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

Research output: Contribution to JournalArticleAcademicpeer-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 languageEnglish
Article number933
Pages (from-to)1-9
Number of pages9
JournalNature Communications
Volume10
DOIs
Publication statusPublished - 25 Feb 2019

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electron transfer
Electrons
electronics
Rhodobacter sphaeroides
Proteobacteria
Solar System
Spectrum Analysis
polarization (charge separation)
Excited states
bacteria
Charge transfer
unity
synchronism
charge transfer
Spectroscopy
life (durability)
spectroscopy
excitation
energy

Cite this

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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’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.",
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Both electronic and vibrational coherences are involved in primary electron transfer in bacterial reaction center. / Ma, Fei; Romero, Elisabet; Jones, Michael R.; Novoderezhkin, Vladimir I.; van Grondelle, Rienk.

In: Nature Communications, Vol. 10, 933, 25.02.2019, p. 1-9.

Research output: Contribution to JournalArticleAcademicpeer-review

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AU - Ma, Fei

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AU - van Grondelle, Rienk

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