臺灣博碩士論文加值系統

　　技術節點隨著科技的進步不斷的縮小，使半導體元件縮小至奈米尺寸，當元件尺寸與電子平均自由徑相當時，會因為晶界散射與電子散射的關係，導致其電阻率急遽上升，使得性能下降。與銅金屬相比，釕金屬與鈷金屬有較短的電子平均自由徑，有機會取代銅成為下一世代連導線。本實驗以電化學原子層沉積的方式置備釕鈷合金薄膜，可應用於高深寬比溝槽連導線製備，解決傳統濺鍍階梯覆蓋率不足的
問題。
　　本實驗以C54-TiSi2做為基板，先以低電位沉積鈷原子，再利用表面侷限氧化還原反應使釕原子與鈷原子置換，調控不同的開路電位時間控制釕原子與鈷原子置換的數量，以獲得純釕薄膜或不同鈷含量的釕鈷薄膜。利用電流密度-時間曲線計算薄膜的總電荷量，並根據電流密度-時間關係圖求得擴散係數，並使用掃描式電子顯微鏡、能量色散光譜儀、四點探針及X射線光電子能譜儀對薄膜進行表面形貌、成分、電性和相結構等分析。
　　實驗結果得知，使用3 mM CoCl2溶液與1 mM RuCl3溶液，當鈷低電位沉積電位為-0.6 V，釕開路電位時間為300秒時，以電化學原子層沉積50個循環後，平均每個循環的原子層沉積量為1.09 Monolayer，Ru薄膜厚度為203 nm，電阻率為46 μΩ-cm。固定鈷低電位沉積電位為-0.6 V，將開路電位時間縮短為20秒時，以電化學原子層沉積50個循環後，可以獲得 Co含量為1.66 at.%的Ru(Co)合金薄膜，平均每個循環的原子層沉積量為0.77 Monolayer，Ru(Co)合金薄膜厚度為133 nm，電阻率為29 μΩ-cm。

　　As the semiconductor technology node continuous decreasing, when line width of Copper (Cu) interconnects similar the average means free path of electrons, the resistivity will be increase of sharp because the scattering of electrons. Cobalt (Co) and Ruthenium (Ru) have low mean free path of electrons than Cu and their properties of high melting point, high oxidation resistance and low resistivity, they are potential as next generation interconnect material. In this study, Ru(Co) thin films were prepared by electrochemical atomic layer deposition, which can apply to
manufacture of nanoscale integrated circuit.
　　In this study, using Co underpotential deposition (UPD) and Ru surface-limited redox replacement (SLRR) prepared Ru(Co) thin films on C54-TiSi2 substrate. By controlling the open circuit potential (OCP) time during the Ru-SLRR to obtain different Co concentration of Ru(Co) thin film or Ru thin film. The charge of Co-UPD can calculate by current density-time curves and the diffusion coefficients of the Co ions in the CoCl2 solution also can calculate. The Ru(Co) thin films electrical properties, phase structure, morphology and composition characterize had been analyzed by four-point probe, X-ray photoelectron spectroscopy, scanning electron microscope and energy dispersive spectrometer.
　　The experimental results show that the best Co-UPD coverage is 1.09 monolayer/cycle in 3 mM CoCl2 + 1 mM RuCl3 solution by using Co-UPD potential at -0.6 V and Ru-OCP time for 300 seconds which obtained resistivity of 46 μΩ-cm. The Co-UPD potential set at -0.6 V and decrease the Ru-OCP time to 20 seconds. We can obtain doping about 1.66 at.% Co in Ru(Co) thin film and it exhibit Co-UPD coverage is 0.77 monolayer/cycle and show lowest resistivity of 29 μΩ-cm.

