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The formation process for planar solid electrolytes in the CeO2-Y2O3 system has been studied using efficient, high-performance, high-resolution microplotter printing technology, using functional ink based on nanopowders (the average size of crystallites was 12–15 nm) of a similar composition obtained by programmed coprecipitation of metal hydroxides. The dependence of the microstructure of the oxide nanoparticles obtained and their crystal structure on yttrium concentration has been studied using a wide range of methods. According to X-ray diffraction (XRD), the nanopowders and coatings produced are single-phase, with a cubic crystal structure of the fluorite type, and the electronic state and content of cerium and yttrium in the printed coatings have been determined using X-ray photoelectron spectroscopy (XPS). The results of scanning electron (SEM) and atomic force microscopy (AFM) have shown that the coatings produced are homogeneous, they do not contain defects in the form of fractures and the height difference over an area of 1 µm2 is 30–45 nm. The local electrophysical characteristics of the oxide coatings produced (the work function of the coating surface, capacitance values, maps of the surface potential and capacitive contrast distribution over the surface) have been studied using Kelvin-probe force microscopy (KPFM) and scanning capacitive microscopy (SCM). Using impedance spectroscopy, the dependence of the electrophysical characteristics of printed planar solid electrolytes in the CeO2-Y2O3 system on yttrium content has been determined and the prospects of the technology developed for the manufacture of modern, intermediate-temperature, solid oxide fuel cells have been demonstrated.

Atomically thin tungsten disulfide (WS2) film is a promising material for flexible electronics and optoelectronics. The ability of its controllable synthesis over a large area is an essential task ...

This work reports a radical-enhanced atomic layer deposition (REALD) process using WH2(Cp)2–O*–H* reaction cycles (Cp = cyclopentadienyl group) to grow WO3–x films with a wide range of tunable oxyg...

Neuromorphic capabilities of a self-aligned complementary metal-oxide-semiconductor compatible W/WOx/HfO2/Ru cell in a 3D vertical memristive structure were investigated. We show that the device exhibits nonfilamentary forming-free multilevel resistive switching with gradual resistance change. In addition, the poor retention of a low resistance state allows integration of these structures in architectures that require short-term memory characteristics such as reservoir computing systems. The ability of the device to rely on the temporal sequence of the stream was tested with the digit recognition task. Since a WOx layer was obtained by thermal oxidization and HfO2 and Ru layers were grown by atomic layer deposition methods, the device is suitable for high-density systems with high connectivity within a neural network.

The feasibility of growing atomically thin MoS2 films (down to two monolayers) on several tens of cm2 area was demonstrated by first depositing the MoO3 thin film by using an atomic layer depositio...

While the conductance of a first-order memristor is defined entirely by the external stimuli, in the second-order memristor it is governed by the both the external stimuli and its instant internal state. As a result, the dynamics of such devices allows to naturally emulate the temporal behavior of biological synapses, which encodes the spike timing information in synaptic weights. Here, we demonstrate a new type of second-order memristor functionality in the ferroelectric HfO2-based tunnel junction on silicon. The continuous change of conductance in the p+-Si/Hf0.5Zr0.5O2/TiN tunnel junction is achieved via the gradual switching of polarization in ferroelectric domains of polycrystalline Hf0.5Zr0.5O2 layer, whereas the combined dynamics of the built-in electric field and charge trapping/detrapping at the defect states at the bottom Si interface defines the temporal behavior of the memristor device, similar to synapses in biological systems. The implemented ferroelectric second-order memristor exhibits various synaptic functionalities, such as paired-pulse potentiation/depression and spike-rate-dependent plasticity, and can serve as a building block for the development of neuromorphic computing architectures.

The formation of NiO nanosheets (average CSR size is 10.4 nm) through the hydrothermal method using a heteroligand complex of composition [Ni(C5H7O2)2-x(C4H9O)x] as a precursor was studied. Using the obtained oxide nanopowder and pneumatic microextrusion printing, NiO coating was applied to the surface of a specialized Pt/Al2O3/Pt chip, and chemosensor properties were investigated in the detection of various gases. It was determined that when CO, NH3, H2, and NO2 were detected, the conductivity of the NiO coating changed from p- to n-type with increasing temperature. Using XPS, XRD, and Raman spectroscopy, it was found that upon exposure to H2S, the surface of NiO coating partially undergoes irreversible chemical modification with the formation of nickel sulfide, resulting in a significant change in the sensory properties of the coating. It was shown that the formed receptor material exhibits the greatest response when detecting H2S, and the proposed approach, combining hydrothermal synthesis and printing technology, is promising for the creation of modern components of resistive gas sensors.

