垂直與水平架構之導電絲電阻記憶元件的製作與導電絲成長暨記憶穩定性機制的探討

熊昌鉑

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垂直與水平架構之導電絲電阻記憶元件的製作與導電絲成長暨記憶穩定性機制的探討

熊昌鉑 , Ph.D　　Advisor：甘炯耀　　

繁體中文

電阻記憶體；固態電解電池元件；氧化鈦；萊里不穩定性；奈米銀導電絲；電致步驟； Resistance switching memory ； Programmable metallization cells ； Titanium oxide ； Rayleigh instability ； Ag nanofilament ； Forming process

Abstract │ Reference (174) │ Altmetrics

Abstract 〈TOP〉

本論文探討下一代非揮發性記憶體的候選之一－可程控金屬化記憶體元件 (Programmable Metallization Cell, PMC) 的製作與導電絲成長與記憶穩定性機制的探討。可程控金屬化記憶體具有可低電壓操作、操作快速、低耗能與高微縮率的優點，非常適合開發為高密度記憶體。然而，有一些重要議題仍不甚瞭解且較無文獻上的探討，但對元件發展卻很關鍵，它們包含：第一，導電絲的形貌或分布為何、導電絲的尺寸可能多小及主導導電絲的成長機制或影響其生長形貌的因素為何等；第二，造成元件記憶態保持性不穩定的機制為何等。基於此，適合上述議題的探討，本研究中我們設計一種「水平式元件」使導電絲在檢測的過程能被觀察與檢測到。我們使用水平式Ag/TiO2/Pt元件作為探討的模型並藉由電致過程的驅動，使銀導電絲以電解電化學的方式形成於TiO2薄膜的表面上，便於觀察。
首先，我們先製作垂直式Ag/TiO2/Pt元件，探討Ag/TiO2/Pt元件的基本電阻轉換特性。此元件為雙極性變阻，電阻轉換的原理是利用電解電化學的反應機制。經多次的電阻轉換後仍能維持穩定的操作特性，其中，SET與RESET的平均電阻轉換電壓分別為0.91 V與-0.47 V，高、低電阻平均分別為4.07×105 Ω與7079 Ω，比例約為57倍左右。此外，低阻態記憶保持性同樣發現具有不穩定的特性而傾向恢復成高阻態，我們發現在較低電流限操作及較厚電解質薄膜厚度下低阻態較為不穩定。
再來，我們製作水平式Ag/TiO2/Pt元件，利用外加電壓或電流輸入進行元件電致步驟的過程，並探討此過程之主要活化限制因子。實驗結果顯示，元件電致步驟速率隨外加電場或溫度的變化呈指數遞增的關係，顯示電致步驟為一種電場輔助熱活化的過程，我們驗證此元件主要的活化過程來自銀離子的遷移。另外，以變溫量測的方式檢測出其遷移活化能約為0.81 eV左右，而其活化能大小與外加電場呈線性遞減的關係，此線性遞減的關係解釋了電致步驟速率隨外加電場呈指數遞增的關係了。
接下來，我們進行經由電致步驟之後所產生的銀結構的形貌與微結構觀察。實驗中發現銀結構物以許多尺寸均勻的奈米銀球體並且彼此以一特定距離成串排列，我們驗證此奈米銀球體是因萊里不穩定性 (Rayleigh instability) 由銀導電絲演變而來。萊里不穩定性是因表面能的存在而使結構體產生不穩定性，理論顯示尺寸愈小、長寬比例較大的物體愈不穩定，而傾向分化為多個球體。實驗結果中，我們得到的銀導電絲尺寸極小 (約直徑7 nm)，經由實際觀察與理論計算證實銀導電絲在室溫下即能迅速造成演化。此外，我們亦觀察元件操作電場與操作電流限值對銀導電絲形成的影響。愈大的電場易形成長柱型的導電絲形貌，而較小電場易形成形狀較為寬廣且分佈鬆散的導電絲結構；另外，較小的電流限則形成尺寸較細小的銀導電絲結構。
最後，我們探討水平式元件經長久的電壓驅動下對銀結構物形貌變化的影響。實驗結果顯示，銀奈米球體在經過適當的電壓驅動 (未達電流限) 將造成球體尺寸的些微增大；相對地，達到電流限後的電壓或電流驅動將造成球體尺寸上的明顯增大，這些形貌演化的過程仍是以電解電化學反應的機制進行。會造成銀結構物的形體變化，都是因元件在後續的電場作用下，電場易集中於銀結構物體週圍，因此後續的電場或電流的作用都只會在銀結構物體周圍造成影響，例如銀離子的遷移或球體結構的變化。

Reference ( 174 ) 〈TOP〉

1 International Technology Roadmap for Semiconductors, 2007 Edition. www.itrs.net/Links/2007ITRS/ExecSum2007.pdf
連結：
2 D. Ielmini, "Reliability issues and modeling of Flash and post-Flash memory (Invited Paper)" Microelectronic Engineering 86, 1870 (2009).
連結：
3 R. Zambrano, "Applications and issues for ferroelectric NVMs" Materials Science in Semiconductor Processing 5, 305 (2002).
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連結：
5 J. G. Zhu, "Magnetoresistive random access memory: The path to competitiveness and scalability" Proceedings of the Ieee 96, 1786 (2008).
連結：

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