Myung-Geun Han

Ferroelectric order in individual nanometre-scale crystals

Ferroelectricity in finite-dimensional systems continues to arouse interest, motivated by predictions of vortex polarization states and the utility of ferroelectric nanomaterials in memory devices, actuators and other applications. Critical to these areas of research are the nanoscale polarization structure and scaling limit of ferroelectric order, which are determined here in individual nanocrystals comprising a single ferroelectric domain. Maps of ferroelectric structural distortions obtained from aberration-corrected transmission electron microscopy, combined with holographic polarization imaging, indicate the persistence of a linearly ordered and monodomain polarization state at nanometre dimensions. Room-temperature polarization switching is demonstrated down to ~5 nm dimensions. Ferroelectric coherence is facilitated in part by control of particle morphology, which along with electrostatic boundary conditions is found to determine the spatial extent of cooperative ferroelectric distortions. This work points the way to multi-Tbit/in(2) memories and provides a glimpse of the structural and electrical manifestations of ferroelectricity down to its ultimate limits.

Ferroelectric Switching Dynamics of Topological Vortex Domains in a Hexagonal Manganite

Field-induced switching of ferroelectric domains with a topological vortex configuration is studied by atomic imaging and electrical biasing in an electron microscope, revealing the role of topological defects on the topologically-guided change of domain-wall pairs in a hexagonal manganite.

Interface-induced nonswitchable domains in ferroelectric thin films

Engineering domains in ferroelectric thin films is crucial for realizing technological applications including non-volatile data storage and solar energy harvesting. Size and shape of domains strongly depend on the electrical and mechanical boundary conditions. Here we report the origin of nonswitchable polarization under external bias that leads to energetically unfavourable head-to-head domain walls in as-grown epitaxial PbZr(0.2)Ti(0.8)O3 thin films. By mapping electrostatic potentials and electric fields using off-axis electron holography and electron-beam-induced current with in situ electrical biasing in a transmission electron microscope, we show that electronic band bending across film/substrate interfaces locks local polarization direction and further produces unidirectional biasing fields, inducing nonswitchable domains near the interface. Presence of oxygen vacancies near the film surface, as revealed by electron-energy loss spectroscopy, stabilizes the charged domain walls. The formation of charged domain walls and nonswitchable domains reported in this study can be an origin for imprint and retention loss in ferroelectric thin films.

Record Surface State Mobility and Quantum Hall Effect in Topological Insulator Thin Films via Interface Engineering

Material defects remain as the main bottleneck to the progress of topological insulators (TIs). In particular, efforts to achieve thin TI samples with dominant surface transport have always led to increased defects and degraded mobilities, thus making it difficult to probe the quantum regime of the topological surface states. Here, by utilizing a novel buffer layer scheme composed of an In2Se3/(Bi0.5In0.5)2Se3 heterostructure, we introduce a quantum generation of Bi2Se3 films with an order of magnitude enhanced mobilities than before. This scheme has led to the first observation of the quantum Hall effect in Bi2Se3.

Origin of 90° domain wall pinning in Pb(Zr0.2Ti0.8)O3 heteroepitaxial thin films

We describe a transmission-electron-microscopy study of the ferroelectric domains in an epitaxial Pb(Zr0.2Ti0.8)O3 (PZT) film grown on La0.7Sr0.3MnO3/SrTiO3(001). We directly observe the pinning of 90° domain walls by pairs of misfit dislocations, respectively, with Burgers vectors a [100] and a [001]. Model calculations based on the elastic theory confirm our finding that, in addition to the depolarization field surrounding the dislocation, the strain field of misfit dislocation-pairs plays the primary role in the formation and pinning of a domains.

Unfolding of Vortices into Topological Stripes in a Multiferroic Material

Multiferroic hexagonal RMnO(3) (R=rare earths) crystals exhibit dense networks of vortex lines at which six domain walls merge. While the domain walls can be readily moved with an applied electric field, the vortex cores so far have been impossible to control. Our experiments demonstrate that shear strain induces a Magnus-type force pulling vortices and antivortices in opposite directions and unfolding them into a topological stripe domain state. We discuss the analogy between this effect and the current-driven dynamics of vortices in superconductors and superfluids.

