Giant conductivity of mobile non-oxide domain walls.

Atomically sharp domain walls in ferroelectrics are considered as an ideal platform to realize easy-to-reconfigure nanoelectronic building blocks, created, manipulated and erased by external fields. However, conductive domain walls have been exclusively observed in oxides, where domain wall mobility and conductivity is largely influenced by stoichiometry and defects. Here, we report on giant conductivity of domain walls in the non-oxide ferroelectric GaV4S8. We observe conductive domain walls forming in zig-zagging structures, that are composed of head-to-head and tail-to-tail domain wall segments alternating on the nanoscale. Remarkably, both types of segments possess high conductivity, unimaginable in oxide ferroelectrics. These effectively 2D domain walls, dominating the 3D conductance, can be mobilized by magnetic fields, triggering abrupt conductance changes as large as eight orders of magnitude. These unique properties demonstrate that non-oxide ferroelectrics can be the source of novel phenomena beyond the realm of oxide electronics.

Interconversion of multiferroic domains and domain walls.

Systems with long-range order like ferromagnetism or ferroelectricity exhibit uniform, yet differently oriented three-dimensional regions called domains that are separated by two-dimensional topological defects termed domain walls. A change of the ordered state across a domain wall can lead to local non-bulk physical properties such as enhanced conductance or the promotion of unusual phases. Although highly desirable, controlled transfer of these properties between the bulk and the spatially confined walls is usually not possible. Here, we demonstrate this crossover by confining multiferroic Dy0.7Tb0.3FeO3 domains into multiferroic domain walls at an identified location within a non-multiferroic environment. This process is fully reversible; an applied magnetic or electric field controls the transformation. Aside from expanding the concept of multiferroic order, such interconversion can be key to addressing antiferromagnetic domain structures and topological singularities.

The ultrathin limit of improper ferroelectricity.

The secondary nature of polarization in improper ferroelectrics promotes functional properties beyond those of conventional ferroelectrics. In technologically relevant ultrathin films, however, the improper ferroelectric behavior remains largely unexplored. Here, we probe the emergence of the coupled improper polarization and primary distortive order parameter in thin films of hexagonal YMnO3. Combining state-of-the-art in situ characterization techniques separately addressing the improper ferroelectric state and its distortive driving force, we reveal a pronounced thickness dependence of the improper polarization, which we show to originate from the strong modification of the primary order at epitaxial interfaces. Nanoscale confinement effects on the primary order parameter reduce the temperature of the phase transition, which we exploit to visualize its order-disorder character with atomic resolution. Our results advance the understanding of the evolution of improper ferroelectricity within the confinement of ultrathin films, which is essential for their successful implementation in nanoscale applications.

Depolarizing-Field Effects in Epitaxial Capacitor Heterostructures.

We identify a transient enhancement of the depolarizing field, leading to an unexpected quench of net polarization, during the growth of a prototypical metal-ferroelectric-metal epitaxial system made of BaTiO_{3} and SrRuO_{3}. Reduced conductivity and, hence, charge screening efficiency in the early growth stage of the SrRuO_{3} top electrode promotes a breakdown of ferroelectric BaTiO_{3} into domains. We demonstrate how a thermal annealing procedure can recover the single-domain state. By tracking the polarization state in situ, using optical second harmonic generation, we bring new understanding to interface-related electrostatic effects in ferroelectric capacitors.

Fermi Volume Evolution and Crystal-Field Excitations in Heavy-Fermion Compounds Probed by Time-Domain Terahertz Spectroscopy.

We measure the quasiparticle weight in the heavy-fermion compound CeCu_{6-x}Au_{x} (x=0, 0.1) by time-resolved terahertz spectroscopy for temperatures from 2 up to 300 K. This method distinguishes contributions from the heavy Kondo band and from the crystal-electric-field satellite bands by different terahertz response delay times. We find that the formation of heavy bands is controlled by an exponentially enhanced, high-energy Kondo scale once the crystal-electric-field states become thermally occupied. We corroborate these observations by temperature-dependent dynamical mean-field calculations for the multiorbital Anderson lattice model and discuss consequences for quantum-critical scenarios.

Publisher Correction: Magnetoelectric inversion of domain patterns.

Four incorrect figure citations in this Letter have been corrected online.

Magnetoelectric inversion of domain patterns.

The inversion of inhomogeneous physical states has great technological importance; for example, active noise reduction relies on the emission of an inverted sound wave that interferes destructively with the noise of the emitter1, and inverting the evolution of a spin system by using a magnetic-field pulse enables magnetic resonance tomography2. In contrast to these examples, inversion of a distribution of ferromagnetic or ferroelectric domains within a material is surprisingly difficult: field poling creates a single-domain state, and piece-by-piece inversion using a scanning tip is impractical. Here we report inversion of entire ferromagnetic and ferroelectric domain patterns in the magnetoelectric material Co3TeO6 and the multiferroic material Mn2GeO4, respectively. In these materials, an applied magnetic field reverses the magnetization or polarization, respectively, of each domain, but leaves the domain pattern intact. Landau theory indicates that this type of magnetoelectric inversion is universal across materials that exhibit complex ordering, with one order parameter holding the memory of the domain structure and another setting its overall sign. Domain-pattern inversion is only one example of a previously unnoticed effect in systems such as multiferroics, in which several order parameters are available for combination. Exploring these effects could therefore advance multiferroics towards new levels of functionality.

