Simulations of the Two-Dimensional Electronic Spectroscopy of the Photosystem II Reaction Center
We report simulations of the two-dimensional electronic spectroscopy of the Q y band of the D1-D2-Cyt b559 photosystem II reaction center at 77 K. We base the simulations on an existing Hamiltonian that was derived by simultaneous fitting to a wide range of linear spectroscopic measurements and desc...
Gespeichert in:
| Veröffentlicht in: | The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Molecules, spectroscopy, kinetics, environment, & general theory, 2013-01, Vol.117 (1), p.34-41 |
|---|---|
| Hauptverfasser: | , , , , , , |
| Format: | Artikel |
| Sprache: | eng |
| Schlagworte: | |
| Online-Zugang: | Volltext |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| container_end_page | 41 |
|---|---|
| container_issue | 1 |
| container_start_page | 34 |
| container_title | The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory |
| container_volume | 117 |
| creator | Lewis, K. L. M Fuller, F. D Myers, J. A Yocum, C. F Mukamel, S Abramavicius, D Ogilvie, J. P |
| description | We report simulations of the two-dimensional electronic spectroscopy of the Q y band of the D1-D2-Cyt b559 photosystem II reaction center at 77 K. We base the simulations on an existing Hamiltonian that was derived by simultaneous fitting to a wide range of linear spectroscopic measurements and described within modified Redfield theory. The model obtains reasonable agreement with most aspects of the two-dimensional spectra, including the overall peak shapes and excited state absorption features. It does not reproduce the rapid equilibration from high energy to low energy excitonic states evident by a strong cross-peak below the diagonal. We explore modifications to the model to incorporate new structural data and improve agreement with the two-dimensional spectra. We find that strengthening the system–bath coupling and lowering the degree of disorder significantly improves agreement with the cross-peak feature, while lessening agreement with the relative diagonal/antidiagonal width of the 2D spectra. We conclude that two-dimensional electronic spectroscopy provides a sensitive test of excitonic models of the photosystem II reaction center and discuss avenues for further refinement of such models. |
| doi_str_mv | 10.1021/jp3081707 |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_pubme</sourceid><recordid>TN_cdi_pubmedcentral_primary_oai_pubmedcentral_nih_gov_3702820</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>1273392258</sourcerecordid><originalsourceid>FETCH-LOGICAL-a534t-ecb4240ce02f74cd479b3590817f3bb5e51392bb54872da2046fab073f0274d03</originalsourceid><addsrcrecordid>eNqFkV9v0zAUxa0JtI1tD3wBlBck9hC4vrbr5AUJlf2pNAm0bs_GcR3qKokzO2Hqt8dduw4kJJ58ZP907rk-hLyl8JEC0k-rnkFBJcgDckwFQi6QildJQ1HmYsLKI_ImxhUAUIb8kBwhQwp8wo7Jj7lrx0YPzncx83U2LG129-jzr661XUy3uskuGmuG4Dtnsnn_JKPx_foZ_770g4_rONg2m82yW6vNxi6b2m6w4ZS8rnUT7dnuPCH3lxd30-v85tvVbPrlJteC8SG3puLIwVjAWnKz4LKsmCg3a9WsqoQVlJWYBC8kLjSm9LWuQLIaUPIFsBPyeevbj1VrFyYND7pRfXCtDmvltVN_v3RuqX76X4pJwAI3Bh92BsE_jDYOqnXR2KbRnfVjVFSmoMWEyfL_KEqW0qIoEnq-RU36tRhsvU9EQW3KU_vyEvvuzxX25HNbCXi_A3Q0uqmD7oyLL1wyKVHIF06bqFZ-DKnF-I-BvwGFuq2W</addsrcrecordid><sourcetype>Open Access Repository</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>1273392258</pqid></control><display><type>article</type><title>Simulations of the Two-Dimensional Electronic Spectroscopy of the Photosystem II Reaction Center</title><source>MEDLINE</source><source>American Chemical Society Journals</source><creator>Lewis, K. L. M ; Fuller, F. D ; Myers, J. A ; Yocum, C. F ; Mukamel, S ; Abramavicius, D ; Ogilvie, J. P</creator><creatorcontrib>Lewis, K. L. M ; Fuller, F. D ; Myers, J. A ; Yocum, C. F ; Mukamel, S ; Abramavicius, D ; Ogilvie, J. P</creatorcontrib><description>We report simulations of the two-dimensional electronic spectroscopy