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    請使用永久網址來引用或連結此文件: https://ir.lib.ncu.edu.tw/handle/987654321/111442


    題名: 利用化學氣相沉積於介電基板選擇性合成二硫化鉬及其元件整合之研究;Investigation of MoS2 Synthesis on Dielectric Substrates by Chemical Vapor Deposition and Subsequent Device Integration
    作者: 陳昱勳;HSUN, CHEN YU
    貢獻者: 機械工程學系
    關鍵詞: 化學氣相沉積;元件;二維材料;CVD;device;2D material
    日期: 2026-08-26
    上傳時間: 2026-10-20 17:33:01 (UTC+8)
    出版者: 國立中央大學
    摘要: 隨著半導體元件持續微縮,傳統矽基通道材料逐漸面臨短通道效應、載子遷移率衰退與界面散射等限制。二維半導體材料因具備原子級厚度、良好能帶特性與優異閘極控制能力,被視為次世代通道材料之重要候選。其中,二硫化鉬(MoS2)具有約 1.8-1.9 eV 直接能隙、低漏電與良好結構穩定性,具備應用於邏輯元件、光電元件與感測器之潛力。然而,傳統 CVD 成長 MoS₂ 仍常伴隨隨機成核、晶體尺寸不均、層數控制困難與轉印缺陷等問題,限制其製程整合性。
    本研究提出以金點陣列(Au seed array)作為選擇性成核模板之 APCVD 製程,透過紫外光雷射直寫微影定義金點圖案,並結合單側封閉式石英內管與碳布遮罩,以調控 MoO3 前驅物釋放與氣體流場穩定性。經製程參數最佳化後,於 Ar 40 sccm、MoO3 10 mg、反應時間 12 min 條件下,可獲得 lateral size 約 25 μm 之 MoS₂ 晶體,其 Raman peak separation 約為 20.42 cm-1,PL FWHM 可降低至約 74.22 meV,顯示材料具有接近單層至少層之結構特徵與良好光學品質。
    此外,本研究比較 Wet SiO2、Dry SiO2 與 HfO2 等介電基板對 MoS₂ 選擇性成長之影響。表面能分析顯示三者分別為 54.35、50.39 與 62.51 mJ/m²,證實基板表面能會透過改變前驅物吸附、表面擴散長度與區域飽和,影響成核位置與層數分布。Dry SiO2 因表面能較低,可抑制非金點區域均質成核,使選擇性成核良率達 92.7%;Wet SiO2 可形成厚度約 0.72 nm 之單層 MoS2,但良率約為 75.7%;HfO2 則兼具 high-κ 特性與較佳光學再現性,良率約為 85.3 %,PL FWHM 集中於 92-96 meV,顯示其具較佳製程容忍度與元件整合潛力。最後,將所成長 MoS2 製作為背閘式場效電晶體,元件呈現明顯 n-type gate modulation behavior,元件關態電流約為10-7 A,開關電流比達106,場效遷移率為 10.7 cm² V-1 s-1。整體而言,本研究建立具位置控制性、高成核良率與介電基板適配性之 MoS2 直接成長平台,可作為未來二維半導體元件整合之基礎。;This study successfully established an Au seed array-assisted APCVD process for the site-selective growth of MoS2 on dielectric substrates. Regularly patterned Au seed arrays were fabricated by ultraviolet laser direct-write lithography and metal evaporation. A single-end-sealed quartz inner tube combined with a carbon cloth cover was employed to regulate the evaporation rate of the MoO3 precursor, stabilize the gas transport direction, and suppress local precursor supersaturation, thereby enabling position-controlled MoS2 growth on dielectric substrates. The process optimization results indicate that preheating the sulfur source effectively improves the S/Mo precursor supply timing, increasing the MoS2 crystal size from less than 3 μm without sulfur preheating to over 20 μm. By further optimizing the carrier gas flow rate, MoO3 precursor amount, and reaction time, the growth condition of Ar 40 sccm, 10 mg MoO3, and 12 min reaction time was identified as the optimized parameter set. Under this condition, MoS2 crystals with a lateral size of approximately 25 μm were obtained, with a Raman peak separation of approximately 20.42 cm-1 and a PL FWHM reduced to approximately 74.22 meV, indicating a near-monolayer to few-layer structure with good optical quality.
    Regarding the influence of dielectric substrates, this study demonstrates that substrate surface energy plays a critical role in modulating precursor adsorption, surface diffusion length, and local supersaturation, thereby affecting the nucleation density, site selectivity, and layer number distribution of MoS₂. The measured surface energies of Wet SiO2, Dry SiO2, and HfO2 were approximately 54.35, 50.39, and 62.51 mJ/m2, respectively. Among these substrates, Dry SiO2, with the lowest surface energy, effectively suppressed homogeneous nucleation in non-seeded regions and achieved the highest selective nucleation yield of approximately 92.7%. However, the accumulation of reactants near the Au seeds may also promote local vertical growth, resulting in an AFM-measured thickness of approximately 1.38 nm. In contrast, Wet SiO2 enabled the formation of monolayer MoS2 with a thickness of approximately 0.72 nm, but its stronger background nucleation led to a lower yield of approximately 75.7 %. HfO2, which possesses the highest surface energy and high-κ dielectric characteristics, exhibited a nucleation yield of approximately 85.3 %. Moreover, the PL FWHM of MoS2 grown on HfO2 was concentrated within 92-96 meV, indicating superior optical reproducibility, process tolerance, and potential for device integration.
    For device fabrication, the selectively grown MoS2 crystals were further integrated into back-gated field-effect transistors. The devices employed highly doped Si as the back gate, 100 nm SiO2 as the gate dielectric, and Y/Au as the source/drain contacts. Electrical measurements revealed clear n-type gate modulation behavior, where the drain current increased with increasing positive gate voltage, confirming that the MoS2 channel can be effectively modulated by the back-gate electric field. The output characteristics also exhibited stable current conduction without obvious abnormal leakage or current breakdown. Based on the transconductance extracted from the linear region of the transfer curve, the field-effect mobility was preliminarily estimated to be approximately 10.7 cm2 V-1 s-1. The on/off current ratio reached the order of 106, while the off-state current remained at a low level, indicating that MoS2 directly grown on dielectric substrates retains promising carrier transport properties. Overall, this work integrates Au seed-mediated nucleation, precursor supply control, and dielectric substrate surface energy engineering to establish a position-controlled, high-yield, and substrate-compatible MoS2 direct growth platform, demonstrating its feasibility for BEOL-compatible two-dimensional semiconductor device integration.
    顯示於類別:[機械工程研究所] 博碩士論文

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