The formation process for planar solid electrolytes in the CeO

Hf0.5Zr0.5O2 thin films are one of the most appealing HfO2-based ferroelectric thin films, which have been researched extensively for their applications in ferroelectric memory devices. In this work, a 1 mol % La-doped Hf0.5Zr0.5O2 thin film was grown by plasma-assisted atomic layer deposition and annealed at temperatures of 450 and 500 °C to crystallize the film into the desired orthorhombic phase. Despite the use of a lower temperature than that used in previous reports, the film showed highly promising ferroelectric properties—a remnant polarization of ∼30 μC/cm2 and switching cycle endurance up to 4 × 1010. The performance was much better than that of undoped Hf0.5Zr0.5O2 thin films, demonstrating the positive influence of La doping. Such improvements were mainly attributed to the decreased coercive field (by ∼30% compared to the undoped film), which allowed for the use of a lower applied field to drive the cycling tests while maintaining a high polarization value. La doping also decreased the leakage...

We study the charge transport mechanism in ferroelectric Hf0.5Zr0.5O2 thin films. Transport properties of the leakage currents in Hf0.5Zr0.5O2 are described by phonon-assisted tunneling between traps. Comparison with transport properties of amorphous Hf0.5Zr0.5O2 demonstrates that the transport mechanism does not depend on the crystal structure. The thermal trap energy of 1.25 eV and optical trap energy of 2.5 eV in Hf0.5Zr0.5O2 were determined based on comparison of experimentally measured data on transport with simulations within phonon-assisted tunneling between traps in dielectric films. We found that the trap density in ferroelectric Hf0.5Zr0.5O2 is slightly less that one in amorphous Hf0.5Zr0.5O2. A hypothesis that oxygen vacancies are responsible for the charge transport in Hf0.5Zr0.5O2 is confirmed by electronic structure ab initio simulation.

Pairing two-dimensional semiconductors with ferroelectric films may allow for the development of hybrid electronic devices that would not only exhibit a combination of the functional properties of both material groups but would also reveal unusual characteristics emerging from coupling between these properties. Here, we report the observation of a considerable (up to 103 at 0.8 V read bias) polarization-mediated tunneling electroresistance (TER) effect in Hf0.5Zr0.5O2 (HZO) ferroelectric tunnel junctions (FTJs) employing MoS2 as one of the electrodes. It was found that for this type of hybrid FTJs, a change in resistance upon polarization reversal could be described by Fowler–Nordheim tunneling. The underlying mechanism for the enhanced TER effect is a polarization-mediated accumulation or depletion of the majority carriers at the MoS2/HZO interface, which results in a change in the effective barrier shape seen by the tunneling electrons. Given the compatibility of HfO2-family ferroelectrics with CMOS technology and a possibility of large scale growth and transfer of MoS2 films, our results provide a pathway for fabrication of high-density nonvolatile memory and data storage systems based on hybrid FTJs.

For the decade, ferroelectric hafnium oxide films are attracting the interest as a promising functional material for nonvolatile ferroelectric random access memory due to full scalability and complementary metal-oxide-semiconductor integratability. Despite the significant progress in key performance parameters, particularly, the readout charge and voltage as well as the endurance, the developed devices can only be implemented by the electronics industry if they exhibit a standard retention time of 10 years. Material engineering modifies not only target ferroelectric properties, but also the retention time. To understand how to maintain the sufficient retention, the physical mechanism behind it should be clarified. For this purpose, we have fabricated the capacitor memory cell with a high rate of retention loss. Comparing the device performance with the results of capacitance transient spectroscopy, operando hard X-ray photoelectron spectroscopy and in situ piezoresponse force microscopy, we have concluded that the retention loss is caused by the accumulation of the positively charged oxygen vacancies at the interfaces with capacitor electrodes. The redistribution of charges during long-term storage of information is fully defined by the domain structure in memory cell.

