Polariton‐Induced Enhanced Emission from an Organic Dye under the Strong Coupling Regime

Ballarini, Dario; Giorgi, Milena De; Gambino, Salvatore; Lerario, Giovanni; Mazzeo, Marco; Genco, Armando; Accorsi, Gianluca; Giansante, Carlo; Colella, Silvia; D’Agostino, Stefania; Cazzato, Paolo; Sanvitto, D.; Gigli, Giuseppe

doi:10.1002/adom.201400226

Cited by 54 publications

(53 citation statements)

References 48 publications

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“…Ballarini et al [28] fabricated a series of strongly coupled microcavities using a squaraine dye having a low PLQY of < 0.01%, and observed large enhancements in PLQY from the cavity (up to an order of magnitude for resonant pumping); a result in direct contrast with the small reduction in PLQY observed here. The difference between such findings can be understood on the basis of the relative magnitudes of radiative decay of uncoupled reservoir excitons and the exciton to polariton scattering rate.…”

Section: (4)contrasting

confidence: 65%

“…Here, our model indicates that direct radiative pumping of polaritons by weak-coupled excimer decay is a much more efficient process than phonon-assisted excitonpolariton scattering process, and thus the net yield of photons emitted from the cavity is largely unchanged in the strong-coupling regime. In contrast, in cavities containing materials having a low radiative rate (or reduced PLQY) [28] , the exciton to polariton scattering rate can be comparable to radiative decay and thus the additional generation of additional highly-radiative polaritons can increase the overall photon yield substantially.…”

Section: (4)mentioning

confidence: 99%

“…A series of organic materials have been explored in strong-coupled microcavities, ranging from porphyrin [4] and phthalocyanine dyes [22] , molecular dyes such as anthracene [23] , conjugated polymers [24] and oligomers [25] , to J-aggregates of cyanine dyes [26] . Recent work has demonstrated polariton lasing from microcavities containing anthracene crystals, conjugated-polymers and a conjugated oligomer [24,27,28] . Polariton electroluminescence has also been evidenced from a number of organicsemiconductor based devices [2,29] .…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Efficient Radiative Pumping of Polaritons in a Strongly Coupled Microcavity by a Fluorescent Molecular Dye

Grant

Michetti

Musser

et al. 2016

Advanced Optical Materials

105

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Abstract:We have explored the optical properties of a series of strongly-coupled microcavities containing the fluorescent molecular dye BODIPY-Br (bromine-substituted boron-dipyrromethene) dispersed into a transparent dielectric matrix with each cavity having a different exciton-photon detuning. Using temperature dependent emission, time-resolved spectroscopy, white-light reflectivity and measurements of fluorescence quantum yield, we explore the population of polaritons along the lower polariton branch. We find that both the cavity fluorescence quantum efficiency and the distribution of polariton states along the lower polariton branch is a function of exciton-photon detuning. Importantly, we show that in the most negatively detuned cavities, the emission quantum efficiency approaches that of a control (non-cavity) film. We develop a simple fitting model based upon direct radiative pumping of polariton states along the LPB and use it to obtain an excellent agreement with measured photoluminescence as a function of temperature and excitonphoton detuning, and qualitative agreement with the measured photoluminescence quantum efficiency. The radiative pumping mechanism that we identify indicates that to facilitate the formation of a non-equilibrium polariton condensate in an organic-semiconductor microcavity, it is important to utilize materials having high fluorescent quantum efficiency and fast radiative rates.A semiconductor-microcavity is an optical structure that can be used to control interactions between light and matter [1] . A typical cavity structure is composed of two mirrors separated by a layer of semiconducting material having a thickness commensurate with the wavelength of light (~100 nm). Such structures confine the local electromagnetic field, and if the energy of the confined photon and excitonic transition are degenerate, interactions can occur in the strong-coupling regime [2][3][4][5] . Here exchange of energy between excitons and photons is faster than the photon damping or exciton-photon dephasing, with the eigenstates of the system being cavity polaritons (a coherent superposition between light and matter). Polaritons are observed through an anticrossing 3 around the resonant energy of the exciton and photon modes in optical reflectivity or photoluminescence (PL) emission measurements [6] . Polaritons are bosonic quasi-particles that exhibit properties of both their excitonic and photonic components, namely the ability undergo scattering through their matter component, to form a coherent polariton condensate [7] . The ability to create and manipulate such condensates offers significant opportunities to create low threshold lasers that operate without the need for a population inversion and devices for quantumsimulations [8][9][10][11] .Most studies of strong-coupling have been performed using cavities containing inorganic-based semiconductors such as GaAs [12] , CdTe [13] , ZnO [14] and GaN [15] , either using a bulk semiconductor layer or in more sophisticated quantum well-based structures ...

