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Mechanism of adiabatic primary electron transfer in photosystem I: Femtosecond spectroscopy upon excitation of reaction center in the far-red edge of the QY band
The ultrafast primary charge separation in Photosystem I (PS I) excited by femtosecond pulses centered at 720 and 760nm was studied by pump-to-probe laser spectroscopy. The absorbance in the red edge of PS I absorption spectrum has an unusual exponential dependence on wavelength. The cutoff of short...
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| Published in: | Biochimica et biophysica acta. Bioenergetics 2017-11, Vol.1858 (11), p.895-905 |
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| cites | cdi_FETCH-LOGICAL-c381t-d38e035596e209fbd86dbd79d5c4a957da889a45953966ef127d0ac242f45ce63 |
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| container_title | Biochimica et biophysica acta. Bioenergetics |
| container_volume | 1858 |
| creator | Cherepanov, Dmitry A. Shelaev, Ivan V. Gostev, Fedor E. Mamedov, Mahir D. Petrova, Anastasia A. Aybush, Arseniy V. Shuvalov, Vladimir A. Semenov, Alexey Yu Nadtochenko, Victor A. |
| description | The ultrafast primary charge separation in Photosystem I (PS I) excited by femtosecond pulses centered at 720 and 760nm was studied by pump-to-probe laser spectroscopy. The absorbance in the red edge of PS I absorption spectrum has an unusual exponential dependence on wavelength. The cutoff of short wavelength components of 760nm pulse allows direct excitation of reaction center chlorophyll molecules without involvement of light-harvesting antenna. The transient spectrum manifests the features of the primary ion-radical pair P700+A0− at time delay |
| doi_str_mv | 10.1016/j.bbabio.2017.08.008 |
| format | article |
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•Femtosecond pump-to-probe laser spectroscopy of photosystem I exited at 760nm.•Direct excitation of primary donor P700 without involvement of antenna.•The primary charge separation in photosystem I proceeds faster than in 200fs.•Exponential asymptotic decline of photosystem I absorption in the red edge.•Three-state adiabatic model of electron transfer between P700 and A0.</description><identifier>ISSN: 0005-2728</identifier><identifier>EISSN: 1879-2650</identifier><identifier>DOI: 10.1016/j.bbabio.2017.08.008</identifier><language>eng</language><publisher>Elsevier B.V</publisher><subject>Adiabatic electron transfer ; Far-red light ; Femtosecond laser spectroscopy ; Photosynthesis, photosystem I, charge separation</subject><ispartof>Biochimica et biophysica acta. Bioenergetics, 2017-11, Vol.1858 (11), p.895-905</ispartof><rights>2017 Elsevier B.V.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c381t-d38e035596e209fbd86dbd79d5c4a957da889a45953966ef127d0ac242f45ce63</citedby><cites>FETCH-LOGICAL-c381t-d38e035596e209fbd86dbd79d5c4a957da889a45953966ef127d0ac242f45ce63</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>315,786,790,27957,27958</link.rule.ids></links><search><creatorcontrib>Cherepanov, Dmitry A.</creatorcontrib><creatorcontrib>Shelaev, Ivan V.</creatorcontrib><creatorcontrib>Gostev, Fedor E.</creatorcontrib><creatorcontrib>Mamedov, Mahir D.</creatorcontrib><creatorcontrib>Petrova, Anastasia A.</creatorcontrib><creatorcontrib>Aybush, Arseniy V.</creatorcontrib><creatorcontrib>Shuvalov, Vladimir A.</creatorcontrib><creatorcontrib>Semenov, Alexey Yu</creatorcontrib><creatorcontrib>Nadtochenko, Victor A.</creatorcontrib><title>Mechanism of adiabatic primary electron transfer in photosystem I: Femtosecond spectroscopy upon excitation of reaction center in the far-red edge of the QY band</title><title>Biochimica et biophysica acta. Bioenergetics</title><description>The ultrafast primary charge separation in Photosystem I (PS I) excited by femtosecond pulses centered at 720 and 760nm was studied by pump-to-probe laser spectroscopy. The absorbance in the red edge of PS I absorption spectrum has an unusual exponential dependence on wavelength. The cutoff of short wavelength components of 760nm pulse allows direct excitation of reaction center chlorophyll molecules without involvement of light-harvesting antenna. The transient spectrum manifests the features of the primary ion-radical pair P700+A0− at time delay <180fs, followed by formation of the secondary pair P700+A1− with a characteristic time of 26ps. The obtained data are rationalized in the framework of adiabatic three-state model that includes the chlorophyll dimer P700 and two symmetrically arranged nearest chlorophyll molecules of A0. The arrangement of chlorophylls results in strong electronic coupling between P700 and A0. Excitation in the maximum of P700 absorption generates electronic states with the highest contribution from P700*, whereas excitation in the far-red edge predominantly generates charge transfer state P700+A0− in both branches of redox-cofactors. The three-level model accounts for a flat-bottomed potential surface of the excited state and adiabatic character of electron transfer between P700 and A0, providing a microscopic explanation of the ultrafast formation of P700+A0− and exponential decline of PS I absorption.
