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Oxygen vacancies play a crucial role in stabilizing the ferroelectric phase in hafnium (Hf) oxide-based thin films and in shaping the evolution of their ferroelectric properties. In this study, we directly manipulated the oxygen vacancy concentration in Hf0.5Zr0.5O2−x (HZO) ferroelectric thin films in situ using oxygen plasma treatment. We scrutinized the variations in the ferroelectric properties of HZO films across different oxygen vacancy concentrations by integrating the findings from ferroelectric performance tests. Additionally, we elucidated the mechanism underlying the influence of oxygen vacancies on the coercive field and polarization properties of HZO ferroelectric films through the first-principles density functional theory (DFT) calculations. Finally, to study the impact of oxygen vacancies on the practical application of HZO ferroelectric synaptic devices, leveraging the plasticity of the ferroelectric polarization, we constructed a multilayer perceptron (MLP) network. We simulated its recognition accuracy and convergence speed under different oxygen vacancy concentrations in the MNIST recognition task. [ABSTRACT FROM AUTHOR]

Oxygen ions' migration is the fundamental resistive switching (RS) mechanism of the binary metal oxides-based memristive devices, and recent studies have found that the RS performance can be enhanced through appropriate oxygen plasma treatment (OPT). However, the lack of experimental evidence observed directly from the microscopic level of materials and applicable understanding of how OPT improves the RS properties will cause significant difficulties in its further application. In this work, we apply scanning probe microscope (SPM)-based techniques to study the OPT-enhanced RS performance in prototypical HfOx based memristive devices through in situ morphology and electrical measurements. It is first found that the structural deformations in HfOx nanofilm induced by migration of oxygen ions and interfacial electrochemical reactions can be recovered by OPT effectively. More importantly, such structural deformations no longer occur after OPT due to the strengthening in lattice structure, which directly illustrates the enhanced quantity of HfOx nanofilm and the nature of enhanced RS properties after OPT. Finally, the underlying mechanisms of OPT-enhanced RS performance are analyzed by the results of X-ray photoelectron spectroscopic (XPS) surface analysis. In the OPT-enhanced HfOx nanofilm, oxygen vacancies in crystalline regions can be remarkably reduced by active oxygen ions' implantation. The oxygen ions transport will depend considerably on the grain boundaries and OPT-enhanced lattice structure will further guarantee the stability of conductive filaments, both of which ensure the uniformity and repeatability in RS processes. This study could provide a scientific basis for improving RS performance of oxides-based memristive devices by utilizing OPT. [ABSTRACT FROM AUTHOR]

Bi4Ti2.99Mn0.01O12 (BTM) thin films with different ratio of neodymium (Nd) doping were prepared on Pt(111)/Ti/SiO2/Si(100) substrates through a sol-gel method. The effects of Nd doping on domain dynamics and temperature-dependent fatigue behaviors of BTM thin films were systematically studied. The polarization fatigues of BTM (not doped) and Bi3.5Nd0.5Ti2.99Mn0.01O12 (BNTM05) thin films first get better with the increasing temperature (T) from 300 to 350 K and then become worse from 350 to 400 K, while Bi3.15Nd0.85Ti2.99Mn0.01O12 (BNTM85) thin films show enhanced fatigue endurance from 300 to 400 K. It can be shown that the long-range diffusion of oxygen vacancies in BTM thin film happens more easily through the impedance spectra analysis with T from 300 to 475 K, which can be verified by a lower activation energies (0.13–0.14 eV) compared to those of BNTM05 and BNTM85 (0.17–0.21 eV). Using a temperature-dependent piezoresponse force microscopy (PFM), we have found more responsive domain fragments in Nd-substituted films. The microscopic domain evolution from 298 to 448 K was done to further explain that the domain wall unpinning effect has been enhanced with increasing T. The correlation between microscopic domain dynamics and macroscopic electrical properties clearly demonstrates the effects of charged domain wall in Nd-doped BTM thin films during the fatigue tests. [ABSTRACT FROM AUTHOR]

Bi₄Ti 2.99 Mn 0.01 O 12 (BTM) thin films with different ratio of neodymium (Nd) doping were prepared on Pt(111)/Ti/SiO₂/Si(100) substrates through a sol-gel method. The effects of Nd doping on domain dynamics and temperature-dependent fatigue behaviors of BTM thin films were systematically studied. The polarization fatigues of BTM (not doped) and Bi 3.5 Nd 0.5 Ti 2.99 Mn 0.01 O 12 (BNTM05) thin films first get better with the increasing temperature ( T ) from 300 to 350 K and then become worse from 350 to 400 K, while Bi 3.15 Nd 0.85 Ti 2.99 Mn 0.01 O 12 (BNTM85) thin films show enhanced fatigue endurance from 300 to 400 K. It can be shown that the long-range diffusion of oxygen vacancies in BTM thin film happens more easily through the impedance spectra analysis with T from 300 to 475 K, which can be verified by a lower activation energies (0.13⁻0.14 eV) compared to those of BNTM05 and BNTM85 (0.17⁻0.21 eV). Using a temperature-dependent piezoresponse force microscopy (PFM), we have found more responsive domain fragments in Nd-substituted films. The microscopic domain evolution from 298 to 448 K was done to further explain that the domain wall unpinning effect has been enhanced with increasing T . The correlation between microscopic domain dynamics and macroscopic electrical properties clearly demonstrates the effects of charged domain wall in Nd-doped BTM thin films during the fatigue tests.