Ferroelectric Barrier Research Articles

Interfacial Ion Intermixing Effect on Four-Resistance States in La0.7Sr0.3MnO3/BaTiO3/La0.7Sr0.3MnO3 Multiferroic Tunnel Junctions.

A multiferroic tunnel junction (MFTJ), employing a ferroelectric barrier layer sandwiched between two ferromagnetic layers, presents at least four resistance states in a single memory cell and therefore opens an avenue for the development of the next generation of high-density nonvolatile memory devices. Here, using the all-perovskite-oxide La0.7Sr0.3MnO3/BaTiO3/La0.7Sr0.3MnO3 as a model MFTJ system, we demonstrate asymmetrical Mn-Ti sublattice intermixing at the La0.7Sr0.3MnO3/BaTiO3 interfaces by direct local measurements of the structure and valence, which reveals the relationship between ferroelectric polarization directions and four-resistance states, and the low temperature anomalous tunneling behavior in the MFTJ. These findings emphasize the crucial role of the interfaces in MFTJs and are quite important for understanding the electric transport of MFTJs as well as designing high-density multistates storage devices.

First-principles study of interface doping in ferroelectric junctions.

Effect of atomic monolayer insertion on the performance of ferroelectric tunneling junction is investigated in SrRuO3/BaTiO3/SrRuO3 heterostrucutures. Based on first-principles calculations, the atomic displacement, orbital occupancy, and ferroelectric polarization are studied. It is found that the ferroelectricity is enhanced when a (AlO2)− monolayer is inserted between the electrode SRO and the barrier BTO, where the relatively high mobility of doped holes effectively screen ferroelectric polarization. On the other hand, for the case of (LaO)+ inserted layer, the doped electrons resides at the both sides of middle ferroelectric barrier, making the ferroelectricity unfavorable. Our findings provide an alternative avenue to improve the performance of ferroelectric tunneling junctions.

Ferroelectric and flexible barrier resistive switching of epitaxial BiFeO3 films studied by temperature-dependent current and capacitance spectroscopy

The resistive switching of epitaxial ferroelectric BiFeO3 thin films was investigated by the combined current and capacitance spectroscopy, in addition with the piezoresponse force microscopy and conducting atomic force microscopy. A strong correlation between the resistance states and the capacitance states was found in the temperature range from 77 to 300 K, revealing the role of interface traps. It is demonstrated that the trap-assisted current transport contributes to the large ON current of the ferroelectric and flexible barrier resistive switching. The combination of ferroelectric polarization reversal, electromigration of oxygen vacancies, and interface traps leads to the nonvolatile memory performance with the ON/OFF ratio of 102 for >105 s and the endurance of over 8000 cycles at room temperature.

(Invited) Emerging Ferroelectric Devices

Ferroelectrics comprise a class of polar materials with an electrically switchable spontaneous polarization allowing their use as binary data storage media in nonvolatile ferroelectric random access memories (FeRAMs). Currently available FeRAMs utilize a destructive read process of stored information, which requires the memory cells to be re-written by a relatively high voltage, increases the read time and limits the scalability. An alternative approach to the read operation is based on the polarization-driven resistive switching, known as the tunneling electroresistance (TER) effect. If the ferroelectric film is sufficiently thin (of the order of several nanometers), conduction electrons can quantum-mechanically tunnel through the ferroelectric barrier. By flipping the polarization of the ferroelectric barrier it is possible to change an internal electronic potential profile and, hence, alter the transmission probability and produce the TER effect. Using this effect, reading of the polarization state can be performed in a non-destructive manner by measuring the resistance of the memory cell to a relatively low voltage. Since TER does not depend on the amount of the stored charge it allows a much better scalability. In addition to being highly relevant to technological applications, the TER effect concerns the fundamental issues of the critical behavior and switching dynamics in ultrathin ferroelectric films, role of structural defects and interfacial properties in the transport behavior. Maintaining a stable polarization in ultrathin ferroelectric films is essential for exploiting the functionality of these materials in nonvolatile memory applications. This talk will focus on investigation of the polarization-controlled tunneling conductance in the FTJ devices that incorporate both ferroelectric films and 2D transition metal dichalcogenides (TMD). In addition, the in-plane transport of the TMD conducting channel in the ferroelectric field effect transistor (FE-FET) devices modulated by polarization reversal will be discussed. We show that interface engineering in these hybrid TMD-FE systems provides a possibility of successfully addressing the most serious challenges relevant to ferroelectric device performance, such as ON/OFF ratio, lifetime, operation endurance and reliability.

