為了提升記憶體特性並達成尺寸微縮的目標，需要不斷引進新的半導體製程技術，其中電漿製程的高能離子就可能對元件造成輻射傷害。所以輻射效應除了在太空工業、核能發展、軍事用途，半導體製程中的輻射環境也可能造成元件故障。因此本篇論文藉由三面閘極多晶矽無接面式快閃記憶體元件觀察輻射傷害對於操作特性的影響，並照射10 k、100 k、1000 k（rad）之鈷（Co）-60輻射劑量了解劑量效應；另外，再透過含氮與鋁之氧化鋯堆疊式電荷儲存層來提升記憶體的操作特性及抗輻射能力。
本論文分為三個部份，首先製備氮化矽/二氧化鋯堆疊式電荷儲存層並應用於多晶矽通道電荷捕捉式快閃記憶體，探討該元件經三種鈷（Co）-60輻射劑量照射前後的影響。由實驗結果得知，ZrO2樣品的導通電流、開關電流比、寫入速度以及抹除速度特性，皆會隨著輻射照射劑量增加而劣化；但電荷保持力變得更好，推測是因輻射所產生的界面缺陷捕捉了欲從通道或閘極端流失的電荷，另一種猜測是元件的電荷儲存層受到輻射破壞，進而增加ZrO2內較深的能階缺陷。
為了減低輻射對於記憶體保持力的影響，論文第二部分將氮與鋁摻入元件之氮化矽/二氧化鋯堆疊式電荷儲存層中。ZrON樣品與ZrAlON樣品皆有較好的電荷保持力，推測氨電漿處理使電荷儲存層中的淺缺陷數量減少，也讓薄膜中的漏電流路徑被氮摻雜鈍化。而ZrAlON樣品相較於ZrO2樣品能有效提升可靠度特性，且不會犧牲太多的操作速度。此外，ZrAlON樣品可能是Al元素的加入使電洞陷阱數量增加，因此具有比ZrON樣品更快的抹除速度。
最後一部份，探討氮、鋁摻雜對ZrO2電荷儲存層之抗輻射能力的影響。結果顯示，ZrAlON樣品的寫入/抹除速度皆於輻射後明顯劣化，而ZrON樣品則不受輻射影響。在可靠度方面，三個樣品的耐久力皆沒有隨著輻射劑量增大而變化。而ZrON樣品及ZrAlON樣品的電荷保持力特性會隨著輻射劑量增大而劣化，可能是因為氨電漿處理可提升材料熱穩定性並強化電荷儲存層的鍵結，而降低輻射對於電荷儲存層的破壞。也證實輻射效應對於記憶體元件是一種全面性的傷害，可能直接破壞界面，或是破壞電荷儲存層中原子的鍵結及改變了缺陷狀況，皆可能導致記憶體特性產生不同程度的劣化。ZrON樣品在記憶體操作速度以及可靠度特性方面，較不易受輻射照射或劑量影響，為抗輻射能力最佳的元件。

In order to improve the memory characteristics and achieve the goal of miniaturization, some new semiconductor process technologies should be used. Among them, plasma process with high-energy ions may cause radiation damage on the device. In addition to the radiation effects in space, nuclear power, and military applications, the radiation exposure during semiconductor manufacturing process may result in malfunction of device. In this thesis, the effects of radiation damage on operation characteristics of poly-Si charge trapping flash memory device are studied by applying Co-60 radiation with total doses of 10 k, 100 k and 1000 k (rad). In addition, the operation characteristics and radiation hardness of charge-trapping flash device can be improved by incorporating nitrogen or aluminum into ZrO2 stacked charge trapping layer.
This thesis consists of three parts. In the first part, the Si3N4/ZrO2 stacked charge trapping layer is applied to the poly-Si charge trapping flash memory device, and the effects of Co -60 radiation on this device are studied. The experimental results show that the on-current, On/Off current ratio, program speed and erase speed of ZrO2 sample are degraded with increasing radiation dose. However, the retention characteristics are better, probably because radiation-induced interface defects may capture the charge to be escaped from the channel or gate. Another possible reason may be that the charge trapping layer of the device is damaged by radiation. Thus, some traps with deep energy level in ZrO2 are formed.
In the second part, in order to reduce the radiation damage on memory retention, nitrogen or aluminum is incorporated into ZrO2 stacked charge trapping layer. ZrON and ZrAlON samples show better retention, probably because NH3 plasma treatment reduces amount of shallow trap in high-k trapping layer, and the leakage paths are passivated by nitrogen and hydrogen. The retention characteristic of ZrAlON sample is better than that of ZrO2 one without sacrificing much operating speed. And the erasing speed of ZrAlON sample is faster than that of ZrON one due to the increased hole traps provided by incorporating aluminum into ZrO2 stacked charge trapping layer.
In the last part, radiation hardness of charge trapping flash devices with nitrogen or aluminum incorporation in ZrO2 stacked trapping layer are studied. The results show that the program and erase speeds of ZrAlON sample are easily degraded after radiation, but ZrON sample wasn’t affected by radiation. In terms of reliability, endurance characteristic of the three samples didn’t change with increasing radiation dose. Retention characteristic of ZrON and ZrAlON samples are degraded with increasing radiation dose, because NH3 plasma treatment can improve the thermal stability and the bonding of the charge trapping layer. Thus, NH3 plasma treatment can reduce radiation damage on the charge trapping layer. It is also found that the radiation effect is a global damage to the memory devices. Radiation effect may directly damage the interface, or destroy the bond of atoms in the charge trapping layer and change the defect status, which all cause somewhat degradation on the memory characteristics.
Hence, operating speed and reliability characteristics of ZrON sample are less susceptible to radiation effects. Therefore, a flash memory device with ZrON trapping layer is promising for radiation hardness applications.