of the Q y band of the D1-D2-Cyt b559 photosystem II reaction center at 77 K. We base the simulations on an existing Hamiltonian that was derived by simultaneous fitting to a wide range of linear spectroscopic measurements and described within modified Redfield theory. The model obtains reasonable agreement with most aspects of the two-dimensional spectra, including the overall peak shapes and excited state absorption features. It does not reproduce the rapid equilibration from high energy to low energy excitonic states evident by a strong cross-peak below the diagonal. We explore modifications to the model to incorporate new structural data and improve agreement with the two-dimensional spectra. We find that strengthening the system–bath coupling and lowering the degree of disorder significantly improves agreement with the cross-peak feature, while lessening agreement with the relative diagonal/antidiagonal width of the 2D spectra. We conclude that two-dimensional electronic spectroscopy provides a sensitive test of excitonic models of the photosystem II reaction center and discuss avenues for further refinement of such models.</description><identifier>ISSN: 1089-5639</identifier><identifier>EISSN: 1520-5215</identifier><identifier>DOI: 10.1021/jp3081707</identifier><identifier>PMID: 23210463</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>Biological and medical sciences ; Computer Simulation ; Electronics ; Energy Transfer ; Excitation spectra ; Fittings ; Fundamental and applied biological sciences. Psychology ; General aspects, investigation technics, apparatus ; Mathematical models ; Models, Molecular ; Photosystem II Protein Complex - chemistry ; Protein Conformation ; Spectra ; Spectroscopy ; Spectrum Analysis - methods ; Tissues, organs and organisms biophysics ; Two dimensional</subject><ispartof>The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory, 2013-01, Vol.117 (1), p.34-41</ispartof><rights>Copyright © 2012 American Chemical Society</rights><rights>2014 INIST-CNRS</rights><rights>2012 American Chemical Society 2012</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a534t-ecb4240ce02f74cd479b3590817f3bb5e51392bb54872da2046fab073f0274d03</citedby><cites>FETCH-LOGICAL-a534t-ecb4240ce02f74cd479b3590817f3bb5e51392bb54872da2046fab073f0274d03</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/jp3081707$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/jp3081707$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,776,780,881,2752,27055,27903,27904,56716,56766</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=27079257$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/23210463$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Lewis, K. L. M</creatorcontrib><creatorcontrib>Fuller, F. D</creatorcontrib><creatorcontrib>Myers, J. A</creatorcontrib><creatorcontrib>Yocum, C. F</creatorcontrib><creatorcontrib>Mukamel, S</creatorcontrib><creatorcontrib>Abramavicius, D</creatorcontrib><creatorcontrib>Ogilvie, J. P</creatorcontrib><title>Simulations of the Two-Dimensional Electronic Spectroscopy of the Photosystem II Reaction Center</title><title>The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory</title><addtitle>J. Phys. Chem. A</addtitle><description>We report simulations of the two-dimensional electronic spectroscopy of the Q y band of the D1-D2-Cyt b559 photosystem II reaction center at 77 K. We base the simulations on an existing Hamiltonian that was derived by simultaneous fitting to a wide range of linear spectroscopic measurements and described within modified Redfield theory. The model obtains reasonable agreement with most aspects of the two-dimensional spectra, including the overall peak shapes and excited state absorption features. It does not reproduce the rapid equilibration from high energy to low energy excitonic states evident by a strong cross-peak below the diagonal. We explore modifications to the model to incorporate new structural data and improve agreement with the two-dimensional spectra. We find that strengthening the system–bath coupling and lowering the degree of disorder significantly improves agreement with the cross-peak feature, while lessening agreement with the relative diagonal/antidiagonal width of the 2D spectra. We conclude that two-dimensional electronic spectroscopy provides a sensitive test of excitonic models of the photosystem II reaction center and discuss avenues for further refinement of such models.