Jason Hoffman

Magnetoelectric Coupling Effects in Multiferroic Complex Oxide Composite Structures

The study of magnetoelectric materials has recently received renewed interest, in large part stimulated by breakthroughs in the controlled growth of complex materials and by the search for novel materials with functionalities suitable for next generation electronic devices. In this Progress Report, we present an overview of recent developments in the field, with emphasis on magnetoelectric coupling effects in complex oxide multiferroic composite materials.

Origin of the magnetoelectric coupling effect in Pb(Zr0.2Ti0.8)O{3}/La{0.8}Sr{0.2}MnO{3} Multiferroic heterostructures.

The electronic valence state of Mn in Pb(Zr0.2Ti0.8)O{3}/La{0.8}Sr{0.2}MnO{3} multiferroic heterostructures is probed by near edge x-ray absorption spectroscopy as a function of the ferroelectric polarization. We observe a temperature independent shift in the absorption edge of Mn associated with a change in valency induced by charge carrier modulation in the La0.8Sr0.2MnO3, demonstrating the electronic origin of the magnetoelectric effect. Spectroscopic, magnetic, and electric characterization shows that the large magnetoelectric response originates from a modified interfacial spin configuration, opening a new pathway to the electronic control of spin in complex oxide materials.

Ferroelectric Field Effect Transistors for Memory Applications

The non-volatile polarization of a ferroelectric is a promising candidate for digital memory applications. Ferroelectric capacitors have been successfully integrated with silicon electronics, where the polarization state is read out by a device based on a field effect transistor configuration. Coupling the ferroelectric polarization directly to the channel of a field effect transistor is a long-standing research topic that has been difficult to realize due to the properties of the ferroelectric and the nature of the interface between the ferroelectric and the conducting channel. Here, we report on the fabrication and characterization of two promising capacitor-less memory architectures.

Unusual resistance hysteresis in n-layer graphene field effect transistors fabricated on ferroelectric Pb(Zr0.2Ti0.8)O3

We have fabricated n-layer graphene field effect transistors on epitaxial ferroelectric Pb(Zr_0.2Ti_0.8)O_3 (PZT) thin films. At low gate voltages, PZT behaves as a high-k dielectric with k up to 100. An unusual resistance hysteresis occurs in gate sweeps at high voltages, with its direction opposite to that expected from the polarization switching of PZT. The relaxation of the metastable state is thermally activated, with an activation barrier of 50-110 meV and a time constant of 6 hours at 300 K. We attribute its origin to the slow dissociation/recombination dynamics of water molecules adsorbed at the graphene-PZT interface. This robust hysteresis can potentially be used to construct graphene-ferroelectric hybrid memory devices.

Non-volatile ferroelastic switching of the Verwey transition and resistivity of epitaxial Fe3O4/PMN-PT (011).

A central goal of electronics based on correlated materials or ‘Mottronics’ is the ability to switch between distinct collective states with a control voltage. Small changes in structure and charge density near a transition can tip the balance between competing phases, leading to dramatic changes in electronic and magnetic properties. In this work, we demonstrate that an electric field induced two-step ferroelastic switching pathway in (011) oriented 0.71Pb(Mg1/3Nb2/3)O3-0.29PbTiO3 (PMN-PT) substrates can be used to tune the Verwey metal-insulator transition in epitaxial Fe3O4 films in a stable and reversible manner. We also observe robust non-volatile resistance switching in Fe3O4 up to room temperature, driven by ferroelastic strain. These results provides a framework for realizing non-volatile and reversible tuning of order parameters coupled to lattice-strain in epitaxial oxide heterostructures over a broad range of temperatures, with potential device applications.

Magnetic anisotropy modulation of magnetite in Fe3O4/BaTiO3(100) epitaxial structures

Temperature dependent magnetometry and transport measurements on epitaxial Fe3O4 films grown on BaTiO3(100) single crystals by molecular beam epitaxy show a series of discontinuities, due to changes in the magnetic anisotropy induced by strain from the different crystal phases of BaTiO3. The magnetite film is under tensile strain at room temperature, which is ascribed to the lattice expansion of BaTiO3 at the cubic to tetragonal transition, indicating that the magnetite film is relaxed at the growth temperature. From the magnetization versus temperature curves, the variation in the magnetic anisotropy is determined and compared with the magnetoelastic anisotropies. These results demonstrate the possibility of using the piezoelectric response of BaTiO3 to modulate the magnetic anisotropy of magnetite films.

Temperature dependence of the magnetoelectric effect in Pb(Zr0.2Ti0.8)O3/La0.8Sr0.2MnO3 multiferroic heterostructures

The magnetoelectric response of Pb(Zr0.2Ti0.8)O3/La0.8Sr0.2MnO3 (PZT/LSMO) artificial multiferroic heterostructures as a function of temperature, electric, and magnetic field, shows that the largest magnetoelectric coupling is attained at temperatures near the magnetic critical point of LSMO, at ∼180 K (−13.5 Oe cm kV−1). The magnetoelectric coupling displays a strong temperature dependence, changing sign at 150 K and saturating to positive values below ∼100 K (+6 Oe cm kV−1). The magnetoelectric curve switches hysteretically between two states in response to the ferroelectric switching. The peak in the magnetoelectric response coincides with the observation of on/off switching of magnetism in LSMO near the critical region, where the sensitivity to electric field is largest, making it a promising approach for device applications.

Charge transfer and interfacial magnetism in (LaNiO3)n/(LaMnO3)2superlattices

(LaNiO3)n/(LaMnO3)2 superlattices were grown using ozone-assisted molecular beam epitaxy, where LaNiO3 is a paramagnetic metal and LaMnO3 is an antiferromagnetic insulator. The superlattices exhibit excellent crystallinity and interfacial roughness of less than 1 unit cell. X-ray spectroscopy and dichroism measurements indicate that electrons are transferred from the LaMnO3 to the LaNiO3, inducing magnetism in LaNiO3. Magnetotransport measurements reveal a transition from metallic to insulating behavior as the LaNiO3 layer thickness is reduced from 5 unit cells to 2 unit cells and suggest a modulated magnetic structure within LaNiO3.

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.

Device performance of ferroelectric/correlated oxide heterostructures for non-volatile memory applications.

Ferroelectric field effect devices offer the possibility of non-volatile data storage. Attempts to integrate perovskite ferroelectric materials with silicon semiconductors, however, have been largely unsuccessful in creating non-volatile, nondestructive read memory elements because of difficulties in controlling the ferroelectric/semiconductor interface. Correlated oxide systems have been explored as alternative channel materials to form all-perovskite field effect devices. We examine a non-volatile memory using an electric-field-induced metal-insulator transition in PbZr(0.2)Ti(0.8)O(3)/La(1 - x)Sr(x)MnO(3) (PZT/LSMO), PZT/La(1 - x)Ca(x)MnO(3) (PZT/LCMO) and PZT/La(1 - x)Sr(x)CoO(3) (PZT/LSCO) devices. The performance of these devices in the areas of switching time and retention are discussed.