We studied how an additional layer of the high T-C superconductor YBCO affects the magneto-transport across a LSMO/Alq(3)/Co spin-valve structure. We found that up to a thickness of at least 10 nm the YBCO layer on top of LSMO hardly changes the spin-valve effect, since the device resistance still depends on the relative orientation of the LSMO and Co magnetization. The spin-valve effect persists even when the superconducting YBCO layer acts as bottom electrode, with no spin-polarized current injected from LSMO into YBCO. This highlights that the charge carriers of a thin YBCO layer on top of LSMO are strongly spin- polarized, most likely due to a magnetic proximity effect involving a transfer of spin-polarized electrons from LSMO to YBCO. Evidence for a strongly underdoped state of the YBCO layers close to the interface with LSMO is indeed obtained from the dI/dV curves in zero magnetic field which reveal a pseudogap persisting well above T-C.

With dc magnetization and polarized neutron reflectometry we studied the ferromagnetic response of YBa₂Cu₃O₇/La_2/3Ca_1/3MnO₃ (YBCO/LCMO) multilayers that are grown with pulsed laser deposition. We found that whereas for certain growth conditions (denoted as A type) the ferromagnetic moment of the LCMO layer is strongly dependent on the structural details of the YBCO layer on which it is deposited, for others (B type) the ferromagnetism of LCMO is much more robust. Both kinds of multilayers are of similar structural quality, but electron energy-loss spectroscopy studies with a scanning transmission electron microscope reveal an enhanced average Mn oxidation state of +3.5 for the A-type as opposed to the B-type samples, for which it is close to the nominal value of +3.33. The related, additional hole doping of the A-type LCMO layers, which likely originates from La and/or Mn vacancies, can explain their fragile ferromagnetic order, since it places them close to the boundary of the ferromagnetic order at which even weak perturbations can induce an antiferromagnetic or glassy state. On the other hand, we show that the B-type samples allow one to obtain YBCO/LCMO heterostructures with very thick YBCO layers and, yet, strongly ferromagnetic LCMO layers.

We fabricate and study experimentally all-perovskite-oxide superconductor/ferromagnetic insulator/superconductor (S/FI/S) tunnel junctions made out of the high-temperature cuprate superconductor YBa₂Cu₃O_7−y (YBCO) and the colossal magnetoresistive manganite LaMnO₃ (LMO) in the ferromagnetic insulator state. YBCO/LMO/YBCO heterostructures with different LMO thicknesses (5, 10, and 20 nm) are grown epitaxially via pulsed laser deposition. Nanoscale S/FI/S junctions with sizes down to 300 nm are made by three-dimensional nano-sculpturing with focused ion beam. Junctions with a thick (20 nm) LMO barrier exhibit a large negative magnetoresistance below T_Curie∼160 K, typical for colossal magnetoresistive manganites, as well as a kink in the current-voltage characteristics at large bias (V∼1–2 Volts), attributed to Zener-type tunneling. However, they do not show a measurable Josephson current. On the contrary, junctions with the thinnest 5-nm LMO barrier exhibit a large supercurrent and no signs of magnetism. The latter may indicate the presence of pinholes due to thickness inhomogeneity and/or a ∼ 2 nm dead magnetic layer at the YBCO / LMO interface caused, e.g., by interdiffusion or strain. The junction with an intermediate 10-nm LMO barrier exhibited a desired S/FI/S junction behavior with significant negative magnetoresistance and signatures of a small Josephson current.

Complex oxides exhibit a variety of unusual physical properties, which can be used for designing novel electronic devices. Here we fabricate and study experimentally nanoscale superconductor/ferromagnet/ superconductor junctions with the high-T_c cuprate superconductors YBa₂Cu₃O_7−x and the colossal magnetoresistive (CMR) manganite ferromagnets La_2/3X_1/3MnO_3+δ(X=CaorSr). We demonstrate that in a broad temperature range the magnetization of a manganite nanoparticle, forming the junction interface, switches abruptly in a monodomain manner. The CMR phenomenon translates the magnetization loop into a hysteretic magnetoresistance loop. The latter facilitates a memory functionality of such a junction with just a single CMR ferromagnetic layer. The orientation of the magnetization (stored information) can be read out by simply measuring the junction resistance in a finite magnetic field. The CMR facilitates a large readout signal in a small applied field. We argue that such a simple single-layer CMR junction can operate as a memory cell both in the superconducting state at cryogenic temperatures and in the normal state up to room temperature.

This thesis explores the growth, the nano-fabrication and the study of the magneto-transport properties of Superconductor/Ferromagnet/Superconductor (SFS) structures from complex oxides such as the high T_c superconducting cuprate YBa₂Cu₃O₇ (YBCO) and the ferromagnetic manganites La_2/3Ca_1/3MnO₃ and La_2/3Sr_1/3MnO₃ (LCMO and LSMO), deposited with the pulsed laser deposition (PLD) technique.The present work has been possible thanks to the collaboration between the “Magnetism and Superconductivity” Group at the University of Fribourg, in Switzerland, and the “Experimentell Kondenserade Materiens Fysik” Group at Stockholm University, in Sweden.

