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  • Coherent two-dimensional (2D) spectroscopy at 80 K was used to study chlorosomes isolated from green sulfur bacterium Chlorobaculum tepidum. Two distinct processes in the evolution of the 2D spectrum are observed. The first being exciton diffusion, seen in the change of the spectral shape occurring on a 100-fs timescale, and the second being vibrational coherences, realized through coherent beatings with frequencies of 91 and 145 cm(-1) that are dephased during the first 1.2 ps. The distribution of the oscillation amplitude in the 2D spectra is independent of the evolution of the 2D spectral shape. This implies that the diffusion energy transfer process does not transfer coherences within the chlorosome. Remarkably, the oscillatory pattern observed in the negative regions of the 2D spectrum (dominated by the excited state absorption) is a mirror image of the oscillations found in the positive part (originating from the stimulated emission and ground state bleach). This observation is surprising since it is expected that coherences in the electronic ground and excited states are generated with the same probability and the latter dephase faster in the presence of fast diffusion. Moreover, the relative amplitude of coherent beatings is rather high compared to non-oscillatory signal despite the reported low values of the Huang-Rhys factors. The origin of these effects is discussed in terms of the vibronic and Herzberg-Teller couplings. (C) 2014 AIP Publishing LLC.
  • Coherent two-dimensional (2D) spectroscopy at 80 K was used to study chlorosomes isolated from green sulfur bacterium Chlorobaculum tepidum. Two distinct processes in the evolution of the 2D spectrum are observed. The first being exciton diffusion, seen in the change of the spectral shape occurring on a 100-fs timescale, and the second being vibrational coherences, realized through coherent beatings with frequencies of 91 and 145 cm(-1) that are dephased during the first 1.2 ps. The distribution of the oscillation amplitude in the 2D spectra is independent of the evolution of the 2D spectral shape. This implies that the diffusion energy transfer process does not transfer coherences within the chlorosome. Remarkably, the oscillatory pattern observed in the negative regions of the 2D spectrum (dominated by the excited state absorption) is a mirror image of the oscillations found in the positive part (originating from the stimulated emission and ground state bleach). This observation is surprising since it is expected that coherences in the electronic ground and excited states are generated with the same probability and the latter dephase faster in the presence of fast diffusion. Moreover, the relative amplitude of coherent beatings is rather high compared to non-oscillatory signal despite the reported low values of the Huang-Rhys factors. The origin of these effects is discussed in terms of the vibronic and Herzberg-Teller couplings. (C) 2014 AIP Publishing LLC. (en)
Title
  • Unraveling the nature of coherent beatings in chlorosomes
  • Unraveling the nature of coherent beatings in chlorosomes (en)
skos:prefLabel
  • Unraveling the nature of coherent beatings in chlorosomes
  • Unraveling the nature of coherent beatings in chlorosomes (en)
skos:notation
  • RIV/60076658:12310/14:43887166!RIV15-GA0-12310___
http://linked.open...avai/riv/aktivita
http://linked.open...avai/riv/aktivity
  • P(GAP205/10/0989), P(GBP501/12/G055)
http://linked.open...iv/cisloPeriodika
  • 11
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  • 52026
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  • RIV/60076658:12310/14:43887166
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http://linked.open.../riv/klicovaSlova
  • resonance raman-spectra; excitation-energy transfer; light-harvesting complexes; bacterium chloroflexus-aurantiacus; 2-dimensional electronic spectroscopy (en)
http://linked.open.../riv/klicoveSlovo
http://linked.open...odStatuVydavatele
  • US - Spojené státy americké
http://linked.open...ontrolniKodProRIV
  • [EB9F29FE0C52]
http://linked.open...i/riv/nazevZdroje
  • Journal of Chemical Physics
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http://linked.open...ichTvurcuVysledku
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http://linked.open...vavai/riv/projekt
http://linked.open...UplatneniVysledku
http://linked.open...v/svazekPeriodika
  • 140
http://linked.open...iv/tvurceVysledku
  • Vácha, František
  • Dostal, Jakub
  • Mancal, Tomas
  • Psencik, Jakub
  • Zigmantas, Donatas
http://linked.open...ain/vavai/riv/wos
  • 000334168400044
issn
  • 0021-9606
number of pages
http://bibframe.org/vocab/doi
  • 10.1063/1.4868557
http://localhost/t...ganizacniJednotka
  • 12310
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