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Oliver Paull

Publications and source records attributed to Oliver Paull.

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Rashba engineering at van der Waals interfaces

Two-dimensional transition metal dichalcogenide (TMD) interfaces offer a versatile platform for studying emergent quantum phenomena and enabling novel device functionalities. When distinct TMD monolayers are stacked vertically or laterally stitched, their interfaces can exhibit unique electronic band alignments, giving rise to long-lived interlayer excitons, charge transfer effects, and moir\'e superlattices with correlated states. Here, we demonstrate that the interface between a large variety of two different epitaxially grown TMD monolayers controls the intensity and sign of the Rashba spin splitting, which is probed using THz spintronic emission. Optimized TMD heterobilayers, such as HfSe$_2$/PtSe$_2$, show enhanced THz emission that surpass the spin-to-charge conversion efficiency of bulk TMDs, confirming the presence of Rashba states with large spin splitting at the interface. By combining spin- and angle-resolved photoemission spectroscopy with density functional theory, we reveal that the electronic hybridization between the two different TMD monolayers gives rise to extended in-gap states with strong Rashba spin-orbit coupling. The choice of TMD layers enables to engineer the sign and strength of spin-to-charge conversion in van der Waals heterobilayers opening up perspectives to build efficient and tunable THz spintronic emitters.

cond-mat.mes-hall

An empirical approach to measuring interface energies in mixed-phase bismuth ferrite

In complex oxide heteroepitaxy, strain engineering is a powerful tool to obtain phases in thin films that may be otherwise unstable in bulk. A successful example of this approach is mixed phase bismuth ferrite (BiFeO3) epitaxial thin films. The coexistence of a tetragonal-like (T-like) matrix and rhombohedral-like (R-like) striations provides an enhanced electromechanical response, along with other attractive functional behaviors. In this paper, we compare the energetics associated with two thickness dependent strain relaxation mechanisms in this system: domain walls arising from monoclinic distortion in the T-like phase, and the interphase boundary between the host T-like matrix and tilted R-like phases. Combining x-ray diffraction measurements with scanning probe microscopy, we extract quantitative values using an empirical energy balance approach. The domain wall and phase boundary energies are found to be 113 $\pm$ 21 and 426 $\pm$ 23 mJ.m$^{-2}$, respectively. These numerical estimates will help us realize designer phase boundaries in multiferroics, which possess colossal responses to external stimuli, attractive for a diverse range of functional applications.

cond-mat.mtrl-sci

Super-R BiFeO$_3$: Epitaxial stabilization of a low-symmetry phase with giant electromechanical response

Piezoelectrics interconvert mechanical energy and electric charge and are widely used in actuators and sensors. The best performing materials are ferroelectrics at a morphotropic phase boundary (MPB), where several phases can intimately coexist. Switching between these phases by electric field produces a large electromechanical response. In the ferroelectric BiFeO$_3$, strain can be used to create an MPB-like phase mixture and thus to generate large electric field dependent strains. However, this enhanced response occurs at localized, randomly positioned regions of the film, which potentially complicates nanodevice design. Here, we use epitaxial strain and orientation engineering in tandem - anisotropic epitaxy - to craft a hitherto unavailable low-symmetry phase of BiFeO$_3$ which acts as a structural bridge between the rhombohedral-like and tetragonal-like polymorphs. Interferometric displacement sensor measurements and first-principle calculations reveal that under external electric bias, this phase undergoes a transition to the tetragonal-like polymorph, generating a piezoelectric response enhanced by over 200%, and associated giant field-induced reversible strain. These results offer a new route to engineer giant electromechanical properties in thin films, with broader perspectives for other functional oxide systems.

cond-mat.mtrl-sci