Both electronic and vibrational coherences are involved in primary electron transfer in bacterial reaction center

Fei Ma; Elisabet Romero; Michael R. Jones; Vladimir I. Novoderezhkin; Rienk van Grondelle

doi:10.1038/s41467-019-08751-8

Both electronic and vibrational coherences are involved in primary electron transfer in bacterial reaction center

Fei Ma^*, Elisabet Romero, Michael R. Jones, Vladimir I. Novoderezhkin, Rienk van Grondelle

^*Corresponding author for this work

Research output: Contribution to Journal › Article › Academic › peer-review

Abstract

Understanding the mechanism behind the near-unity efficiency of primary electron transfer in reaction centers is essential for designing performance-enhanced artificial solar conversion systems to fulfill mankind’s growing demands for energy. One of the most important challenges is distinguishing electronic and vibrational coherence and establishing their respective roles during charge separation. In this work we apply two-dimensional electronic spectroscopy to three structurally-modified reaction centers from the purple bacterium Rhodobacter sphaeroides with different primary electron transfer rates. By comparing dynamics and quantum beats, we reveal that an electronic coherence with dephasing lifetime of ~190 fs connects the initial excited state, P*, and the charge-transfer intermediate PA+PB-; this P*→PA+PB- step is associated with a long-lived quasi-resonant vibrational coherence; and another vibrational coherence is associated with stabilizing the primary photoproduct, P+BA-. The results show that both electronic and vibrational coherences are involved in primary electron transfer process and they correlate with the super-high efficiency.

Original language	English
Article number	933
Pages (from-to)	1-9
Number of pages	9
Journal	Nature Communications
Volume	10
DOIs	https://doi.org/10.1038/s41467-019-08751-8
Publication status	Published - 25 Feb 2019

Funding

F.M., E.R. and R.v.G. were supported by an Advanced Investigator grant from the European Research Council (No. 267333, PHOTPROT) to R.v.G. and the TOP-grant (700.58.305) from the Foundation of Chemical Science part of NWO. R.v.G. gratefully acknowledges his Academy Professor grant from the Netherlands Royal Academy of Sciences (KNAW). M.R.J. acknowledges support from the Biotechnology and Biological Sciences Research Council of the UK (project BB/I022570/1). V.I.N. was supported by the Russian Foundation for Basic Research (Grant No. 18-04-00105).

Funders	Funder number
Foundation of Chemical Science
Netherlands Royal Academy of Sciences
Seventh Framework Programme	267333
Biotechnology and Biological Sciences Research Council	BB/I022570/1
European Research Council	700.58.305
Koninklijke Nederlandse Akademie van Wetenschappen
Russian Foundation for Basic Research	18-04-00105
Nederlandse Organisatie voor Wetenschappelijk Onderzoek

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1038/s41467-019-08751-8

https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6389996

Persistent URL (handle)

Copy link address

Cite this

@article{f83a1290267f463aac41e74f1cc5f641,

title = "Both electronic and vibrational coherences are involved in primary electron transfer in bacterial reaction center",

abstract = "Understanding the mechanism behind the near-unity efficiency of primary electron transfer in reaction centers is essential for designing performance-enhanced artificial solar conversion systems to fulfill mankind{\textquoteright}s growing demands for energy. One of the most important challenges is distinguishing electronic and vibrational coherence and establishing their respective roles during charge separation. In this work we apply two-dimensional electronic spectroscopy to three structurally-modified reaction centers from the purple bacterium Rhodobacter sphaeroides with different primary electron transfer rates. By comparing dynamics and quantum beats, we reveal that an electronic coherence with dephasing lifetime of ~190 fs connects the initial excited state, P*, and the charge-transfer intermediate PA+PB-; this P*→PA+PB- step is associated with a long-lived quasi-resonant vibrational coherence; and another vibrational coherence is associated with stabilizing the primary photoproduct, P+BA-. The results show that both electronic and vibrational coherences are involved in primary electron transfer process and they correlate with the super-high efficiency.",

author = "Fei Ma and Elisabet Romero and Jones, {Michael R.} and Novoderezhkin, {Vladimir I.} and {van Grondelle}, Rienk",

year = "2019",

month = feb,

day = "25",

doi = "10.1038/s41467-019-08751-8",

language = "English",

volume = "10",

pages = "1--9",

journal = "Nature Communications",

issn = "2041-1723",

publisher = "Nature Publishing Group",

}

TY - JOUR

T1 - Both electronic and vibrational coherences are involved in primary electron transfer in bacterial reaction center

AU - Ma, Fei

AU - Romero, Elisabet

AU - Jones, Michael R.

AU - Novoderezhkin, Vladimir I.

AU - van Grondelle, Rienk

PY - 2019/2/25

Y1 - 2019/2/25

N2 - Understanding the mechanism behind the near-unity efficiency of primary electron transfer in reaction centers is essential for designing performance-enhanced artificial solar conversion systems to fulfill mankind’s growing demands for energy. One of the most important challenges is distinguishing electronic and vibrational coherence and establishing their respective roles during charge separation. In this work we apply two-dimensional electronic spectroscopy to three structurally-modified reaction centers from the purple bacterium Rhodobacter sphaeroides with different primary electron transfer rates. By comparing dynamics and quantum beats, we reveal that an electronic coherence with dephasing lifetime of ~190 fs connects the initial excited state, P*, and the charge-transfer intermediate PA+PB-; this P*→PA+PB- step is associated with a long-lived quasi-resonant vibrational coherence; and another vibrational coherence is associated with stabilizing the primary photoproduct, P+BA-. The results show that both electronic and vibrational coherences are involved in primary electron transfer process and they correlate with the super-high efficiency.

AB - Understanding the mechanism behind the near-unity efficiency of primary electron transfer in reaction centers is essential for designing performance-enhanced artificial solar conversion systems to fulfill mankind’s growing demands for energy. One of the most important challenges is distinguishing electronic and vibrational coherence and establishing their respective roles during charge separation. In this work we apply two-dimensional electronic spectroscopy to three structurally-modified reaction centers from the purple bacterium Rhodobacter sphaeroides with different primary electron transfer rates. By comparing dynamics and quantum beats, we reveal that an electronic coherence with dephasing lifetime of ~190 fs connects the initial excited state, P*, and the charge-transfer intermediate PA+PB-; this P*→PA+PB- step is associated with a long-lived quasi-resonant vibrational coherence; and another vibrational coherence is associated with stabilizing the primary photoproduct, P+BA-. The results show that both electronic and vibrational coherences are involved in primary electron transfer process and they correlate with the super-high efficiency.

UR - http://www.scopus.com/inward/record.url?scp=85062069020&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85062069020&partnerID=8YFLogxK

U2 - 10.1038/s41467-019-08751-8

DO - 10.1038/s41467-019-08751-8

M3 - Article

C2 - 30804346

AN - SCOPUS:85062069020

SN - 2041-1723

VL - 10

SP - 1

EP - 9

JO - Nature Communications

JF - Nature Communications

M1 - 933

ER -

Both electronic and vibrational coherences are involved in primary electron transfer in bacterial reaction center

Abstract

Funding

UN SDGs

Access to Document

Persistent URL (handle)

Other files and links

Fingerprint

Cite this