Conductivity Contrast and Tunneling Charge Transport in the Vortexlike Ferroelectric Domain Patterns of Multiferroic Hexagonal YMnO_{3}.

We deduce the intrinsic conductivity properties of the ferroelectric domain walls around the topologically protected domain vortex cores in multiferroic YMnO_{3}. This is achieved by performing a careful equivalent-circuit analysis of dielectric spectra measured in single-crystalline samples with different vortex densities. The conductivity contrast between the bulk domains and the less conducting domain boundaries is revealed to reach up to a factor of 500 at room temperature, depending on the sample preparation. Tunneling of localized defect charge carriers is the dominant charge-transport process in the domain walls that are depleted of mobile charge carriers. This work demonstrates that, via equivalent-circuit analysis, dielectric spectroscopy can provide valuable information on the intrinsic charge-transport properties of ferroelectric domain walls, which is of high relevance for the design of new domain-wall-based microelectronic devices.

Terahertz-Driven Nonlinear Spin Response of Antiferromagnetic Nickel Oxide.

Terahertz magnetic fields with amplitudes of up to 0.4 Tesla drive magnon resonances in nickel oxide while the induced dynamics is recorded by femtosecond magneto-optical probing. We observe distinct spin-mediated optical nonlinearities, including oscillations at the second harmonic of the 1 THz magnon mode. The latter originate from coherent dynamics of the longitudinal component of the antiferromagnetic order parameter, which are probed by magneto-optical effects of second order in the spin deflection. These observations allow us to dynamically disentangle electronic from lattice-related contributions to magnetic linear birefringence and dichroism-information so far only accessible by ultrafast THz spin control. The nonlinearities discussed here foreshadow physics that will become essential in future subcycle spin switching.

Functional ferroic heterostructures with tunable integral symmetry.

The relation between symmetry and functionality was pinpointed by Pierre Curie who stated that it is the symmetry breaking that creates physical properties. This fundamental principle is nowadays used for engineering heterostructures whose integral symmetry leads to exotic phenomena such as one-way transparency. For switching devices, however, such symmetry-related functionalities cannot be used because the symmetry in conventional heterostructures is immutable once the material has been synthesized. Here we demonstrate a concept for post-growth symmetry control in PbZr0.2Ti0.8O3 and BiFeO3-based heterostructures. A conducting oxide is sandwiched between two ferroelectric layers, and inversion symmetry is reversibly switched on or off by layer-selective electric-field poling. The generalization of our approach to other materials and symmetries is discussed. We thus establish ferroic trilayer structures as device components with reversibly tunable symmetry and demonstrate their use as light emitters that can be activated and deactivated by applying moderate electric voltages.

Piezoresponse force microscopy at sub-room temperatures.

Piezoresponse force microscopy is demonstrated at temperatures between -80 °C and +120 °C using a commercial room temperature atomic force microscope upgraded with a home-built cooling/heating-stage. We applied temperature-ramp-synchronized piezoresponse force microscope (PFM) for tracing the temperature dependence of the formation of ferroelectric domains. The potential of our sub-room temperature PFM is demonstrated by investigating the formation and evolution of ferroelectric domains in RbHSO4 as a function of temperature and time, respectively.

Anisotropic conductance at improper ferroelectric domain walls.

Transition metal oxides hold great potential for the development of new device paradigms because of the field-tunable functionalities driven by their strong electronic correlations, combined with their earth abundance and environmental friendliness. Recently, the interfaces between transition-metal oxides have revealed striking phenomena, such as insulator-metal transitions, magnetism, magnetoresistance and superconductivity. Such oxide interfaces are usually produced by sophisticated layer-by-layer growth techniques, which can yield high-quality, epitaxial interfaces with almost monolayer control of atomic positions. The resulting interfaces, however, are fixed in space by the arrangement of the atoms. Here we demonstrate a route to overcoming this geometric limitation. We show that the electrical conductance at the interfacial ferroelectric domain walls in hexagonal ErMnO(3) is a continuous function of the domain wall orientation, with a range of an order of magnitude. We explain the observed behaviour using first-principles density functional and phenomenological theories, and relate it to the unexpected stability of head-to-head and tail-to-tail domain walls in ErMnO(3) and related hexagonal manganites. As the domain wall orientation in ferroelectrics is tunable using modest external electric fields, our finding opens a degree of freedom that is not accessible to spatially fixed interfaces.

