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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 陳俊顯 | zh_TW |
dc.contributor.advisor | Chun-hsien Chen | en |
dc.contributor.author | 甯鼎軒 | zh_TW |
dc.contributor.author | Ting-Hsuan Ning | en |
dc.date.accessioned | 2023-12-20T16:20:21Z | - |
dc.date.available | 2023-12-21 | - |
dc.date.copyright | 2023-12-20 | - |
dc.date.issued | 2023 | - |
dc.date.submitted | 2023-09-14 | - |
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/91290 | - |
dc.description.abstract | 量子干涉(quantum interference, QI)在單分子的電子傳輸領域中有建設性(constructive, CQI)與破壞性(distructive, DQI)兩種現象。5,15-二氧雜卟啉(5,15-dioxaporphyrin, DOP)是個反芳香性分子(antiaromatics),其meso位置被氧原子取代,在氧化還原前後皆具鉗合金屬的能力,並能維持芳香性分子的平面結構,比一般卟啉分子擁有更高的電化學操作耐受性。本研究以軌域對稱性法則(orbital symmetry rule)和延伸彎箭頭法則(extended curly arrow rules)預測三種DOP分子在反芳香性的20個π電子(簡稱20π)氧化成為芳香性的18個π電子(簡稱18π)時,發生的CQI和DQI現象。通過第一原理計算分析頭基接點對3,13-雙對胺基苯基DOP(3,13-bis(4-aminophenyl)DOP, 3,13-DOP)、3,17-雙對胺基苯基DOP (3,17-DOP)與10,20-雙對胺基苯基DOP (10,20-DOP)的量子干涉特性。我們發現DOP分子由20π氧化為18π時,因為分子軌域相位的加乘或抵消,使得3,17-DOP的電荷傳輸能譜由DQI轉變成CQI,而10,20-DOP的轉換則相反。3,13-DOP在兩種氧化態均呈現DQI特徵。模擬電化學電位控制下的改變工作電極電位(Ewk)獲得的I-Ewk圖顯示在DQI特徵附近,呈現四個數量級以上的電流開關比值。 | zh_TW |
dc.description.abstract | Constructive and destructive quantum interference (CQI and DQI) are especially featured in the charge transport of single-molecule junctions. 5,15-dioxaporphyrin (DOP) is a meso-oxygen-substituted counterpart of highly π-conjugated porphyrin which can maintain planar structure and ability to chelate nickel ion during redox reactions. In this study, we utilized orbital symmetry rule to predict the CQI and DQI features of the DOP when it was oxidized from 20π-electron neutral specie to 18π-electron dication. Through first-principles calculation, the switches between DQI and CQI caused by altering contact-positions of anchoring groups on 3,13-bis(4-aminophenyl)DOP (3,13-DOP), 3,17-bis(4-aminophenyl)DOP (3,17-DOP) and 10,20-bis(4-aminophenyl)DOP (10,20-DOP) were analyzed. When the 20π-electron 3,17-DOP was oxidized to the 18π-electron state, the QI patterns in the transmission spectra would turn from DQI to CQI by the addition and the offset of the phases of certain molecular orbitals, and vice versa for 10,20-DOP. 3,13-DOP feature DQI at both oxidation state. Calculated electrochemical gating I-Ewk curves result in up to 4 orders of current on/off ratio near the DQI pattern. | en |
