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<p>A multi-layer graphene (MLG) nanosheet with extremely high thermal conductivity was implemented as the top electrode (TE) of ZrO<sub>2</sub> capacitors and their ferroelectric properties were stabilized by inserting a ZrN interlayer (IL) at the MLG and ZrO<sub>2</sub> interface to achieve superior electrocaloric characteristics for future in-chip cooling. By replacing the traditional TiN TE with an MLG nanosheet, a transition from tetragonal to orthorhombic ZrO<sub>2</sub> thin films was realized, contributing to the modified characteristics from antiferroelectricity to ferroelectricity. The phase transition can be ascribed to the strain-induced lattice transformation as confirmed by grazing-incidence X-ray diffraction, high-angle annular bright-field and annular dark-field micrographs, and nano-beam electron diffraction. Hence, a high remnant polarization of 14.8 µC/cm<sup>2</sup> and an excellent electrocaloric temperature change (Δ<i>T</i>) of 22.3&#xa0;K at 298&#xa0;K were obtained for the ferroelectric ZrO<sub>2</sub> capacitors with a high thermal conductivity of the MLG TE and superior phase stabilization in crystallinity of the ZrN IL with nine atomic layer deposition cycles, promising to serve as a cooling unit in monolithic high-density integrated circuits (ICs).</p>

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Multi-layer graphene induced orthorhombic zirconia stabilized by ZrN interlayer for superior heat transfer and electrocaloric cooling

  • 期刊论文

  • 发表日期：

    2025年11月19日

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  • Yu-Hua Liu,
  • Kuan-Lin Chen,
  • Jing-En Lin,
  • Han-Hsiang Tai,
  • Jer-Chyi Wang

摘要

A multi-layer graphene (MLG) nanosheet with extremely high thermal conductivity was implemented as the top electrode (TE) of ZrO2 capacitors and their ferroelectric properties were stabilized by inserting a ZrN interlayer (IL) at the MLG and ZrO2 interface to achieve superior electrocaloric characteristics for future in-chip cooling. By replacing the traditional TiN TE with an MLG nanosheet, a transition from tetragonal to orthorhombic ZrO2 thin films was realized, contributing to the modified characteristics from antiferroelectricity to ferroelectricity. The phase transition can be ascribed to the strain-induced lattice transformation as confirmed by grazing-incidence X-ray diffraction, high-angle annular bright-field and annular dark-field micrographs, and nano-beam electron diffraction. Hence, a high remnant polarization of 14.8 µC/cm2 and an excellent electrocaloric temperature change (ΔT) of 22.3 K at 298 K were obtained for the ferroelectric ZrO2 capacitors with a high thermal conductivity of the MLG TE and superior phase stabilization in crystallinity of the ZrN IL with nine atomic layer deposition cycles, promising to serve as a cooling unit in monolithic high-density integrated circuits (ICs).