[Display omitted]
•Femtosecond pump-to-probe laser spectroscopy of photosystem I exited at 760nm.•Direct excitation of primary donor P700 without involvement of antenna.•The primary charge separation in photosystem I proceeds faster than in 200fs.•Exponential asymptotic decline of photosystem I absorption in the red edge.•Three-state adiabatic model of electron transfer between P700 and A0.</description><subject>Adiabatic electron transfer</subject><subject>Far-red light</subject><subject>Femtosecond laser spectroscopy</subject><subject>Photosynthesis, photosystem I, charge separation</subject><issn>0005-2728</issn><issn>1879-2650</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2017</creationdate><recordtype>article</recordtype><recordid>eNp9UU1v1DAQtRBIXVr-QQ8-cknqjzixOSChipZKRVUlOHCyHHvCerWxg-2tuj-Hf4q36ZnTvBm990YzD6FLSlpKaH-1a8fRjD62jNChJbIlRL5BGyoH1bBekLdoQwgRDRuYPEPvc96RKusY36C_38FuTfB5xnHCxnkzmuItXpKfTTpi2IMtKQZckgl5goR9wMs2lpiPucCM7z7hG5hrCzYGh_Pyws82Lkd8WKoQnq0v1bPCuiGBsS_YQiirW9kCnkxqEjgM7jecaKfZ4y88muAu0LvJ7DN8eK3n6OfN1x_X35r7h9u76y_3jeWSlsZxCYQLoXpgRE2jk70b3aCcsJ1RYnBGSmU6oQRXfQ8TZYMjxrKOTZ2w0PNz9HH1XVL8c4Bc9Oyzhf3eBIiHrKniRHHOB1Wp3Uq19dKcYNKv79KU6FMieqfXRPQpEU2krolU2edVBvWMJw9JZ-shWHA-1a9pF_3_Df4B4jCZZQ</recordid><startdate>201711</startdate><enddate>201711</enddate><creator>Cherepanov, Dmitry A.</creator><creator>Shelaev, Ivan V.</creator><creator>Gostev, Fedor E.</creator><creator>Mamedov, Mahir D.</creator><creator>Petrova, Anastasia A.</creator><creator>Aybush, Arseniy V.</creator><creator>Shuvalov, Vladimir A.</creator><creator>Semenov, Alexey Yu</creator><creator>Nadtochenko, Victor A.</creator><general>Elsevier B.V</general><scope>6I.</scope><scope>AAFTH</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope></search><sort><creationdate>201711</creationdate><title>Mechanism of adiabatic primary electron transfer in photosystem I: Femtosecond spectroscopy upon excitation of reaction center in the far-red edge of the QY band</title><author>Cherepanov, Dmitry A. ; Shelaev, Ivan V. ; Gostev, Fedor E. ; Mamedov, Mahir D. ; Petrova, Anastasia A. ; Aybush, Arseniy V. ; Shuvalov, Vladimir A. ; Semenov, Alexey Yu ; Nadtochenko, Victor A.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c381t-d38e035596e209fbd86dbd79d5c4a957da889a45953966ef127d0ac242f45ce63</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2017</creationdate><topic>Adiabatic electron transfer</topic><topic>Far-red light</topic><topic>Femtosecond laser spectroscopy</topic><topic>Photosynthesis, photosystem I, charge separation</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Cherepanov, Dmitry A.</creatorcontrib><creatorcontrib>Shelaev, Ivan V.</creatorcontrib><creatorcontrib>Gostev, Fedor E.</creatorcontrib><creatorcontrib>Mamedov, Mahir D.</creatorcontrib><creatorcontrib>Petrova, Anastasia A.</creatorcontrib><creatorcontrib>Aybush, Arseniy V.</creatorcontrib><creatorcontrib>Shuvalov, Vladimir A.</creatorcontrib><creatorcontrib>Semenov, Alexey Yu</creatorcontrib><creatorcontrib>Nadtochenko, Victor A.</creatorcontrib><collection>ScienceDirect Open Access Titles</collection><collection>Elsevier:ScienceDirect:Open Access</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>Biochimica et biophysica acta. Bioenergetics</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Cherepanov, Dmitry A.