Ying-Hui Hsieh

Epitaxial Photostriction-Magnetostriction Coupled Self-Assembled Nanostructures

Self-assembled vertical nanostructures take advantage of high interface-to-volume ratio and can be used to design new functionalities by the choice of a proper combination of constituents. However, most of the studies to date have emphasized the functional controllability of the nanostructures using external electric or magnetic fields. In this study, to introduce light (or photons) as an external control parameter in a self-assembled nanostructure system, we have successfully synthesized oxide nanostructures with CoFe(2)O(4) nanopillars embedded in a SrRuO(3) matrix. The combination of photostrictive SrRuO(3) and magnetostrictive CoFe(2)O(4) in the intimately assembled nanostructures leads to a light-induced, ultrafast change in magnetization of the CoFe(2)O(4) nanopillars. Our work demonstrates a novel concept on oxide nanostructure design and opens an alternative pathway for the explorations of diverse functionalities in heteroepitaxial self-assembled oxide nanostructures.

Deep Data Analysis of Conductive Phenomena on Complex Oxide Interfaces: Physics from Data Mining

Spatial variability of electronic transport in BiFeO3-CoFe2O4 (BFO-CFO) self-assembled heterostructures is explored using spatially resolved first-order reversal curve (FORC) current voltage (IV) mapping. Multivariate statistical analysis of FORC-IV data classifies statistically significant behaviors and maps characteristic responses spatially. In particular, regions of grain, matrix, and grain boundary responses are clearly identified. k-Means and Bayesian demixing analysis suggest the characteristic response be separated into four components, with hysteretic-type behavior localized at the BFO-CFO tubular interfaces. The conditions under which Bayesian components allow direct physical interpretation are explored, and transport mechanisms at the grain boundaries and individual phases are analyzed. This approach conjoins multivariate statistical analysis with physics-based interpretation, actualizing a robust, universal, data-driven approach to problem solving, which can be applied to exploration of local transport and other functional phenomena in other spatially inhomogeneous systems.

Large Magnetoresistance in Magnetically Coupled SrRuO3 –CoFe2O4 Self-Assembled Nanostructures

A new way to induce a large magnetoresistance has been achieved by self-assembled nanostructures consisting of ferromagnetic spinel CoFe₂O₄ (CFO) and metallic perovskite SrRuO₃ (SRO). The interdiffused Fe³⁺ ions in SRO have paved the way to strong magnetic couplings with CFO nanopillars, resulting in the suppression of spin-polarized electron scattering.

Flexible ferroelectric element based on van der Waals heteroepitaxy

A flexible ferroelectric memory element based on oxide heteroepitaxy has been demonstrated with superior performance. We present a promising technology for nonvolatile flexible electronic devices: A direct fabrication of epitaxial lead zirconium titanate (PZT) on flexible mica substrate via van der Waals epitaxy. These single-crystalline flexible ferroelectric PZT films not only retain their performance, reliability, and thermal stability comparable to those on rigid counterparts in tests of nonvolatile memory elements but also exhibit remarkable mechanical properties with robust operation in bent states (bending radii down to 2.5 mm) and cycling tests (1000 times). This study marks the technological advancement toward realizing much-awaited flexible yet single-crystalline nonvolatile electronic devices for the design and development of flexible, lightweight, and next-generation smart devices with potential applications in electronics, robotics, automotive, health care, industrial, and military systems.

Flexible Multiferroic Bulk Heterojunction with Giant Magnetoelectric Coupling via van der Waals Epitaxy

Magnetoelectric nanocomposites have been a topic of intense research due to their profound potential in the applications of electronic devices based on spintronic technology. Nevertheless, in spite of significant progress made in the growth of high-quality nanocomposite thin films, the substrate clamping effect still remains a major hurdle in realizing the ultimate magnetoelectric coupling. To overcome this obstacle, an alternative strategy of fabricating a self-assembled ferroelectric-ferrimagnetic bulk heterojunction on a flexible muscovite via van der Waals epitaxy is adopted. In this study, we investigated the magnetoelectric coupling in a self-assembled BiFeO3 (BFO)-CoFe2O4 (CFO) bulk heterojunction epitaxially grown on a flexible muscovite substrate. The obtained heterojunction is composed of vertically aligned multiferroic BFO nanopillars embedded in a ferrimagnetic CFO matrix. Moreover, due to the weak interaction between the flexible substrate and bulk heterojunction, the interface is incoherent and, hence, the substrate clamping effect is greatly reduced. The phase-field simulation model also complements our results. The magnetic and electrical characterizations highlight the improvement in magnetoelectric coupling of the BFO-CFO bulk heterojunction. A magnetoelectric coupling coefficient of 74 mV/cm·Oe of this bulk heterojunction is larger than the magnetoelectric coefficient reported earlier on flexible substrates. Therefore, this study delivers a viable route of fabricating a remarkable magnetoelectric heterojunction and yet flexible electronic devices that are robust against extreme conditions with optimized performance.

