Room Temperature Polariton Emission from Strongly Coupled Organic Semiconductor Microcavities

Lidzey, David G.; Bradley, Donal D. C.; Virgili, Tersilla; Armitage, A.; Skolnick, M. S.; Walker, Sara

doi:10.1103/physrevlett.82.3316

Cited by 334 publications

(293 citation statements)

References 17 publications

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“…Such a gap could occur in organic semiconductors. 6,7 In these systems, excitons are strongly bound and therefore small ͑Frenkel͒. They readily self-trap on local lattice distortions and on impurities in these, often highly disordered, materials.…”

Section: Discussionmentioning

confidence: 99%

“…2 In this example, wave-vector conservation ensures that each exciton is coupled only to a single mode of the electromagnetic field, leading to the formation of polaritons which are superpositions of a single exciton and photon. Recently, there has been a lot of interest in polaritons formed from photons confined in cavities: such cavity polaritons have now been observed for confined photons coupled to atoms, 3 to two-dimensional excitons in quantum wells, 4 to bulk excitons, 5 to excitons in films of organic semiconductors, 6,7 and to charged exciton complexes. 8 Since polaritons are photons coupled to other excitations, they are bosons, and so are candidates for Bose condensation.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Bose condensation of cavity polaritons beyond the linear regime: The thermal equilibrium of a model microcavity

Eastham¹,

Littlewood²

2001

Phys. Rev. B

154

199

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We consider a generalization of the Dicke model. This model describes localized, physically separated, saturable excitations, such as excitons bound on impurities, coupled to a single long-lived mode of an optical cavity. We consider the thermal equilibrium of this model at a fixed total number of excitons and photons. We find a phase in which both the cavity field and the excitonic polarization are coherent. This phase corresponds to a Bose condensate of cavity polaritons, generalized to allow for the fermionic internal structure of the excitons. It is separated from the normal state by an unusual reentrant phase boundary. We calculate the excitation energies of the model, and hence the optical absorption spectra of the cavity. In the condensed phase the absorption spectrum is gapped. The presence of this gap distinguishes the polariton condensate from the normal state and from a conventional laser, even when the inhomogeneous linewidth of the excitons is so large that there is no observable polariton splitting in the normal state.

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Bose condensation of cavity polaritons beyond the linear regime: The thermal equilibrium of a model microcavity

Eastham¹,

Littlewood²

2001

Phys. Rev. B

154

199

View full text Add to dashboard Cite

show abstract

“…Organic materials possess Frenkel excitons, instead of Wannier ones, with large binding energy and oscillator strength. Because of this, organic MCs allow obtaining values of the Rabi splitting up to 300 meV 5 and offer the possibility of easily observing polaritons at room temperature 6 . Electroluminescence was demonstrated in a J-aggregate strongly coupled microcavity LED 7 at room temperature.…”

Section: Introductionmentioning

confidence: 99%

Exciton-phonon scattering and photoexcitation dynamics inJ-aggregate microcavities

Michetti

Rocca

2009

Phys. Rev. B

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We have developed a model accounting for the photo-excitation dynamics and the photoluminescence of strongly coupled J-aggregate microcavities. Our model is based on a description of the J-aggregate film as a disordered Frenkel exciton system in which relaxation occurs due to the presence of a thermal bath of molecular vibrations. In a strongly coupled microcavity exciton-polaritons are formed, mixing superradiant excitons and cavity photons. The calculation of the microcavity steady-state photoluminescence, following a CW non resonant pumping, is carried out. The experimental photoluminescence intensity ratio between upper and lower polariton branches is accurately reproduced. In particular both thermal activation of the photoluminescence intensity ratio and its Rabi splitting dependence are a consequence of the bottleneck in the relaxation, occurring at the bottom of the excitonic reservoir. The effects due to radiative channels of decay of excitons and to the presence of a paritticular set of discrete optical molecular vibrations active in relaxation processes are investigared.