How do long-term development and periodical changes of river-floodplain systems affect the fate of contaminants? Results from European rivers.

In many densely populated areas, riverine floodplains have been strongly impacted and degraded by river channelization and flood protection dikes. Floodplains act as buffers for flood water and as filters for nutrients and pollutants carried with river water and sediment from upstream source areas. Based on results of the EU-funded "AquaTerra" project (2004-2009), we analyze changes in the dynamics of European river-floodplain systems over different temporal scales and assess their effects on contaminant behaviour and ecosystem functioning. We find that human-induced changes in the hydrologic regime of rivers have direct and severe consequences on nutrient cycling and contaminant retention in adjacent floodplains. We point out the complex interactions of contaminants with nutrient availability and other physico-chemical characteristics (pH, organic matter) in determining ecotoxicity and habitat quality, and draw conclusions for improved floodplain management.

Observation and coupling of domains in a spin-spiral multiferroic.

The coexistence, coupling, and manipulation of magnetic spiral domains and magnetically induced ferroelectric domains are spatially resolved by optical second harmonic generation in multiferroic MnWO4. Eight types of magnetic domains couple to two ferroelectric domains. An electric field uniquely creates a magnetic single-domain state. A magnetic field quenches the spontaneous polarization while retaining its magnetic origin so that the ferroelectric domains are concealed instead of destroyed.

Anisotropy of antiferromagnetic 180 degrees domains in LiCoPO4 and LiNiPO4.

Unexpected three-dimensional distributions of antiferromagnetic 180 degrees domains are observed in LiCoPO4 and LiNiPO4 by optical second harmonic generation. Domains in LiCoPO4 are isotropic in spite of the quasi-two-dimensional magnetic structure whereas domains in LiNiPO4 are distinctly anisotropic, but in contrast to the anisotropy of the magnetic structure. The diversity reveals a potential for fine-tuning magnetic properties determined by the distribution of domains or domain walls and the urgent need for an improved understanding of spatial correlations in antiferromagnets.

Ultrafast exciton relaxation in microcrystalline pentacene films.

The exciton dynamics in microcrystalline pentacene films is investigated by transient absorption measurements with 30 fs time resolution. It is found that the emission from photoexcited Frenkel excitons decays within 70 fs due to the ultrafast formation of an excitonic species with a strongly reduced transition dipole to the ground state and an absorption dipole in the plane of the film. We propose that an excimer exciton is formed and stabilized by changes of the local crystal structure. The subsequent dynamics is dominated by diffusion controlled annihilation and trapping.

Ultrafast manipulation of antiferromagnetism of NiO.

Photoexcitation of antiferromagnetic NiO leads to ultrafast reorientation of Ni2+ spins due to change of the magnetic anisotropy. Recovery of the magnetic ground state occurs as coherent oscillation of the antiferromagnetic order parameter between hard- and easy-axis states manifesting itself as quantum beating. The coherence time is approximately 1 ns with the beating frequency being determined by the anisotropy energy.

Magnetic-field induced second harmonic generation in CuB2O4.

Three types of optical magnetic-field induced second harmonic (MFISH) generation are observed in CuB2O4. Unusually sharp and intense electronic transitions in MFISH and linear absorption spectra provide selective access to the two nonequivalent Cu2+ sublattices. The magnetic phase diagram for both sublattices is determined by MFISH. Magnetic structure is dominated by antiferromagnetic order at the 4b site. Sublattice interactions transfer it to the 8d site where it coexists with a discoupled paramagnetic component.

Structure and interaction of antiferromagnetic domain walls in hexagonal YMnO3.

The structure of antiferromagnetic (AFM) domain walls and their interaction with lattice strain are derived taking the multiple-order-parameter compound YMnO3 as a model example. Contrary to the conviction that AFM domain walls are energetically unfavorable, their interaction with lattice strain lowers the total energy of the system and leads to a piezomagnetic clamping of the electric and magnetic order parameters in good agreement with the available experimental data.

Observation of coupled magnetic and electric domains.

Ferroelectromagnets are an interesting group of compounds that complement purely (anti-)ferroelectric or (anti-)ferromagnetic materials--they display simultaneous electric and magnetic order. With this coexistence they supplement materials in which magnetization can be induced by an electric field and electrical polarization by a magnetic field, a property which is termed the magnetoelectric effect. Aside from its fundamental importance, the mutual control of electric and magnetic properties is of significant interest for applications in magnetic storage media and 'spintronics'. The coupled electric and magnetic ordering in ferroelectromagnets is accompanied by the formation of domains and domain walls. However, such a cross-correlation between magnetic and electric domains has so far not been observed. Here we report spatial maps of coupled antiferromagnetic and ferroelectric domains in YMnO3, obtained by imaging with optical second harmonic generation. The coupling originates from an interaction between magnetic and electric domain walls, which leads to a configuration that is dominated by the ferroelectromagnetic product of the order parameters.