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Hafnium zirconium oxide (HZO) has attracted attention for applications in nonvolatile memory and energy harvesting devices. However, it faces practical challenges such as insufficient endurance. One promising strategy to address this limitation is the utilization of antiferroelectric (AFE) behavior in HZO‐based materials. Previous studies have shown that various metal substitutions into HZO can result in AFE‐like properties within specific substitution concentration windows. While AFE‐like properties have often been attributed to the tetragonal phase of ZrO₂, recent studies suggest that the antipolar orthorhombic phase (space groupPbca) may instead be responsible for the observed AFE behavior. This study investigates how varying aluminum substitution concentration influences the phase and electrical properties of HZO devices to clarify the origin of AFE behavior. The results demonstrate that low aluminum concentrations in HZO, particularly in 8:1 and 6:1 HZO:Al composition ratio HZO devices, lead to pronounced real AFE behavior associated with the formation of thePbcaphase. 

Hafnium oxide-based thin films, in particular hafnium zirconium oxide (HZO), have potential for applications in nonvolatile memory and energy harvesting. Atomic layer deposition (ALD) is the most widely used method for HZO deposition due to its precise thickness control and ability to provide conformal coverage. Previous studies have shown the effects of different metal precursors, oxidizer precursors, and process temperatures on the ferroelectric properties of HZO. However, no mechanism has been identified to describe the different phase stabilities as the metal precursor purge time varies. This study investigates how varying the metal precursor purge time during plasma-enhanced ALD (PE-ALD) influences the phases and properties of the HZO thin films. Grazing incidence X-ray diffraction, Fourier transform infrared spectroscopy, and scanning transmission electron microscopy are used to study the changes in phase of HZO with variation of the metal precursor purge time during the PE-ALD process. The phases observed are correlated with polarization and relative permittivity responses under an electric field, including wake-up and endurance effects. The resulting phases and properties are linked to changes in composition, as measured using time-of-flight secondary ion mass spectrometry and X-ray photoelectron spectroscopy. It is shown that short metal precursor purge times result in increased carbon and nitrogen impurities and stabilization of the antipolar Pbca phase. Long purge times lead to films comprising predominantly the ferroelectric Pca21 phase. 

The discovery of ferroelectricity in hafnia based thin films has catalyzed significant research focused on understanding the ferroelectric property origins and means to increase stability of the ferroelectric phase. Prior studies have revealed that biaxial tensile stress via an electrode “capping effect” is a suspected ferroelectric phase stabilization mechanism. This effect is commonly reported to stem from a coefficient of thermal expansion (CTE) incongruency between the hafnia and top electrode. Despite reported correlations between ferroelectric phase fraction and electrode CTE, the thick silicon substrate dominates the mechanics and CTE-related stresses, negating any dominant contribution from an electrode CTE mismatch toward the capping effect. In this work, these discrepancies are reconciled, and the origin of these differences deriving from electrode elastic modulus, not CTE, is demonstrated. Pt/M/TaN/Hf0.5Zr0.5O2/TaN/Si devices, where M is platinum, TaN, iridium, tungsten, and ruthenium, were fabricated. Sin2(ψ)-based X-ray diffraction measurements of biaxial stress in the HZO layer reveal a strong correlation between biaxial stress, remanent polarization, and electrode elastic modulus. Conversely, a low correlation exists between the electrode CTE, HZO biaxial stress, and remanent polarization. A higher elastic modulus enhances the resistance to electrode elastic deformation, which intensifies the capping effect during crystallization, and culminates in the tandem restriction of out-of-plane hafnia volume expansion and preferential orientation of the polar c-axis normal to the plane. These behaviors concomitantly increase the ferroelectric phase stability and polarization magnitude. This work provides electrode material selection guidelines toward the development of high-performing ferroelectric hafnia into microelectronic devices, such as nonvolatile memories. 

