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Register a new userOn the persistence of polar domains in ultrathin ferroelectric capacitors
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The instability of ferroelectric ordering in ultra-thin films is one of the most important fundamental issues pertaining realization of a number of electronic devices with enhanced functionality, such as ferroelectric and multiferroic tunnel junctions or ferroelectric field effect transistors. In this paper, we investigate the polarization state of archetypal ultrathin (several nanometres) ferroelectric heterostructures: epitaxial single-crystalline BaTiO$_3$ films sandwiched between the most habitual perovskite electrodes, SrRuO$_3$, on top of the most used perovskite substrate, SrTiO$_3$. We use a combination of piezoresponse force microscopy, dielectric measurements and structural characterization to provide conclusive evidence for the ferroelectric nature of the relaxed polarization state in ultrathin BaTiO$_3$ capacitors. We show that even the high screening efficiency of SrRuO$_3$ electrodes is still insufficient to stabilize polarization in SrRuO$_3$/BaTiO$_3$/SrRuO$_3$ heterostructures at room temperature. We identify the key role of domain wall motion in determining the macroscopic electrical properties of ultrathin capacitors and discuss their dielectric response in the light of the recent interest in negative capacitance behaviour.
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The epitaxial growth of multifunctional oxides on semiconductors has opened a pathway to introduce new functionalities to semiconductor device technologies. In particular, ferroelectric materials integrated on semiconductors could lead to low-power field-effect devices that can be used for logic and memory. Essential to realizing such field-effect devices is the development of ferroelectric metal-oxide-semiconductor (MOS) capacitors, in which the polarization of a ferroelectric gate is coupled to the surface potential of a semiconducting channel. Here we demonstrate that ferroelectric MOS capacitors can be realized using single crystalline SrZrxTi1-xO3 (x = 0.7) that has been epitaxially grown on Ge. We find that the ferroelectric properties of SrZrxTi1-xO3 are exceptionally robust, as gate layers as thin as 5 nm corresponding to an equivalent-oxide-thickness of just 1.0 nm exhibit a ~ 2 V hysteretic window in the capacitance-voltage characteristics. The development of ferroelectric MOS capacitors with nanoscale gate thicknesses opens new vistas for nanoelectronic devices.
Structural studies on ultrathin SrRuO3/BaTiO3/SrRuO3 capacitors, with BaTiO3 thicknesses of between 5 nm and 30 nm, show well-defined interfaces between ferroelectric BaTiO3 and electrode SrRuO3 layers. In these capacitors, we cannot observe any extrinsic electrical effects due to either the formation of an insulating interfacial passive layer or passive-layer-induced charge injection. Such high quality interfaces result in very good fatigue endurance, even for the 5 nm thick BaTiO3 capacitor.
Thickness-dependence of coercive field (EC) was investigated in ultrathin BaTiO3 capacitors with thicknesses (d) between 30 and 5 nm. The EC appears nearly independent of d below 15 nm, and decreases slowly as d increases above 15 nm. This behavior cannot be explained by extrinsic effects, such as interfacial passive layers or strain relaxation, nor by homogeneous domain models. Based on domain nuclei formation model, the observed EC behavior is explainable via a quantitative level. A crossover of domain shape from a half-prolate spheroid to a cylinder is also suggested at d~ 15 nm, exhibiting good agreement with experimental results.
The response of polar nanoregions (PNR) in the relaxor compound Pb[(Zn$_{1/3}$Nb$_{2/3}$)$_{0.92}$Ti$_{0.08}$]O$_3$ subject to a [111]-oriented electric field has been studied by neutron diffuse scattering. Contrary to classical expectations, the diffuse scattering associated with the PNR persists, and is even partially enhanced by field cooling. The effect of the external electric field is retained by the PNR after the field is removed. The ``memory of the applied field reappears even after heating the system above $T_C$, and cooling in zero field.
The possibility of reconciliation between seemingly mutually exclusive properties in one system can not only lead to theoretical breakthroughs but also potential novel applications. The research on the coexistence of two purportedly contra-indicated properties, ferroelectricity/polarity and conductivity, proposed by Anderson and Blount over 50 years ago was recently revitalized by the discovery of the first unambiguous polar metal LiOsO3 and further fueled by the demonstration of the first switchable ferroelectric metal WTe2. In this review, we first discuss the reasons why the coexistence of ferroelectricity/polarity and conductivity have been deemed incompatible, followed by a review on the history of ferroelectric/polar metals. Secondly, we review the important milestones along with the corresponding mechanisms for the ferroelectric/polar metallic phases in these materials. Thirdly, we summarize the design approaches for ferroelectric/polar metals. Finally, we discuss the future prospects and potential applications of ferroelectric/polar metals.
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