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Title: Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer

Authors:
; ; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1372716
Grant/Contract Number:
SC0001035
Resource Type:
Journal Article: Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 114; Journal Issue: 32; Related Information: CHORUS Timestamp: 2017-08-08 12:47:46; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English

Citation Formats

Duan, Hong-Guang, Prokhorenko, Valentyn I., Cogdell, Richard J., Ashraf, Khuram, Stevens, Amy L., Thorwart, Michael, and Miller, R. J. Dwayne. Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer. United States: N. p., 2017. Web. doi:10.1073/pnas.1702261114.
Duan, Hong-Guang, Prokhorenko, Valentyn I., Cogdell, Richard J., Ashraf, Khuram, Stevens, Amy L., Thorwart, Michael, & Miller, R. J. Dwayne. Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer. United States. doi:10.1073/pnas.1702261114.
Duan, Hong-Guang, Prokhorenko, Valentyn I., Cogdell, Richard J., Ashraf, Khuram, Stevens, Amy L., Thorwart, Michael, and Miller, R. J. Dwayne. 2017. "Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer". United States. doi:10.1073/pnas.1702261114.
@article{osti_1372716,
title = {Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer},
author = {Duan, Hong-Guang and Prokhorenko, Valentyn I. and Cogdell, Richard J. and Ashraf, Khuram and Stevens, Amy L. and Thorwart, Michael and Miller, R. J. Dwayne},
abstractNote = {},
doi = {10.1073/pnas.1702261114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 32,
volume = 114,
place = {United States},
year = 2017,
month = 7
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1073/pnas.1702261114

Citation Metrics:
Cited by: 2works
Citation information provided by
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  • We demonstrate that the coupling of excitonic and vibrational motion in biological complexes can provide mechanisms to explain the long-lived oscillations that have been obtained in nonlinear spectroscopic signals of different photosynthetic pigment protein complexes and we discuss the contributions of excitonic versus purely vibrational components to these oscillatory features. Considering a dimer model coupled to a structured spectral density we exemplify the fundamental aspects of the electron-phonon dynamics, and by analyzing separately the different contributions to the nonlinear signal, we show that for realistic parameter regimes purely electronic coherence is of the same order as purely vibrational coherence inmore » the electronic ground state. Moreover, we demonstrate how the latter relies upon the excitonic interaction to manifest. These results link recently proposed microscopic, non-equilibrium mechanisms to support long lived coherence at ambient temperatures with actual experimental observations of oscillatory behaviour using 2D photon echo techniques to corroborate the fundamental importance of the interplay of electronic and vibrational degrees of freedom in the dynamics of light harvesting aggregates.« less
  • Recently, nuclear vibrational contribution signatures in two-dimensional (2D) electronic spectroscopy have attracted considerable interest, in particular as regards interpretation of the oscillatory transients observed in light-harvesting complexes. These transients have dephasing times that persist for much longer than theoretically predicted electronic coherence lifetime. As a plausible explanation for this long-lived spectral beating in 2D electronic spectra, quantum-mechanically mixed electronic and vibrational states (vibronic excitons) were proposed by Christensson et al. [J. Phys. Chem. B 116, 7449 (2012)] and have since been explored. Here in this work, we address a dimer which produces little beating of electronic origin in the absencemore » of vibronic contributions, and examine the impact of protein-induced fluctuations upon electronic-vibrational quantum mixtures by calculating the electronic energy transfer dynamics and 2D electronic spectra in a numerically accurate manner. It is found that, at cryogenic temperatures, the electronic-vibrational quantum mixtures are rather robust, even under the influence of the fluctuations and despite the small Huang-Rhys factors of the Franck-Condon active vibrational modes. This results in long-lasting beating behavior of vibrational origin in the 2D electronic spectra. At physiological temperatures, however, the fluctuations eradicate the mixing, and hence, the beating in the 2D spectra disappears. Further, it is demonstrated that such electronic-vibrational quantum mixtures do not necessarily play a significant role in electronic energy transfer dynamics, despite contributing to the enhancement of long-lived quantum beating in 2D electronic spectra, contrary to speculations in recent publications.« less
  • Recently, nuclear vibrational contribution signatures in two-dimensional (2D) electronic spectroscopy have attracted considerable interest, in particular as regards interpretation of the oscillatory transients observed in light-harvesting complexes. These transients have dephasing times that persist for much longer than theoretically predicted electronic coherence lifetime. As a plausible explanation for this long-lived spectral beating in 2D electronic spectra, quantum-mechanically mixed electronic and vibrational states (vibronic excitons) were proposed by Christensson et al. [J. Phys. Chem. B 116, 7449 (2012)] and have since been explored. In this work, we address a dimer which produces little beating of electronic origin in the absence ofmore » vibronic contributions, and examine the impact of protein-induced fluctuations upon electronic-vibrational quantum mixtures by calculating the electronic energy transfer dynamics and 2D electronic spectra in a numerically accurate manner. It is found that, at cryogenic temperatures, the electronic-vibrational quantum mixtures are rather robust, even under the influence of the fluctuations and despite the small Huang-Rhys factors of the Franck-Condon active vibrational modes. This results in long-lasting beating behavior of vibrational origin in the 2D electronic spectra. At physiological temperatures, however, the fluctuations eradicate the mixing, and hence, the beating in the 2D spectra disappears. Further, it is demonstrated that such electronic-vibrational quantum mixtures do not necessarily play a significant role in electronic energy transfer dynamics, despite contributing to the enhancement of long-lived quantum beating in 2D electronic spectra, contrary to speculations in recent publications.« less
  • Cited by 6
  • We investigated the spin coherence of high-mobility two-dimensional electron gases confined in multilayer GaAs quantum wells. The dynamics of the spin polarization was optically studied using pump-probe techniques: time-resolved Kerr rotation and resonant spin amplification. For double and triple quantum wells doped beyond the metal-to-insulator transition, the spin-orbit interaction was tailored by the sample parameters of structural symmetry (Rashba constant), width, and electron density (Dresselhaus linear and cubic constants) which allow us to attain long dephasing times in the nanoseconds range. The determination of the scales, namely, transport scattering time, single-electron scattering time, electron-electron scattering time, and spin polarization decaymore » time further supports the possibility of using n-doped multilayer systems for developing spintronic devices.« less