Yijia Gu

Domain Dynamics During Ferroelectric Switching

The role of defects and interfaces on switching in ferroelectric materials is observed with high-resolution microscopy. The utility of ferroelectric materials stems from the ability to nucleate and move polarized domains using an electric field. To understand the mechanisms of polarization switching, structural characterization at the nanoscale is required. We used aberration-corrected transmission electron microscopy to follow the kinetics and dynamics of ferroelectric switching at millisecond temporal and subangstrom spatial resolution in an epitaxial bilayer of an antiferromagnetic ferroelectric (BiFeO3) on a ferromagnetic electrode (La0.7Sr0.3MnO3). We observed localized nucleation events at the electrode interface, domain wall pinning on point defects, and the formation of ferroelectric domains localized to the ferroelectric and ferromagnetic interface. These results show how defects and interfaces impede full ferroelectric switching of a thin film.

Extended Mapping and Exploration of the Vanadium Dioxide Stress-Temperature Phase Diagram

Single-crystal micro- and nanomaterials often exhibit higher yield strength than their bulk counterparts. This enhancement is widely recognized in structural materials but is rarely exploited to probe fundamental physics of electronic materials. Vanadium dioxide exhibits coupled electronic and structural phase transitions that involve different structures existing at different strain states. Full understanding of the driving mechanism of these coupled transitions necessitates concurrent structural and electrical measurements over a wide phase space. Taking advantages of the superior mechanical property of micro/nanocrystals of VO(2), we map and explore its stress-temperature phase diagram over a phase space that is more than an order of magnitude broader than previously attained. New structural and electronic aspects were observed crossing phase boundaries at high-strain states. Our work shows that the actively tuning strain in micro/nanoscale electronic materials provides an effective route to investigate their fundamental properties beyond what can be accessed in their bulk counterpart.

Emergence of room-temperature ferroelectricity at reduced dimensions

Thinning films induces ferroelectricity Thin ferroelectric films are needed in computers and medical devices. However, traditional ferroelectric films typically become less and less polarized the thinner the films become. Instead of using a good ferroelectric and making it thinner, Lee et al. started with SrTiO3, which in its bulk form is not ferroelectric. This material does have naturally occurring nanosized polarized regions. and when the thickness of the SrTiO3 films reaches the typical size of these regions, the whole film aligns and becomes ferroelectric. Science, this issue p. 1314 Strontium titanate films become ferroelectric when they are as thin as naturally occurring nanosized polarized regions. The enhancement of the functional properties of materials at reduced dimensions is crucial for continuous advancements in nanoelectronic applications. Here, we report that the scale reduction leads to the emergence of an important functional property, ferroelectricity, challenging the long-standing notion that ferroelectricity is inevitably suppressed at the scale of a few nanometers. A combination of theoretical calculations, electrical measurements, and structural analyses provides evidence of room-temperature ferroelectricity in strain-free epitaxial nanometer-thick films of otherwise nonferroelectric strontium titanate (SrTiO3). We show that electrically induced alignment of naturally existing polar nanoregions is responsible for the appearance of a stable net ferroelectric polarization in these films. This finding can be useful for the development of low-dimensional material systems with enhanced functional properties relevant to emerging nanoelectronic devices.

Thermodynamics of strained vanadium dioxide single crystals

Vanadium dioxide undergoes a metal–insulator transition, in which the strain condition plays an important role. To investigate the strain contribution, a phenomenological thermodynamic potential for the vanadium dioxide single crystal was constructed. The transformations under the uniaxial stress, wire, and thin film boundary conditions were analyzed, and the corresponding phase diagrams were constructed. The calculated phase diagrams agree well with existing experimental data, and show that the transformation temperature (and Curie temperature) strongly depends on the strain condition.

Composition- and pressure-induced ferroelectric to antiferroelectric phase transitions in Sm-doped BiFeO3 system

A three-dimensional phenomenological model is proposed to describe both ferroelectricity and antiferroelectricity based on the Ginzburg-Landau-Devonshire theory. Its application to the multiferroic Sm-doped BiFeO3 system describes the temperature-, pressure-, and composition-induced ferroelectric to antiferroelectric phase transitions. The constructed temperature-composition and temperature-pressure phase diagrams show that compressive hydrostatic pressure and Sm doping have similar effects on the ferroelectric and antiferroelectric phase transitions. It is also indicated from the temperature-pressure phase diagram that the experimentally observed phase of BiFeO3 under the hydrostatic pressure from 3 GPa to 10 GPa is a PbZrO3-like antiferroelectric phase.