</description><subject>Biological and medical sciences</subject><subject>Computer Simulation</subject><subject>Electronics</subject><subject>Energy Transfer</subject><subject>Excitation spectra</subject><subject>Fittings</subject><subject>Fundamental and applied biological sciences. Psychology</subject><subject>General aspects, investigation technics, apparatus</subject><subject>Mathematical models</subject><subject>Models, Molecular</subject><subject>Photosystem II Protein Complex - chemistry</subject><subject>Protein Conformation</subject><subject>Spectra</subject><subject>Spectroscopy</subject><subject>Spectrum Analysis - methods</subject><subject>Tissues, organs and organisms biophysics</subject><subject>Two dimensional</subject><issn>1089-5639</issn><issn>1520-5215</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2013</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNqFkV9v0zAUxa0JtI1tD3wBlBck9hC4vrbr5AUJlf2pNAm0bs_GcR3qKokzO2Hqt8dduw4kJJ58ZP907rk-hLyl8JEC0k-rnkFBJcgDckwFQi6QildJQ1HmYsLKI_ImxhUAUIb8kBwhQwp8wo7Jj7lrx0YPzncx83U2LG129-jzr661XUy3uskuGmuG4Dtnsnn_JKPx_foZ_770g4_rONg2m82yW6vNxi6b2m6w4ZS8rnUT7dnuPCH3lxd30-v85tvVbPrlJteC8SG3puLIwVjAWnKz4LKsmCg3a9WsqoQVlJWYBC8kLjSm9LWuQLIaUPIFsBPyeevbj1VrFyYND7pRfXCtDmvltVN_v3RuqX76X4pJwAI3Bh92BsE_jDYOqnXR2KbRnfVjVFSmoMWEyfL_KEqW0qIoEnq-RU36tRhsvU9EQW3KU_vyEvvuzxX25HNbCXi_A3Q0uqmD7oyLL1wyKVHIF06bqFZ-DKnF-I-BvwGFuq2W</recordid><startdate>20130110</startdate><enddate>20130110</enddate><creator>Lewis, K. L. M</creator><creator>Fuller, F. D</creator><creator>Myers, J. A</creator><creator>Yocum, C. F</creator><creator>Mukamel, S</creator><creator>Abramavicius, D</creator><creator>Ogilvie, J. P</creator><general>American Chemical Society</general><scope>IQODW</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>7X8</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><scope>5PM</scope></search><sort><creationdate>20130110</creationdate><title>Simulations of the Two-Dimensional Electronic Spectroscopy of the Photosystem II Reaction Center</title><author>Lewis, K. L. M ; Fuller, F. D ; Myers, J. A ; Yocum, C. F ; Mukamel, S ; Abramavicius, D ; Ogilvie, J. P</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a534t-ecb4240ce02f74cd479b3590817f3bb5e51392bb54872da2046fab073f0274d03</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2013</creationdate><topic>Biological and medical sciences</topic><topic>Computer Simulation</topic><topic>Electronics</topic><topic>Energy Transfer</topic><topic>Excitation spectra</topic><topic>Fittings</topic><topic>Fundamental and applied biological sciences. Psychology</topic><topic>General aspects, investigation technics, apparatus</topic><topic>Mathematical models</topic><topic>Models, Molecular</topic><topic>Photosystem II Protein Complex - chemistry</topic><topic>Protein Conformation</topic><topic>Spectra</topic><topic>Spectroscopy</topic><topic>Spectrum Analysis - methods</topic><topic>Tissues, organs and organisms biophysics</topic><topic>Two dimensional</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Lewis, K. L. M</creatorcontrib><creatorcontrib>Fuller, F. D</creatorcontrib><creatorcontrib>Myers, J. A</creatorcontrib><creatorcontrib>Yocum, C. F</creatorcontrib><creatorcontrib>Mukamel, S</creatorcontrib><creatorcontrib>Abramavicius, D</creatorcontrib><creatorcontrib>Ogilvie, J. P</creatorcontrib><collection>Pascal-Francis</collection><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>PubMed