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Spectroscopic characterization of ch...

Yale University.

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Spectroscopic characterization of charge localization and delocalization in ionic clusters.

紀錄類型:	書目-語言資料,印刷品 : Monograph/item
正題名/作者:	Spectroscopic characterization of charge localization and delocalization in ionic clusters./
作者:	Roscioli, Joseph R.
面頁冊數:	311 p.
附註:	Adviser: Mark A. Johnson.
Contained By:	Dissertation Abstracts International70-01B.
標題:	Chemistry, Physical. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3342666
ISBN:	9780549977421

Spectroscopic characterization of charge localization and delocalization in ionic clusters.
Roscioli, Joseph R.

Spectroscopic characterization of charge localization and delocalization in ionic clusters. - 311 p.

Adviser: Mark A. Johnson.

Thesis (Ph.D.)--Yale University, 2008.

This thesis presents an overview of studies aimed at resolving the molecular-level conceptual framework required to understand charge localization and delocalization in ionic clusters. These begin with a series of experiments in which the detailed structures and electron binding motifs of hydrated electron clusters, (H 2O)n-, are explored using one- and two-laser isomer selection techniques. The delocalized excess electron binds to the neutral water cluster scaffold by one of two general mechanisms, which are spectrally characterized over a wide range of cluster sizes. In contrast to these studies, proton delocalization plays a dominant role in the energetics of clusters of the form [A·H·B] +/-, where A and B comprise a variety of chemical species from halides to ammonia to ethers. The transitions associated with the shared proton vary between 700 and 3500 cm-1, depending upon the identities of A and B, and isotopic substitution is used to understand how the motions responsible for this spectral activity are intimately coupled to the other vibrational modes in the complex. This work is extended to larger proton-bound clusters, H+·[A·B·C], where excitation of the shared H atoms leads to intermolecular charge transfer reminiscent of the Grotthus mechanism.

ISBN: 9780549977421Subjects--Topical Terms:

560527
Chemistry, Physical.

Spectroscopic characterization of charge localization and delocalization in ionic clusters.
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502 $a Thesis (Ph.D.)--Yale University, 2008.
520 $a This thesis presents an overview of studies aimed at resolving the molecular-level conceptual framework required to understand charge localization and delocalization in ionic clusters. These begin with a series of experiments in which the detailed structures and electron binding motifs of hydrated electron clusters, (H 2O)n-, are explored using one- and two-laser isomer selection techniques. The delocalized excess electron binds to the neutral water cluster scaffold by one of two general mechanisms, which are spectrally characterized over a wide range of cluster sizes. In contrast to these studies, proton delocalization plays a dominant role in the energetics of clusters of the form [A·H·B] +/-, where A and B comprise a variety of chemical species from halides to ammonia to ethers. The transitions associated with the shared proton vary between 700 and 3500 cm-1, depending upon the identities of A and B, and isotopic substitution is used to understand how the motions responsible for this spectral activity are intimately coupled to the other vibrational modes in the complex. This work is extended to larger proton-bound clusters, H+·[A·B·C], where excitation of the shared H atoms leads to intermolecular charge transfer reminiscent of the Grotthus mechanism.
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