The mechanism responsible for the charge transport in thin ferroelectric Hf0.5Zr0.5O2 films has been studied. It is shown that in these films the transport mechanism is phonon-assisted tunneling between the traps. The optimal thickness of dielectric film for TiN/Hf0.5Zr0.5O2/Pt structures is determined. As a result of comparing the experimental current–voltage (I–V) characteristics of TiN/Hf0.5Zr0.5O2/Pt structures with the calculated ones, the thermal and optical energies of the traps are determined and the concentration of the traps is estimated. A comparison between the transport properties of ferroelectric and amorphous Hf0.5Zr0.5O2 films is carried out. It is shown that the charge transport mechanism in this dielectric does not depend on its crystalline phase. A method for decreasing leakage currents in Hf0.5Zr0.5O2 is proposed. A study of the resource of repolarization cycles for TiN/Hf0.5Zr0.5O2/TiN metal-dielectric-metal (MDM) structures fully grown by atomic layer deposition (ALD) has been carried out.

We report the influence of an ultrathin Ru bottom electrode on ferroelectric properties of fully atomic layer deposition (ALD)-grown Hf0.5Zr0.5O2 (HZO) and La-doped Hf0.5Zr0.5O2 (HZLO)-based ferroelectric capacitors. We show that the Ru bottom electrode deposited by radical enhanced ALD (REALD) improves the remanent polarization of both capacitors considerably. The origin of such a phenomenon is established by grazing-incidence and symmetrical θ–2θ x-ray diffraction measurements. HZO films on Ru exhibit the orthorhombic phase, which is highly (002)-textured in the out-of-plane direction as compared to HZO on TiN. HZLO films demonstrate the rise of (111) intensity of the orthorhombic phase when it is grown on Ru. Both types of capacitors with Ru exhibit a lower wake-up degree as compared to the ones with TiN, which is assumed to be due to the difference in the bottom interface properties. At the same time, both HZO and HZLO on Ru suffer from the relatively early breakdown during electric field cycling, which is presumably due to the high surface roughness of REALD Ru. Taking into account the continuous search for the new precursor's chemicals and ALD processes for Ru, which would be able to provide smother films, ALD Ru might be promising for the hafnium oxide-based ferroelectric random access memory.

Сombining the sol–gel method and pen plotter printing, using the hydrolytically active heteroligand complex [Co(C5H7O2)2-x(C4H9O)x] as a component of a new functional ink, Co3O4 thin films were produced on the surface of substrates of various types. The influence of synthesis conditions and print modes on the microstructure, optical, electrophysical and sensor properties of planar nanomaterials was comprehensively studied. The optical band gap energies associated with charge transfer for transitions O2-→Co3+ and O2-→Co2+ of the obtained thin films were evaluated. Using Kelvin probe force microscopy and impedance spectroscopy, the electrophysical characteristics (the electronic work function of the film surface, the temperature dependence of electrical conductivity, and the activation energy of electrical conductivity) of the obtained Co3O4 films were determined. The sensitivity of printed cobalt(II, III) oxide thin films with respect to various gases (Н2, СН4, СО and NO2) was studied. It was established that the obtained samples demonstrated the highest sensor response when detecting CO and NO2 in the operating temperature range of 150–200°С. The prospects of the proposed synthesis method and printing technology when forming Co3O4 thin-film nanostructures to create electrodes of supercapacitors and receptor components of resistive CO and NO2 gas sensors were shown.

Hf

Display Omitted Hf0.5Zr0.5O2 films with wide range of thickness were grown by ALD.Structural and electrical properties were studied after PMA and PDA.Ferroelectricity achievement in case of electrode-free annealing was demonstrated.The difference of structural properties in case of PMA and PDA was provided.The explanation of films structural difference after PMA and PDA was proposed. The structural and electrical properties of Hf0.5Zr0.5O2 thin films after post deposition and post metallization annealing were investigated. The possibility of the annealing without top electrodes for attainment of ferroelectric properties in Hf0.5Zr0.5O2 thin films was demonstrated. It was, however, shown, that the annealing in presence of top electrode leads to the more preferable crystallization to polar o-phase and the increase in the remanent polarization value. The influence of the film thickness on the structural and ferroelectric properties was studied both after post metallization and post deposition annealing. The optimal Hf0.5Zr0.5O2 thickness was found to be equal to ~19nm for electrode free annealing, which is promising value for modern nanoscale ferroelectric devices.

The charge transport mechanism in thin amorphous and ferroelectric Hf0.5Zr0.5O2 films has been studied. It has been shown that the transport mechanism in studied materials does not depend on the crystal phase and is phonon-assisted tunneling between traps. The comparison of the experimental current–voltage characteristics of TiN/Hf0.5Zr0.5O2/Pt structures with the calculated ones provides the trap parameters: thermal energy of 1.25 eV and the optical energy of 2.5 eV. The trap concentration has been estimated as ~1019–1020 cm–3.