Flexible Heteroepitaxy of CoFe2O4/Muscovite Bimorph with Large Magnetostriction

A bimorph composed of ferrimagnetic cobalt ferrite (CoFe2O4, CFO) and flexible muscovite was fabricated via van der Waals epitaxy. The combination of X-ray diffraction and transmission electron microscopy was conducted to reveal the heteroepitaxy of the CFO/muscovite system. The robust magnetic behaviors against mechanical bending were characterized by hysteresis measurements and magnetic force microscopy, which maintain a saturation magnetization (Ms) of ∼120-150 emu/cm3 under different bending states. The large magnetostrictive response of the CFO film was then determined by digital holographic microscopy, where the difference of magnetostrction coefficient (Δλ) is -104 ppm. The superior performance of this bimorph is attributed to the nature of weak interaction between film and substrate. Such a flexible CFO/muscovite bimorph provides a new platform to develop next-generation flexible magnetic devices.

Constraining Data Mining with Physical Models: Voltage- and Oxygen Pressure-Dependent Transport in Multiferroic Nanostructures.

Development of new generation electronic devices necessitates understanding and controlling the electronic transport in ferroic, magnetic, and optical materials, which is hampered by two factors. First, the complications of working at the nanoscale, where interfaces, grain boundaries, defects, and so forth, dictate the macroscopic characteristics. Second, the convolution of the response signals stemming from the fact that several physical processes may be activated simultaneously. Here, we present a method of solving these challenges via a combination of atomic force microscopy and data mining analysis techniques. Rational selection of the latter allows application of physical constraints and enables direct interpretation of the statistically significant behaviors in the framework of the chosen physical model, thus distilling physical meaning out of raw data. We demonstrate our approach with an example of deconvolution of complex transport behavior in a bismuth ferrite-cobalt ferrite nanocomposite in ambient and ultrahigh vacuum environments. Measured signal is apportioned into four electronic transport patterns, showing different dependence on partial oxygen and water vapor pressure. These patterns are described in terms of Ohmic conductance and Schottky emission models in the light of surface electrochemistry. Furthermore, deep data analysis allows extraction of local dopant concentrations and barrier heights empowering our understanding of the underlying dynamic mechanisms of resistive switching.

Orientation-tuning in self-assembled heterostructures induced by a buffer layer

Anisotropic nano-plate structures in self-assembled perovskite-spinel thin films, BiFeO3-NiFe2O4 and BiFeO3-CoFe2O4, which were deposited on (001)c SrRuO3/SrTiO3 and DyScO3 substrates, respectively, have been demonstrated using transmission electron microscopy combined with strain analysis. Unlike the unitary cube-on-cube orientation relationship reported widely, the growth direction of the CoFe2O4 and NiFe2O4 plates was tuned to [011]c while the BiFeO3 matrix kept [001]c in both systems. In particular, a thin stress-sensitive BiFeO3 buffer layer between the spinel nanostructure and the substrate was introduced for providing a complex strain state in both film systems. The novel orientation tuning and the pattern configuration of the heterostructures are mainly attributed to the strain imposed on the films and the anisotropic ledge growth mechanism of spinels.

Self-assembled perovskite-spinel heterostructure on a highly distorted substrate

The pattern configuration and interface structure in epitaxial BiFeO3-CoFe2O4 heterostructures grown on (010)pc NdGaO3 substrates have been investigated systematically by transmission electron microscopy and chemical analysis. The crystal orientation of CoFe2O4 variants was tuned to [111]CFO, while BiFeO3 kept [010]pc matching the substrate. Triangular prism-shaped CoFe2O4 embedded in the BiFeO3 matrix grew as an equilibrium island mode with {111}CFO as its surfaces and interfaces. Two types of BiFeO3-CoFe2O4 orientation relationships were determined as (001)[010]BFO//(0-22)[111]CFO and (101)[010]BFO//(−220)[111]CFO. The results reveal that the dominant factors controlling the growth orientation of the present vertical heterostructures are surface energy anisotropy and atomic structure continuity.

Photostriction of CH3NH3PbBr3 Perovskite Crystals

Organic-inorganic hybrid perovskite materials exhibit a variety of physical properties. Pronounced coupling between phonon, organic cations, and the inorganic framework suggest that these materials exhibit strong light-matter interactions. The photoinduced strain of CH3 NH3 PbBr3 is investigated using high-resolution and contactless in situ Raman spectroscopy. Under illumination, the material exhibits large blue shifts in its Raman spectra that indicate significant structural deformations (i.e., photostriction). From these shifts, the photostrictive coefficient of CH3 NH3 PbBr3 is calculated as 2.08 × 10-8 m2 W-1 at room temperature under visible light illumination. The significant photostriction of CH3 NH3 PbBr3 is attributed to a combination of the photovoltaic effect and translational symmetry loss of the molecular configuration via strong translation-rotation coupling. Unlike CH3 NH3 PbI3 , it is noted that the photostriction of CH3 NH3 PbBr3 is extremely stable, demonstrating no signs of optical decay for at least 30 d. These results suggest the potential of CH3 NH3 PbBr3 for applications in next-generation optical micro-electromechanical devices.