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Title: Excited State Structural Dynamics of Carotenoids and ChargeTransfer Systems

Abstract

This dissertation describes the development andimplementation of a visible/near infrared pump/mid-infrared probeapparatus. Chapter 1 describes the background and motivation ofinvestigating optically induced structural dynamics, paying specificattention to solvation and the excitation selection rules of highlysymmetric molecules such as carotenoids. Chapter 2 describes thedevelopment and construction of the experimental apparatus usedthroughout the remainder of this dissertation. Chapter 3 will discuss theinvestigation of DCM, a laser dye with a fluorescence signal resultingfrom a charge transfer state. By studying the dynamics of DCM and of itsmethyl deuterated isotopomer (an otherwise identical molecule), we areable to investigate the origins of the charge transfer state and provideevidence that it is of the controversial twisted intramolecular (TICT)type. Chapter 4 introduces the use of two-photon excitation to the S1state, combined with one-photon excitation to the S2 state of thecarotenoid beta-apo-8'-carotenal. These 2 investigations show evidencefor the formation of solitons, previously unobserved in molecular systemsand found only in conducting polymers Chapter 5 presents an investigationof the excited state dynamics of peridinin, the carotenoid responsiblefor the light harvesting of dinoflagellates. This investigation allowsfor a more detailed understanding of the importance of structuraldynamics of carotenoids in light harvesting.

Authors:
 [1]
  1. Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National ScienceFoundation
OSTI Identifier:
925609
Report Number(s):
LBNL-63796
R&D Project: 449A01; BnR: KC0301010; TRN: US0803066
DOE Contract Number:  
AC02-05CH11231; NSF:CHE0131524-FLEMING
Resource Type:
Thesis/Dissertation
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CAROTENOIDS; CONSTRUCTION; DYES; EXCITATION; EXCITED STATES; FLUORESCENCE; HARVESTING; IMPLEMENTATION; LASERS; POLYMERS; PROBES; SELECTION RULES; SOLITONS; SOLVATION; visible/near infrared pump/mid infrared apparatus opticallyinduced structural dynamics carotenoids charge transfer systems solitonsexcited state dynamics of peridinin light harvesting

Citation Formats

Van Tassle, Aaron Justin. Excited State Structural Dynamics of Carotenoids and ChargeTransfer Systems. United States: N. p., 2006. Web. doi:10.2172/925609.
Van Tassle, Aaron Justin. Excited State Structural Dynamics of Carotenoids and ChargeTransfer Systems. United States. doi:10.2172/925609.
Van Tassle, Aaron Justin. Sun . "Excited State Structural Dynamics of Carotenoids and ChargeTransfer Systems". United States. doi:10.2172/925609. https://www.osti.gov/servlets/purl/925609.
@article{osti_925609,
title = {Excited State Structural Dynamics of Carotenoids and ChargeTransfer Systems},
author = {Van Tassle, Aaron Justin},
abstractNote = {This dissertation describes the development andimplementation of a visible/near infrared pump/mid-infrared probeapparatus. Chapter 1 describes the background and motivation ofinvestigating optically induced structural dynamics, paying specificattention to solvation and the excitation selection rules of highlysymmetric molecules such as carotenoids. Chapter 2 describes thedevelopment and construction of the experimental apparatus usedthroughout the remainder of this dissertation. Chapter 3 will discuss theinvestigation of DCM, a laser dye with a fluorescence signal resultingfrom a charge transfer state. By studying the dynamics of DCM and of itsmethyl deuterated isotopomer (an otherwise identical molecule), we areable to investigate the origins of the charge transfer state and provideevidence that it is of the controversial twisted intramolecular (TICT)type. Chapter 4 introduces the use of two-photon excitation to the S1state, combined with one-photon excitation to the S2 state of thecarotenoid beta-apo-8'-carotenal. These 2 investigations show evidencefor the formation of solitons, previously unobserved in molecular systemsand found only in conducting polymers Chapter 5 presents an investigationof the excited state dynamics of peridinin, the carotenoid responsiblefor the light harvesting of dinoflagellates. This investigation allowsfor a more detailed understanding of the importance of structuraldynamics of carotenoids in light harvesting.},
doi = {10.2172/925609},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2006},
month = {1}
}

Thesis/Dissertation:
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