• journal/journal.article
• aip/jcp
• /content/aip/journal/jcp/136/22/10.1063/1.4719210
• jcp.aip.org
1887
No data available.
Please log in to see this content.
You have no subscription access to this content.
No metrics data to plot.
The attempt to load metrics for this article has failed.
The attempt to plot a graph for these metrics has failed.
Photon emission statistics and photon tracking in single-molecule spectroscopy of molecular aggregates: Dimers and trimers
USD
10.1063/1.4719210
View Affiliations Hide Affiliations
Affiliations:
1 Centre for Theoretical Physics and Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 4, 9747 AG Groningen, The Netherlands
a) Electronic mail: j.knoester@rug.nl.
J. Chem. Phys. 136, 224507 (2012)
/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

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.

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).

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.

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.

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.

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.

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.

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.

Article metrics loading...

/content/aip/journal/jcp/136/22/10.1063/1.4719210
2012-06-13
2014-04-25

Full text loading...

### Most read this month

Article
content/aip/journal/jcp
Journal
5
3

### Most cited this month

More Less
This is a required field
Please enter a valid email address
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
SEARCH_EXPAND_ITEM