</au><au>Shelaev, Ivan V.</au><au>Gostev, Fedor E.</au><au>Mamedov, Mahir D.</au><au>Petrova, Anastasia A.</au><au>Aybush, Arseniy V.</au><au>Shuvalov, Vladimir A.</au><au>Semenov, Alexey Yu</au><au>Nadtochenko, Victor A.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Mechanism of adiabatic primary electron transfer in photosystem I: Femtosecond spectroscopy upon excitation of reaction center in the far-red edge of the QY band</atitle><jtitle>Biochimica et biophysica acta. Bioenergetics</jtitle><date>2017-11</date><risdate>2017</risdate><volume>1858</volume><issue>11</issue><spage>895</spage><epage>905</epage><pages>895-905</pages><issn>0005-2728</issn><eissn>1879-2650</eissn><notes>ObjectType-Article-1</notes><notes>SourceType-Scholarly Journals-1</notes><notes>ObjectType-Feature-2</notes><notes>content type line 23</notes><abstract>The ultrafast primary charge separation in Photosystem I (PS I) excited by femtosecond pulses centered at 720 and 760nm was studied by pump-to-probe laser spectroscopy. The absorbance in the red edge of PS I absorption spectrum has an unusual exponential dependence on wavelength. The cutoff of short wavelength components of 760nm pulse allows direct excitation of reaction center chlorophyll molecules without involvement of light-harvesting antenna. The transient spectrum manifests the features of the primary ion-radical pair P700+A0− at time delay <180fs, followed by formation of the secondary pair P700+A1− with a characteristic time of 26ps. The obtained data are rationalized in the framework of adiabatic three-state model that includes the chlorophyll dimer P700 and two symmetrically arranged nearest chlorophyll molecules of A0. The arrangement of chlorophylls results in strong electronic coupling between P700 and A0. Excitation in the maximum of P700 absorption generates electronic states with the highest contribution from P700*, whereas excitation in the far-red edge predominantly generates charge transfer state P700+A0− in both branches of redox-cofactors. The three-level model accounts for a flat-bottomed potential surface of the excited state and adiabatic character of electron transfer between P700 and A0, providing a microscopic explanation of the ultrafast formation of P700+A0− and exponential decline of PS I absorption.
[Display omitted]
•Femtosecond pump-to-probe laser spectroscopy of photosystem I exited at 760nm.•Direct excitation of primary donor P700 without involvement of antenna.•The primary charge separation in photosystem I proceeds faster than in 200fs.•Exponential asymptotic decline of photosystem I absorption in the red edge.•Three-state adiabatic model of electron transfer between P700 and A0.</abstract><pub>Elsevier B.V</pub><doi>10.1016/j.bbabio.2017.08.008</doi><tpages>11</tpages><oa>free_for_read</oa></addata></record> |
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| subjects | Adiabatic electron transfer Far-red light Femtosecond laser spectroscopy Photosynthesis, photosystem I, charge separation |
| title | Mechanism of adiabatic primary electron transfer in photosystem I: Femtosecond spectroscopy upon excitation of reaction center in the far-red edge of the QY band |
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