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Abstract: Antimony selenide (Sb2Se3) is a promising absorber material for thin-film photovoltaics. However, certain areas of fundamental understanding of this material remain incomplete and this presents a barrier to further efficiency gains. In particular, recent studies have highlighted the role of majority carrier type and extrinsic doping in drastically changing the performance of high efficiency devices [1]. Herein, Sndoped Sb2Se3 bulk crystals are shown to exhibit p-type conductivity using Hall effect and hot-probe measurements. The measured conductivities are higher than those achieved through native defects alone, but with a carrier density (up to 7.4 × 1014 cm−3) several orders of magnitude smaller than the quantity of Sn included in the source material. Additionally, a combination of ultraviolet, X-ray and hard X-ray photoemission spectroscopies are employed to obtain a non-destructive depth profile of the valence band maximum, confirming p-type conductivity and indicating a majority carrier type inversion layer at the surface. Finally, these results are supported by density functional theory calculations of the defect formation energies in Sn-doped Sb2Se3, showing a possible limit on the carrier concentration achievable with Sn as a dopant. This study sheds light on the effectiveness of Sn as a p-type dopant in Sb2Se3 and highlights avenues for further optimisation of doped Sb2Se3 for solar energy devices.

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Abstract: In antiferromagnetic (AF) materials, magnetic moments align in a regular pattern such that the moments cancel perfectly in each magnetic unit cell. Hence AF materials do not show a net magnetisation and are largely inert against magnetic fields. Thus, the hidden order of antiferromagnets has only been revealed in the last century. For spintronic applications, the use of antiferromagnets promises numerous advantages compared to conventional spintronics based primarily on ferromagnetic (FM) materials. Amongst the key materials for AF spintronics research are tetragonal, antiferromagnetic CuMnAs films, because in addition to being antiferromagnetically ordered at room-temperature, tetragonal CuMnAs is one of only two conductive AF materials, for which it has been shown that the AF order can be manipulated with electrical currents. This has raised hopes for antiferromagnetic memory devices where the AF order in CuMnAs is switched electrical between two different states. The magnetic moments in CuMnAs films form ferromagnetic sheets (parallel alignment) which are stacked antiparallel along the crystallographic c-direction. The spin axis is confined within the ab-plane, but varies on a microscopic scale, which produces a variety of different AF domain structures. This thesis adresses the question: “what underlies the AF domain structures and how can they be manipulated efficiently?” Visualising antiferromagnetic domain structures remains experimentally challenging, because the domains do not show a net magnetisation. Here, it is realised by combining photoemission electron microscopy (PEEM) with x-ray magnetic linear dichroism (XMLD), which yields sensitivity to the spin axis. These measurements require x-rays with precisely tunable energy. Therefore, this work has largely been performed at a synchrotron, namely Diamond Light Source. Here, direct imaging of the response of the AF domain structure upon the application of electrical current pulses is used to study the microscopic mechanisms of electric switching in CuMnAs films. In the films studied here, the most efficient switching was found to occur via reversible AF domain wall motion induced by electrical current pulses of alternating polarity. The measurements also reveal the limiting factors of electrical switching in CuMnAs films, namely domain pinning which limits device efficiency and domain relaxation which hinders long-term memory. This illustrates that one needs to be able to precisely tune the material properties for a specific application in order to build efficient AF spintronic devices. Hence, the factors, which govern the AF spin textures in the CuMnAs films, need to be revealed. This is done by combining direct imaging of the AF domain structure with complementary techniques including electrical measurements, scanning X-ray diffraction and low-energy electron microscopy and diffraction (LEEM, LEED). The measurements reveal that the AF domain patterns are highly sensitive to the crystallographic microstructure including patterned edges and crystallographic defects. In particular, crystallographic microtwin defects are found to largely define the AF domain structure in non-patterned films. The coupling between defects and AF domains can lead to magnetostructural kinetics, where defects and AF domains grow together over weeks at room temperature and over minutes at slightly elevated temperatures of 50°C -70°C. In devices, patterned edges are found to influence the AF domains over tens of micrometers. Combining the knowledge about the effects of microtwin defects and patterned edges on the AF structure helps to understand the microscopic effects of electric current pulses and can form the basis for targeted AF domain engineering.

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Abstract: Silicene, the two-dimensional (2D) allotrope of silicon, is a promising material for electronics. So far, the most direct synthesis strategy has been to grow it epitaxially on metal surfaces; however, the effect of the strong silicon-metal interaction on the structure and electronic properties of the metal-supported silicene is generally poorly understood. In this work, we consider the 4×4-silicene monolayer grown on Ag(111), probably the most illustrious representative of the 2D silicon family, and show that our experimental results refute the common interpretation of this system as a simple buckled, honeycomb monolayer with a sharp interface to the Ag substrate. Instead, the presented analysis demonstrates the pervasive presence of a second silicon species, which we conclude to be a Si‑Ag alloy stacked between the 2D silicene and the silver substrate and scaffolding the 2D silicene layer. These findings question the current structural understanding of the silicene/Ag(111) interface and may raise expectations of analogous alloy systems in the stabilization of other 2D materials grown epitaxially on metal surfaces.

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Abstract: In materials science, much effort has been devoted to the reproduction of superconductivity in chemical compositions, analogous to cuprate superconductors since their discovery over 30 years ago. This approach was recently successful in realising superconductivity in infinite-layer nickelates1,2,3,4,5,6. Although differing from cuprates in electronic and magnetic properties, strong Coulomb interactions suggest that infinite-layer nickelates have a propensity towards various symmetry-breaking orders that populate cuprates7,8,9,10. Here we report the observation of charge density waves (CDWs) in infinite-layer NdNiO2 films using Ni L3 resonant X-ray scattering. Remarkably, CDWs form in Nd 5d and Ni 3d orbitals at the same commensurate wavevector (0.333, 0) reciprocal lattice units, with non-negligible out-of-plane dependence and an in-plane correlation length of up to ~60 Å. Spectroscopic studies reveal a strong connection between CDWs and Nd 5d–Ni 3d orbital hybridization. Upon entering the superconducting state at 20% Sr doping, the CDWs disappear. Our work demonstrates the existence of CDWs in infinite-layer nickelates with a multiorbital character distinct from cuprates, which establishes their low-energy physics.

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Abstract: We combine state-of-the-art oxide epitaxial growth by hybrid molecular beam epitaxy with transport, x-ray photoemission, and surface diffraction, along with classical and first-principles quantum mechanical modeling to investigate the nuances of insulating layer formation in otherwise high-mobility homoepitaxial n-SrTiO3(001) films. Our analysis points to charge immobilization at the buried n-SrTiO3/undoped SrTiO3(001) interface as well as within the surface contamination layer resulting from air exposure as the drivers of electronic dead-layer formation. As Fermi level equilibration occurs at the surface and the buried interface, charge trapping reduces the sheet carrier density (n2D) and renders the n-STO film insulating if n2D falls below the critical value for the metal-to-insulator transition.