Persistent photoconductance is a phenomenon found in many semiconductors, by which light induces long-lived excitations in electronic states. Commonly, persistent photoexcitation leads to an increase of carriers (accumulation), though occasionally it can be negative (depletion). Here, we present the quantum well at the LaAlO_{3}/SrTiO_{3} interface, where in addition to photoinduced accumulation, a secondary photoexcitation enables carrier depletion. The balance between both processes is wavelength dependent, and allows tunable accumulation or depletion in an asymmetric manner, depending on the relative arrival time of photons of different frequencies. We use Green's function formalism to describe this unconventional photoexcitation, which paves the way to an optical implementation of neurobiologically inspired spike-timing-dependent plasticity.
Oxide growth with semiconductor-like accuracy allows the fabrication of atomically precise thin films and interfaces displaying a wide range of phases and functionalities that are absent in the corresponding oxide bulk materials. Among the other properties it was found that a two-dimensional electronic gas is formed under some circumstances at the LaAlO3/SrTiO3(0 0 1) interface separating two typical insulating perovskite crystals. The origin of this conducting state has been discussed at length, since different doping mechanisms can act in these material systems. Many experimental results point to the so-called polar catastrophe scenario as the principal mechanism driving the formation of the two-dimensional electronic gas. According to this mechanism, the existence of an interfacial polar discontinuity is the key ingredient to drive an electronic reconstruction at the LaAlO3/SrTiO3(0 0 1) interface and the consequent formation of a two-dimensional electron gas. This simple picture has been often questioned by the existence of material systems whose interface are predicted being non-polar according to the simplistic 'ionic' limit but that display an electrical behavior analogous to that of LaAlO3/SrTiO3(0 0 1) interfaces. This is the case of the LaAlO3/SrTiO3(1 1 0), i.e., a LaAlO3/SrTiO3 interface with a different in-plane orientation. It is evident that to solve such kind of controversies a detailed investigation of the polar or non-polar state of these interfaces is needed, although this is not simple for the lack of experimental tools that are specifically sensitive to interfacial polarity. Here we apply Optical Second Harmonic Generation to investigate LaAlO3/SrTiO3 interfaces with different in-plane orientations to bridge this gap. By comparing our results with recent theoretical findings, we will arrive to the conclusion that the real LaAlO3/SrTiO3(1 1 0) interface is strongly polar.
Photonic crystals are periodic nanostructures that can support a variety of confined electromagnetic modes. Such confined modes are usually accompanied by local enhancement of electric field intensity that strengthens light-matter interactions, enabling applications such as surface-enhanced Raman scattering (SERS) and surface plasmon enhanced sensing. In the presence of magneto-optically active materials, the local field enhancement gives rise to anomalous magneto-optical activity. Typically, the confined modes of a given photonic crystal depend strongly on the wavelength and incidence angle of the incident electromagnetic radiation. Thus, spectral and angular-resolved measurements are needed to fully identify them as well as to establish their relationship with the magneto-optical activity of the crystal. In this article, we describe how to use a Fourier-plane (back focal plane) microscope to characterize magneto-optically active samples. As a model system, here we use a plasmonic grating built out of magneto-optically active Au/Co/Au multilayer. In the experiments, we apply a magnetic field on the grating in situ and measure its reciprocal space response, obtaining the magneto-optical response of the grating over a range of wavelengths and incident angles. This information enables us to build a complete map of the plasmonic band structure of the grating and the angle and wavelength dependent magneto-optical activity. These two images allow us to pinpoint the effect that the plasmon resonances have on the magneto-optical response of the grating. The relatively small magnitude of magneto-optical effects requires a careful treatment of the acquired optical signals. To this end, an image processing protocol for obtaining magneto-optical response from the acquired raw data is laid out.