Central (Full Participant titles)</collection><jtitle>The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Lewis, K. L. M</au><au>Fuller, F. D</au><au>Myers, J. A</au><au>Yocum, C. F</au><au>Mukamel, S</au><au>Abramavicius, D</au><au>Ogilvie, J. P</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Simulations of the Two-Dimensional Electronic Spectroscopy of the Photosystem II Reaction Center</atitle><jtitle>The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory</jtitle><addtitle>J. Phys. Chem. A</addtitle><date>2013-01-10</date><risdate>2013</risdate><volume>117</volume><issue>1</issue><spage>34</spage><epage>41</epage><pages>34-41</pages><issn>1089-5639</issn><eissn>1520-5215</eissn><abstract>We report simulations of the two-dimensional electronic spectroscopy of the Q y band of the D1-D2-Cyt b559 photosystem II reaction center at 77 K. We base the simulations on an existing Hamiltonian that was derived by simultaneous fitting to a wide range of linear spectroscopic measurements and described within modified Redfield theory. The model obtains reasonable agreement with most aspects of the two-dimensional spectra, including the overall peak shapes and excited state absorption features. It does not reproduce the rapid equilibration from high energy to low energy excitonic states evident by a strong cross-peak below the diagonal. We explore modifications to the model to incorporate new structural data and improve agreement with the two-dimensional spectra. We find that strengthening the system–bath coupling and lowering the degree of disorder significantly improves agreement with the cross-peak feature, while lessening agreement with the relative diagonal/antidiagonal width of the 2D spectra. We conclude that two-dimensional electronic spectroscopy provides a sensitive test of excitonic models of the photosystem II reaction center and discuss avenues for further refinement of such models.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><pmid>23210463</pmid><doi>10.1021/jp3081707</doi><tpages>8</tpages><oa>free_for_read</oa></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 1089-5639 |
| ispartof | The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory, 2013-01, Vol.117 (1), p.34-41 |
| issn | 1089-5639 1520-5215 |
| language | eng |
| recordid | cdi_pubmedcentral_primary_oai_pubmedcentral_nih_gov_3702820 |
| source | MEDLINE; American Chemical Society Journals |
| subjects | Biological and medical sciences Computer Simulation Electronics Energy Transfer Excitation spectra Fittings Fundamental and applied biological sciences. Psychology General aspects, investigation technics, apparatus Mathematical models Models, Molecular Photosystem II Protein Complex - chemistry Protein Conformation Spectra Spectroscopy Spectrum Analysis - methods Tissues, organs and organisms biophysics Two dimensional |
| title | Simulations of the Two-Dimensional Electronic Spectroscopy of the Photosystem II Reaction Center |
| url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2025-01-27T20%3A24%3A15IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_pubme&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Simulations%20of%20the%20Two-Dimensional%20Electronic%20Spectroscopy%20of%20the%20Photosystem%20II%20Reaction%20Center&rft.jtitle=The%20journal%20of%20physical%20chemistry.%20A,%20Molecules,%20spectroscopy,%20kinetics,%20environment,%20&%20general%20theory&rft.au=Lewis,%20K.%20L.%20M&rft.date=2013-01-10&rft.volume=117&rft.issue=1&rft.spage=34&rft.epage=41&rft.pages=34-41&rft.issn=1089-5639&rft.eissn=1520-5215&rft_id=info:doi/10.1021/jp3081707&rft_dat=%3Cproquest_pubme%3E1273392258%3C/proquest_pubme%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=1273392258&rft_id=info:pmid/23210463&rfr_iscdi=true |