audience; We use coupled micropillars etched out of a semiconductor microcavity to engineer a spin-orbit Hamiltonian for photons and polaritons in a microstructure. The coupling between the spin and orbital momentum arises from the polarization-dependent confinement and tunneling of photons between adjacent micropillars arranged in the form of a hexagonal photonic molecule. It results in polariton eigenstates with distinct polarization patterns, which are revealed in photoluminescence experiments in the regime of polariton condensation. Thanks to the strong polariton nonlinearities, our system provides a photonic workbench for the quantum simulation of the interplay between interactions and spin-orbit effects, particularly when extended to two-dimensional lattices.

International audience; We describe the first implementation of a coupled atom transistor where two shallow donors (P or As) are implanted in a nanoscale silicon nanowire and their electronic levels are controlled with three gate voltages. Transport spectroscopy through these donors placed in series is performed both at zero and microwave frequencies. The coherence of the charge transfer between the two donors is probed by Landau-Zener-Stuckelberg interferometry. Single-charge transfer at zero bias (electron pumping) has been performed and the crossover between the adiabatic and non-adiabatic regimes is studied.

The origin of superconductivity in bulk SrTiO$_{3}$ is a mystery, since the non-monotonous variation of the critical transition with carrier concentration defies the expectations of the crudest version of the BCS theory. Here, employing the Nernst effect, an extremely sensitive probe of tiny bulk Fermi surfaces, we show that down to concentrations as low as $5.5 \times 10^{17}cm^{-3}$, the system has both a sharp Fermi surface and a superconducting ground state. The most dilute superconductor currently known has therefore a metallic normal state with a Fermi energy as little as 1.1 meV on top of a band gap as large as 3 eV. Occurrence of a superconducting instability in an extremely small, single-component and barely anisotropic Fermi surface implies strong constraints for the identification of the pairing mechanism., Final version

A densely and monolithically integrated photonic chip on indium phosphide is greatly in need for data transmission but the present day’s level of integration in InP is very low. Silicon enjoys a unique position among all the semiconductors in its level of integration. But it suffers from its slow signal transmission between the circuit boards and between the chips as it uses conventional electronic wire connections. This being the bottle-neck that hinders enhanced transmission speed, optical-interconnects in silicon have been the dream for several years. Suffering from its inherent deficient optical properties, silicon is not supposed to offer this feasibility in the near future. Hence, integration of direct bandgap materials, such as indium phosphide on silicon, is one of the viable alternatives. This thesis addresses these two issues, namely monolithic integration on indium phosphide and monolithic integration of indium phosphide on silicon. To this end, we use two techniques, namely selective epitaxy and heteroepitaxy by employing hydride vapor phase epitaxy method. The first part deals with the exploitation of selective epitaxy for fabricating a discrete and an integrated chip based on InP. The former is a multi-quantum well buried heterostructure laser emitting at 1.55 µm that makes use of AlGaInAs and InGaAsP as the barrier and well, respectively. We demonstrate that even though it contains Al in the active region, semi-insulating InP:Fe can be regrown. The lasers demonstrate threshold as low as 115A/cm2/quantum well, an external quantum efficiency of 45% and a characteristic temperature of 78 K, all at 20 oC. Concerning the integrated device, we demonstrate complex and densely packed buried arrayed waveguide (AWG) structures found in advanced systems-on-the-chip for optical code-division multiple-access (O-CDMA). We present a case of an error-free 10 Gb/s encoding and decoding operation from an eight-channel AWGs with 180 GHz channel spacing. Selective epitaxial growth aspects specific to these complicated structures are also described and guidance on design implementation of these AWGs is given. Mass transport studies on these AWGs are also presented. The second part deals with various studies on and relevant to epitaxial lateral overgrowth (ELOG) of high quality InP on silicon. (i) ELOG often encounters cases where most part of the surface is covered by mask. From the modeling on large mask area effects, their impact on the transport and kinetic properties has been established. (ii) It is known that ELOG causes strain in the materials. From synchrotron X-ray measurements, strain is shown to have large effect on the mask edges and the underlying substrate. (iii) The combination of strain and the influence of image forces when reducing the opening dimensions in ELOG has been modeled. It is found to be very beneficial to reduce openings down to ~100 nm where effective filtering of dislocations is predicted to take place even in vicinity of the openings. We call it nano-ELOG. (iv) By combining the modeling results of nano-ELOG and of a pre-study of ELOG on pure InP, a novel net pattern design is invented and experimented for nano-ELOG of InP on Si. PL measurements together with transmission electron microscopy observations indicate beneficial effects of small size openings (200 nm) compared to 1000 nm openings. (v) ELOG of InP on silicon-on-insulators together with a multi-quantum well structure grown on it has been demonstrated for the first time. This is particularly interesting for integrating silicon/silicon dioxide waveguides with InP. QC 20100902