Recently, doped HfO2 thin films have attracted considerable attention because of promising applications in complementary metal–oxide–semiconductor (CMOS)‐compatible ferroelectric memories. Herein, the ferroelectric properties and polarization fatigue of La:HfO2 thin‐film capacitors are reported. By varying the substrate lattice constant and film thickness, a robust remanent polarization of ≈16 μC cm−2 is achieved in a 12 nm‐thick Pt/La:HfO2/La0.67Sr0.33MnO3 capacitor. Fatigue measurements are conducted using designed pulse sequences, in which the voltage, pulse width, and interval time are changed to observe the evolution of switchable polarization with increasing cycles. Severe fatigue is observed when the La:HfO2 capacitors are partially switched and the interval between the bipolar switching is elongated. These behaviors may be ascribed to the domain wall pinning scenario, in which domain switching is blocked by the migration and aggregation of charges on non‐electroneutral walls. Further analysis of the fatigue behaviors with a nucleation‐limited‐switching model shows that the mean time and activation field for polarization switching are increased in fatigued La:HfO2 capacitors because electrical stimuli are required to disperse the aggregated charges before the domains are set free. These results facilitate the design and fabrication of HfO2‐based ferroelectric memories with improved device reliability.
As nanoelectronic synapses, memristive ferroelectric tunnel junctions (FTJs) have triggered great interest due to the potential applications in neuromorphic computing for emulating biological brains. Here, we demonstrate multiferroic FTJ synapses based on the ferroelectric modulation of spin-filtering BaTiO3/CoFe2O4 composite barriers. Continuous conductance change with an ON/OFF current ratio of ∼54 400% and long-term memory with the spike-timing-dependent plasticity (STDP) of synaptic weight for Hebbian learning are achieved by controlling the polarization switching of BaTiO3. Supervised learning simulations adopting the STDP results as database for weight training are performed on a crossbar neural network and exhibit a high accuracy rate above 97% for recognition. The polarization switching also alters the band alignment of CoFe2O4 barrier relative to the electrodes, giving rise to the change of tunneling magnetoresistance ratio by about 10 times and even the reversal of its sign depending upon the resistance states. These results, especially the electrically switchable spin polarization, provide a new approach toward multiferroic neuromorphic devices with energy-efficient electrical manipulations through potential barrier design. In addition, the availability of spinel ferrite barriers epitaxially grown with ferroelectric oxides also expends the playground of FTJ devices for a broad scope of applications.
Role of charged defects in resistance fatigue of ferroelectric tunnel junctions has been revealed at atomic scale.
Recently, tunnel junction devices adopting semiconducting Nb:SrTiO3 electrodes have attracted considerable attention for their potential applications in resistive data storage and neuromorphic computing. In this work, we report on a comparative study of Pt/insulator/Nb:SrTiO3 tunnel junctions between ferroelectric BaTiO3 and nonferroelectric SrTiO3 and LaAlO3 barriers to reveal the role of polarization in resistance switching properties. Although hysteretic behaviors appear in current–voltage measurements of all devices regardless of the barrier character, significantly improved current ratios by more than three orders of magnitude are observed in the Pt/BaTiO3/Nb:SrTiO3 tunnel junctions due to the dominance of polarization in modulation of junction barrier profiles between the low and high resistance states. The switchable polarization also gives rise to enhanced resistance retention since the electron diffusion that smears the barrier contrast of the bistable resistance states is suppressed by the polar BaTiO3/Nb:SrTiO3 interface associated with the ferroelectric bound charges. These polarization-induced effects are absent in the nonferroelectric Pt/SrTiO3/Nb:SrTiO3 and Pt/LaAlO3/Nb:SrTiO3 devices in which serious resistance state decay, described by Fick’s second law, is observed since there are no switchable interface charges on SrTiO3/Nb:SrTiO3 and LaAlO3/Nb:SrTiO3 to block the electron diffusion. In addition, the Pt/BaTiO3/Nb:SrTiO3 device also exhibits an excellent switching endurance up to ∼4.0 × 106 bipolar cycles. These enhancements indicate the importance of ferroelectric polarization for achieving high-performance resistance switching and suggest that metal/ferroelectric/Nb:SrTiO3 tunnel junctions are promising candidates for nonvolatile memory applications.
Freestanding perovskite thin films display many unprecedented properties and exhibit the potential to be easily integrated on other non-oxide substrates or layers. In this work, we demonstrated a pathway to synthesis freestanding perovskite oxide thin films by using brownmillerite SrCoO2.5 as a sacrificial layer. Four representative freestanding perovskite oxide films, e.g., ferromagnetic SrRuO3, La0.7Sr0.3MnO3, dielectric SrTiO3, and ferroelectric Pb(Zr0.2Ti0.8)O3, were produced by etching SrCoO2.5 in Fe(NO3)3 weak acidic solution at room temperature. A 80 nm SrRuO3, which served as an H+ conduction channel, was deposited as a bottom layer of SrCoO2.5 to trigger a quick dissolution for the exfoliation of SrTiO3 and Pb(Zr0.2Ti0.8)O3 poor H+ conductor. Their crystal structure and physical properties were well retained in transferred films. Our work demonstrated the wide applicability of SrCoO2.5 as a sacrificial layer on the synthesis of freestanding perovskite oxide thin films.
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