Ultrahigh Dielectric Permittivity of a Micron-Sized Hf0.5Zr0.5O2 Thin-Film Capacitor After Missing of a Mixed Tetragonal Phase

Published in Materials and Physics

Ultrahigh Dielectric Permittivity of a Micron-Sized Hf0.5Zr0.5O2 Thin-Film Capacitor After Missing of a Mixed Tetragonal Phase
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Ultrahigh Dielectric Permittivity of a Micron-Sized Hf0.5Zr0.5O2 Thin-Film Capacitor After Missing of a Mixed Tetragonal Phase - Nano-Micro Letters

Innovative use of HfO2-based high-dielectric-permittivity materials could enable their integration into few-nanometre-scale devices for storing substantial quantities of electrical charges, which have received widespread applications in high-storage-density dynamic random access memory and energy-efficient complementary metal–oxide–semiconductor devices. During bipolar high electric-field cycling in numbers close to dielectric breakdown, the dielectric permittivity suddenly increases by 30 times after oxygen-vacancy ordering and ferroelectric-to-nonferroelectric phase transition of near-edge plasma-treated Hf0.5Zr0.5O2 thin-film capacitors. Here we report a much higher dielectric permittivity of 1466 during downscaling of the capacitor into the diameter of 3.85 μm when the ferroelectricity suddenly disappears without high-field cycling. The stored charge density is as high as 183 μC cm−2 at an operating voltage/time of 1.2 V/50 ns at cycle numbers of more than 1012 without inducing dielectric breakdown. The study of synchrotron X-ray micro-diffraction patterns show missing of a mixed tetragonal phase. The image of electron energy loss spectroscopy shows the preferred oxygen-vacancy accumulation at the regions near top/bottom electrodes as well as grain boundaries. The ultrahigh dielectric-permittivity material enables high-density integration of extremely scaled logic and memory devices in the future.

A research team led by Professors Yan Cheng and An Quan Jiang has published a breakthrough study in Nano-Micro Letters on the dielectric properties of micron-sized Hf0.5Zr0.5O2 (HZO) thin-film capacitors. Their work reveals how the elimination of a mixed tetragonal phase induces an unprecedented dielectric response, offering a new paradigm for integrating hafnia-based materials into advanced memory and logic devices.

Key Findings

  • Ferroelectric–Nonferroelectric Transition: When the capacitor size is reduced to 3.85 μm, ferroelectricity vanishes and an ultrahigh dielectric permittivity of 1466 emerges, without requiring high-field fatigue cycling.
  • Phase Evolution: Synchrotron X-ray micro-diffraction demonstrates the disappearance of the tetragonal phase, leaving a stabilized orthorhombic structure that underpins the dielectric enhancement.
  • Charge Storage: The capacitor achieves a stored charge density of 183 μC cm-2 at 1.2 V/50 ns, sustaining over 1012 cycles without breakdown—an order of magnitude higher than conventional ferroelectric counterparts.
  • Oxygen Vacancy Engineering: Electron energy loss spectroscopy shows preferential oxygen-vacancy accumulation near electrodes and grain boundaries, which lowers energy barriers for spontaneous oxygen migration and facilitates the phase transition.

Why It Matters

  • Scalable Integration: The findings enable high-density integration of capacitors within nanoscale logic and memory architectures, surpassing limitations of conventional ferroelectric films.
  • Energy Efficiency: The giant permittivity and robust cycling stability are highly attractive for dynamic random access memory (DRAM), energy-efficient CMOS devices, and future low-power electronics.
  • Mechanistic Insights: By correlating dielectric performance with oxygen-vacancy ordering and phase stability, the study provides a fundamental roadmap for tailoring hafnia-based materials beyond their traditional ferroelectric role.

Future Outlook

This discovery signals a shift from incremental improvements in ferroelectric hafnia to deliberate manipulation of phase composition and defect chemistry for extreme dielectric responses. Potential research directions include:

  • Reducing leakage current density through defect passivation and interface optimization.
  • Extending the concept to sub-micron geometries for ultra-scaled devices.
  • Exploring multifunctional coupling of dielectric, ferroelectric, and resistive switching behaviors in a single platform.

By demonstrating a fatigue-free pathway to ultrahigh permittivity, this work redefines the technological landscape of hafnium-based dielectrics. It highlights how nanoscale structural engineering and defect management can unlock new functionalities in widely used CMOS-compatible materials, bridging fundamental condensed-matter physics with urgent demands in advanced electronics.

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Surfaces, Interfaces and Thin Film
Physical Sciences > Materials Science > Surfaces, Interfaces and Thin Film
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  • Nano-Micro Letters Nano-Micro Letters

    Nano-Micro Letters is a peer-reviewed, international, interdisciplinary and open-access journal that focus on science, experiments, engineering, technologies and applications of nano- or microscale structure and system in physics, chemistry, biology, material science, and pharmacy.