Superradiance of 2D Frenkel exciton-polaritons: mixing of molecular configurations and resonance interaction with the substrate

Agranovich, V.M.; Dubovsky, O. A.; Grigorishin, K.I.; Leskova, T. A.; Neidlinger, Th.; Reineker, P.

doi:10.1016/0301-0104(96)88026-8

Cited by 6 publications

(6 citation statements)

References 11 publications

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“…Finally, the low coverage of anthracene, with islands on the order of the wavelength of light or smaller, prevents the formation of polaritons in these samples, which would complicate the interpretation of the optical spectra. [53][54][55] While the absorption lineshape is largely temperature independent, the steady state fluorescence spectrum changes significantly as the temperature is lowered. Previous work has shown how the temperature dependence of the fluorescence can provide valuable information about the Frenkel exciton delocalization in organic solids.…”

Section: Resultsmentioning

confidence: 99%

Experimental and theoretical study of temperature dependent exciton delocalization and relaxation in anthracene thin films

Ahn

Müller

Al‐Kaysi

et al. 2008

The Journal of Chemical Physics

101

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The spectroscopy of solid anthracene is examined both experimentally and theoretically. To avoid experimental complications such as self-absorption and polariton effects, ultrathin polycrystalline films deposited on transparent substrates are studied. To separate the contributions from different emitting species, the emission is resolved in both time and wavelength. The spectroscopic data are interpreted in terms of a three-state kinetic model, where two excited states, a high energy state 1 and a low energy state 2, both contribute to the luminescence and are kinetically coupled. Using this model, we analyze the spectral lineshape, relative quantum yield, and relaxation rates as a function of temperature. For state 1, we find that the ratio of the 0-0 vibronic peak to the 0-1 peak is enhanced by roughly a factor of 3.5 at low temperature, while the quantum yield and decay rates also increase by a similar factor. These observations are explained using a theoretical model previously developed for herringbone polyacene crystals. The early-time emission lineshape is consistent with that expected for a linear aggregate corresponding to an edge-dislocation defect. The results of experiment and theory are quantitatively compared at different temperatures in order to estimate that the singlet exciton in our polycrystalline films is delocalized over about ten molecules. Within these domains, the exciton's coherence length steadily increases as the temperature drops, until it reaches the limits of the domain, whereupon it saturates and remains constant as the temperature is lowered further. While the theoretical modeling correctly reproduces the temperature dependence of the fluorescence spectral lineshape, the decay of the singlet exciton appears to be determined by a trapping process that becomes more rapid as the temperature is lowered. This more rapid decay is consistent with accelerated trapping due to increased delocalization of the exciton at lower temperatures. These observations suggest that exciton coherence can play an important role in both radiative and nonradiative decay channels in these materials. Our results show that the spectroscopy of polyacene solids can be analyzed in a self-consistent fashion to obtain information about electronic delocalization and domain sizes.

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Section: Resultsmentioning

confidence: 99%

Experimental and theoretical study of temperature dependent exciton delocalization and relaxation in anthracene thin films

Ahn

Müller

Al‐Kaysi

et al. 2008

The Journal of Chemical Physics

101

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“…Because the interlayer interaction holds for all the layers together in the slab, it does not seem a good approximation to fully neglect it as was done in Ref. [10]. Nevertheless, as a well-known fact [15,6], R n,n' falls off very quickly against |n -n' ^ so that one can limit oneself to the interaction within a few numbers of nearest layers only.…”

Section: Size Dependence Versus Surface-to-buik Ratiosmentioning

confidence: 99%

“…Theoretical investigations of unique properties of future composite organic-inorganic quantum structures, where the Wannier-Mott and the Frenkel excitons hybridize, have just been started [7][8][9]. ' One type of the available heterostructure-based molecular systems is multilayer molecular slabs which have currently attracted a lot of interest [10][11][12]. Reference [10] evaluated the superradiance rate neglecting interaction between the layers.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

On Number of Exciton Surface States in Multilayer Molecular Slabs

1997

Acta Phys. Pol. A

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Criteria for the possible number of exciton surface states in a multilayer molecular slab are elucidated in detail. Namely, we explicitly determine the domains of system parameters where the size dependence plays a role. We further clarify the way a surface state is localized in the slab in both asymmetric and symmetric configurations. Basing on our results which are obtained within the first nearest layer approximation, we also conjecture properties to be expected when further nearest layers are taken into consideration.

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“…In this paper we are concerned with the electronic structure of a multilayer OQW. The super-radiance property of OQWs has been investigated recently in [9]; however, the interaction between crystalline layers was neglected in the investigation. Super-radiant decay can be described in terms of the imaginary part of the second-order self-energy due to exciton-photon interaction, while its real part gives the dipole-dipole interaction.…”

Section: Introductionmentioning

confidence: 99%

Size-dependent electronic eigenstates of multilayer organic quantum wells

An¹,

Hanamura²

1996

J. Phys.: Condens. Matter

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A detailed theoretical treatment is given of eigenfunctions and eigenenergies of a multilayer organic quantum well sandwiched between two different dielectric media. The abrupt change of dielectric constants at the interfaces distorts the wave function and results in there being possible surface states in addition to propagating states. The proper boundary conditions are accounted for by the method of image charges. Analytic criteria for the existence of surface states are established using the nearest-layer approximation; they depend not only on the intralayer and interlayer parameters but also on the number of layers. The size dependence together with the dependence on signs and relative magnitudes of the structure parameters fully determine the energy spectrum of propagating states as well as the number and the location of surface states.

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Superradiance of 2D Frenkel exciton-polaritons: mixing of molecular configurations and resonance interaction with the substrate

Cited by 6 publications

References 11 publications

Experimental and theoretical study of temperature dependent exciton delocalization and relaxation in anthracene thin films

Experimental and theoretical study of temperature dependent exciton delocalization and relaxation in anthracene thin films

On Number of Exciton Surface States in Multilayer Molecular Slabs

Size-dependent electronic eigenstates of multilayer organic quantum wells

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