Nanostructures , Crystallization , Electromagnetic Phenomena , Nanostructures/chemistry , Optical Phenomena
Strontium titanate (SrTiO_{3}) is the quintessential material for oxide electronics. One of its hallmark features is the transition, driven by antiferrodistortive (AFD) lattice modes, from a cubic to a ferroelastic low-temperature phase. Here we investigate the evolution of the ferroelastic twin walls upon application of an electric field. Remarkably, we find that the dielectric anisotropy of tetragonal SrTiO_{3}, rather than the intrinsic domain wall polarity, is the main driving force for the motion of the twins. Based on a combined first-principles and Landau-theory analysis, we show that such anisotropy is dominated by a trilinear coupling between the polarization, the AFD lattice tilts, and a previously overlooked antiferroelectric (AFE) mode. We identify the latter AFE phonon with the so-called "R mode" at â¼440 cm^{-1}, which was previously detected in IR experiments, but whose microscopic nature was unknown.
Phase-matching conditions-used to bridge the wave vector mismatch between light and surface plasmon polaritons (SPPs)-have been exploited recently to enable nonreciprocal optical propagation and enhanced magneto-optic responses in magnetoplasmonic systems. Here we show that using diffraction in conjunction with plasmon excitations leads to a photonic system with a more versatile and flexible response. As a testbed, we analyzed diffracted magneto-optical effects in magnetoplasmonic gratings, where broken time-reversal symmetry induces frequency shifts in the energy and angular spectra of plasmon resonance. These result in exceptionally large responses in the diffracted magneto-optical effect. The concepts presented here can be used to develop non-reciprocal optical devices that exploit diffraction, in order to achieve tailored electromagnetic responses.
The multifunctional (ferromagnetic and ferroelectric) response at room temperature that is elusive in single phase multiferroic materials can be achieved in a proper combination of ferroelectric perovskites and ferrimagnetic spinel oxides in horizontal heterostructures. In this work, lead-free CoFe2O4/BaTiO3 bilayers are integrated with Si(001) using LaNiO3/CeO2/YSZ as a tri-layer buffer. They present structural and functional properties close to those achieved on perovskite substrates: the bilayers are fully epitaxial with extremely flat surface, and exhibit robust ferromagnetism and ferroelectricity at room temperature.
We have uncovered a giant gyrotropic magneto-optical response for doped ferromagnetic manganite La_{2/3}Ca_{1/3}MnO_{3} around the near room-temperature paramagnetic-to-ferromagnetic transition. At odds with current wisdom, where this response is usually assumed to be fundamentally fixed by the electronic band structure, we point to the presence of small polarons as the driving force for this unexpected phenomenon. We explain the observed properties by the intricate interplay of mobility, Jahn-Teller effect, and spin-orbit coupling of small polarons. As magnetic polarons are ubiquitously inherent to many strongly correlated systems, our results provide an original, general pathway towards the generation of magnetic-responsive gigantic gyrotropic responses that may open novel avenues for magnetoelectric coupling beyond the conventional modulation of magnetization.
Magnetoelectric coupling at multiferroic interfaces is a promising route toward the nonvolatile electric-field control of magnetization. Here, we use optical measurements to study the static and dynamic variations of the interface magnetization induced by an electric field in Co/PbZr0.2Ti0.8O3 (Co/PZT) bilayers at room temperature. The measurements allow us to identify different coupling mechanisms. We further investigate the local electronic and magnetic structure of the interface by means of transmission electron microscopy, soft X-ray magnetic circular dichroism, and density functional theory to corroborate the coupling mechanism. The measurements demonstrate a mixed linear and quadratic optical response to the electric field, which results from a magneto-electro-optical effect. We propose a decomposition method of the optical signal to discriminate between different components involved in the electric field-induced polarization rotation of the reflected light. This allows us to extract a signal that we can ascribe to interface magnetoelectric coupling. The associated surface magnetization exhibits a clear hysteretic variation of odd symmetry with respect to the electric field and nonzero remanence. The interface coupling is remarkably stable over a wide frequency range (1-50 kHz), and the application of a bias magnetic field is not necessary for the coupling to occur. These results show the potential of exploiting interface coupling with the prospect of optimizing the performance of magnetoelectric memory devices in terms of stability, as well as fast and dissipationless operation.
