Recently, relaxor ferroelectric thin-film capacitors have attracted considerable attention for energy storage applications since their slim-type polarization–electric field hysteresis loops can yield large recoverable energy density ( Wrec) and high efficiency ( η). In this work, we study the effects of buffer layers on energy storage properties of 0.93Pb(Mg1/3Nb2/3)O3-0.07PbTiO3 (PMN-PT) thin-film capacitors with a 5 nm-thick SrTiO3 (STO) and LaAlO3 (LAO) films. The energy storage properties of Pt/PMN-PT/SrRuO3 (SRO) capacitors are found to be significantly changed by incorporating the STO or LAO buffer layer at the top Pt/PMN-PT interface, while inserting the buffer layer at bottom PMN-PT/SRO interface shows negligible effects on the electrical properties. Specifically, with the STO buffering, the breakdown field is dramatically increased in the Pt/STO/PMN-PT/SRO capacitor due to the existence of an internal field in the STO, which prevents the growth of electrical trees from the bottom SRO to the top Pt electrode, and a large Wrec of ∼48.91 J/cm3, more than three times of that of the PMN-PT capacitor, is achieved. However, buffered by the LAO, the Pt/LAO/PMN-PT/SRO capacitor exhibits a reduced relaxor character, which may be ascribed to a pinning effect of nanodomains associated with the charged LAO/PMN-PT interface. As a result, both Wrec and η are significantly lowered, compared to the non-buffered PMN-PT capacitor. These results provide physical insights into the modulation of relaxor and dielectric behaviors by designing the characteristics of buffer layers, demonstrating a way for enhancing energy storage properties in thin-film capacitors.
Recently, ion-doped HfO2 thin films are highly desirable for the next-generation nonvolatile memories due to excellent compatibility with current complementary metal-oxide-semiconductor processes and robust ferroelectricity persisted down to the nanoscale. In this work, we study conduction mechanisms of 4 and 8 nm-thick La:HfO2 ultrathin films sandwiched between Pt and (La0.67,Sr0.33)MnO3 (LSMO) electrodes based on band alignments of the Pt/La:HfO2/LSMO, measured by x-ray photoelectron spectroscopy, and temperature-dependent current-voltage curves from 50 to 300 K. In a 4 nm-thick La:HfO2 thin-film capacitor, the conduction mechanism is found to be governed by direct tunneling at 50–100 K and phonon-assisted indirect tunneling when the temperature is further increased to 300 K in which the [Formula: see text] acceptors are served as localized states, facilitating hole hopping through the La:HfO2 barrier. When the thickness is increased to 8 nm, the tunneling through a La:HfO2 layer is suppressed, and the current-voltage character becomes rectifying, which is regulated by the dominated La:HfO2/LSMO interfacial barrier. The transport for a forward bias of the La:HfO2/LSMO barrier is found to be governed by thermionic-field emission, exhibiting a temperature-independent build-in potential of ∼2.77 V. For the reverse bias, the Fowler–Nordheim tunneling is observed. The revealing of conduction mechanisms in terms of band alignments sheds light on leakage problems and facilitates the design of HfO2-based ferroelectric devices with excellent insulating character for high-performance memory applications.
Ferroelectric tunnel junctions (FTJs) are promising candidates for the next-generation memory technologies. The electroresistance mechanism, however, has been reported not only from the polarization-modulation of barrier profiles. Electrical migration of charged defects has also been observed as a possible origin for the resistive switching. Here, we achieve two kinds of electroresistance behaviors in Pt/Pb(Zr,Ti)O3/(La,Sr)MnO3 tunnel junctions by introducing oxygen vacancies in the Pb(Zr,Ti)O3 barrier. The oxygen vacancies are observed by x-ray photoelectron spectroscopy, and their effects on the widely adopted piezoresponse force microscopy characterizations of ultrathin ferroelectric films have been analyzed by AC voltage-dependent hysteresis loops. For the Pt/Pb(Zr,Ti)O3/(La,Sr)MnO3 device that is modulated by the polarization reversal, a counterclockwise resistance–voltage ( R– V) relationship is observed due to the tunneling between high and low barriers, whereas the R– V hysteresis loop is changed to clockwise with the existence of oxygen vacancies, in which conductive filaments are formed in the Pb(Zr,Ti)O3 barrier. However, such an ionic electroresistance is not stable during repetitive switching. Further investigation on memristive behaviors is, thus, performed on the ferroelectric-controlled Pt/Pb(Zr,Ti)O3/(La,Sr)MnO3 tunnel junctions. An excellent linearity is achieved in continuous resistance change owing to the nucleation-limited-switching mode of domain switching in the Pb(Zr,Ti)O3 barrier, giving rise to spike-timing-dependent plasticity behaviors for the Hebbian rule of learning and memory. These results provide insight into the distinguishing of ferroelectric and ionic contributions in electroresistance of FTJ devices, facilitating deep understanding of nonvolatile resistive memories.
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