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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 陳俊顯(Chun-hsien Chen) | |
dc.contributor.author | Ho-Sung Tsao | en |
dc.contributor.author | 曹何嵩 | zh_TW |
dc.date.accessioned | 2022-11-25T07:29:04Z | - |
dc.date.available | 2023-12-31 | |
dc.date.copyright | 2021-08-20 | |
dc.date.issued | 2021 | |
dc.date.submitted | 2021-08-06 | |
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/82309 | - |
dc.description.abstract | "單分子接點(single-molecule junctions)中的閃爍雜訊(flicker noise),被認為是原子運動造成的電流雜訊。電子經由空間傳輸(through-space)或是經由鍵結傳輸(through-bond),受到原子運動的影響程度不同,而得到不同的閃爍雜訊,因此閃爍雜訊用來鑑定分子由through-space或是through-bond傳輸電子,是近年來被開發的新研究方法。在本論文中,我們以閃爍雜訊分析法,研究三核銠金屬串錯合物[Rh3(dpa)4X2] (X = CN, NCS; dpa = dipyridylamido anion)以及五核金屬串錯合物[M5(tpda)4(NCS)2] (M = Cr, Co, Ni; tpda = tripyridyldiamido dianion),判斷金屬串錯合物的電子傳輸路徑屬於through-space或是through-bond,期望藉由分析金屬串錯合物的電子傳輸路徑,使我們對於分子內電子傳輸機制能更加瞭解,並設計出更導電的單分子電子元件。 我們透過理論計算,發現中性態的[Rh3(dpa)4X2] (X = CN, NCS),其電子在金屬核具有定域化(localized)的特性,而+1價的[Rh3(dpa)4(NCS)2]+則具有非定域化(delocalized)的特性。然而閃爍雜訊分析法顯示它們的電子傳輸皆屬於through-space,因此我們推測金屬核間的交互作用不是唯一影響電子傳輸方式的因素。在五核金屬串錯合物中,Ni5、Co5和Cr5的金屬核間的鍵級分別為0、0.5和1.5,由於Ni5的金屬間的鍵級為0,因此可以假設電子傾向以through-space傳輸,Cr5的鍵級最大,因此可以假設電子傾向以through-bond傳輸,Co5則同時有兩種電子傳輸機制。有趣的是,閃爍雜訊分析法顯示相反的趨勢,Ni5透過through-bond傳輸,Cr5透過through-space傳輸,Co5則介於兩者之間,顯示並非金屬核間的交互作用主導電子傳輸,而是其他因素主導。 我們藉由閃爍雜訊分析法的結果,配合單分子導電值以及金屬核間的鍵級、金屬核與NCS軸向配基間的鍵長,提出了一種機制:NCS軸向配基的能階與金屬核的能階之能量差距,主導了金屬串的電子傳輸,若能量差距小則偏向through-bond,差距大則偏向through-space。M5和NCS之間的能量差Δ應為Cr5 > Co5 > Ni5,當∆大時,例如Cr5,為through-space傳輸;而當∆小時,例如Ni5,則為through-bond傳輸。Co5的∆介於兩者之間,因此同時具有兩種途徑。此機制解釋了金屬串錯合物的導電值以及電子傳輸機制的趨勢。我們的研究結果提供了一種研究金屬串錯合物電子傳輸的方法。 " | zh_TW |
dc.description.provenance | Made available in DSpace on 2022-11-25T07:29:04Z (GMT). No. of bitstreams: 1 U0001-0608202115562700.pdf: 4341640 bytes, checksum: d48424062e5151ffd7bcf3e99d1d02df (MD5) Previous issue date: 2021 | en |
dc.description.tableofcontents | 口試委員會審定書 i 誌謝 ii 摘要 iii ABSTRACT v 總目錄 vii 圖目錄 ix 表目錄 xi 第1章 緒論 1 1.1 前言 1 1.2 Landauer formula、量子導電值與穿透係數 1 1.3 掃描式穿隧顯微術破裂接合法 2 1.4 金屬串錯合物之簡介 4 1.5 電化學掃描式穿隧顯微術破裂接合法 5 1.6 MMM junctions的電流雜訊 6 1.6.1 Thermal noise 7 1.6.2 Shot noise 7 1.6.3 Random telegraph noise (隨機電報雜訊) 8 1.6.4 Flicker noise (1/f noise) 9 1.6.5 雜訊功率與電子耦合的關聯 11 1.7 Flicker noise分析法的應用 14 1.7.1 DQI檢測 15 1.7.2 π-stacking檢測 17 1.7.3 構型異構物之指認 19 1.7.4 分子設計調控電子耦合 21 1.8 研究動機 24 第2章 實驗方法 25 2.1 藥品及耗材 25 2.2 儀器 26 2.3 電性測量 26 2.3.1 製作金電極 26 2.3.2 裝設樣品槽 27 2.3.3 參考電極與Luggin capillary之製備 28 2.3.4 裝置架設與下針。 29 2.3.5 測量單分子導電值對探針位移關係曲線 30 2.3.6 測量單分子導電值對時間關係曲線 31 2.3.7 EC-STM循環伏安法 32 2.4 數據處理 33 2.4.1 導電值對探針位移之二維統計圖 33 2.4.2 標準化雜訊功率對平均導電值之二維統計圖 34 第3章 結果與討論 36 3.1 三核銠金屬串錯合物之電性表現 36 3.1.1 中性態[Rh3(dpa)4(CN)2]與[Rh3(dpa)4(NCS)2]之電性表現 36 3.1.2 [Rh3(dpa)4(NCS)2]+之電性表現 40 3.2 五核鉻、鈷及鎳金屬串錯合物之電性表現 43 3.3 金屬串錯合物的電子傳輸機制 46 第4章 結論 50 參考資料 52 附錄 58 | |
dc.language.iso | zh-TW | |
dc.title | 以閃爍雜訊分析金屬串錯合物之電子傳輸機制 | zh_TW |
dc.title | Flicker Noise Analysis on Electron Transport of Single-Molecule Junctions of Metal-String Complexes | en |
dc.date.schoolyear | 109-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 彭旭明(Hsin-Tsai Liu),許良彥(Chih-Yang Tseng) | |
dc.subject.keyword | 閃爍雜訊分析法,電化學,金屬串錯合物,分子電子學,掃描式穿隧顯微術破裂接合法, | zh_TW |
dc.subject.keyword | Flicker Noise,Electrochemistry,Metal-string Complexes,Molecular Electronics,Scanning Tunneling Microscope-based Break-Junction, | en |
dc.relation.page | 60 | |
dc.identifier.doi | 10.6342/NTU202102156 | |
dc.rights.note | 同意授權(全球公開) | |
dc.date.accepted | 2021-08-09 | |
dc.contributor.author-college | 理學院 | zh_TW |
dc.contributor.author-dept | 化學研究所 | zh_TW |
dc.date.embargo-lift | 2023-12-31 | - |
顯示於系所單位: | 化學系 |
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