Study on multi-logic polarization and inverse piezoelectric effect of ferroelectric tunnel junction with a composite barrier

By adjusting different polarization status in ferroelectric thin films, effect of saturation polarization, bias voltage, dielectric barrier width, and ferroelectric barrier width on electrical properties of a metal-dielectric-ferroelectric-metal structure are investigated in detail. Our simulation results show that the electrical properties of the tunnel junction can be effectively improved by utilizing the inverse piezoelectric effect of ferroelectric thin films. When the strain effect is taken into account, by controlling the polarization of the ferroelectric layer, the number of logic values could be modulated flexibly.

Elemental intermixing within an ultrathin SrRuO3 electrode layer in epitaxial heterostructure BaTiO3/SrRuO3/SrTiO3

Aberration corrected scanning transmission electron microscopy is used to directly observe atom columns in an epitaxial BaTiO3 thin film deposited on a 3.6 nm-thick SrRuO3 electrode layer above an SrTiO3 (001) substrate. Compositional gradients across the heterointerfaces were examined using electron energy-loss spectroscopy techniques. It was found that a small amount of Ba and Ti had diffused into the SrRuO3 layer, and that this layer contained a non-negligible concentration of oxygen vacancies. Such point defects are expected to degrade the electrode’s electronic conductivity drastically, resulting in a much longer screening length. This may explain the discrepancy between experimental measurements and theoretical estimates of the ferroelectric critical thickness of a BaTiO3 ferroelectric barrier sandwiched between metallic SrRuO3 electrodes, since theoretical calculations generally assume ideal (stoichiometric) perovskite SrRuO3.

Interfacial structure, ferroelectric stability, and magnetoelectric effect of magnetoelectric junction FeCo/BaTiO3/FeCo with alloy electrode

The interfacial structures, ferroelectric instability, and magnetoelectric coupling effect of FeCo/BaTiO3/FeCo junction with alloy electrode have been studied systematically using the first-principles calculations within density functional theory. Owing to different interfacial coupling between the electrode and BaTiO3 barrier layer, there are four possible interfacial structures, including TiO2/Fe, BaO/Fe, TiO2/Co, and BaO/Co interfaces. Among the four interfacial structures, the TiO2/Fe interface is the most stable one. With the decreasing thickness of BaTiO3 barrier layer in the junction, there exists a critical size of ferroelectricity with a thickness of ~4.5 formula unit cells. However, the ferroelectric polarization of magnetoelectric junction with the alloy FeCo electrode is larger than that of the junction with the Co electrode using a same size due to the stronger screening ability of alloy FeCo electrode. Meanwhile, we find that the induced magnetic moments of Ti atoms are nearly from the contribution of the first TiO2 layer adjacent to the interfaces irrespective of the thickness of ferroelectric barrier. In other words, the induced magnetic moments of Ti atoms only maintain an atom-layer thickness. Moreover, the induced magnetic moments of Ti atoms and local magnetic moments of Fe atoms at the two interfaces of tunneling junction depend on the polarization orientation, leading to a sizable ME coupling effect.

Space-charge Effect on Electroresistance in Metal-Ferroelectric-Metal capacitors.

Resistive switching through electroresistance (ER) effect in metal-ferroelectric-metal (MFM) capacitors has attracted increasing interest due to its potential applications as memories and logic devices. However, the detailed electronic mechanisms resulting in large ER when polarisation switching occurs in the ferroelectric barrier are still not well understood. Here, ER effect up to 1000% at room temperature is demonstrated in C-MOS compatible MFM nanocapacitors with a 8.8 nm-thick poly(vinylidene fluoride) (PVDF) homopolymer ferroelectric, which is very promising for silicon industry integration. Most remarkably, using theory developed for metal-semiconductor rectifying contacts, we derive an analytical expression for the variation of interfacial barrier heights due to space-charge effect that can interpret the observed ER response. We extend this space-charge model, related to the release of trapped charges by defects, to MFM structures made of ferroelectric oxides. This space-charge model provides a simple and straightforward tool to understand recent unusual reports. Finally, this work suggests that defect-engineering could be an original and efficient route for tuning the space-charge effect and thus the ER performances in future electronic devices.

Electric field control of magnetic properties and electron transport in BaTiO3-based multiferroic heterostructures

In this paper, we report on a purely electric mechanism for achieving the electric control of the interfacial spin polarization and magnetoresistance in multiferroic tunneling junctions. We investigate micrometric devices based on the Co/Fe/BaTiO3/La0.7Sr0.3MnO3 heterostructure, where Co/Fe and La0.7Sr0.3MnO3 are the magnetic electrodes and BaTiO3 acts both as a ferroelectric element and tunneling barrier. We show that, at 20 K, devices with a 2 nm thick BaTiO3 barrier present both tunneling electroresistance (TER = 12 ± 0.1%) and tunneling magnetoresistance (TMR). The latter depends on the direction of the BaTiO3 polarization, displaying a sizable change of the TMR from −0.32 ± 0.05% for the polarization pointing towards Fe, to −0.12 ± 0.05% for the opposite direction. This is consistent with the on-off switching of the Fe magnetization at the Fe/BaTiO3 interface, driven by the BaTiO3 polarization, we have previously demonstrated in x-ray magnetic circular dichroism experiments.

