研究生: |
胡銘顯 Ming-shien Hu |
---|---|
論文名稱: |
低維光電晶體的合成與特性分析 Synthesis and Characterization of Low-Dimensional Optoelectronic Crystals |
指導教授: |
林麗瓊
Li-Chyong Chen 洪儒生 Lu-Sheng Hong 陳貴賢 Kuei-Hsien Chen |
口試委員: |
果尚志
none 馮哲川 none 吳季珍 none 陳永芳 none 黃鶯聲 none |
學位類別: |
博士 Doctor |
系所名稱: |
工程學院 - 化學工程系 Department of Chemical Engineering |
論文出版年: | 2006 |
畢業學年度: | 94 |
語文別: | 英文 |
論文頁數: | 183 |
中文關鍵詞: | 磊晶 、 化學氣相沈積 、 一維奈米材料 、 碳化矽 、 表面電漿共振 、 奈米帶 |
外文關鍵詞: | surface plasmon resonance, epitaxy, chemical vapor deposition, one-dimensional nanomaterial, silicon carbide, nanobelt |
相關次數: | 點閱:356 下載:0 |
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本論文的主題分為三部分: (1)以矽甲烷、乙炔為反應物的冷壁式低壓化學氣相沈積法於矽(111)基板表面碳化改質並成長碳化矽異質磊晶的探討與評估 ; (2)以氣流引導式化學氣相沈積法(GSCVD)及有機金屬化學氣相沈積法(MOCVD)成長一維氮化銦奈米帶 (InN nanobelt)及其光學性質的研究與探討 ; (3) 以微波電漿輔助化學氣相沈積法(MWCVD)成長一維介電材料包覆金顆粒複合奈米線的合成與光電性質的研究。
第一部份的實驗中,不但成功的以乙炔於矽單晶Si(111)基板上碳化出無孔洞且表面平坦的碳化矽緩衝層,且也於此緩衝層表面成長出碳化矽的磊晶薄膜,我們發現於此一系統中碳化膜的表面粗糙度對於之後成長的碳化矽磊晶品質具有決定性的影響。此外也針對進料氣體通入反應器的方式,探討其對於碳化矽薄膜的成長模式及結晶性質的影響。我們發現,在室溫即通入氣體原料時,有助於薄膜以二維的模式成長出高品質的磊晶膜,而高溫時才通入原料的方式卻導致三維的成長,造成多晶薄膜的沈積。這乃是因為室溫通入氣體原料不僅在熱力學上有助於乙炔在已經碳化的矽表面上作化學性吸附,且有效的抑制了氣體原料的氣相成核,而導致薄膜呈現二維的成長模式。
第二部份的實驗中,成功的以GSCVD法成長出一維的單晶氮化銦奈米帶。結構上我們利用氮化銦奈米帶表面能量的差異,解釋了奈米帶為何呈現特定晶面的帶狀表面形態。在光學性質方面以光激發光譜測量結果發現,以GSCVD法成長出的氮化銦奈米帶具有本質能隙(0.76 eV)的紅外光發光行為,其發光訊號的線寬為目前文獻值中最低(14meV)。由發光強度與激發功率成線性增加以及線寬與激發功率成線性減少的結果。我們推論出此一行為為增幅自發放射(amplified spontaneous emission)所造成。此外我們也成功的利用MOCVD法成長出氮化銦奈米帶。以穿透式電子顯微鏡分析其微結構發現,無論是成長方向或表面晶相皆與GSCVD法所成長的氮化銦奈米帶相同。值得一提的是,在改變激發能量密度(pumping intensity) 於20 K下的光激發光譜 (PL) 測量結果發現,在低激發能量密度下,PL為一半高寬 (linewidth) 較寬約 60nm的波形。隨著激發能量密度持續增加,於PL的光譜中觀察到發光強度與激發能量密度呈現一門檻行為 (threshold behavior),這是由於InN nanobelt的PL由自發性放射轉變為受激放射 (stimulated emission) 的緣故。 隨著激發能量密度更進一步增加至73kW/cm2時,此時PL由原本線寬為60nm的光譜出現了具有週期性且線寬銳減為只有2.3 nm的光譜,這意味著氮化銦奈米帶的PL由自發性發光(spontaneous emission)轉變為雷射。
第三部份中,我們開發了微型反應器(microreactor)的方法,以MWCVD製程合成出一維介電材料包覆金顆粒之複合奈米線 (Au@SiOx nanowire),並利用穿透式電子顯微鏡觀察其成長的機制。此外發現,此一複合奈米線具有表面電漿共振吸收的特性。在不同波長的雷射光源照射時,此一複合奈米線於表面電漿共振吸收的頻率,呈現出強烈的波長選擇性以及可逆的光敏感特性,據此推測所觀察到的增強性光敏感行為可能是由於光誘導所形成之表面電漿子衰退為熱電子並經由介電層穿遂所造成。
The subject of this research is focused on: (1) investigating the surface carbonization of Si(111) and the subsequent heteroepitaxial growth of SiC(111) using SiH4 and C2H2 as gaseous reactants in a cold-wall type low pressure chemical vapor deposition (LPCVD) reactor, (2) fabricating one-dimensional (1D) InN nanobelts by using gas-stream guided thermal CVD (GSCVD) and metal organic chemical vapor deposition (MOCVD), (3) synthesizing of photosensitive Au nanoparticle-embedded dielectric nanowires by microwave plasma assisted CVD.
