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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 彭旭明 | |
dc.contributor.author | Po-Chun Liu | en |
dc.contributor.author | 劉柏君 | zh_TW |
dc.date.accessioned | 2021-06-13T15:37:38Z | - |
dc.date.available | 2008-07-21 | |
dc.date.copyright | 2008-07-21 | |
dc.date.issued | 2008 | |
dc.date.submitted | 2008-07-09 | |
dc.identifier.citation | [1] The 1997 National Technology Roadmap for Semiconductors (SEMATCH, Austin, TX, 1997).
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/37665 | - |
dc.description.abstract | Over the past few decades, a considerable number of studies have been made on metal strings which are believed to have the potential to be used for future nano-electronics. In order to develop new generation of metal strings, two series of them, which contain a mixed-valence pentanickel backbone or a heterometallic framework, have been studied. The first study concerns two new linear pentanickel complexes, [Ni5(bna)4(Cl)2](PF6)2 (6) and [Ni5(bna)4(Cl)2](PF6)4 (7) (bna = binaphthyridylamide), which were synthesized and structurally characterized. The metal framework of complex 7 has a standard [Ni5]10+ core, isoelectronic and isostructural with the metal core of Ni5(tpda)4Cl2, (12) (tpda = tripyridyldiamide). The terminal nickel atoms of 7 are in high-spin state (S = 1) and antiferromagnetic coupled (J = -15.86 cm -1). Complex 6, however, displays the first characterized linear nickel framework in which the usual sequence of NiII atoms has been reduced by two electrons. Each dinickel unit attached to the naphthyridyl moieties is assumed to undergo a one-electron reduction, whereas the central nickel formally remains NiII. Magnetism, NIR spectroscopy and DFT calculation suggest that the metal framework of the mixed-valence complex 6 should be described as intermediate between a localized picture corresponding to NiII-NiI-NiII-NiI-NiII and a fully delocalized model represented as (Ni2)3+-NiII-(Ni2)3+, and is assigned to Robin-Day Class II of mixed-valence complexes. Scanning tunnelling microscopy (STM) methodology was used to assess the conductance and the resistance of single molecules of [Ni5(bna)4(NCS)2](NCS)2 (8) and Ni5(tpda)4Cl2 (11) which are the derivative of complexes 6 and 12. Compound 8 was found to be ~40% more conductive than 11. This result that could be assigned to the electron mobility induced by mixed-valency in the naphthyridyl fragments.
In the second part, two heteronuclear compounds CuPdCu(dpa)4Cl2 (9) and CuPtCu(dpa)4Cl2 (10) were obtained. They are isoelectronic to the oxidized form of the tricopper complex [Cu3(dpa)4Cl2]+ (13), previously characterized and investigated by Berry et al. The magnetic properties and the EPR spectra of 9 and 10 were reported. For 9, there is a weak antiferromagnetic interaction (J = -7.45 cm-1) between the Cu(II) magnetic centers. For 10, the antiferromagnetic interaction sharply decreased to -0.77 cm-1. These properties are at variance with those of 13, for which a relatively strong antiferromagnetic interaction (J = -34 cm-1) has been reported. DFT calculations reproduce the decrease of the magnetic interaction from 9 to 13 and assign it to the role of the nonmagnetic metal (CuIII and PdII) in the transference of the superexchange interaction. | en |
dc.description.provenance | Made available in DSpace on 2021-06-13T15:37:38Z (GMT). No. of bitstreams: 1 ntu-97-D94223010-1.pdf: 6476021 bytes, checksum: f66e4c5f349eccc8925cd1f1d48e657e (MD5) Previous issue date: 2008 | en |
dc.description.tableofcontents | Chapter 1 Introduction 1
1.1 Molecular Electronic Device – The Future Electronic Devices 1 1.2 Molecular Wires 2 1.3 One Dimensional Metal Chain Complexes 2 1.4 A Brief Introduction of the Research Interests of the Metal Strings 6 1.5 Concept of Designing and Studying the New Metal Strings in These Studies 8 Chapter 2 Experimental Section 11 2.1 Chemicals 11 2.2 Techniques 12 2.3 Preparations 16 Chapter 3 Mixed-Valence Linear [Ni5]8+ Complex .23 3.1 Concept of Designing New Linear Pentanickel Complex 23 3.2 Synthesis and Structure Results 26 3.3 Magnetic Properties 31 3.4 NMR Spectroscopy 36 3.5 Near-IR Spectra 39 3.6 Electrochemistry 42 3.7 DFT Calculations 43 3.8 Single Molecular Conductance of [Ni5(bna)4(NCS)2](NCS)2 (8) and Ni5(tpda)4(NCS)2 (11) 51 Chapter 4 Heteronuclear Cu-Pd-Cu And Cu-Pt-Cu Complexes 55 4.1 Concept of Studying the Exchange Interaction of Metal Strings 55 4.2 Structural Results 57 4.3 Magnetic Properties 60 4.4 Electronic Paramagnetic Resonance 63 4.5 DFT Calculations 68 Chapter 5 Conclusions 77 Reference 82 Appendix 90 | |
dc.language.iso | en | |
dc.title | 新世代混價及混金屬分子導線的合成與理論研究 | zh_TW |
dc.title | New Generations of Metal Strings: Synthesis, Structure, Magnetism, Spectroscopy and Theoretical Analysis of the Mixed-Valence [Ni5]8+ Compound and Two Mixed-Metal (Cu-Pd-Cu and Cu-Pt-Cu) Complexes. | en |
dc.type | Thesis | |
dc.date.schoolyear | 96-2 | |
dc.description.degree | 博士 | |
dc.contributor.oralexamcommittee | 王瑜,金必耀,葉震宇,陳俊顯,馬克柏納德(Marc Benard),瑪麗瑪德蓮何摩(Marie-Madeleine Rohmer) | |
dc.subject.keyword | 分子導線,密度泛函數計算,分子磁性,混價化合物,金屬鍵,混金屬化合物,磁交換作用, | zh_TW |
dc.subject.keyword | molecular wires,density functional theory calculation,molecular magnetism,mixed-valence compound,metal-metal interaction,mixed-metal compound,exchange interaction, | en |
dc.relation.page | 141 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2008-07-10 | |
dc.contributor.author-college | 理學院 | zh_TW |
dc.contributor.author-dept | 化學研究所 | zh_TW |
顯示於系所單位: | 化學系 |
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