skip to main content


Title: Emergence of the Vortex State in Confined Ferroelectric Heterostructures
Abstract

The manipulation of charge and lattice degrees of freedom in atomically precise, low‐dimensional ferroelectric superlattices can lead to exotic polar structures, such as a vortex state. The role of interfaces in the evolution of the vortex state in these superlattices (and the associated electrostatic and elastic boundary conditions they produce) has remained unclear. Here, the toroidal state, arranged in arrays of alternating clockwise/counterclockwise polar vortices, in a confined SrTiO3/PbTiO3/SrTiO3trilayer is investigated. By utilizing a combination of transmission electron microscopy, synchrotron‐based X‐ray diffraction, and phase‐field modeling, the phase transition as a function of layer thickness (number of unit cells) demonstrates how the vortex state emerges from the ferroelectric state by varying the thickness of the confined PbTiO3layer. Intriguingly, the vortex state arises at head‐to‐head domain boundaries in ferroelectrica1/a2twin structures. In turn, by varying the total number of PbTiO3layers (moving from trilayer to superlattices), it is possible to manipulate the long‐range interactions among multiple confined PbTiO3layers to stabilize the vortex state. This work provides a new understanding of how the different energies work together to produce this exciting new state of matter and can contribute to the design of novel states and potential memory applications.

 
more » « less
NSF-PAR ID:
10453800
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Materials
Volume:
31
Issue:
36
ISSN:
0935-9648
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Transition metal dichalcogenide (TMDC) moiré superlattices, owing to the moiré flatbands and strong correlation, can host periodic electron crystals and fascinating correlated physics. The TMDC heterojunctions in the type-II alignment also enable long-lived interlayer excitons that are promising for correlated bosonic states, while the interaction is dictated by the asymmetry of the heterojunction. Here we demonstrate a new excitonic state, quadrupolar exciton, in a symmetric WSe2-WS2-WSe2trilayer moiré superlattice. The quadrupolar excitons exhibit a quadratic dependence on the electric field, distinctively different from the linear Stark shift of the dipolar excitons in heterobilayers. This quadrupolar exciton stems from the hybridization of WSe2valence moiré flatbands. The same mechanism also gives rise to an interlayer Mott insulator state, in which the two WSe2layers share one hole laterally confined in one moiré unit cell. In contrast, the hole occupation probability in each layer can be continuously tuned via an out-of-plane electric field, reaching 100% in the top or bottom WSe2under a large electric field, accompanying the transition from quadrupolar excitons to dipolar excitons. Our work demonstrates a trilayer moiré system as a new exciting playground for realizing novel correlated states and engineering quantum phase transitions.

     
    more » « less
  2. Abstract

    Polar skyrmions are predicted to emerge from the interplay of elastic, electrostatic and gradient energies, in contrast to the key role of the anti-symmetric Dzyalozhinskii-Moriya interaction in magnetic skyrmions. Here, we explore the reversible transition from a skyrmion state (topological charge of −1) to a two-dimensional, tetratic lattice of merons (with topological charge of −1/2) upon varying the temperature and elastic boundary conditions in [(PbTiO3)16/(SrTiO3)16]8membranes. This topological phase transition is accompanied by a change in chirality, from zero-net chirality (in meronic phase) to net-handedness (in skyrmionic phase). We show how scanning electron diffraction provides a robust measure of the local polarization simultaneously with the strain state at sub-nm resolution, while also directly mapping the chirality of each skyrmion. Using this, we demonstrate strain as a crucial order parameter to drive isotropic-to-anisotropic structural transitions of chiral polar skyrmions to non-chiral merons, validated with X-ray reciprocal space mapping and phase-field simulations.

     
    more » « less
  3. Abstract

    Complex‐oxide superlattices provide a pathway to numerous emergent phenomena because of the juxtaposition of disparate properties and the strong interfacial interactions in these unit‐cell‐precise structures. This is particularly true in superlattices of ferroelectric and dielectric materials, wherein new forms of ferroelectricity, exotic dipolar textures, and distinctive domain structures can be produced. Here, relaxor‐like behavior, typically associated with the chemical inhomogeneity and complexity of solid solutions, is observed in (BaTiO3)n/(SrTiO3)n(n= 4–20 unit cells) superlattices. Dielectric studies and subsequent Vogel–Fulcher analysis show significant frequency dispersion of the dielectric maximum across a range of periodicities, with enhanced dielectric constant and more robust relaxor behavior for smaller periodn. Bond‐valence molecular‐dynamics simulations predict the relaxor‐like behavior observed experimentally, and interpretations of the polar patterns via 2D discrete‐wavelet transforms in shorter‐period superlattices suggest that the relaxor behavior arises from shape variations of the dipolar configurations, in contrast to frozen antipolar stripe domains in longer‐period superlattices (n= 16). Moreover, the size and shape of the dipolar configurations are tuned by superlattice periodicity, thus providing a definitive design strategy to use superlattice layering to create relaxor‐like behavior which may expand the ability to control desired properties in these complex systems.

     
    more » « less
  4. Abstract

    The ability to produce atomically precise, artificial oxide heterostructures allows for the possibility of producing exotic phases and enhanced susceptibilities not found in parent materials. Typical ferroelectric materials either exhibit large saturation polarization away from a phase boundary or large dielectric susceptibility near a phase boundary. Both large ferroelectric polarization and dielectric permittivity are attained wherein fully epitaxial (PbZr0.8Ti0.2O3)n/(PbZr0.4Ti0.6O3)2n(n= 2, 4, 6, 8, 16 unit cells) superlattices are produced such that the overall film chemistry is at the morphotropic phase boundary, but constitutive layers are not. Long‐ (n≥ 6) and short‐period (n= 2) superlattices reveal large ferroelectric saturation polarization (Ps= 64 µC cm−2) and small dielectric permittivity (εr≈ 400 at 10 kHz). Intermediate‐period (n= 4) superlattices, however, exhibit both large ferroelectric saturation polarization (Ps= 64 µC cm−2) and dielectric permittivity (εr= 776 at 10 kHz). First‐order reversal curve analysis reveals the presence of switching distributions for each parent layer and a third, interfacial layer wherein superlattice periodicity modulates the volume fraction of each switching distribution and thus the overall material response. This reveals that deterministic creation of artificial superlattices is an effective pathway for designing materials with enhanced responses to applied bias.

     
    more » « less
  5. The ferroelectric domain pattern within lithographically defined PbTiO 3 /SrTiO 3 ferroelectric/dielectric heteroepitaxial superlattice nanostructures is strongly influenced by the edges of the structures. Synchrotron X-ray nanobeam diffraction reveals that the spontaneously formed 180° ferroelectric stripe domains exhibited by such superlattices adopt a configuration in rectangular nanostructures in which domain walls are aligned with long patterned edges. The angular distribution of X-ray diffuse scattering intensity from nanodomains indicates that domains are aligned within an angular range of approximately 20° with respect to the edges. Computational studies based on a time-dependent Landau–Ginzburg–Devonshire model show that the preferred direction of the alignment results from lowering of the bulk and electrostrictive contributions to the free energy of the system due to the release of the lateral mechanical constraint. This unexpected alignment appears to be intrinsic and not a result of distortions or defects caused by the patterning process. Our work demonstrates how nanostructuring and patterning of heteroepitaxial superlattices allow for pathways to create and control ferroelectric structures that may appear counterintuitive. 
    more » « less