本研究針對 HfO₂–ZrO₂ 疊層薄膜之組成、氫流量與界面工程進行系統性探討,建立其介電充電行為、高頻穩定性與缺陷行為之關聯性。結果顯示,位於 MPB 近旁的氫處理後HZZ53 組成具有最高介電常數與最低耗散因子,並由 XPS 分析確認其具較低氧缺陷比例與較佳晶格穩定性。脈衝操作顯示該組成具備完整的快速介電響應,可有效避免準靜態 C–V 於高頻下之 dipole-lag 侷限,使動態介電常數遠高於傳統量測值。除高頻性能外,低缺陷密度(Dit)亦使其在耐久性與熱穩定性上保持優異表現,並在極薄 EOT 下仍維持低漏電特性。透過 鐵電畴方向示意圖建立之模型顯示,其快速可翻轉極化與溫度誘發極化變化具一致性,為後續焦電效應與高頻介電整合奠定物理基礎。本研究提出一套兼具高 k、高頻穩定與高可靠度之 HfO₂–ZrO₂ 疊層工程策略,對記憶體與超薄介電元件具有高度應用潛力。;This study systematically investigates the composition, hydrogen-flow conditions, and interfacial engineering of HfO₂–ZrO₂ stacked films, establishing the correlation between dielectric charging behavior, high-frequency stability, and defect characteristics. The hydrogen-treated HZZ53 composition located near the MPB exhibits the highest dielectric constant and the lowest dissipation factor, confirmed by XPS analysis showing reduced oxygen-related defects and improved lattice stability. Pulse-based measurements reveal a fully activated fast dielectric response, effectively avoiding the dipole-lag limitations observed in high-frequency quasi-static C–V and resulting in significantly enhanced dynamic dielectric constants. In addition to its high-frequency performance, the low defect density (Dit) contributes to excellent endurance and thermal stability, while maintaining low leakage even at ultrathin EOT. A domain-orientation model further illustrates that the fast switchable polarization is consistent with temperature-induced polarization variations, providing the physical basis for future pyroelectric and high-frequency dielectric integration. This work presents a robust engineering strategy for achieving high-k, high-frequency-stable, and highly reliable HfO₂–ZrO₂ dielectric stacks, demonstrating strong potential for memory and ultrathin capacitor applications.