In this paper atomic-layer deposition (ALD) HfxAl1–xOy thin films with a wide range of metal components concentrations (x = 0.2−0.8) for metal–insulator–metal (MIM) capacitors were investigated with emphasis on the chemical properties and phase composition. It was shown by X-ray diffraction (XRD) that all films are amorphous. X-ray photoelectron spectroscopy (XPS) revealed the same energy position with respect to the valence-band maximum of Al2p and Hf4f lines and a continuous shift of O1s and O-KLL lines toward the higher binding energy (0.45 and 2.2 eV, respectively) with increase of Al content. Both the shape and position of O1s and O-KLL lines indicated the inability to deconvolute it on sublines related to the binary oxides. The calculated modified Auger parameter indicated the change of the ionicity of the bonding in HfxAl1–xOy films with change of the composition. Thus, it was proposed that HfxAl1–xOy films in all the studied composition range represent amorphous solid solutions. The continuous change of energy bandgap measured by reflected electron energy loss spectroscopy (REELS) from ∼6.5 eV for Al2O3 to ∼5.4 eV for HfO2 and XRD data do not contradict this assumption. Correlation between structural properties of HfxAl1–xOy films and electrical properties of MIM capacitors based on them was also shown, that is, continuous change in capacitance density (from 3.1 to 7.4fF/µm2), leakage current density and quadratic voltage coefficient of capacitance with composition change was observed.

This work demonstrates by in vacuo X-ray photoelectron spectroscopy and grazing-incidence X-ray diffraction that Ru(EtCp)2 and O* radical-enhanced atomic layer deposition, where EtCp means the ethylcyclopentadienyl group, provides the growth of either RuO2 or Ru thin films depending on the deposition temperature (Tdep), while different mechanisms are responsible for the growth of RuO2 and Ru. The thin films deposited at temperatures ranging from 200 to 260 °C consisted of polycrystalline rutile RuO2 phase revealing, according to atomic force microscopy and the four-point probe method, a low roughness (∼1.7 nm at 15 nm film thickness) and a resistivity of ≈83 µΩ cm. This low-temperature RuO2 growth was based on Ru(EtCp)2 adsorption, subsequent ligand removal, and Ru oxidation by active oxygen. The clear saturative behavior with regard to the precursor and reactant doses and each purge time, as well as the good step coverage of the film growth onto 3D structures, inherent to genuine surface-controlled atomic layer deposition, were confirmed for the lowest Tdep of 200 °C. However, at Tdep = 260 °C, a competition between film growth and etching was found, resulted in not-saturative growth. At higher deposition temperatures (300-340 °C), the growth of metallic Ru thin films with a resistivity down to ≈12 µΩ cm was demonstrated, where the film growth was proved to follow a combustion mechanism known for molecular oxygen-based Ru growth processes. However, this process lacked the truly saturative growth with regard to the precursor and reactant doses due to the etching predominance.

The crystalline structure and electrical response of La-doped HfO2-ZrO2 thin films of which processing temperature did not exceed 400 °C were examined, where the La-doping concentration was varied from zero to ≈2 mol. %. The film structure and associated properties were found to vary sensitively with the minute variation in the La-concentration, where the ferroelectric response at low La-concentration ( ≈1 mol. %, which was accompanied by a significant increase in dielectric permittivity. La-doping was found to be very effective in inhibiting the monoclinic phase formation and in decreasing the leakage current. Notably, the high coercive field, which was one of the most significant problems in this material system, could be decreased by ∼35% at the most promising La-concentration of 0.7 mol. %. As a result, a highly promising field cycling endurance up to 1011 cycles could be secured while maintaining a high remnant polarization value (≥25 μC/cm2). This is one of the best results in this field of the authors' knowledge.

