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Photon emission statistics and photon tracking in single-molecule spectroscopy of molecular aggregates: Dimers and trimers
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10.1063/1.4719210
/content/aip/journal/jcp/136/22/10.1063/1.4719210
http://aip.metastore.ingenta.com/content/aip/journal/jcp/136/22/10.1063/1.4719210
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

Level diagram of the dimer. In the special case of a homogeneous dimer, the dotted anti-symmetric state |−⟩ is optically dark and the dimer can be regarded as an effective three-level system.

Image of FIG. 2.
FIG. 2.

(a) I L ) and (b) Q L ) versus (ω L − ω0)/J in the small Rabi frequency limit for the homogeneous dimer. Chosen parameters are ω0 = 10J, Γ0 = 2 × 10−2 J, Ω0 = −1 × 10−3 J. Calculated parameters based on Eqs. (A3) and (A4) are Γ g + = 5.3 × 10−2 J, Γ+e = 2.9 × 10−2 J, Ω+ = −1.4 × 10−3 J. (Inset) Our numerical results for the super-Poissonian peak (solid line) compared to the results derived from Eq. (20).

Image of FIG. 3.
FIG. 3.

(a) I L ) and (b) Q L ) for the homogeneous dimer as a function of (ω L − ω0)/J for intermediate Rabi frequencies, Ω0 = −4 × 10−2 J, −8 × 10−2 J, and −1.2 × 10−1 J. Parameters are the same as those of Fig. 2, leading to Ω+ = −5.7 × 10−2 J, −1.1 × 10−1 J, and −1.7 × 10−1 J, respectively. (Inset) Transition from super- to sub-Poissonian behavior in more detail.

Image of FIG. 4.
FIG. 4.

Plots of I L ) and Q L ) versus (ω L − ω0)/J for the dimer in both limits of inhomogeneity. Panels (a) and (c) present the data for small inhomogeneity, with parameter choices ω1 = 10J, ω2 = 10.2J (i.e., σ = 0.1J), Γ0 = 2 × 10−2 J, and Ω0 = −2 × 10−3 J. From this it follows that Γ g + = 5.3 × 10−2 J, Γ+e = 2.9 × 10−2 J, Γ g = 7.2 × 10−5 J, Γe = 1.3 × 10−4 J, Ω g + = Ω+e = −2.8 × 10−3 J, and Ω g = Ωe = −1.4 × 10−4 J. Panels (b) and (d) present data for large inhomogeneity, with parameter choices ω1 = 10J, ω2 = 30J (i.e., σ = 10J), Γ0 = 2 × 10−2 J, and Ω0 = −2 × 10−3 J. From this we have Γ g + = 7.5 × 10−2 J, Γ+e = 2.7 × 10−3 J, Γ g = 2.2 × 10−3 J, Γe = 6.1 × 10−2 J, Ω g + = Ω+e = −2.1 × 10−3 J, and Ω g = Ωe = −1.9 × 10−3 J. Inset (a): details of the |g⟩ → |−⟩ transition line shape. Inset (d): observation of the small super-Poissonian peak for ω L ≈ ω0.

Image of FIG. 5.
FIG. 5.

Maximum value of the observed super-Poissonian peak Q max as a function of the disorder parameter σ. Numerical results (squares) are compared with those obtained from Eq. (22) (solid line). Chosen parameters are ω1 = 10J, Γ0 = 2 × 10−2 J, Ω0 = −1 × 10−3 J. (Inset) Same as the main plot, but now the energy dependence of the spontaneous decay rates Γ ij is neglected.

Image of FIG. 6.
FIG. 6.

Level diagram of the linear homogeneous trimer with all molecules having equal transition dipole vectors. The arrows correspond to the optically allowed transitions.

Image of FIG. 7.
FIG. 7.

(a) I L ) and (b) Q L ) versus (ω L − ω0)/J for the homogeneous trimer in the limit of small Rabi frequency. Chosen parameters are ω0 = 10J, Γ0 = 2 × 10−2 J, and Ω0 = −1 × 10−3 J.

Image of FIG. 8.
FIG. 8.

(a) I L ) and (b) Q L ) for the trimer plotted against (ω L − ω0)/J for Ω0 = −0.05J and −0.1J. Chosen parameters are the same as those of Fig. 7. The range for ω L is chosen to reflect the characteristics of multi-exciton influences in more detail. (Inset) Detailed behavior of the frequency regime near , which is the transition frequency between the ground state and the |1; 1⟩ one-exciton state.

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/content/aip/journal/jcp/136/22/10.1063/1.4719210
2012-06-13
2014-04-25
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Photon emission statistics and photon tracking in single-molecule spectroscopy of molecular aggregates: Dimers and trimers
http://aip.metastore.ingenta.com/content/aip/journal/jcp/136/22/10.1063/1.4719210
10.1063/1.4719210
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