Direct Visualization of Exciton Reequilibration in the LH1 and LH2 Complexes of Rhodobacter sphaeroides by Multipulse Spectroscopy
The dynamics of the excited states of the light-harvesting complexes LH1 and LH2 of Rhodobacter sphaeroides are governed, mainly, by the excitonic nature of these ring-systems. In a pump-dump-probe experiment, the first pulse promotes LH1 or LH2 to its excited state and the second pulse dumps a port...
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creator | Cohen Stuart, Thomas A. Vengris, Mikas Novoderezhkin, Vladimir I. Cogdell, Richard J. Hunter, C. Neil van Grondelle, Rienk |
description | The dynamics of the excited states of the light-harvesting complexes LH1 and LH2 of
Rhodobacter sphaeroides are governed, mainly, by the excitonic nature of these ring-systems. In a pump-dump-probe experiment, the first pulse promotes LH1 or LH2 to its excited state and the second pulse dumps a portion of the excited state. By selective dumping, we can disentangle the dynamics normally hidden in the excited-state manifold. We find that by using this multiple-excitation technique we can visualize a 400-fs reequilibration reflecting relaxation between the two lowest exciton states that cannot be directly explored by conventional pump-probe. An oscillatory feature is observed within the exciton reequilibration, which is attributed to a coherent motion of a vibrational wavepacket with a period of ∼150 fs. Our disordered exciton model allows a quantitative interpretation of the observed reequilibration processes occurring in these antennas. |
doi_str_mv | 10.1016/j.bpj.2011.02.048 |
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Rhodobacter sphaeroides are governed, mainly, by the excitonic nature of these ring-systems. In a pump-dump-probe experiment, the first pulse promotes LH1 or LH2 to its excited state and the second pulse dumps a portion of the excited state. By selective dumping, we can disentangle the dynamics normally hidden in the excited-state manifold. We find that by using this multiple-excitation technique we can visualize a 400-fs reequilibration reflecting relaxation between the two lowest exciton states that cannot be directly explored by conventional pump-probe. An oscillatory feature is observed within the exciton reequilibration, which is attributed to a coherent motion of a vibrational wavepacket with a period of ∼150 fs. Our disordered exciton model allows a quantitative interpretation of the observed reequilibration processes occurring in these antennas.</description><identifier>ISSN: 0006-3495</identifier><identifier>EISSN: 1542-0086</identifier><identifier>DOI: 10.1016/j.bpj.2011.02.048</identifier><identifier>PMID: 21539791</identifier><language>eng</language><publisher>United States: Elsevier Inc</publisher><subject>BASIC BIOLOGICAL SCIENCES ; Biophysics ; Electrons ; Experiments ; Gram-negative bacteria ; Kinetics ; Light-Harvesting Protein Complexes - chemistry ; Protein ; Protein Conformation ; Rhodobacter sphaeroides ; Rhodobacter sphaeroides - metabolism ; solar (fuels), photosynthesis (natural and artificial), biofuels (including algae and biomass), bio-inspired, charge transport, membrane, synthesis (novel materials), synthesis (self-assembly) ; spectroscopy ; Spectrum analysis ; Spectrum Analysis - methods ; Thermodynamics ; Vibration</subject><ispartof>Biophysical journal, 2011-05, Vol.100 (9), p.2226-2233</ispartof><rights>2011 Biophysical Society</rights><rights>Copyright © 2011 Biophysical Society. Published by Elsevier Inc. All rights reserved.</rights><rights>Copyright Biophysical Society May 4, 2011</rights><rights>2011 by the Biophysical Society. 2011 Biophysical Society</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c626t-236377583b1338ac824d0d959a7264be8dda47ff5f470325ae15067a00a728f63</citedby><cites>FETCH-LOGICAL-c626t-236377583b1338ac824d0d959a7264be8dda47ff5f470325ae15067a00a728f63</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC3149263/pdf/$$EPDF$$P50$$Gpubmedcentral$$H</linktopdf><linktohtml>$$Uhttps://www.sciencedirect.com/science/article/pii/S0006349511002992$$EHTML$$P50$$Gelsevier$$Hfree_for_read</linktohtml><link.rule.ids>230,314,723,776,780,881,3537,27903,27904,53768,53770,65308</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/21539791$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/1065533$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Cohen Stuart, Thomas A.