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1.
Adv Mater ; 36(23): e2312437, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38341379

ABSTRACT

Light is an effective tool to probe the polarization and domain distribution in ferroelectric materials passively, that is, non-invasively, for example, via optical second harmonic generation (SHG). With the emergence of oxide electronics, there is now a strong demand to expand the role of light toward active control of the polarization. In this work, optical control of the ferroelectric polarization is demonstrated in prototypical epitaxial PbZrxTi1-xO3 (PZT)-based heterostructures. This is accomplished in three steps, using above-bandgap UV light, while tracking the response of the polarization with optical SHG. First, it is found that UV-light exposure induces a transient enhancement or suppression of the ferroelectric polarization in films with an upward- or downward-oriented polarization, respectively. This behavior is attributed to a modified charge screening driven by the separation of photoexcited charge carriers at the Schottky interface of the ferroelectric thin film. Second, by taking advantage of this optical handle on electrostatics, remanent optical poling from a pristine multi-domain into a single-domain configuration is accomplished. Third, via thermal annealing or engineered electrostatic boundary conditions, a complete reversibility of the optical poling is further achieved. Hence, this work paves the way for the all-optical control of the spontaneous polarization in ferroelectric thin films.

2.
Faraday Discuss ; 237(0): 186-197, 2022 Sep 15.
Article in English | MEDLINE | ID: mdl-35687084

ABSTRACT

Recent advances in the field of THz spectroscopy allow for controlled experiments to measure signatures of collective excitations in the conventional s-wave superconductor in the fifth harmonic generation current (FHG). Here, we analyze this process theoretically within the Anderson pseudospin formalism and use a periodic multicycle pulse setup, where the driving electromagnetic field points in the direction of a lattice vector. We investigate the interplay of the Higgs mode contribution to the fifth harmonic generation current and compare it to other contributing mechanisms, such as charge density fluctuations (CDF). Similar to the third harmonic generating current we show that the signal in the FHG is also dominated by the CDF. Most importantly, we predict a double peak signature in the frequency dependence of the intensity amplitude of the FHG current with one peak located at Ω = Δ0 (4Ω = 4Δ0) and another one at Ω = Δ0/2 (4Ω = 2Δ0). The resonant enhancement in the latter case is indicative of the higher order coupling to the Higgs mode or CDF, while the former is reminiscent of the THG describing the coupling of CDF and the Higgs mode with 2 single photons.

3.
J Chem Phys ; 156(9): 094103, 2022 Mar 07.
Article in English | MEDLINE | ID: mdl-35259902

ABSTRACT

We investigate molecular plasmonic excitations sustained in hollow spherical gold nanoparticles using time-dependent density functional theory (TD-DFT). Specifically, we consider Au60 spherical, hollow molecules as a toy model for single-shell plasmonic molecules. To quantify the plasmonic character of the excitations obtained from TD-DFT, the energy-based plasmonicity index is generalized to the framework of DFT, validated on simple systems such as the sodium Na20 chain and the silver Ag20 compound, and subsequently successfully applied to more complex molecules. We also compare the quantum mechanical TD-DFT simulations to those obtained from a classical Mie theory that relies on macroscopic electrodynamics to model the light-matter interaction. This comparison allows us to distinguish those features that can be explained classically from those that require a quantum-mechanical treatment. Finally, a double-shell system obtained by placing a C60 buckyball inside the hollow spherical gold particle is further considered. It is found that the double-shell, while increasing the overall plasmonic character of the excitations, leads to significantly lowered absorption cross sections.

4.
J Health Psychol ; 27(7): 1635-1645, 2022 06.
Article in English | MEDLINE | ID: mdl-33198516

ABSTRACT

Among N = 165 14-22-year-old bearers of celiac disease (CD), the German-based study examined if participation in camps for children with CD is related to higher CD-related quality of life (CD-QoL); N = 48 of the study participants attended at least one camp. Camp participation was found to be related to higher CD-QoL, an effect mediated by having more friends with CD and by perceiving higher social support. Camp participation was also associated with higher illness acceptance and lower anxiety. Results show the potential benefits of recreational activities in CD treatment, to be further examined in experimental research.


Subject(s)
Celiac Disease , Quality of Life , Adolescent , Child , Diet, Gluten-Free , Humans , Social Support , Surveys and Questionnaires
5.
Adv Mater ; 33(52): e2104688, 2021 Dec.
Article in English | MEDLINE | ID: mdl-34606122

ABSTRACT

The functionalities of BiFeO3 -based magnetoelectric multiferroic heterostructures rely on the controlled manipulation of their ferroelectric domains and of the corresponding net in-plane polarization, as this aspect guides the voltage-controlled magnetic switching. Chemical substitution has emerged as a key to push the energy dissipation of the BiFeO3 into the attojoule range but appears to result in a disordered domain configuration. Using non-invasive optical second-harmonic generation on heavily La-substituted BiFeO3 films, it is shown that a weak net in-plane polarization remains imprinted in the pristine films despite the apparent domain disorder. It is found that this ingrained net in-plane polarization can be trained with out-of-plane electric fields compatible with applications. Operando studies on capacitor heterostructures treated in this way show the full restoration of the domain configuration of pristine BiFeO3 along with a giant net in-plane polarization enhancement. Thus, the experiments reveal a surprising robustness of the net in-plane polarization of BiFeO3 against chemical modification, an important criterion in ongoing attempts to integrate magnetoelectric materials into energy-efficient devices.