Robust topological surface states of Bi2Se3 thin films on amorphous SiO2/Si substrate and a large ambipolar gating effect

The recent emergence of topological insulators (TI) has spurred intensive efforts to grow TI thin films on various substrates. However, little is known about how robust the topological surface states (TSS) are against disorders and other detrimental effects originating from the substrates. Here, we report the observation of a well-defined TSS on Bi2Se3 films grown on amorphous SiO2 (a-SiO2) substrates and a large gating effect on these films using the underneath doped-Si substrate as the back gate. The films on a-SiO2 were composed of c-axis ordered but random in-plane domains. However, despite the in-plane randomness induced by the amorphous substrate, the transport properties of these films were superior to those of similar films grown on single-crystalline Si(111) substrates, which are structurally better matched but chemically reactive with the films. This work sheds light on the importance of chemical compatibility, compared to lattice matching, for the growth of TI thin films, and also demonstrates ...

Hollandites as a new class of multiferroics

Discovery of new complex oxides that exhibit both magnetic and ferroelectric properties is of great interest for the design of functional magnetoelectrics, in which research is driven by the technologically exciting prospect of controlling charges by magnetic fields and spins by applied voltages, for sensors, 4-state logic, and spintronics. Motivated by the notion of a tool-kit for complex oxide design, we developed a chemical synthesis strategy for single-phase multifunctional lattices. Here, we introduce a new class of multiferroic hollandite Ba-Mn-Ti oxides not apparent in nature. BaMn3Ti4O14.25, designated BMT-134, possesses the signature channel-like hollandite structure, contains Mn4+ and Mn3+ in a 1:1 ratio, exhibits an antiferromagnetic phase transition (TN ~ 120 K) with a weak ferromagnetic ordering at lower temperatures, ferroelectricity, a giant dielectric constant at low frequency and a stable intrinsic dielectric constant of ~200 (1-100 MHz). With evidence of correlated antiferromagnetic and ferroelectric order, the findings point to an unexplored family of structures belonging to the hollandite supergroup with multifunctional properties, and high potential for developing new magnetoelectric materials.

Magnetoelectricity in CoFe2O4 nanocrystal-P(VDF-HFP) thin films

Transition metal ferrites such as CoFe2O4, possessing a large magnetostriction coefficient and high Curie temperature (Tc > 600 K), are excellent candidates for creating magnetic order at the nanoscale and provide a pathway to the fabrication of uniform particle-matrix films with optimized potential for magnetoelectric coupling. Here, a series of 0–3 type nanocomposite thin films composed of ferrimagnetic cobalt ferrite nanocrystals (8 to 18 nm) and a ferroelectric/piezoelectric polymer poly(vinylidene fluoride-co-hexafluoropropene), P(VDF-HFP), were prepared by multiple spin coating and cast coating over a thickness range of 200 nm to 1.6 μm. We describe the synthesis and structural characterization of the nanocrystals and composite films by XRD, TEM, HRTEM, STEM, and SEM, as well as dielectric and magnetic properties, in order to identify evidence of cooperative interactions between the two phases. The CoFe2O4 polymer nanocomposite thin films exhibit composition-dependent effective permittivity, loss tangent, and specific saturation magnetization (Ms). An enhancement of the effective permittivity and saturation magnetization of the CoFe2O4-P(VDF-HFP) films was observed and directly compared with CoFe2O4-polyvinylpyrrolidone, a non-ferroelectric polymer-based nanocomposite prepared by the same method. The comparison provided evidence for the observation of a magnetoelectric effect in the case of CoFe2O4-P(VDF-HFP), attributed to a magnetostrictive/piezoelectric interaction. An enhancement of Ms up to +20.7% was observed at room temperature in the case of the 10 wt.% CoFe2O4-P(VDF-HFP) sample.

Topologically Allowed Nonsixfold Vortices in a Sixfold Multiferroic Material: Observation and Classification

We report structural transformation of sixfold vortex domains into two-, four-, and eightfold vortices via a different type of topological defect in hexagonal manganites. Combining high-resolution electron microscopy and Landau-theory-based numerical simulations, we investigate the remarkable atomic arrangement and the intertwined relationship between the vortex structures and the topological defects. The roles of their displacement field, formation temperature, and nucleation sites are revealed. All conceivable vortices in the system are topologically classified using homotopy group theory, and their origins are identified.