Earlier, the two research groups in Fribourg and Stockholm had studied SFS structures from YBCO/LaMnO₃/YBCO multilayers with 20 nm thick ferromagnetic and insulating LaMnO₃ barriers, and obtained signs of an unconventional spin-triplet current across these structures. This finding motivated the present thesis work with a focus on two main aspects.

Firstly, to explore other candidate materials suitable as barriers and optimise their growth conditions as to maintain a large ferromagnetic moment and thus a high spin polarisation of the charge carriers. Secondly, to study what happens when the thickness of the ferromagnetic and insulating LaMnO₃ barrier is reduced well below 20 nm to enable larger supercurrents.

It has been shown for a series of YBCO/LCMO multilayers that the ferromagnetic moment of LCMO depends critically on the PLD growth conditions as well as on the thickness and even structural details of the YBCO layer on which they are grown. Furthermore, a protocol has been established to grow heterostructures with strongly ferromagnetic manganite layers embedded in thick YBCO layers by optimising the PLD growth conditions and by substituting the bottom YBCO layer with a Co and Ca substituted version of YBCO that has a tetragonal structure (tYBCO) instead of the orthorhombic one of plain YBCO.

Devices suitable for perpendicular magneto-transport measurements have been nano-fabricated from YBCO/manganite/YBCO multilayers with ~10 nm thick LCMO and LSMO layers as the F barriers. While no clear indications of a spin-triplet component of the superconducting order parameter have been obtained yet, a negative and hysteretic magneto-resistance has been observed that is indicative of a strong ferromagnetic order in the thin manganite barrier. The latter suggests a potential memory functionality of such structures that could be exploited in future spintronic memory devices.

Moreover, devices have been fabricated on SFS structures with a reduced thickness of the LaMnO₃ barrier of 10 nm and 5 nm. These samples were grown prior to the beginning of this PhD work using non optimised growth conditions, and it was found that the ferromagnetic properties of these LaMnO₃ barriers are strongly deteriorated. It remains to be seen whether the ferromagnetic order of such thin LaMnO₃ layers can be also recovered by using the optimised growth conditions as for LSMO and LCMO.

We studied the structural, magnetic and electronic properties of SrFeO3-delta (SFO) thin films and SrFeO3-delta/La2/3Ca1/3MnO3 (LCMO) superlattices that have been grown with pulsed laser deposition (PLD) on La0.3Sr0.7Al0.65Ta0.35O3 (LSAT) substrates. X-ray reflectometry and scanning transmission electron microscopy (STEM) confirm the high structural quality of the films and flat and atomically sharp interfaces of the superlattices. The STEM data also reveal a difference in the interfacial layer stacking with a SrO layer at the LCMO/SFO and a LaO layer at the SFO/LCMO interfaces along the PLD growth direction. The x-ray diffraction (XRD) data suggest that the as grown SFO films and SFO/LCMO superlattices have an oxygen-deficient SrFeO3-delta structure with I4/mmm space group symmetry (delta <= 0.2). Subsequent ozone annealed SFO films are consistent with an almost oxygen stoichiometric structure (delta approximate to 0). The electronic and magnetic properties of these SFO films are similar to the ones of corresponding single crystals. In particular, the as grown SrFeO3-delta films are insulating whereas the ozone annealed films are metallic. The magneto-resistance effects of the as grown SFO films have a similar magnitude as in the single crystals, but extend over a much wider temperature range. Last but not least, for the SFO/LCMO superlattices we observe a rather large exchange bias effect that varies as a function of the cooling field.

La1.85Sr0.15CuO4/La2CuO4 (LSCO15/LCO) bilayers with a precisely controlled thickness of N unit cells (UCs) of the former and M UCs of the latter ([LSCO15_N/LCO_M]) were grown on (001)-oriented SrLaAlO4 (SLAO) substrates with pulsed laser deposition (PLD). X-ray diffraction and reciprocal space map (RSM) studies confirmed the epitaxial growth of the bilayers and showed that a [LSCO15_2/LCO_2] bilayer is fully strained, whereas a [LSCO15_2/LCO_7] bilayer is already partially relaxed. The in situ monitoring of the growth with reflection high energy electron diffraction (RHEED) revealed that the gas environment during deposition has a surprisingly strong effect on the growth mode and thus on the amount of disorder in the first UC of LSCO15 (or the first two monolayers of LSCO15 containing one CuO2 plane each). For samples grown in pure N2O gas (growth type B), the first LSCO15 UC next to the SLAO substrate is strongly disordered. This disorder is strongly reduced if the growth is performed in a mixture of N2O and O2 gas (growth type A). Electric transport measurements confirmed that the first UC of LSCO15 next to the SLAO substrate is highly resistive and shows no sign of superconductivity for growth type B, whereas it is superconducting for growth type A. Furthermore, we found, rather surprisingly, that the conductivity of the LSCO15 UC next to the LCO capping layer strongly depends on the thickness of the latter. A LCO capping layer with 7 UCs leads to a strong localization of the charge carriers in the adjacent LSCO15 UC and suppresses superconductivity. The magnetotransport data suggest a similarity with the case of weakly hole doped LSCO single crystals that are in a so-called ‘cluster-spin-glass state.’ We discussed several mechanisms that could lead to such a localization of holes that are embedded in a short-range ordered antiferromagnetic background for the case of a thick LCO capping layer with M=7 but not for a thin one with M=2.