6.
J Appl Phys ; 129(9)2021.
Article in English | MEDLINE | ID: mdl-36575704

ABSTRACT

Plasmonic nanostructures attract tremendous attention as they confine electromagnetic fields well below the diffraction limit while simultaneously sustaining extreme local field enhancements. To fully exploit these properties, the identification and classification of resonances in such nanostructures is crucial. Recently, a novel figure of merit for resonance classification has been proposed1 and its applicability was demonstrated mostly to toy model systems. This novel measure, the energy-based plasmonicity index (EPI), characterizes the nature of resonances in molecular nanostructures. The EPI distinguishes between either a single-particle-like or a plasmonic nature of resonances based on the energy space coherence dynamics of the excitation. To advance the further development of this newly established measure, we present here its exemplary application to characterize the resonances of graphene nanoantennas. In particular, we focus on resonances in a doped nanoantenna. The structure is of interest, as a consideration of the electron dynamics in real space might suggest a plasmonic nature of selected resonances in the low doping limit but our analysis reveals the opposite. We find that in the undoped and moderately doped nanoantenna, the EPI classifies all emerging resonances as predominantly single-particle-like and only after doping the structure heavily, the EPI observes plasmonic response.

7.
Nat Commun ; 11(1): 1081, 2020 Feb 26.
Article in English | MEDLINE | ID: mdl-32102995

ABSTRACT

Modern high-resolution microscopes are commonly used to study specimens that have dense and aperiodic spatial structure. Extracting meaningful information from images obtained from such microscopes remains a formidable challenge. Fourier analysis is commonly used to analyze the structure of such images. However, the Fourier transform fundamentally suffers from severe phase noise when applied to aperiodic images. Here, we report the development of an algorithm based on nonconvex optimization that directly uncovers the fundamental motifs present in a real-space image. Apart from being quantitatively superior to traditional Fourier analysis, we show that this algorithm also uncovers phase sensitive information about the underlying motif structure. We demonstrate its usefulness by studying scanning tunneling microscopy images of a Co-doped iron arsenide superconductor and prove that the application of the algorithm allows for the complete recovery of quasiparticle interference in this material.

8.
Nat Commun ; 10(1): 4750, 2019 10 18.
Article in English | MEDLINE | ID: mdl-31628309

ABSTRACT

Recent reports of current-induced switching of ferrimagnetic oxides coupled to heavy metals have opened prospects for implementing magnetic insulators into electrically addressable devices. However, the configuration and dynamics of magnetic domain walls driven by electrical currents in insulating oxides remain unexplored. Here we investigate the internal structure of the domain walls in Tm3Fe5O12 (TmIG) and TmIG/Pt bilayers, and demonstrate their efficient manipulation by spin-orbit torques with velocities of up to 400 ms-1 and minimal current threshold for domain wall flow of 5 × 106 A cm-2. Domain wall racetracks are defined by Pt current lines on continuous TmIG films, which allows for patterning the magnetic landscape of TmIG in a fast and reversible way. Scanning nitrogen-vacancy magnetometry reveals that the domain walls of TmIG thin films grown on Gd3Sc2Ga3O12 exhibit left-handed Néel chirality, changing to an intermediate Néel-Bloch configuration upon Pt deposition. These results indicate the presence of interfacial Dzyaloshinskii-Moriya interaction in magnetic garnets, opening the possibility to stabilize chiral spin textures in centrosymmetric magnetic insulators.

9.
Nano Lett ; 19(9): 5930-5937, 2019 Sep 11.
Article in English | MEDLINE | ID: mdl-31419382

ABSTRACT

Memory and logic devices that encode information in magnetic domains rely on the controlled injection of domain walls to reach their full potential. In this work, we exploit the chiral coupling, which is induced by the Dzyaloshinskii-Moriya interaction, between in-plane and out-of-plane magnetized regions of a Pt/Co/AlOx trilayer in combination with current-driven spin-orbit torques to control the injection of domain walls into magnetic conduits. We demonstrate that the current-induced domain nucleation is strongly inhibited for magnetic configurations stabilized by the chiral coupling and promoted for those that have the opposite chirality. These configurations allow for efficient domain wall injection using current densities of the order of 4 × 1011 A m-2, which are lower than those used in other injection schemes. Furthermore, by setting the orientation of the in-plane magnetization using an external field, we demonstrate the use of a chiral domain wall injector to create a controlled sequence of alternating domains in a racetrack structure driven by a steady stream of unipolar current pulses.

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