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Section: (4)contrasting

confidence: 65%

Section: (4)mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Efficient Radiative Pumping of Polaritons in a Strongly Coupled Microcavity by a Fluorescent Molecular Dye

Grant

Michetti

Musser

et al. 2016

Advanced Optical Materials

105

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“…Therefore, within the homogeneous model considered in this work, emission near the lower polariton frequency can be due to direct radiative transitions (photon leakage) from polariton states at higher energies that leave the material with ν ≥ 1 vibrational quanta. Non-radiative relaxation is thus not the only mechanism that can account for the observed emission enhancements at the lower polariton frequency, under off-resonant pumping [41,71]. For large molecular ensembles in metallic cavities, we expect sub-picosecond radiative relaxation to be the dominant polariton decay channel, due to a predicted size-enhanced fluorescence rate into bound modes of the nanostructure, and the short photon lifetime of low-Q microcavities [4].…”

Section: Discussionmentioning

confidence: 95%

Absorption and photoluminescence in organic cavity QED

2017

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Organic microcavities can be engineered to reach exotic quantum regimes of strong and ultrastrong light-matter coupling. However, the microscopic interpretation of their spectroscopic signals can be challenging due to the competition between coherent and dissipative processes involving electrons, vibrations and cavity photons. We develop here a theoretical framework based on the Holstein-Tavis-Cummings model and a Markovian treatment of dissipation to account for previously unexplained spectroscopic features of organic microcavities consistently. We identify conditions for the formation of dark vibronic polaritons, a new class of light-matter excitations that are not visible in absorption but lead to strong photoluminescence lines. We show that photon leakage from dark vibronic polaritons can be responsible for enhancing photoluminescence at the lower polariton frequency, and also explain the apparent breakdown of reciprocity between absorption and emission in the vicinity of the bare molecular transition frequency. Successful comparison with experimental data demonstrates the applicability of our theory.

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“…The resonant, reversible exchange of energy between the semiconductor exciton and confined cavity-photon yields a splitting of these states into lower and upper polaritons, separated by the Rabi splitting energy (ħΩ). This phenomenon has been widely investigated in both inorganic [3][4][5][6] and organic semiconductors [7][8][9][10], the latter of which have the advantage of strongly bound excitons that are stable at room temperature. Recent advances have seen the development of organic exciton-polariton condensates and room-temperature polariton lasing [11,12], and an everexpanding field of molecules capable of undergoing strong exciton-photon coupling [13].…”

Section: Introductionmentioning

confidence: 99%

Strong coupling in a microcavity containing β-carotene

Grant¹,

Jayaprakash²,

Coles³

et al. 2018

Opt. Express

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Abstract:We have fabricated an open-cavity microcavity structure containing a thin film of the biologically-derived molecule β-carotene. We show that the β-carotene absorption can be described in terms of a series of Lorentzian functions that approximate the 0-0, 0-1, 0-2, 0-3 and 0-4 electronic and vibronic transitions. On placing this molecular material into a microcavity, we obtain anti-crossing between the cavity mode and the 0-1 vibronic transition, however other electronic and vibronic transitions remain in the intermediate or weak-coupling regime due to their lower oscillator strength and broader linewidth. We discuss the consequences of strong-coupling for the possible modification of photosynthetic processes, or a re-ordering of allowed and optically-forbidden states.

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Polariton‐Induced Enhanced Emission from an Organic Dye under the Strong Coupling Regime

Cited by 54 publications

References 48 publications

Efficient Radiative Pumping of Polaritons in a Strongly Coupled Microcavity by a Fluorescent Molecular Dye

Efficient Radiative Pumping of Polaritons in a Strongly Coupled Microcavity by a Fluorescent Molecular Dye

Absorption and photoluminescence in organic cavity QED

Strong coupling in a microcavity containing β-carotene

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