摘要 i
Abstract iii
目錄 v
表目錄 ix
圖目錄 x
第一章 緒論 1
1.1 非揮發性記憶體 1
1.2 快閃記憶體元件 2
1.2.1 浮動閘極式快閃記憶體元件 2
1.2.2 電荷捕捉式快閃記憶體元件 3
1.3 多晶矽薄膜電晶體 5
1.3.1 低溫多晶矽之結晶方法 6
1.4 多向式閘極結構與奈米線通道快閃記憶體元件 7
1.5 介電係數材料與能帶工程 8
1.5.1 高介電系數材料 8
1.5.2 能帶工程 9
1.6 無接面式快閃記憶體元件 10
1.7 三維結構可堆疊式NAND快閃記憶體 12
1.8 輻射效應 13
1.8.1 金氧半元件輻射後之影響 14
1.9 各章摘要 15
第二章 快閃記憶體元件製程與操作方法 21
2.1 快閃記憶體元件之製程 21
2.1.1 三面閘極無接面式通道元件（Tri-Gate） 21
2.1.2 原子層沉積系統（Atomic Layer Deposition, ALD） 23
2.1.3 實驗之輻射來源（Radiation） 24
2.1.4 物性分析-穿透式電子顯微鏡（TEM） 25
2.2 快閃記憶體元件之基本操作原理與機制 25
2.2.1 載子穿隧機制 27
2.2.1.1 福勒-諾德海姆穿隧（F-N Tunneling） 27
2.2.1.2 直接穿隧（Direct Tunneling） 29
2.2.2 通道熱載子注入（Channel Hot Electron Injection, CHEI） 30
2.2.3 本實驗元件使用之操作機制（寫入/抹除） 31
2.2.3.1 福勒-諾德海姆穿隧（F-N Tunneling）寫入 31
2.2.3.2 福勒-諾德海姆穿隧（F-N Tunneling）抹除 31
2.3 快閃記憶體元件之可靠度特性 33
2.3.1 電荷保持力 33
2.3.2 耐久力 34
2.4 元件之輻射機制 36
2.4.1 氧化層正電荷（ΔQot）的產生 36
2.4.2 界面陷阱（Interface Trapped）的產生 37
2.5 快閃記憶體元件之量測方法 38
2.5.1 基本特性曲線量測方法 38
2.5.2 F-N穿隧之寫入與抹除量測 39
2.5.3 電荷保持力量測 39
2.5.4 耐久力量測 40
第三章 氮化矽/二氧化鋯堆疊電荷儲存層之多晶矽無接面式快閃記憶體經不同劑量輻射傷害之研究 56
3.1 研究動機與背景 57
3.2 實驗樣品製作流程 58
3.3 實驗結果與討論 60
3.3.1 元件汲極電流對閘極電壓特性圖 60
3.3.2 元件之寫入與抹除特性 61
3.3.3 元件之可靠度特性 62
3.3.3.1 耐久力特性 62
3.3.3.2 電荷保持力特性 63
3.4 本章結論 64
第四章 將氮與鋁摻入氮化矽/二氧化鋯堆疊電荷儲存層對多晶矽無接面式快閃記憶體元件特性之研究 73
4.1 研究動機與背景 74
4.2 實驗樣品製作流程 75
4.3 實驗結果與討論 77
4.3.1 元件汲極電流對閘極電壓特性圖 77
4.3.2 元件寫入與抹除特性 77
4.3.3 元件可靠度特性 79
4.4 結論 80
第五章 將氮與鋁摻入氮化矽/二氧化鋯堆疊電荷儲存層之多晶矽無接面式快閃記憶體元件經不同劑量輻射傷害之研究 89
5.1 研究動機與背景 90
5.2 實驗樣品製作流程 90
5.3 實驗結果與討論 91
5.3.1 元件汲極電流對閘極電壓特性圖 91
5.3.2 元件之寫入與抹除特性 91
5.3.2.1 ZrON元件的寫入與抹除特性受輻射之影響 92
5.3.2.2 ZrAlON元件的寫入與抹除特性受輻射之影響 92
5.3.2.3 三個元件的寫入與抹除特性受輻射之影響 93
5.3.3 元件之可靠度特性 95
5.3.3.1 耐久力特性受輻射之影響 95
5.3.3.2 電荷保持力特性受輻射之影響 96
5.4 本章結論 97
第六章 總結 110
參考文獻 113

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