</creatorcontrib><creatorcontrib>Vengris, Mikas</creatorcontrib><creatorcontrib>Novoderezhkin, Vladimir I.</creatorcontrib><creatorcontrib>Cogdell, Richard J.</creatorcontrib><creatorcontrib>Hunter, C. Neil</creatorcontrib><creatorcontrib>van Grondelle, Rienk</creatorcontrib><creatorcontrib>Energy Frontier Research Centers (EFRC)</creatorcontrib><creatorcontrib>Photosynthetic Antenna Research Center (PARC)</creatorcontrib><title>Direct Visualization of Exciton Reequilibration in the LH1 and LH2 Complexes of Rhodobacter sphaeroides by Multipulse Spectroscopy</title><title>Biophysical journal</title><addtitle>Biophys J</addtitle><description>The dynamics of the excited states of the light-harvesting complexes LH1 and LH2 of
Rhodobacter sphaeroides are governed, mainly, by the excitonic nature of these ring-systems. In a pump-dump-probe experiment, the first pulse promotes LH1 or LH2 to its excited state and the second pulse dumps a portion of the excited state. By selective dumping, we can disentangle the dynamics normally hidden in the excited-state manifold. We find that by using this multiple-excitation technique we can visualize a 400-fs reequilibration reflecting relaxation between the two lowest exciton states that cannot be directly explored by conventional pump-probe. An oscillatory feature is observed within the exciton reequilibration, which is attributed to a coherent motion of a vibrational wavepacket with a period of ∼150 fs. Our disordered exciton model allows a quantitative interpretation of the observed reequilibration processes occurring in these antennas.</description><subject>BASIC BIOLOGICAL SCIENCES</subject><subject>Biophysics</subject><subject>Electrons</subject><subject>Experiments</subject><subject>Gram-negative bacteria</subject><subject>Kinetics</subject><subject>Light-Harvesting Protein Complexes - chemistry</subject><subject>Protein</subject><subject>Protein Conformation</subject><subject>Rhodobacter sphaeroides</subject><subject>Rhodobacter sphaeroides - metabolism</subject><subject>solar (fuels), photosynthesis (natural and artificial), biofuels (including algae and biomass), bio-inspired, charge transport, membrane, synthesis (novel materials), synthesis (self-assembly)</subject><subject>spectroscopy</subject><subject>Spectrum analysis</subject><subject>Spectrum Analysis - methods</subject><subject>Thermodynamics</subject><subject>Vibration</subject><issn>0006-3495</issn><issn>1542-0086</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2011</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNqFksFu1DAQhiMEoqXwAFwg4sJpl7Ed24mQkNBSKNIipJZytRxn0vUqG6d2UnU58uTMsmWBC5xseb6Z8fzzZ9lTBnMGTL1az-thPefA2Bz4HIryXnbMZMFnAKW6nx0DgJqJopJH2aOU1gCMS2APsyPOpKh0xY6z7-98RDfmX32abOe_2dGHPg9tfnrr_EjXc8TryXe-jvuQ7_NxhfnyjOW2b-jk-SJshg5vMe3yzlehCbV1I8Y8DSuLMfiGQvU2_zR1ox-mLmF-MVDTGJILw_Zx9qC19Pjk7jzJLt-fflmczZafP3xcvF3OnOJqnHGhhNayFDUTorSu5EUDTSUrq7kqaiybxha6bWVbaBBcWmQSlLYABJStEifZm33dYao32Djsx2g7M0S_sXFrgvXm70jvV-Yq3BjBioorQQVe7AuENHqTSB90Kxf6nmYxDJSUYge9vOsSw_WEaTQbnxx2ne0xTMlUoJliCuR_yVLR5qoC4HfjA7kOU-xJLIK05EJDSRDbQ450TRHbw2QMzM4uZm3ILmZnFwPckF0o59mfkhwyfvmDgOd7oLXB2Kvok7m8oAqSvMSYVpqI13sCaXU3HuNOGOwdNj-NZZrg__GBH_t72Zc</recordid><startdate>20110504</startdate><enddate>20110504</enddate><creator>Cohen Stuart, Thomas A.</creator><creator>Vengris, Mikas</creator><creator>Novoderezhkin, Vladimir I.</creator><creator>Cogdell, Richard J.</creator><creator>Hunter, C. Neil</creator><creator>van Grondelle, Rienk</creator><general>Elsevier Inc</general><general>Biophysical Society</general><general>Elsevier</general><general>The Biophysical Society</general><scope>6I.</scope><scope>AAFTH</scope><scope>FBQ</scope><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7QO</scope><scope>7QP</scope><scope>7TK</scope><scope>7TM</scope><scope>7U9</scope><scope>8FD</scope><scope>FR3</scope><scope>H94</scope><scope>K9.