Phenomenological thermodynamic potential for CaTiO3 single crystals

The antiferrodistortive (AFD) structural transitions of calcium titanate (CaTiO3) at ambient pressure have been extensively studied during the last few years. It has been found that none of the AFD polymorphs is polar or ferroelectric. However, it was recently shown theoretically and later experimentally confirmed that a ferroelectric transition in CaTiO3 can be induced by tensile strains. The ferroelectric instability is believed to be strongly coupled to the AFD soft modes. In this paper, we present a complete thermodynamic potential for describing the coupling between the AFD and ferroelectric phase transitions. We analyzed the dependence of transition temperatures on stress and strain condition. Based on this potential, a (001) CaTiO3 thin film diagram was constructed. The results show good agreement with available experimental observations. The strong suppression of ferroelectric transition by the AFD transition is discussed.

Nanoscale mechanical switching of ferroelectric polarization via flexoelectricity

Flexoelectric coefficient is a fourth-rank tensor arising from the coupling between strain gradient and electric polarization and thus exists in all crystals. It is generally ignored for macroscopic crystals due to its small magnitude. However, at the nanoscale, flexoelectric contributions may become significant and can potentially be utilized for device applications. Using the phase-field method, we study the mechanical switching of electric polarization in ferroelectric thin films by a strain gradient created via an atomic force microscope tip. Our simulation results show good agreement with existing experimental observations. We examine the competition between the piezoelectric and flexoelectric effects and provide an understanding of the role of flexoelectricity in the polarization switching. Also, by changing the pressure and film thickness, we reveal that the flexoelectric field at the film bottom can be used as a criterion to determine whether domain switching may happen under a mechanical force.

Direct observation of nanoscale Peltier and Joule effects at metal-insulator domain walls in vanadium dioxide nanobeams.

The metal to insulator transition (MIT) of strongly correlated materials is subject to strong lattice coupling, which brings about the unique one-dimensional alignment of metal-insulator (M-I) domains along nanowires or nanobeams. Many studies have investigated the effects of stress on the MIT and hence the phase boundary, but few have directly examined the temperature profile across the metal-insulating interface. Here, we use thermoreflectance microscopy to create two-dimensional temperature maps of single-crystalline VO2 nanobeams under external bias in the phase coexisting regime. We directly observe highly localized alternating Peltier heating and cooling as well as Joule heating concentrated at the M-I domain boundaries, indicating the significance of the domain walls and band offsets. Utilizing the thermoreflectance technique, we are able to elucidate strain accumulation along the nanobeam and distinguish between two insulating phases of VO2 through detection of the opposite polarity of their respective thermoreflectance coefficients. Microelasticity theory was employed to predict favorable domain wall configurations, confirming the monoclinic phase identification.

Impact of symmetry on the ferroelectric properties of CaTiO3 thin films

Epitaxial strain is a powerful tool to induce functional properties such as ferroelectricity in thin films of materials that do not possess ferroelectricity in bulk form. In this work, a ferroelectric state was stabilized in thin films of the incipient ferroelectric, CaTiO3, through the careful control of the biaxial strain state and TiO6 octahedral rotations. Detailed structural characterization was carried out by synchrotron x-ray diffraction and scanning transmission electron microscopy. CaTiO3 films grown on La0.18Sr0.82Al0.59Ta0.41O3 (LSAT) and NdGaO3 (NGO) substrates experienced a 1.1% biaxial strain state but differed in their octahedral tilt structures. A suppression of the out-of-plane rotations of the TiO6 octahedral in films grown on LSAT substrates resulted in a robust ferroelectric I4 mm phase with remnant polarization ∼5 μC/cm2 at 10 K and Tc near 140 K. In contrast, films grown on NGO substrates with significant octahedral tilting showed reduced polarization and Tc. These results highlight ...

Electric field-induced tetragonal to orthorhombic phase transitions in [110]c-oriented BaTiO3 single crystals

Electric field-induced phase transitions in [110]c-oriented BaTiO3 single crystals were studied by macroscopic electrical measurements in the temperature range from 20 °C to 50 °C. Discontinuous, hysteretic jumps in the polarization and strain were observed, indicating a tetragonal ↔ orthorhombic phase transition. The critical electric field to induce the transition was found to shift to higher values with increasing temperature. The Landau-Devonshire theory was used to analyze the observed electric field-induced T ↔ O phase transitions.