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dc.description.provenance | Made available in DSpace on 2023-12-20T16:20:21Z (GMT). No. of bitstreams: 0 | en |
dc.description.tableofcontents | 誌謝 i
中文摘要 ii ABSTRACT iii 目錄 iv 圖目錄 vii 表目錄 x 第1章 緒論 1 1.1 分子電子學的傳輸機制與基本模型 1 1.2 量子干涉原理與預測方法 3 1.2.1 軌域對稱性法則 5 1.2.2 延伸彎箭頭法則 7 1.2.3 量子干涉與量子傳輸途徑關係 10 1.3 本研究探討之5,15-二氧雜卟啉分子 12 1.3.1 芳香性與反芳香性 14 1.3.2 卟啉類化合物的光譜與氧化還原性質 17 1.3.3 具異原子卟啉的氧化態穩定性 19 1.3.4 頭基與卟啉接點對電子傳輸之影響 20 1.4 非電中性分子之電性計算 22 1.4.1 單分子靜電勢模擬 22 1.4.2 非電中性分子的電子傳輸模擬 24 1.4.3 相反離子的種類選擇 26 1.5 研究動機 27 第2章 研究方法 28 2.1 計算原理 28 2.1.1 哈特里−福克方法 28 2.1.2 密度泛函理論 29 2.1.3 非平衡格林函數−密度泛函方法 29 2.1.4 泛函 29 2.1.5 基底函數 30 2.2 計算軟體與條件 30 2.2.1 Gaussian 09之計算條件設定 30 2.2.2 QuantumATK之計算條件設定 30 2.3 模型建構 31 2.3.1 電極設計 31 2.3.2 分子設計 32 2.3.3 模擬電化學環境下的相反離子設定 32 2.3.4 電極−分子−電極系統 33 第3章 結果與討論 34 3.1 DOP的氧化還原特性與分子軌域能階 34 3.1.1 相反離子與DOP之相對位置討論 36 3.2 DOP的量子干涉特徵預測 38 3.2.1 軌域對稱性法則對DOP之量子干涉預測 38 3.2.2 延伸彎箭頭法則對DOP之量子干涉預測 41 3.2.3 頭基接點與量子干涉的關係 44 3.3 DOP分子接點衍生物與相反離子之相對位置關係 45 3.3.1 DOP分子接點衍生物的能階 45 3.3.2 DOP分子接點衍生物的靜電勢模擬 48 3.3.3 相反離子與DOP分子接點衍生物之空間位置討論 49 3.3.4 相反離子使用與否及其種類之討論 52 3.4 DOP的電子傳輸性質 54 3.4.1 DOP分子接點衍生物於電極−分子−電極系統內之空間位置討論 54 3.4.2 DOP分子接點衍生物之電子傳輸能譜 56 3.4.3 DOP分子接點衍生物之分子軌域節點與軌域對稱性法則討論 61 3.5 DOP分子接點衍生物之電子傳輸途徑討論 62 3.5.1 DOP分子接點衍生物之量子干涉特徵與延伸彎箭頭法則討論 67 3.6 電位控制下之分子導電值討論 68 3.6.1 費米能量處的傳輸值比較與定偏壓不同電位下之I-Ewk圖 69 第4章 結論 71 參考資料 72 | - |
dc.language.iso | zh_TW | - |
dc.title | 5,15-二氧雜卟啉之頭基接點影響單分子電性的量子干涉模擬 | zh_TW |
dc.title | Computational Study on Electron Transport for Single-Molecule Junctions of 5,15-Dioxaporphyrin: Peripheral Substituent Position-dependent Quantum Interference | en |
dc.type | Thesis | - |
dc.date.schoolyear | 112-1 | - |
dc.description.degree | 碩士 | - |
dc.contributor.oralexamcommittee | 陳以文;許良彥 | zh_TW |
dc.contributor.oralexamcommittee | I-Wen Chen;Liang-Yan Hsu | en |
dc.subject.keyword | 第一原理計算,分子電性,卟啉,二氧雜卟啉,量子干涉, | zh_TW |
dc.subject.keyword | First-principles Calculation,Molecular Electronics,Porphyrin,Quantum Interference, | en |
dc.relation.page | 77 | - |
dc.identifier.doi | 10.6342/NTU202304220 | - |
dc.rights.note | 同意授權(限校園內公開) | - |
dc.date.accepted | 2023-09-14 | - |
dc.contributor.author-college | 理學院 | - |
dc.contributor.author-dept | 化學系 | - |
顯示於系所單位: | 化學系 |
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