ABSTRACT
Unusual features in the Hall Resistivity of thin film systems are frequently associated with whirling spin textures such as Skyrmions. A host of recent investigations of Hall Hysteresis loops in SrRuO3 heterostructures have provided conflicting evidence for different causes for such features. We have constructed an SrRuO3-PbTiO3 (Ferromagnetic - Ferroelectric) bilayer that exhibits features in the Hall Hysteresis previously attributed to a Topological Hall Effect, and Skyrmions. Here we show field dependent Magnetic Force Microscopy measurements throughout the key fields where the 'THE' presents, revealing the emergence to two periodic, chiral spin textures. The zero-field cycloidal phase, which then transforms into a 'double-q' incommensurate spin crystal appears over the appearance of the 'Topological-like' Hall effect region, and develop into a ferromagnetic switching regime as the sample reaches saturation, and the 'Topological-like' response diminishes. Scanning Tunnelling Electron Microscopy and Density Functional Theory is used to observe and analyse surface inversion symmetry breaking and confirm the role of an interfacial Dzyaloshinskii-Moriya interaction at the heart of the system.
ABSTRACT
Bulk crystals and thin films of PbTi(1-x)FexO3(-δ) (PTFO) are multiferroic, exhibiting ferroelectricity and ferromagnetism at room temperature. Here we report that the Ruddlesden-Popper phase Pbn+1(Ti(1-x)Fex)nO3(n+1)-δ forms spontaneously during pulsed laser deposition of PTFO on LaAlO3 substrates. High-resolution transmission electron microscopy, x-ray diffraction and x-ray photoemission spectroscopy were utilised to perform a structural and compositional analysis, demonstrating that n ≃ 8 and x ≃ 0.5. The complex dielectric function of the films was determined from far-infrared to ultraviolet energies using a combination of terahertz time-domain spectroscopy, Fourier transform spectroscopy, and spectroscopic ellipsometry. The simultaneous Raman and infrared activity of phonon modes and the observation of second harmonic generation establishes a non-centrosymmetric point group for Pbn+1(Ti0.5Fe0.5)nO3(n+1)-δ, a prerequisite for (but not proof of) ferroelectricity. No evidence of macroscopic ferromagnetism was found in SQUID magnetometry. The ultrafast optical response exhibited coherent magnon oscillations compatible with local magnetic order, and additionally was used to study photocarrier cooling on picosecond timescales. An optical gap smaller than that of BiFeO3 and long photocarrier lifetimes may make this system interesting as a ferroelectric photovoltaic.