The influence of La content on the ferroelectric properties of HfO2-ZrO2 thin films was examined for integrated electrostatic supercapacitor applications. A transition from ferroelectric to antiferroelectric-like behavior, accompanied by a significant increase of energy storage density value and efficiency, was observed with the increasing La concentration in La-doped HfO2-ZrO2-based capacitor structures, where the processing temperature remained below 400 °C. The combination of high energy storage density value (≈50 J/cm3) with high efficiency (70%) was obtained for the film with the highest La content (2.0 mol. %). The 2.0 mol. % La-doped HfO2-ZrO2-based capacitor structures were field cycled up to 109 times and were found to provide >40 J/cm3 energy storage density along with up to 80% efficiency. Moreover, the high thermal stability of such capacitors was confirmed. The founded property combination makes the La-doped HfO2-ZrO2 thin films suitable for integrated energy storage and pulse-power devices.The influence of La content on the ferroelectric properties of HfO2-ZrO2 thin films was examined for integrated electrostatic supercapacitor applications. A transition from ferroelectric to antiferroelectric-like behavior, accompanied by a significant increase of energy storage density value and efficiency, was observed with the increasing La concentration in La-doped HfO2-ZrO2-based capacitor structures, where the processing temperature remained below 400 °C. The combination of high energy storage density value (≈50 J/cm3) with high efficiency (70%) was obtained for the film with the highest La content (2.0 mol. %). The 2.0 mol. % La-doped HfO2-ZrO2-based capacitor structures were field cycled up to 109 times and were found to provide >40 J/cm3 energy storage density along with up to 80% efficiency. Moreover, the high thermal stability of such capacitors was confirmed. The founded property combination makes the La-doped HfO2-ZrO2 thin films suitable for integrated energy storage and pulse-power devices.

We create thin metallic films formed as a size-ordered deposition of Ni nanoclusters whose sizes are distributed over the range of 2–7 nm. The morphology, chemical composition, and electrical characteristics of the films are measured. The conductivity of the films under investigation changes approximately as the inverse square root of the average nanocluster size. We observe experimentally that, under irradiation by electrons with energies of 10–25 keV, the films show signs of being subjected to the electromotive force. We discuss how this effect is connected with the size-ordered spatial distribution of metallic nanoclusters. We analyze the possibility of using 63Ni nanocluster films in betavoltaic battery units and estimate the expected efficiency of converting β-decay energy into electricity.

The structural and ferroelectric properties of lightly La-doped (1 mol. %) HfO2 thin films grown by plasma-assisted atomic layer deposition were examined. An annealing temperature as low as 400 °C crystallized the film into the desired orthorhombic phase, which resulted in it displaying promising ferroelectric performance. The remanent polarization (Pr) increased with annealing temperature, but the performance enhancement seemed to saturate at 500 °C. A slight decrease in the dielectric constant, which was associated with the preferential formation of a polar orthorhombic phase at higher temperatures, was also observed. The long-term wake-up effect, i.e., a marked rise in the 2Pr value during field cycling, was demonstrated for films processed at all annealing temperatures. The presence of domain groups with opposite internal electric biases was found in the pristine state, while the internal bias distribution became more uniform during wake-up. The endurance of up to 4 × 108 switching cycles without marked fatigue using bipolar pulses with a duration of 600 ns, and an amplitude of ±3 MV/cm was demonstrated.

In this work chemical and electrical properties of TiN films, grown by low temperature plasma-enhanced atomic layer deposition (PE-ALD) process from TiCl4 and NH3, were investigated. Electrical resistivity as low as 250 μOhm × cm, as well as the lowest Cl impurity content, was achieved at 320 °C. Full-ALD Hf0.5Zr0.5O2-based metal-ferroelectric-metal capacitor with TiN electrodes was fabricated and its electrical properties were investigated. It was also shown that the proposed PE-ALD process provides an early film continuity, which was confirmed by ultrathin fully continuous film growth. Such ultrathin (3 nm) and fully continuous TiN film was also successfully implemented as the top electrode to Hf0.5Zr0.5O2-based ferroelectric capacitor. Angle-resolved X-ray photoelectron spectroscopy (AR-XPS) was used for its thickness determination and a visible wake-up effect in underlying Hf0.5Zr0.5O2 layer was clearly observed.

