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Self-assembly, redox activity, and c...

Skomski, Daniel.

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Self-assembly, redox activity, and charge transport of functional surface nano-architectures by molecular design.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Self-assembly, redox activity, and charge transport of functional surface nano-architectures by molecular design./
Author:	Skomski, Daniel.
Description:	250 p.
Notes:	Source: Dissertation Abstracts International, Volume: 76-12(E), Section: B.
Contained By:	Dissertation Abstracts International76-12B(E).
Subject:	Materials science. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3718566
ISBN:	9781321984378

Self-assembly, redox activity, and charge transport of functional surface nano-architectures by molecular design.
Skomski, Daniel.

Self-assembly, redox activity, and charge transport of functional surface nano-architectures by molecular design. - 250 p.

Source: Dissertation Abstracts International, Volume: 76-12(E), Section: B.

Thesis (Ph.D.)--Indiana University, 2015.

Surface-assisted molecular self-assembly is a promising strategy to program the structure and chemical state of atoms and molecules in nano-architectures to achieve a specific function. The experiments described in this thesis demonstrate that the design and programming of basic organic components leads to desired characteristics by self-assembly. The fabrication of uniform single-site metal centers at surfaces, important for high selectivity in next-generation catalysts, was accomplished by coordination to redox non-innocent phenanthroline and tetrazine-based ligands. These examples were the first demonstrating tuning of the metal oxidation state in surface coordination architectures through rational ligand design. The molecular-scale coordination architectures were the first formed from chromium and vanadium, and the first from platinum in a non-porphyrin system. The first mixed valence metal-ligand surface structure was fabricated that attained the same ligand coordination number for all metal sites. A new surface reaction method was demonstrated between an inexpensive sodium chloride reagent and carboxylate ligands. High-temperature, molecular-resolution microscopy and spectroscopy of the ordered metal-organic structures demonstrated thermal stability up to 300 °C, the highest molecular-level thermal stability in organic surface nanostructures yet achieved, making such systems potential candidates for moderate-temperature catalytic reactions. Molecular self-assembly was expanded into organic semiconductor thin films. In a two-component, bi-layered system, hydrogen bonding between carboxylates and carboxylic acid-substituted thiophenes was utilized, yielding the first real-space images of phenyl-thiophene stacking. In a one-component system, multiple donor-acceptor pi-pi contacts between phenyltriazole building blocks accomplished assembly of flat-lying molecules from a surface with molecular-scale precision through more than twenty molecular layers. Sufficient inter-layer charge transport allowed electronic property characterization with the scanning tunneling microscope, demonstrating a narrowing of the film bandgap with increasing thickness which evidenced electron conjugation in the film. These results have advanced our understanding of supramolecular self-assembly at surfaces and how it can impact future technologies from organic-based materials.

ISBN: 9781321984378Subjects--Topical Terms:

543314
Materials science.

Self-assembly, redox activity, and charge transport of functional surface nano-architectures by molecular design.
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500 $a Adviser: Steven L. Tait.
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