摘要......i
Abstract......iii
誌謝......v
目錄......vi
表目錄......x
圖目錄......xi
第一章 緒論......1
1.1前言......1
1.1.1連導線鈷製程......1
1.1.2連導線釕製程......2
1.2研究動機......3
第二章 理論基礎及文獻回顧......7
2.1 薄膜沉積......7
2.1.1物理氣相沉積 (Physical Vapor Deposition, PVD)......7
2.1.2電化學沉積 (Electrochemical Deposition, ECD)......9
2.1.3原子層沉積 (Atomic Layer Deposition, ALD)......9
2.2電化學原子層沉積 (Electrochemical Atomic Layer Deposition, EC-ALD)......10
2.2.1電化學原子層沉積初步概念......10
2.2.2低電位沉積 (Underpotential Deposition, UPD)......10
2.2.3表面侷限氧化還原反應 (Surface Limited Redox Replacement, SLRR)......12
2.2.4 EC-ALD文獻探討......13
2.3電化學分析原理......14
2.3.1工作電極 (Working Electrode, WE)......15
2.3.2輔助電極 (Auxiliary Electrode, AE)......15
2.3.3參考電極 (Reference Electrode, RE)......16
2.3.4循環伏安法 (Cyclic Voltammetry, CV)......16
2.3.5計時電流法 (Chrono Amperometry, CA)......17
2.4電化學成核原理......18
2.4.1電化學反應過程......18
2.4.2電化學成核理論......19
2.4.3影響電化學成核因素......21
第三章 實驗流程與儀器介紹......31
3.1實驗材料......31
3.1.1 實驗基板......31
3.1.2 濺鍍靶材......31
3.1.3 製程氣體......31
3.1.4 化學藥品......31
3.2 實驗設備......32
3.2.1 磁控濺鍍系統 (Magnetron Sputter System)......32
3.2.2 熱處理系統 (Annealing System)......32
3.2.3 電化學原子層沉積 (Electrochemical Atomic Layer Deposition System, EC-ALD)......33
3.3實驗流程......33
3.3.1 前處理......33
3.3.2 矽基板清洗......34
3.3.3 C54-TiSi2基板製備......34
3.3.4 電化學溶液配置......35
3.3.5 EC-ALD實驗步驟設定......35
3.4分析儀器及原理......36
3.4.1表面輪廓儀 (α-step)......36
3.4.2四點探針 (Four-Point Probe, FPP)......36
3.4.3 掃描式電子顯微鏡 (Scanning Electron Microscope, SEM)......37
3.4.4場發射掃描式電子顯微鏡 (Field Emission Scanning Electron Microscope, FE-SEM)......37
3.4.5 能量散射光譜儀 (Energy Dispersive Spectroscopy, EDS)......38
3.4.6 X光繞射儀 (X-ray Diffraction, XRD)......38
3.4.7 X光光電子能譜儀 (X-ray Photoelectron Spectroscopy, XPS)......39
第四章 實驗結果與討論......51
4.1不同沉積電位對Co電化學沉積特性......51
4.1.1鈷溶液在C54-TiSi2基板上之循環伏安圖......51
4.1.2不同Co-UPD電位與覆蓋率分析......52
4.2以Ru-SLRR置換Co-UPD沉積Ru薄膜之特性......53
4.2.1以Ru-SLRR置換Co-UPD持續不同時間之電壓-電流-時間關係......53
4.2.2 Co-UPD沉積之電流密度-時間關係......55
4.2.3 Ru-SLRR沉積之電位-時間關係......58
4.2.4 Ru薄膜成分分析......59
4.2.5 Ru薄膜形貌分析......59
4.2.6 Ru薄膜電性分析......61
4.2.7 Ru薄膜之電流瞬態曲線......61
4.2.8 Ru薄膜之Cottrell曲線......62
4.3以Ru-SLRR置換Co-UPD沉積Ru(Co) 合金薄膜之特性......64
4.3.1 Ru(Co)合金薄膜之電壓-電流-時間關係......64
4.3.2 Ru(Co)合金薄膜之電流密度-時間關係......66
4.3.3 Ru(Co)合金薄膜之電位-時間關係......67
4.3.4 Ru(Co)合金薄膜結構分析......68
4.3.5 Ru(Co)合金薄膜成分分析......68
4.3.6 Ru(Co)合金薄膜形貌分析......68
4.3.7 Ru(Co)合金薄膜電性分析......69
4.3.8 Ru(Co)薄膜之電流瞬態曲線......70
4.3.9 Ru(Co)薄膜之Cottrell曲線......70
第五章 結論......109
參考文獻......110
Extended Abstract......120

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