</scope><scope>P64</scope><scope>7X8</scope><scope>7QL</scope><scope>C1K</scope><scope>OTOTI</scope><scope>5PM</scope></search><sort><creationdate>20110504</creationdate><title>Direct Visualization of Exciton Reequilibration in the LH1 and LH2 Complexes of Rhodobacter sphaeroides by Multipulse Spectroscopy</title><author>Cohen Stuart, Thomas A. ; Vengris, Mikas ; Novoderezhkin, Vladimir I. ; Cogdell, Richard J. ; Hunter, C. Neil ; van Grondelle, Rienk</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c626t-236377583b1338ac824d0d959a7264be8dda47ff5f470325ae15067a00a728f63</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2011</creationdate><topic>BASIC BIOLOGICAL SCIENCES</topic><topic>Biophysics</topic><topic>Electrons</topic><topic>Experiments</topic><topic>Gram-negative bacteria</topic><topic>Kinetics</topic><topic>Light-Harvesting Protein Complexes - chemistry</topic><topic>Protein</topic><topic>Protein Conformation</topic><topic>Rhodobacter sphaeroides</topic><topic>Rhodobacter sphaeroides - metabolism</topic><topic>solar (fuels), photosynthesis (natural and artificial), biofuels (including algae and biomass), bio-inspired, charge transport, membrane, synthesis (novel materials), synthesis (self-assembly)</topic><topic>spectroscopy</topic><topic>Spectrum analysis</topic><topic>Spectrum Analysis - methods</topic><topic>Thermodynamics</topic><topic>Vibration</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Cohen Stuart, Thomas A.</creatorcontrib><creatorcontrib>Vengris, Mikas</creatorcontrib><creatorcontrib>Novoderezhkin, Vladimir I.</creatorcontrib><creatorcontrib>Cogdell, Richard J.</creatorcontrib><creatorcontrib>Hunter, C. 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Neil</au><au>van Grondelle, Rienk</au><aucorp>Energy Frontier Research Centers (EFRC)</aucorp><aucorp>Photosynthetic Antenna Research Center (PARC)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Direct Visualization of Exciton Reequilibration in the LH1 and LH2 Complexes of Rhodobacter sphaeroides by Multipulse Spectroscopy</atitle><jtitle>Biophysical journal</jtitle><addtitle>Biophys J</addtitle><date>2011-05-04</date><risdate>2011</risdate><volume>100</volume><issue>9</issue><spage>2226</spage><epage>2233</epage><pages>2226-2233</pages><issn>0006-3495</issn><eissn>1542-0086</eissn><abstract>The dynamics of the excited states of the light-harvesting complexes LH1 and LH2 of
Rhodobacter sphaeroides are governed, mainly, by the excitonic nature of these ring-systems. In a pump-dump-probe experiment, the first pulse promotes LH1 or LH2 to its excited state and the second pulse dumps a portion of the excited state. By selective dumping, we can disentangle the dynamics normally hidden in the excited-state manifold. We find that by using this multiple-excitation technique we can visualize a 400-fs reequilibration reflecting relaxation between the two lowest exciton states that cannot be directly explored by conventional pump-probe. An oscillatory feature is observed within the exciton reequilibration, which is attributed to a coherent motion of a vibrational wavepacket with a period of ∼150 fs. Our disordered exciton model allows a quantitative interpretation of the observed reequilibration processes occurring in these antennas.</abstract><cop>United States</cop><pub>Elsevier Inc</pub><pmid>21539791</pmid><doi>10.1016/j.bpj.2011.02.048</doi><tpages>8</tpages><oa>free_for_read</oa></addata></record> |
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subjects | BASIC BIOLOGICAL SCIENCES Biophysics Electrons Experiments Gram-negative bacteria Kinetics Light-Harvesting Protein Complexes - chemistry Protein Protein Conformation Rhodobacter sphaeroides Rhodobacter sphaeroides - metabolism solar (fuels), photosynthesis (natural and artificial), biofuels (including algae and biomass), bio-inspired, charge transport, membrane, synthesis (novel materials), synthesis (self-assembly) spectroscopy Spectrum analysis Spectrum Analysis - methods Thermodynamics Vibration |
title | Direct Visualization of Exciton Reequilibration in the LH1 and LH2 Complexes of Rhodobacter sphaeroides by Multipulse Spectroscopy |
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