Primary Charge separation in the Photosystem II reaction center revealed by a global analysis of the two-dimensional electronic spectra

Hong Guang Duan, Valentyn I. Prokhorenko, Emilie Wientjes, Roberta Croce, Michael Thorwart, R. J.Dwayne Miller

Research output: Contribution to JournalArticleAcademicpeer-review

Abstract

The transfer of electronic charge in the reaction center of Photosystem II is one of the key building blocks of the conversion of sunlight energy into chemical energy within the cascade of the photosynthetic reactions. Since the charge transfer dynamics is mixed with the energy transfer dynamics, an effective tool for the direct resolution of charge separation in the reaction center is still missing. Here, we use experimental two-dimensional optical photon echo spectroscopy in combination with the theoretical calculation to resolve its signature. A global fitting analysis allows us to clearly and directly identify a decay pathway associated to the primary charge separation. In particular, it can be distinguished from regular energy transfer and occurs on a time scale of 1.5 ps under ambient conditions. This technique provides a general tool to identify charge separation signatures from the energy transport in two-dimensional optical spectroscopy.

Original languageEnglish
Article number12347
JournalScientific Reports
Volume7
Issue number1
DOIs
Publication statusPublished - 1 Dec 2017

Fingerprint

Photosystem II Protein Complex
Energy transfer
Charge transfer
Photons
Spectroscopy

Cite this

Duan, Hong Guang ; Prokhorenko, Valentyn I. ; Wientjes, Emilie ; Croce, Roberta ; Thorwart, Michael ; Miller, R. J.Dwayne. / Primary Charge separation in the Photosystem II reaction center revealed by a global analysis of the two-dimensional electronic spectra. In: Scientific Reports. 2017 ; Vol. 7, No. 1.
@article{7e116420bb764693b029eaa753c0ac24,
title = "Primary Charge separation in the Photosystem II reaction center revealed by a global analysis of the two-dimensional electronic spectra",
abstract = "The transfer of electronic charge in the reaction center of Photosystem II is one of the key building blocks of the conversion of sunlight energy into chemical energy within the cascade of the photosynthetic reactions. Since the charge transfer dynamics is mixed with the energy transfer dynamics, an effective tool for the direct resolution of charge separation in the reaction center is still missing. Here, we use experimental two-dimensional optical photon echo spectroscopy in combination with the theoretical calculation to resolve its signature. A global fitting analysis allows us to clearly and directly identify a decay pathway associated to the primary charge separation. In particular, it can be distinguished from regular energy transfer and occurs on a time scale of 1.5 ps under ambient conditions. This technique provides a general tool to identify charge separation signatures from the energy transport in two-dimensional optical spectroscopy.",
author = "Duan, {Hong Guang} and Prokhorenko, {Valentyn I.} and Emilie Wientjes and Roberta Croce and Michael Thorwart and Miller, {R. J.Dwayne}",
year = "2017",
month = "12",
day = "1",
doi = "10.1038/s41598-017-12564-4",
language = "English",
volume = "7",
journal = "Scientific Reports",
issn = "2045-2322",
publisher = "Nature Publishing Group",
number = "1",

}

Primary Charge separation in the Photosystem II reaction center revealed by a global analysis of the two-dimensional electronic spectra. / Duan, Hong Guang; Prokhorenko, Valentyn I.; Wientjes, Emilie; Croce, Roberta; Thorwart, Michael; Miller, R. J.Dwayne.

In: Scientific Reports, Vol. 7, No. 1, 12347, 01.12.2017.

Research output: Contribution to JournalArticleAcademicpeer-review

TY - JOUR

T1 - Primary Charge separation in the Photosystem II reaction center revealed by a global analysis of the two-dimensional electronic spectra

AU - Duan, Hong Guang

AU - Prokhorenko, Valentyn I.

AU - Wientjes, Emilie

AU - Croce, Roberta

AU - Thorwart, Michael

AU - Miller, R. J.Dwayne

PY - 2017/12/1

Y1 - 2017/12/1

N2 - The transfer of electronic charge in the reaction center of Photosystem II is one of the key building blocks of the conversion of sunlight energy into chemical energy within the cascade of the photosynthetic reactions. Since the charge transfer dynamics is mixed with the energy transfer dynamics, an effective tool for the direct resolution of charge separation in the reaction center is still missing. Here, we use experimental two-dimensional optical photon echo spectroscopy in combination with the theoretical calculation to resolve its signature. A global fitting analysis allows us to clearly and directly identify a decay pathway associated to the primary charge separation. In particular, it can be distinguished from regular energy transfer and occurs on a time scale of 1.5 ps under ambient conditions. This technique provides a general tool to identify charge separation signatures from the energy transport in two-dimensional optical spectroscopy.

AB - The transfer of electronic charge in the reaction center of Photosystem II is one of the key building blocks of the conversion of sunlight energy into chemical energy within the cascade of the photosynthetic reactions. Since the charge transfer dynamics is mixed with the energy transfer dynamics, an effective tool for the direct resolution of charge separation in the reaction center is still missing. Here, we use experimental two-dimensional optical photon echo spectroscopy in combination with the theoretical calculation to resolve its signature. A global fitting analysis allows us to clearly and directly identify a decay pathway associated to the primary charge separation. In particular, it can be distinguished from regular energy transfer and occurs on a time scale of 1.5 ps under ambient conditions. This technique provides a general tool to identify charge separation signatures from the energy transport in two-dimensional optical spectroscopy.

UR - http://www.scopus.com/inward/record.url?scp=85030116276&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85030116276&partnerID=8YFLogxK

U2 - 10.1038/s41598-017-12564-4

DO - 10.1038/s41598-017-12564-4

M3 - Article

VL - 7

JO - Scientific Reports

JF - Scientific Reports

SN - 2045-2322

IS - 1

M1 - 12347

ER -