In the first part, carbonization of Si(111) surface was successfully achieved using C2H2 as a hydrocarbon reactant. The carbonized Si(111) surface was found to have void-free and flat surface. It was suggested that the surface roughness of the carbonized Si(111) layers plays a crucial role in determining the crystalline property of the subsequent SiC epilayers. Furthermore, we also investigated the effect of feeding process on the growth mode and crystalline property of SiC(111) films. The feeding of SiH4 and C2H2 at room temperature followed by a temperature ramping to 1523 K exhibited two-dimensional growth mode, while transformed into three-dimensional growth and showed polycrystalline property when the reactants were directly fed at 1523 K. Kinetic analysis of the film growth rate for the two reactant feeding procedures showed almost the same activation energy (54 Kcal/mol), indicating a gaseous decomposition of SiH4 to form SiH2 and H2 controls the overall film growth process. Nevertheless, feeding reactants from room temperature may favor the chemisorption of the reactants, facilitating the suppression of the gas-phase nucleation in the initial period of film growth, thus leading to two dimensional film growth.
In the second part, single-crystalline indium nitride (InN) nanobelts were synthesized using Au as a catalyst by a guided-stream thermal chemical vapor deposition technique. The facet-selectivity of nanobelt was discussed in view of thermodynamic aspect and was attributed to the difference in surface energy of respective facet. Photoluminescence (PL) spectra of InN nanobelts showed a sharp infrared emission peak at 0.76 eV with a full width at half maximum of 14 meV, the smallest value in comparison with those of the InN epilayers reported to date. The integrated PL intensity was found to increase linearly with the excitation power, which confirms the observed PL is due to the direct band-to-band emission. The linewidth narrowing can be ascribed to amplified spontaneous emission as evidenced by a clear indication of linearly disproportional dependence of linewith on excitation power. On the other hand, we also successfully fabricated InN nanobelts by MOCVD technique. TEM characterization revealed that the growth direction and surface facets of MOCVD-grown InN nanobelts were identical to that grown by GSCVD. At low excitation intensity, the spectrum consisted of a single broad spontaneous emission band with a FWHM of (~60 nm) at 1594 nm. As the pumping intensity increases up to 73 kW/cm2, several sharp peaks emerged in the spectra between 1559 nm and 1644 nm. The typical linewidth of the observed sharp emission peaks at highest pumping intensity of 75.6 kW/cm2 was about 2.3 nm, nearly 25 times narrower than that (~60 nm) of spontaneous emission below the threshold. As the pumping power increases, a strong superlinear dependence of the emission intensity (inset of Fig. 4) and the rapid linewidth narrowing at high pumping power could be observed, suggesting a transition from spontaneous emission to stimulated emission in the MOCVD-grown InN nanobelts. Above the pumping power threshold, the emergence of multiple sharp peaks represented different lasing modes with strong coherent feedback at wavelength between 1559 nm and 1644 nm.
In the final part, we present the use of micro-reactor approach for fabricating self-organized photosensitive Au nanoparticle chain encapsulated by dielectric nanowire in a MWCVD system. The growth mechanism of the hybrid nanowires was unveiled by TEM characterization. It was found that the hybrid nanowire exhibits pronounced surface plasmon resonance absorption. More remarkably, a strong wavelength-dependent and reversible photoresponse has been demonstrated in a two-terminal device using an ensemble of Au nanopeapodded silica nanowires under light illumination, while no photoresponse was observed for the plain silica nanowires. The enhancement of photoresponse is attributed to the generation of hot electrons due to the decay of surface plasmon polariton followed by the drift or diffusion to the dielectric nanowire and tunnel to the conuterelectrode.
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