Hafnia was considered as a paraelectric material until observation of ferroelectric effect in thin films of doped HfO2 after high-temperature annealing (~1000°C). [T.S. Böscke et al., Appl. Phys. Lett. 99, 102903 (2011); S. Mueller et al., Adv. Function. Mater. 22, 2412 (2012)]. Of particular interest is the fact that ferroelectricity was also demonstrated in thin of the solid solution Hf0.5Zr0.5O2 which requires annealing at significantly lower temperatures [J. Müller et al., Appl. Phys. Lett. 99, 112901 (2011); J. Müller et al., Nano Lett. 12, 4318 (2012); M.H. Park et al., Appl. Phys. Lett. 102, 112914 (2013); A. Chernikova et al., Microelectron. Eng. 147, 15 (2015)]. Ferroelectricity in these materials is associated with the ability to stabilize noncentrosymmetric orthorhombic phase Pbc2 1 [J. Müller et al., Nano Lett. 12, 4318 (2012)]. It should be noted that the hafnia-based materials have a number of advantages over conventional ferroelectric regarding compatibility with technological processes used in microelectronics, and has already demonstrated their ability to provide very high density of elements. Taking into account advantages of the ferroelectric random access memory (FeRAM) as non-volatile, high-speed performance, high number of switching cycles, the discovery of ferroelectric effect in these materials gave an impetus for development of universal memory concept, which may lead to a significant breakthrough in the development of memory devices [M.H. Park et al., Adv. Mater. 27, 1811 (2015)]. An unsolved problem in the way of development of FeRAM-based universal memory is the spontaneous depolarization of the active medium, which leads to short data storage time (retention) that is observed in Ref. [C.-H. Cheng, A. Chin, IEEE Electron Dev. Lett. 35, 138 (2014)]. One of the possible reason of spontaneous depolarization is leakage currents through the ferroelectric thin films. High-κ Hf0.5Zr0.5O2 thin films (κ>16 depending on structure phase) can be used as sub-gate dielectrics in MOSFET and FinFET transistors instead of SiO2. Thus, it is very important to know charge transport mechanisms in thin dielectrics films to control the leakage currents for development of high quality memory devices. Purpose of the present work is to study charge transport mechanism in ferroelectric Hf0.5Zr0.5O2. Transport measurements were performed for TiN/Hf0.5Zr0.5O2/Pt structures. Test structure were fabricated with atomic layer deposition (ALD) technique. 10-nm-thick TiN layer was deposited on oxidized Si (100) substrate. Then the 10-nm-thick Hf0.5Zr0.5O2 films we deposited at 240°C from TEMAHf and TEMAZr precursors using H2O as oxygen source. Laser ellipsometry and Rutherford backscattering spectroscopy confirmed the thickness and stoichiometry of as deposited Hf0.5Zr0.5O2 films. Some samples were annealed at 400°C in N2 environment during 30sec (rapid thermal annealing, RTA). The crystalline structures of as deposited and annealed films were examined by symmetrical X-Ray diffraction (XRD). Pt top electrodes (thickness of ~30nm) were deposited through shadow mask with round holes (area is 7.1×104μm2) by electron beam evaporation on as deposited Hf0.5Zr0.5O2films and after RTA. The electronic structure of Hf0.5Zr0.5O2 was calculated within the spin polarized density functional theory using the ab initio simulation code Quantum ESPRESSO [P. Giannozzi et al., J. Phys.: Condens. Matter 21, 395502 (2009)] with B3LYP hybrid exchange-correlation functional. The oxygen vacancy was generated by the removal of an O atom, followed by relaxation of remaining atoms in 96-atom supercell. The XRD spectra of Hf0.5Zr0.5O2 films show that as deposited films have amorphous structure (a-Hf0.5Zr0.5O2), while annealed films are polycrystalline with monoclinic (P2 1/c), tetragonal (P4 2/nmc) and noncentralsymmetric orthorhombic (Pbc2 1) phases. The presence of ferroelectric properties of f-Hf0.5Zr0.5O2 films after RTA is confirmed by observing characteristic hysteresis on the P-V plate for Pt/ Hf0.5Zr0.5O2/TiN structures. Comparison of experimentally measured leakage currents-voltage dependencies at different temperatures (I-V-T) with Frenkel model of charged trap ionization returns overestimated value of dynamic permittivity with respect to predicted by ab initio calculations and underestimated value of frequency factor ν<

We report the possibility of employment of low temperature (≤330 °C) plasma-enhanced atomic layer deposition for the formation of both electrodes and hafnium-oxide based ferroelectric in the metal-insulator-metal structures. The structural and ferroelectric properties of La doped HfO2-based layers and its evolution with the change of both La content (2.1, 3.7 and 5.8 at. %) and the temperature of the rapid thermal processing (550–750 °C) were investigated in detail. Ferroelectric properties emerged only for 2.1 and 3.7 at. % of La due to the structural changes caused by the given doping levels. Ferroelectric properties were also found to depend strongly on annealing temperature, with the most robust ferroelectric response for lowest La concentration and intermediate 650 °C annealing temperature. The long term wake-up effect and such promising endurance characteristics as 3 × 108 switches by bipolar voltage cycles with 30 μs duration and ± 3 MV/cm amplitude without any decrease of remnant polarization value were demonstrated.