Ultrafast polariton relaxation dynamics in an organic semiconductor microcavity

Virgili, Tersilla; Coles, David M.; Adawi, Ali M.; Clark, Caspar; Michetti, Paolo; Rajendran, Sai Kiran; Brida, Daniele; Polli, Dario; Cerullo, Giulio; Lidzey, David G.

doi:10.1103/physrevb.83.245309

Cited by 134 publications

(183 citation statements)

References 32 publications

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“…Here, we provide direct evidence of the transfer of population between the exciton reservoir and upper and lower-branch polariton states using femtosecond pump-probe spectroscopy. We show that UP states are able to scatter to the exciton reservoir with a rate of (150 fs) -1 [2]. We show that our spectroscopy measurements are in good agreement with theoretical models of relaxation processes within strongly-coupled organic semiconductor microcavities, confirming our growing understanding of such photonic systems.…”

Section: Introductionsupporting

confidence: 70%

Ultra-fast polariton dynamics in an organic microcavity

Virgili

Coles

Adawi

et al. 2013

EPJ Web of Conferences

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Abstract:We study an organic semiconductor microcavity operating in the strongcoupling regime using femtosecond pump-probe spectroscopy. By probing the photoinduced absorption bands, we characterize the time-dependent population densities of states in the two polariton branches. We found evidence of a scattering process from the upper-branch cavity polaritons to the exciton reservoir having a rate of (150 fs)−1. A slower process similarly populates lower-branch polaritons with a rate of around (3ps)−1

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Section: Introductionsupporting

confidence: 70%

Ultra-fast polariton dynamics in an organic microcavity

Virgili

Coles

Adawi

et al. 2013

EPJ Web of Conferences

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“…For such large splittings, changes in bulk properties are observed, as already shown for the workfunction [16] and the ground state energy [17]. It has also been noticed over the years that the lifetime of the lowest polariton state, denoted C − , is much longer than the lifetime of the photon in the cavity mode [18][19][20][21][22][23][24][25]. In recent experiments using resonant excitation, this C − lifetime has even been shown to be longer than that of the bare excited molecules [26,27].…”

Section: Introductionmentioning

confidence: 86%

Non-Markovian polariton dynamics in organic strong coupling

et al. 2015

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Strongly coupled organic systems are characterized by unusually large Rabi splittings, even in the vacuum state. They show the counter-intuitive feature of a lifetime of the lower polariton state longer than for all other excited states. Here we build up a new theoretical framework to understand the dynamics of such coupled system. In particular, we show that the non-Markovian character of the relaxation of the dressed organic system explains the long lifetime of the lower polariton state.

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“…[17][18][19][20][21][22][23][24][25] However, the inhomogeneous broadening, practically always present in the assemblies of organic molecules, decreases the observed Rabi splitting if the width of the broadening is close to the coupling strength-and also gives rise to a coexistence of noncoupled MEs and the polaritons. 26 This results in a pure ME fluorescence appearing together with the luminescence of polaritons in a strongly coupled system [18][19][20] (with similar results for the cavity photon polaritons [27][28][29] ). Earlier studies of strongly coupled SPP-ME systems have reported that the luminescence of polaritons with an energy higher than the ME, the so-called upper polariton branch (UPB), is usually very weak despite the large incoupled intensity monitored via reflectance [18][19][20][21] (standard Kretschmann measurement, 30 see Fig.…”

Section: Introductionmentioning

confidence: 90%

“…27 On the contrary, the scattering from the ME to LPB was shown to be much slower than the usual time scale of the vibrational relaxation. 27 Our laser excitation result implies a similar dynamics for the SPP-ME polaritons. This would also explain the observed decrease of the UPB luminescence in previous measurements.…”

Section: Three-level Modelmentioning

confidence: 99%

Absence of mutual polariton scattering for strongly coupled surface plasmon polaritons and dye molecules with a large Stokes shift

et al. 2013

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Absence of mutual polariton scattering for strongly coupled surface plasmon polaritons and dye molecules with large Stokes shift Koponen, Mikko; Hohenester, U.; Hakala, Tommi; Toppari, Jussi Koponen, M., Hohenester, U., Hakala, T., & Toppari, J. (2013 The understanding and control of the dynamics of hybrid modes consisting of strongly coupled surface plasmon polaritons and molecular excitations of dye molecules is of great timely interest, as it allows one to tailor interactions between optical signals as needed for active all-optical devices. Here we utilize dye molecules with an especially large Stokes shift to demonstrate the absence of mutual scatterings among the strongly coupled hybrid modes. We employ a quantum mechanical three-level model and show that the hybrid modes decay via dephasing and internal relaxation of the molecules to a fluorescing state of the dye, which can be used as a measure for the decay. Our results provide essential information about the dynamics of the strongly coupled modes.

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Ultrafast polariton relaxation dynamics in an organic semiconductor microcavity

Cited by 134 publications

References 32 publications

Ultra-fast polariton dynamics in an organic microcavity

Ultra-fast polariton dynamics in an organic microcavity

Non-Markovian polariton dynamics in organic strong coupling

Absence of mutual polariton scattering for strongly coupled surface plasmon polaritons and dye molecules with a large Stokes shift

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