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Inhomogeneous dephasing masks coherence lifetimes in ensemble measurements
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10.1063/1.4704591
/content/aip/journal/jcp/136/16/10.1063/1.4704591
http://aip.metastore.ingenta.com/content/aip/journal/jcp/136/16/10.1063/1.4704591
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

Location of the seven chromophores of FMO, labeled with letters A-G. For clarity, the phytyl chains have been deleted as well as pieces of the protein that obscure the view of the chromophores. We label the chromophores with letters to avoid confusion with the excitons, which we index with numbers. For comparison to literature in which the chromophores are labeled with numbers, A corresponds to 1, B corresponds to 2, etc.

Image of FIG. 2.
FIG. 2.

Oscillations in the ρ12 element over 4 ps for calculations using the Case A density matrix. The trajectory of the ρ12 element for each of the 2500 systems is plotted in pink. The blue line shows the values of the ρ12 element of the averaged density matrix, ⟨ρ12⟩. The red line shows the values of ρ12 for a single (arbitrarily chosen) system. The red dashed line shows an exponential decay curve with a lifetime of ∼630 fs, which corresponds to the lifetime of an exponential curve fitted to the absolute value of the single trajectory shown in red (see supplementary material for details). The blue dashed line represents an exponential curve of lifetime ∼400 fs, the lifetime of a corresponding fit to ⟨ρ12⟩. Comparison of the ensemble average to the individual systems shows that dephasing occurs faster than decoherence.

Image of FIG. 3.
FIG. 3.

Oscillations in the ρ12 element over 4 ps for calculations beginning with the Case B density matrix. The trajectory of the ρ12 element for each of the 2500 systems is plotted in pink. The blue line shows the values of the ρ12 element of the averaged density matrix, ⟨ρ12⟩. The red line shows the values of ρ12 for a single (arbitrarily chosen) system. The red dashed line shows an exponential decay curve with a lifetime of ∼560 fs, which corresponds to the lifetime of an exponential curve fitted to the absolute value of the single trajectory in shown in red (see supplementary material for details). The blue dashed line represents an exponential curve of lifetime ∼310 fs, the lifetime of a corresponding fit to ⟨ρ12⟩. Comparison of the ensemble average to the individual systems shows that dephasing occurs faster than decoherence.

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/content/aip/journal/jcp/136/16/10.1063/1.4704591
2012-04-27
2014-04-20
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Inhomogeneous dephasing masks coherence lifetimes in ensemble measurements
http://aip.metastore.ingenta.com/content/aip/journal/jcp/136/16/10.1063/1.4704591
10.1063/1.4704591
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