We have imaged optically the spatial distributions of ferroelectricity and piezoelectricity at the diffraction limit. Contributions to the birefringence from electro-optics--linked to ferroelectricity--as well as strain--arising from converse piezoelectric effects--have been recorded simultaneously in a BaTiO3 thin film. The concurrent recording of electro-optic and piezo-optic mappings revealed that, far from the ideal uniformity, the ferroelectric and piezoelectric responses were strikingly inhomogeneous, exhibiting significant fluctuations over the scale of the micrometer. The optical methods here described are appropriate to study the variations of these properties simultaneously, which are of great relevance when ferroelectrics are downscaled to small sizes for applications in data storage and processing.
The discovery of two-dimensional electron gases (2DEGs) at oxide interfaces-involving electrons in narrow d-bands-has broken new ground, enabling the access to correlated states that are unreachable in conventional semiconductors based on s- and p- electrons. There is a growing consensus that emerging properties at these novel quantum wells-such as 2D superconductivity and magnetism-are intimately connected to specific orbital symmetries in the 2DEG sub-band structure. Here we show that crystal orientation allows selective orbital occupancy, disclosing unprecedented ways to tailor the 2DEG properties. By carrying out electrostatic gating experiments in LaAlO3/SrTiO3 wells of different crystal orientations, we show that the spatial extension and anisotropy of the 2D superconductivity and the Rashba spin-orbit field can be largely modulated by controlling the 2DEG sub-band filling. Such an orientational tuning expands the possibilities for electronic engineering of 2DEGs at LaAlO3/SrTiO3 interfaces.
We report on an extremely fast and versatile synthetic approach, based on microwave assisted sol-gel chemistry, that allows a conformal nanometric coating of intricate three-dimensional structures. Using this methodology, we have achieved a conformal coverage of large areas of three-dimensional opals with a superparamagnetic manganese ferrite layer, yielding magneto-photonic crystals with excellent quality. The use of a ternary oxide for the ultrathin coating demonstrates the potential of this methodology to realize three-dimensional structures with complex materials that may find applications beyond photonics, such as energy, sensing or catalysis.
Crystallization/methods , Nanostructures/chemistry , Nanostructures/ultrastructure , Light , Macromolecular Substances/chemistry , Magnetics , Materials Testing , Molecular Conformation , Particle Size , Surface Properties
Three-dimensional magnetophotonic crystals (3D-MPCs) are being postulated as appropriate platforms to tailor the magneto-optical spectral response of magnetic materials and to incorporate this functionality in a new generation of optical devices. By infiltrating self-assembled inverse opal structures with monodisperse nickel nanoparticles we have fabricated 3D-MPCs that show a sizable enhancement of the magneto-optical signal at frequencies around the stop-band edges of the photonic crystals. We have established a proper methodology to disentangle the intrinsic magneto-optical spectra from the nonmagnetic optical activity of the 3D-MPCs. The results of the optical and magneto-optical characterization are consistent with a homogeneous magnetic infiltration of the opal structure that gives rise to both a red-shift of the optical bandgap and a modification of the magneto-optical spectral response due to photonic bandgap effects. The results of our investigation demonstrate the potential of 3D-MPCs fabricated following the approach outlined here and offer opportunities to adapt the magneto-optical spectral response at optical frequencies by appropriate design of the opal structure or magnetic field strength.
We report here on a fast magneto-optical characterization method for colloidal liquid dispersions of magnetic nanoparticles. We have applied our methodology to Ni nanoparticles with size equal or below 15 nm synthesized by a ligand stabilized solution-phase synthesis. We have measured the magnetic circular dichroism (MCD) of colloidal dispersions and found that we can probe the intrinsic magnetic properties within a wide concentration range, from 10(-5) up to 10(-2) M, with sensitivity to concentrations below 1 microg/mL of magnetic Ni particles. We found that the measured MCD signal scales up with the concentration thus providing a means of determining the concentration values of highly diluted dispersions. The methodology presented here exhibits large flexibility and versatility and might be suitable to study either fundamental problems related to properties of nanosize particles including surface related effects which are highly relevant for magnetic colloids in biomedical applications or to be applied to in situ testing and integration in production lines.
Colloids/chemistry , Metal Nanoparticles/chemistry , Nickel/chemistry , Circular Dichroism , Magnetics , Nanotechnology