Ferroelectric Schottky barrier tunnel FET with gate-drain underlap: Proposal and investigation

In this paper, for the first time, a novel ferroelectric schottky barrier tunnel FET (Fe SB-TFET) is proposed and investigated. The Fe SB-TFET consists of ferroelectric gate stack with highly doped pocket at the source/drain and channel interface. In addition, for the suppression of ambipolar leakage current (IAMB), gate-drain underlap is employed. By using ferroelectric gate stack, we effectively amplified the applied gate voltage to enhance electric field for the reduction of tunneling barrier width at the source side schottky barrier. As a result, the increased tunneling probability improves the device performance in terms of high ION, high ION/IOFF ratio, reduced IAMB and low subthreshold swing (SS) as compared to the conventional SB-TFET having double pocket. We also investigate the influence of highly doped pocket (HDP) doping concentration and length on the device performance.

Octonary Resistance States in La0.7Sr0.3MnO3/BaTiO3/La0.7Sr0.3MnO3 Multiferroic Tunnel Junctions

General drawbacks of current electronic/spintronic devices are high power consumption and low density storage. A multiferroic tunnel junction (MFTJ), employing a ferroelectric barrier layer sandwiched between two ferromagnetic layers, presents four resistance states in a single device and therefore provides an alternative way to achieve high density memories. Here, an MFTJ device with eight nonvolatile resistance states by further integrating the design of noncollinear magnetization alignments between the ferromagnetic layers is demonstrated. Through the angle‐resolved tunneling magnetoresistance investigations on La0.7Sr0.3MnO3/BaTiO3/La0.7Sr0.3MnO3 junctions, it is found that, besides collinear parallel/antiparallel magnetic configurations, the MFTJ shows at least two other stable noncollinear (45° and 90°) magnetic configurations. Combining the tunneling electroresistance effect caused by the ferroelectricity reversal of the BaTiO3 barrier, an octonary memory device is obtained, representing potential applications in high density nonvolatile storage in the future.

High temperature coefficient of resistance for a ferroelectric tunnel junction

An infrared detector is proposed that is based on a ferroelectric tunnel junction (FTJ) working under bolometer-like principles. Electron tunneling, either direct or indirect, through the ferroelectric barrier depends on the temperature of the devices. During tunneling, infrared radiation alters the polarization of the ferroelectric film via pyroelectricity, resulting in a change in the barrier height of the tunnel junction. A high temperature coefficient of resistance of up to −3.86% was observed at room temperature. These results show that the FTJ structure has potential to be adapted for use in uncooled infrared detectors.

Plasma reforming of methane in a tunable ferroelectric packed-bed dielectric barrier discharge reactor

In a tunable circular parallel plate dielectric barrier discharge reactor with pellets of a ferroelectric material separating the electrodes we investigate the plasma reforming of methane trying to maximize both the reaction yield and the energetic efficiency of the process. The geometrical configuration of the reactor (gap between electrodes, active electrode area) and the ferroelectric pellet size have been systematically varied to determine their influence on the process efficiency. The comparison between wet (with H2O as reactant), oxidative (with O2), and dry (with CO2) reforming reactions reveals a higher efficiency for the former with CO + H2 as main reaction products. The maximum energetic efficiency EE, defined as the produced number of litres of H2 per kWh, found for optimized working conditions at low-level applied power is higher than the up to date best-known results. A comprehensive discussion of the influence of the different parameters affecting the reaction yield is carried out.

Effect of epitaxial strain on tunneling electroresistance in ferroelectric tunnel junctions

We report the effect of compressive strain on the tunneling electroresistance (TER) effect in BaTiO3/SrRuO3 (BTO/SRO) heterostructures. We find that epitaxial strain imposed by the mismatch of NdGaO3 and SrTiO3 lattice parameters with the BTO and SRO layers improves ferroelectric polarization of BTO and concurrently promotes the metallicity of the SRO films. While the enhanced polarization is beneficial for the TER magnitude, the reduced asymmetry in the tunneling barrier due to the shortened screening length of SRO is detrimental for the effect. Thus, a combined effect of strain on the polarization of the ferroelectric barrier and the screening properties of the electrodes needs to be taken into account when considering and predicting the TER effect in ferroelectric tunnel junctions.

Large room-temperature electroresistance in dual-modulated ferroelectric tunnel barriers.

Pt/BaTiO3/La0.7Sr0.3MnO3 tunnel junctions, at negative voltage bias, for two polarization directions are represented. It is demonstrated that reversing the polarization direction of a ferroelectric barrier in a tunnel junction leads to a change of junction conductance and capacitance, with concomitant variations on the barrier height and effective thickness, both contributing to produce larger electroresistance.

