Nonlinear optical diode effect in a magnetic Weyl semimetal.

Diode effects are of great interest for both fundamental physics and modern technologies. Electrical diode effects (nonreciprocal transport) have been observed in Weyl systems. Optical diode effects arising from the Weyl fermions have been theoretically considered but not probed experimentally. Here, we report the observation of a nonlinear optical diode effect (NODE) in the magnetic Weyl semimetal CeAlSi, where the magnetization introduces a pronounced directionality in the nonlinear optical second-harmonic generation (SHG). We demonstrate a six-fold change of the measured SHG intensity between opposite propagation directions over a bandwidth exceeding 250 meV. Supported by density-functional theory, we establish the linearly dispersive bands emerging from Weyl nodes as the origin of this broadband effect. We further demonstrate current-induced magnetization switching and thus electrical control of the NODE. Our results advance ongoing research to identify novel nonlinear optical/transport phenomena in magnetic topological materials and further opens new pathways for the unidirectional manipulation of light.

Origin of the Critical Thickness in Improper Ferroelectric Thin Films.

Improper ferroelectrics are expected to be more robust than conventional ferroelectrics against depolarizing field effects and to exhibit a much-desired absence of critical thickness. Recent studies, however, revealed the loss of ferroelectric response in epitaxial improper ferroelectric thin films. Here, we investigate improper ferroelectric hexagonal YMnO3 thin films and find that the polarization suppression, and hence functionality, in the thinner films is due to oxygen off-stoichiometry. We demonstrate that oxygen vacancies form on the film surfaces to provide the necessary charge to screen the large internal electric field resulting from the positively charged YMnO3 surface layers. Additionally, we show that by modifying the oxygen concentration of the films, the phase transition temperatures can be substantially tuned. We anticipate that our findings are also valid for other ferroelectric oxide films and emphasize the importance of controlling the oxygen content and cation oxidation states in ferroelectrics for their successful integration in nanoscale applications.

In situmonitoring of epitaxial ferroelectric thin-film growth.

In ferroelectric thin films, the polarization state and the domain configuration define the macroscopic ferroelectric properties such as the switching dynamics. Engineering of the ferroelectric domain configuration during synthesis is in permanent evolution and can be achieved by a range of approaches, extending from epitaxial strain tuning over electrostatic environment control to the influence of interface atomic termination. Exotic polar states are now designed in the technologically relevant ultrathin regime. The promise of energy-efficient devices based on ultrathin ferroelectric films depends on the ability to create, probe, and manipulate polar states in ever more complex epitaxial architectures. Because most ferroelectric oxides exhibit ferroelectricity during the epitaxial deposition process, the direct access to the polarization emergence and its evolution during the growth process, beyond the realm of existing structuralin situdiagnostic tools, is becoming of paramount importance. We review the recent progress in the field of monitoring polar states with an emphasis on the non-invasive probes allowing investigations of polarization during the thin film growth of ferroelectric oxides. A particular importance is given to optical second harmonic generationin situ. The ability to determine the net polarization and domain configuration of ultrathin films and multilayers during the growth of multilayers brings new insights towards a better understanding of the physics of ultrathin ferroelectrics and further control of ferroelectric-based heterostructures for devices.

Inversion-Symmetry Engineering in Layered Oxide Thin Films.

Inversion-symmetry breaking is a ubiquitous concept in condensed-matter science: It is a prerequisite for technologically relevant effects such as piezoelectricity, nonlinear optical properties, and spin-transport phenomena. It also determines abstract properties, like the electronic topology in quantum materials. Therefore, the creation of materials where inversion symmetry can be turned on or off by design may be a versatile approach for controlling parity-related functionalities. Here, we engineer inversion symmetry on a sub-unit-cell level in ultrathin hexagonal manganite films. Although an odd number of half-unit-cell layers breaks inversion symmetry, an even number of such layers remains centrosymmetric. Optical second harmonic generation as an inversion-symmetry-sensitive functionality is thus activated and deactivated on demand and at the same time used for in situ tracking of the symmetry state of our films. Symmetry engineering on the sub-unit-cell level thus suggests a new platform for controlled activation and deactivation of symmetry-governed functionalities in oxide-electronic epitaxial thin films.

Design and Manipulation of Ferroic Domains in Complex Oxide Heterostructures.

The current burst of device concepts based on nanoscale domain-control in magnetically and electrically ordered systems motivates us to review the recent development in the design of domain engineered oxide heterostructures. The improved ability to design and control advanced ferroic domain architectures came hand in hand with major advances in investigation capacity of nanoscale ferroic states. The new avenues offered by prototypical multiferroic materials, in which electric and magnetic orders coexist, are expanding beyond the canonical low-energy-consuming electrical control of a net magnetization. Domain pattern inversion, for instance, holds promises of increased functionalities. In this review, we first describe the recent development in the creation of controlled ferroelectric and multiferroic domain architectures in thin films and multilayers. We then present techniques for probing the domain state with a particular focus on non-invasive tools allowing the determination of buried ferroic states. Finally, we discuss the switching events and their domain analysis, providing critical insight into the evolution of device concepts involving multiferroic thin films and heterostructures.