東華大學圖書館 |

語系: 繁體中文

說明(常見問題)

回圖書館首頁

手機版館藏查詢

登入

回首頁

切換: 標籤 | MARC模式 | ISBD

Photosynthetic Design Principles for...

Sohail, Sara Hess.

FindBook

Google Book

Amazon

博客來

Photosynthetic Design Principles for Ultrafast Energy Transfer Processes.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Photosynthetic Design Principles for Ultrafast Energy Transfer Processes./
作者:	Sohail, Sara Hess.
出版者:	Ann Arbor : ProQuest Dissertations & Theses, : 2020,
面頁冊數:	184 p.
附註:	Source: Dissertations Abstracts International, Volume: 81-10, Section: B.
Contained By:	Dissertations Abstracts International81-10B.
標題:	Chemistry. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=27736119
ISBN:	9781658494724

Photosynthetic Design Principles for Ultrafast Energy Transfer Processes.
Sohail, Sara Hess.

Photosynthetic Design Principles for Ultrafast Energy Transfer Processes. - Ann Arbor : ProQuest Dissertations & Theses, 2020 - 184 p.

Source: Dissertations Abstracts International, Volume: 81-10, Section: B.

Thesis (Ph.D.)--The University of Chicago, 2020.

This item must not be sold to any third party vendors.

As chemists, we often aim to solve each new problem with a unique molecule. Biology takes the opposite approach. Photosynthetic organisms have evolved to survive in diverse habitats by densely packing many of the same pigment molecules to spatially delocalize excitations and support vibronic coherence between pigments. Pigment-pigment and pigment-environment interactions tune chromophore absorption to capture broad wavelengths of light. We seek to understand the design principles that govern the ultrafast dynamics of light harvesting on a femtosecond timescale and apply these design principles to develop molecular artificial light harvesting systems. In this thesis, I present two-dimensional electronic spectra on living cells of the anoxygenic purple bacterium Rhodobacter sphaeroides, the fused antenna/reaction center photosystems from the oxygenic cyanobacterium Synechocystsis sp. PCC 6803 in their native membrane environment, and DNA-dye constructs that are candidates for artificial light harvesting applications. In Rhodobacter sphaeroides, we collected the first fully absorptive two-dimensional electronic spectra of a living cell, revealing a sub-100 fs intracomplex relaxation in light harvesting complex 1. We present a synthetic system of coupled cyanine dyes that supports vibronic coherence, a photosynthetic design principle implicated in efficient exciton energy transfer in photosynthetic organisms, by tethering the dyes to a DNA scaffold. It is the first report of using DNA to engineer vibronic coherence. We use singlet-singlet annihilation to track inter-complex energy transfer between isoenergetic complexes in intact thylakoids prepared from wild-type and mutant cyanobacterial cells. We observe diffusion-limited trapping behavior between red Chl pools on neighboring Photosystem I monomers in these Synechocystis sp. PCC 6803 membrane fragments. We also present the first two-dimensional electronic spectra of living cyanobacteria. This represents a major advance in in vivo ultrafast spectroscopy, opening the door to studying regulatory and response mechanisms in these more complex oxygenic phototrophes. Future planned experiments include the investigation of the effects of light quantity and quality on the organization of the photosynthetic machinery in cyanobacteria, experiments to elucidate the molecular mechanics and quantum dynamics of photoprotective quenching in green algae, and engineering efficient energy transfer aided by vibronic coherence in a synthetic dye-DNA assembly.

ISBN: 9781658494724Subjects--Topical Terms:

516420
Chemistry.
Subjects--Index Terms:

Electronic spectroscopy

Photosynthetic Design Principles for Ultrafast Energy Transfer Processes.
LDR:03673nmm a2200361 4500 001 2266105
005 20200608114800.5
008 220629s2020 ||||||||||||||||| ||eng d
020 $a 9781658494724
035 $a (MiAaPQ)AAI27736119
035 $a AAI27736119
040 $a MiAaPQ $c MiAaPQ
100 1 $a Sohail, Sara Hess. $3 3543291
245 1 0 $a Photosynthetic Design Principles for Ultrafast Energy Transfer Processes.
260 1 $a Ann Arbor : $b ProQuest Dissertations & Theses, $c 2020
300 $a 184 p.
500 $a Source: Dissertations Abstracts International, Volume: 81-10, Section: B.
500 $a Advisor: Engel, Gregory S.
502 $a Thesis (Ph.D.)--The University of Chicago, 2020.
506 $a This item must not be sold to any third party vendors.
520 $a As chemists, we often aim to solve each new problem with a unique molecule. Biology takes the opposite approach. Photosynthetic organisms have evolved to survive in diverse habitats by densely packing many of the same pigment molecules to spatially delocalize excitations and support vibronic coherence between pigments. Pigment-pigment and pigment-environment interactions tune chromophore absorption to capture broad wavelengths of light. We seek to understand the design principles that govern the ultrafast dynamics of light harvesting on a femtosecond timescale and apply these design principles to develop molecular artificial light harvesting systems. In this thesis, I present two-dimensional electronic spectra on living cells of the anoxygenic purple bacterium Rhodobacter sphaeroides, the fused antenna/reaction center photosystems from the oxygenic cyanobacterium Synechocystsis sp. PCC 6803 in their native membrane environment, and DNA-dye constructs that are candidates for artificial light harvesting applications. In Rhodobacter sphaeroides, we collected the first fully absorptive two-dimensional electronic spectra of a living cell, revealing a sub-100 fs intracomplex relaxation in light harvesting complex 1. We present a synthetic system of coupled cyanine dyes that supports vibronic coherence, a photosynthetic design principle implicated in efficient exciton energy transfer in photosynthetic organisms, by tethering the dyes to a DNA scaffold. It is the first report of using DNA to engineer vibronic coherence. We use singlet-singlet annihilation to track inter-complex energy transfer between isoenergetic complexes in intact thylakoids prepared from wild-type and mutant cyanobacterial cells. We observe diffusion-limited trapping behavior between red Chl pools on neighboring Photosystem I monomers in these Synechocystis sp. PCC 6803 membrane fragments. We also present the first two-dimensional electronic spectra of living cyanobacteria. This represents a major advance in in vivo ultrafast spectroscopy, opening the door to studying regulatory and response mechanisms in these more complex oxygenic phototrophes. Future planned experiments include the investigation of the effects of light quantity and quality on the organization of the photosynthetic machinery in cyanobacteria, experiments to elucidate the molecular mechanics and quantum dynamics of photoprotective quenching in green algae, and engineering efficient energy transfer aided by vibronic coherence in a synthetic dye-DNA assembly.
590 $a School code: 0330.
650 4 $a Chemistry. $3 516420
650 4 $a Physical chemistry. $3 1981412
653 $a Electronic spectroscopy
653 $a Light harvesting
653 $a Molecular dimers
653 $a Photosynthesis
653 $a Ultrafast
690 $a 0485
690 $a 0494
710 2 $a The University of Chicago. $b Chemistry. $3 1675066
773 0 $t Dissertations Abstracts International $g 81-10B.
790 $a 0330
791 $a Ph.D.
792 $a 2020
793 $a English
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=27736119