Ferroelectric control of spin-transfer torque in multiferroic tunnel junctions

Based on model calculations we predict electric-field control of the spin-transfer torque (STT) in magnetic tunnel junctions with ferroelectric barriers. We demonstrate that the bias dependence of the in-plane ${T}_{\ensuremath{\parallel}}$ and out-of-plane ${T}_{\ensuremath{\perp}}$ components of the STT can be dramatically modified by the ferroelectric polarization. In particular, the magnitude of the STT can be enhanced or suppressed by switching the polarization direction and in some cases the sign of STT can be toggled. The underlying mechanism is the combination of polarization-induced symmetry breaking and the interplay of the bias-induced and polarization-induced spin-dependent screening giving rise to a rich behavior of the electrostatic potential energy profile. These properties could lead to enhanced switching efficiency in STT-based devices and open a new avenue for applications of multiferroic devices.

Multiferroic tunnel junctions and ferroelectric control of magnetic state at interface (invited)

As semiconductor devices reach ever smaller dimensions, the challenge of power dissipation and quantum effect place a serious limit on the future device scaling. Recently, a multiferroic tunnel junction (MFTJ) with a ferroelectric barrier sandwiched between two ferromagnetic electrodes has drawn enormous interest due to its potential applications not only in multi-level data storage but also in electric field controlled spintronics and nanoferronics. Here, we present our investigations on four-level resistance states, giant tunneling electroresistance (TER) due to interfacial magnetoelectric coupling, and ferroelectric control of spin polarized tunneling in MFTJs. Coexistence of large tunneling magnetoresistance and TER has been observed in manganite/(Ba, Sr)TiO3/manganite MFTJs at low temperatures and room temperature four-resistance state devices were also obtained. To enhance the TER for potential logic operation with a magnetic memory, La0.7Sr0.3MnO3/BaTiO3/La0.5Ca0.5MnO3 /La0.7Sr0.3MnO3 MFTJs were designed by utilizing a bilayer tunneling barrier in which BaTiO3 is ferroelectric and La0.5Ca0.5MnO3 is close to ferromagnetic metal to antiferromagnetic insulator phase transition. The phase transition occurs when the ferroelectric polarization is reversed, resulting in an increase of TER by two orders of magnitude. Tunneling magnetoresistance can also be controlled by the ferroelectric polarization reversal, indicating strong magnetoelectric coupling at the interface.

Sub-nA spatially resolved conductivity profiling of surface and interface defects in ceria films

Spatial variability of conductivity in ceria is explored using scanning probe microscopy with galvanostatic control. Ionically blocking electrodes are used to probe the conductivity under opposite polarities to reveal possible differences in the defect structure across a thin film of CeO2. Data suggest the existence of a large spatial inhomogeneity that could give rise to constant phase elements during standard electrochemical characterization, potentially affecting the overall conductivity of films on the macroscale. The approach discussed here can also be utilized for other mixed ionic electronic conductor systems including memristors and electroresistors, as well as physical systems such as ferroelectric tunneling barriers.

Controlling the spin-torque efficiency with ferroelectric barriers

Nonequilibrium spin-dependent transport in magnetic tunnel junctions comprising a ferroelectric barrier is theoretically investigated. The exact solutions of the free electron Schr\"odinger equation for electron tunneling in the presence of interfacial screening are obtained by combining Bessel and Airy functions. We demonstrate that the spin transfer torque efficiency, and more generally the bias dependence of tunneling magneto- and electroresistance, can be controlled by switching the ferroelectric polarization of the barrier. In particular, the critical voltage at which the in-plane torque changes sign can be strongly enhanced or reduced depending on the direction of the ferroelectric polarization of the barrier. This effect provides a supplementary way to electrically control the current-driven dynamic states of the magnetization and related magnetic noise in spin transfer devices.

Ferroelectric tunnel junctions with graphene electrodes.

Polarization-driven resistive switching in ferroelectric tunnel junctions (FTJs)--structures composed of two electrodes separated by an ultrathin ferroelectric barrier--offers new physics and materials functionalities, as well as exciting opportunities for the next generation of non-volatile memories and logic devices. Performance of FTJs is highly sensitive to the electrical boundary conditions, which can be controlled by electrode material and/or interface engineering. Here, we demonstrate the use of graphene as electrodes in FTJs that allows control of interface properties for significant enhancement of device performance. Ferroelectric polarization stability and resistive switching are strongly affected by a molecular layer at the graphene/BaTiO3 interface. For the FTJ with the interfacial ammonia layer we find an enhanced tunnelling electroresistance (TER) effect of 6 × 10(5)%. The obtained results demonstrate a new approach based on using graphene electrodes for interface-facilitated polarization stability and enhancement of the TER effect, which can be exploited in the FTJ-based devices.