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“…Molecular aggregates can also be grown using self-assembly methods in different shapes including pseudo one-dimensional chains [5] two-dimensional films [6] and nanoscale tubes [7,10]. Molecular aggregates can be combined with other photonic structures such as optical cavities [3] or plasmonic nanoparticles [4]. Thus, the interest to molecular aggregates as possible lightprocessing elements grows continuously.…”

Section: Introductionmentioning

confidence: 99%

“…The prediction of optical properties is one of the main challenges for the theoretical characterization of molecular aggregates [1][2][3][4]. The complication originates in the disorder and structural variations that span over a broad length scale and include fluctuations of monomer transition frequencies, domain formation and variations in the aggregate shape on the submicron scale [5][6][7].…”

Section: Introductionmentioning

confidence: 99%

Parametric hierarchical matrix approach for the wideband optical response of large-scale molecular aggregates

Ansari-Oghol-Beig

Rostami

Chernobrovkina

et al. 2013

Journal of Applied Physics

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Fast and efficient calculations of optical responses using electromagnetic models require computational acceleration and compression techniques. A hierarchical matrix approach is adopted for this purpose. In order to model large-scale molecular structures these methods should be applied over wide frequency spectra. Here we introduce a novel parametric hierarchical matrix method that allows one for a rapid construction of a wideband system representation and enables an efficient wideband solution. We apply the developed method to the modeling of the optical response of bacteriochorophyll tubular aggregates as found in green photosynthetic bacteria. We show that the parametric method can provide one with the frequency and time-domain solutions for structures of the size of 100, 000 molecules, which is comparable to the size of the whole antenna complex in a bacterium. The absorption spectrum is calculated and the significance of electrodynamic retardation effects for relatively large structures, i.e. with respect to the wavelength of light, is briefly studied. PACS numbers: INTRODUCTIONThe prediction of optical properties is one of the main challenges for the theoretical characterization of molecular aggregates [1][2][3][4]. The complication originates in the disorder and structural variations that span over a broad length scale and include fluctuations of monomer transition frequencies, domain formation and variations in the aggregate shape on the submicron scale [5][6][7]. The periodic lattice approximation is hardly applicable in this case and one may need to model the complete structure. Quantum mechanical methods, for example, open quantum system approaches [8] or quantum mechanics/molecular mechanics methods [9], that became popular recently, can characterize aggregate-light interaction in great details. However, the application of these methods to large systems is constrained by the exponential complexity growth with respect to the number of monomers composing the structure.Aggregates of pigments molecules and fluorescent dyes possess distinct optical properties such as strong absorbance and fluorescence, coherent interaction with photons, and also fast and long-range diffusion of the absorbed energy among the molecules composing the aggregate [1]. There are a number of examples of molecular aggregates. For instance, light-absorbing complexes in plants and photosynthetic bacteria contain aggregates of pigment molecules, chlorophylls and bacteriochlorophylls respectively [2]. Those structures, constructed by nature, collect and process solar energy with high efficiency. Molecular aggregates can also be grown using self-assembly methods in different shapes including pseudo one-dimensional chains [5] two-dimensional films [6] and nanoscale tubes [7,10]. Molecular aggregates can be combined with other photonic structures such as optical cavities [3] or plasmonic nanoparticles [4]. Thus, the interest to molecular aggregates as possible lightprocessing elements grows continuously.In this context, the classical el...

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Room Temperature Polariton Emission from Strongly Coupled Organic Semiconductor Microcavities

Cited by 334 publications

References 17 publications

Bose condensation of cavity polaritons beyond the linear regime: The thermal equilibrium of a model microcavity

Bose condensation of cavity polaritons beyond the linear regime: The thermal equilibrium of a model microcavity

Exciton-phonon scattering and photoexcitation dynamics inJ-aggregate microcavities

Parametric hierarchical matrix approach for the wideband optical response of large-scale molecular aggregates

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