Abstract Realizing compact and scalable Ising machines that are compatible with CMOS-process technology is crucial to the effectiveness and practicality of using such hardware platforms for accelerating computationally intractable problems. Besides the need for realizing compact Ising spins, the implementation of the coupling network, which describes the spin interaction, is also a potential bottleneck in the scalability of such platforms. Therefore, in this work, we propose an Ising machine platform that exploits the novel behavior of compact bi-stable CMOS-latches (cross-coupled inverters) as classical Ising spins interacting through highly scalable and CMOS-process compatible ferroelectric-HfO 2 -based Ferroelectric FETs (FeFETs) which act as coupling elements. We experimentally demonstrate the prototype building blocks of this system, and evaluate the scaling behavior of the system using simulations. Our work not only provides a pathway to realizing CMOS-compatible designs but also to overcoming their scaling challenges. 

Abstract The Ising model provides a natural mapping for many computationally hard combinatorial optimization problems (COPs). Consequently, dynamical system-inspired computing models and hardware platforms that minimize the Ising Hamiltonian, have recently been proposed as a potential candidate for solving COPs, with the promise of significant performance benefit. However, prior work on designing dynamical systems as Ising machines has primarily considered quadratic interactions among the nodes. Dynamical systems and models considering higher order interactions among the Ising spins remain largely unexplored, particularly for applications in computing. Therefore, in this work, we propose Ising spin-based dynamical systems that consider higher order (> 2) interactions among the Ising spins, which subsequently, enables us to develop computational models to directly solve many COPs that entail such higher order interactions (i.e., COPs on hypergraphs). Specifically, we demonstrate our approach by developing dynamical systems to compute the solution for the Boolean NAE-K-SAT (K ≥ 4) problem as well as solve the Max-K-Cut of a hypergraph. Our work advances the potential of the physics-inspired ‘toolbox’ for solving COPs. 

The rich non‐linear dynamics of the coupled oscillators (under second harmonic injection) can be leveraged to solve computationally hard problems in combinatorial optimization such as finding the ground state of the Ising Hamiltonian. While prior work on the stability of the so‐called Oscillator Ising Machines (OIMs) has used the linearization method, in this letter, the authors present a complementary method to analyze stability using the second‐order derivative test of the energy/cost function. The authors establish the equivalence between the two methods, thus augmenting the tool kit for the design and implementation of OIMs. 

While ferroelectric HfO₂shows promise for use in memory technologies, limited endurance is one factor that challenges its widespread application. In this study, endurance is investigated through field cycling W/Hf_0.5Zr_0.5O₂/W capacitors above the coercive field while manipulating the time‐under‐field using bipolar pulses of varying pulse duration or duty cycle. Both remanent polarization and leakage current increased with increasing pulse duration. Additionally, an order of magnitude decrease in the pulse duration from 20 to 2 μs resulted in an increase in endurance lifetime of nearly two orders of magnitude from 3×10⁶to 2×10⁸cycles. These behaviors are attributed to increasing time‐under–field allowing for charged oxygen vacancy migration, initially unpinning domains, or driving phase transformations before segregating to grain boundaries and electrode interfaces. This oxygen vacancy migration causes increasing polarization before creating conducting percolation paths that result in degradation and premature device failure. This process is suppressed for 2 µs pulse duration field cycling where minimal wake‐up and lower leakage before device failure is observed, suggesting that very short pulses can be used to significantly increase device endurance. These results provide insight into the impact of pulse duration on device performance and highlight consideration of use conditions when endurance testing. This article is protected by copyright. All rights reserved. 

Nonlinear dynamical systems such as coupled oscillators are being actively investigated as Ising machines for solving computationally hard problems in combinatorial optimization. Prior works have established the equivalence between the global minima of the cost function describing the coupled oscillator system and the ground state of the Ising Hamiltonian. However, the properties of the oscillator Ising machine (OIM) from a nonlinear control viewpoint, such as the stability of the OIM solutions, remain unexplored. Therefore, in this work, using nonlinear control-theoretic analysis, we (i) identify the conditions required to ensure the functionality of the coupled oscillators as an Ising machine, (ii) show that all globally optimal phase configurations may not always be stable, resulting in some configurations being more favored over others and, thus, creating a biased OIM, and (iii) elucidate the impact of the stability of locally optimal phase configurations on the quality of the solution computed by the system. Our work, fostered through the unique convergence between nonlinear control theory and analog systems for computing, provides a new toolbox for the design and implementation of dynamical system-based computing platforms.