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In this Letter, the robust ferroelectric properties of low-temperature (350 °C) Hf0.5Zr0.5O2 (HZO) films are investigated. We demonstrate that the lower crystallization temperature of HZO films originates from a densified film deposition with an anhydrous H2O2 oxidant in the atomic layer deposition process. As a consequence of this densification, H2O2-based HZO films showed completely crystallinity with fewer defects at a lower annealing temperature of 350 °C. This reduction in the crystallization temperature additionally suppresses the oxidation of TiN electrodes, thereby improving device reliability. The low-temperature crystallization process produces an H2O2-based HZO capacitor with a high remanent polarization (Pr), reduced leakage current, high breakdown voltage, and better endurance. Furthermore, while an O3-based HZO capacitor requires wake-up cycling to achieve stable Pr, the H2O2-based HZO capacitor demonstrates a significantly reduced wake-up nature. Anhydrous H2O2 oxidant enables the fabrication of a more reliable ferroelectric HZO device using a low process thermal budget (350 °C). [ABSTRACT FROM AUTHOR]

In this Letter, a high-pressure annealing (HPA) process is proposed as a way to reduce the thermal budget of Hf0.5Zr0.5O2 (HZO) thin films with ferroelectric behaviors. The low-thermal-budget process is essential for integrating ferroelectric devices in the back-end-of-line to provide more functionalities and effective memory area. For the HZO film annealed at 300 °C using the HPA process, an orthorhombic phase responsible for ferroelectric behavior was formed with a decrease in film thickness, resulting in a remanent polarization (Pr) of ∼13 μC/cm2 (i.e., 2Pr of ∼26 μC/cm2). Meanwhile, when only the annealing time was increased at 300 °C without applying pressure, the HZO film did not crystallize and exhibited linear dielectric properties. Consequently, the HZO films (<10 nm) can be crystallized by applying pressure (15 atm) even at low temperatures of 300 °C, thereby obtaining ferroelectric properties. [ABSTRACT FROM AUTHOR]

Since HfO2‐based ferroelectric films were reported in 2011, several doping/alloying elements have been introduced to secure interesting ferroelectric/antiferroelectric properties of Hf‐based fluorite‐structured thin films. Using a conventional approach by atomic layer deposition (ALD), an enormous number of experiments would be required to reveal the compositional effects of doping/alloying components in ternary and quaternary systems. Therefore, for a comprehensive study of the ferroelectric properties of HfxZr1−xO2, a novel combinatorial ALD technique that enables the fabrication of multicomponent films with a different composition ratio and thickness via saturated/non‐saturated ALD without changing the supercycle of each material is reported. The gradient of the amount of HfO2 over a 100 mm substrate is achieved using a lower Hf‐precursor temperature that results in an insufficient Hf‐precursor dose for saturated deposition. Systematic study on the HfxZr1−xO2 combinatorial library is carried out by spectroscopic ellipsometry, X‐ray photoelectron spectroscopy, and X‐ray diffraction. Furthermore, TiN/HfxZr1−xO2/TiN capacitors are fabricated to measure the remnant polarization. The obtained results clearly show the ferroelectric–antiferroelectric transition according to continuous composition change instead of discrete research. Therefore, a highly productive method for studying ferroelectricity changes in terms of a doping and a composition of HfO2‐based ferroelectric thin films through a novel ALD combinatorial approach is proposed. [ABSTRACT FROM AUTHOR]

Ferroelectric Hf 0.5 Zr 0.5 O 2 (HZO) capacitors have been extensively explored for in-memory computing (IMC) applications due to their nonvolatility and back-end-of-line (BEOL) compatible process. Several IMC approaches using resistance and capacitance states in ferroelectric HZO have been proposed for vector-matrix multiplication (VMM), but previous approaches suffer from limited accuracy and reliability. In this work, we propose a promising approach centered on the remanent polarization (P r ) switching of binary ferroelectric HZO capacitor synapses. We experimentally demonstrate a simple pattern recognition task showing that the voltage readout of P r switching provides excellent accuracy due to its high on/off ratio and consequent reliability. We also performed large-scale simulations on a complex inference task, achieving high accuracy and immunity to device variations. We therefore believe that our proposed paradigm is promising for near-term neuromorphic IMC.