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Microscopic theory of singlet exciton fission. I. General formulation
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View: Figures


Image of FIG. 1.
FIG. 1.

Population dynamics of the two-state singlet fission model described in the text with meV, V = 50 meV, ℏΩ = 150 meV (Ω−1 ≈ 4 fs), and T = 300 K (k B T ≈ 26 meV), for increasing system-bath coupling strength. Approximate results are shown for the time-local (TL) Redfield equation, the secular and Markovian (SM) Redfield equation, and for the noninteracting blip approximation (NIBA).

Image of FIG. 2.
FIG. 2.

The same as in Fig. 1 , but with λ = 25 meV and scanning the electronic coupling, V. Note the changing scale of the time axis.

Image of FIG. 3.
FIG. 3.

Population dynamics of the three-state model described in the text. While both Redfield theory and NIBA provide a reliable description of dynamics in the two-step sequential regime, NIBA is qualitatively unable to describe the superexchange regime. Redfield equation dynamics employ the secular and Markov approximations and exact results are calculated with the HEOM approach.

Image of FIG. 4.
FIG. 4.

Calculated and experimental absorption spectrum of a single pentacene molecule at T = 100 K in solution. The calculation parameters are E(S 1) = 2.3 eV, ℏΩ = 170 meV, and λ = 120 meV (S = 0.7). The bath is modeled by a single phonon frequency and a homogeneous broadening of 30 meV has been applied. Experimental spectrum is from Ref. 109 .

Image of FIG. 5.
FIG. 5.

Single molecule absorption spectra at T = 0 for a single vibrational frequency, Ω, with the Huang-Rhys parameter, S, as given. Spectra have been artificially broadened for clarity and normalized to the value of the S = 0.5 zero-phonon (0–0) line.


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Microscopic theory of singlet exciton fission. I. General formulation