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Non-classical Stark effects of photosynthetic reaction centers.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Non-classical Stark effects of photosynthetic reaction centers.
Author:	Treynor, Thomas Pirrie.
Description:	241 p.
Notes:	Adviser: Steven G. Boxer.
Notes:	Source: Dissertation Abstracts International, Volume: 64-09, Section: B, page: 4379.
Contained By:	Dissertation Abstracts International64-09B.
Subject:	Chemistry, Physical.
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3104165
ISBN:	0496517333

Non-classical Stark effects of photosynthetic reaction centers.
Treynor, Thomas Pirrie.

Non-classical Stark effects of photosynthetic reaction centers. [electronic resource] - 241 p.

Adviser: Steven G. Boxer.

Thesis (Ph.D.)--Stanford University, 2003.

For each non-classical Stark effect its theoretical basis is considered in detail and quantitative analytical tools are developed. Also, each of these non-classical Stark effects is applied to the characterization of the electronic structure of photosynthetic reaction centers. Some of the results include the following: new constraints on the organization of the carotenoids in photosystem II core complexes are determined; the dielectric screening is found to be greater in the vicinity of the special pair than in the vicinity of the strongly bound quinone in bacterial reaction centers; the dipole strength of the intervalence band of the special pair radical cation in bacterial reaction centers is found to be strongly affected by intensity borrowing; comparisons of Stark spectra among wild-type and perturbed bacterial reaction centers support a two-step mechanism over a superexchange mechanism for the primary electron transfer event.

ISBN: 0496517333Subjects--Topical Terms:

226924
Chemistry, Physical.

Non-classical Stark effects of photosynthetic reaction centers.
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245 1 0 $a Non-classical Stark effects of photosynthetic reaction centers. $h [electronic resource]
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500 $a Adviser: Steven G. Boxer.
500 $a Source: Dissertation Abstracts International, Volume: 64-09, Section: B, page: 4379.
502 $a Thesis (Ph.D.)--Stanford University, 2003.
520 # $a For each non-classical Stark effect its theoretical basis is considered in detail and quantitative analytical tools are developed. Also, each of these non-classical Stark effects is applied to the characterization of the electronic structure of photosynthetic reaction centers. Some of the results include the following: new constraints on the organization of the carotenoids in photosystem II core complexes are determined; the dielectric screening is found to be greater in the vicinity of the special pair than in the vicinity of the strongly bound quinone in bacterial reaction centers; the dipole strength of the intervalence band of the special pair radical cation in bacterial reaction centers is found to be strongly affected by intensity borrowing; comparisons of Stark spectra among wild-type and perturbed bacterial reaction centers support a two-step mechanism over a superexchange mechanism for the primary electron transfer event.
520 # $a Three methods are developed for characterizing charge transfer processes in organized systems, whether organic, inorganic or biological. They are similar in that each utilizes the experimental technique of Stark spectroscopy, in which the perturbation to a spectrum by an applied electric field is measured, but they differ in the kind of charge transfer process studied. Thermally activated charge transfer processes, as described by Marcus theory, are shown to give rise to field-modulated population effects. Excited-state tunneling processes, as described by radiationless relaxation theory, are shown to give rise to resonance Stark effects. Intervalence band absorption spectra, as described by PKS theory, are shown to give rise to intervalence band Stark effects. Collectively these phenomena are referred to as non-classical Stark effects in order to distinguish their information content from that of so-called classical Stark effects. Whereas classical Stark effects have been used widely to characterize the electronic properties of atoms or molecules in vacuo or in situ, non-classical Stark effects have been underutilized considering their unique abilities to inform those aspects of electronic structure which are peculiar to charge transfer processes: their driving forces, reorganization energies and electronic couplings.
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