Control over Energy Transfer between Fluorescent BODIPY Dyes in a Strongly Coupled Microcavity

Georgiou, Kyriacos; Michetti, Paolo; Gai, Lizhi; Cavazzini, Marco; Shen, Zhen

doi:10.1021/acsphotonics.7b01002

Cited by 85 publications

(106 citation statements)

References 29 publications

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“…We investigate the potential of dye‐filled microcavities for broadband tunable polariton lasers using BODIPY‐G1 dye molecules dispersed in a transparent polystyrene (PS) matrix as the intracavity material host. The molecular dye BODIPY‐G1 is a typical representative of the BODIPY family and combines both high extinction coefficients and high photoluminescence (PL) quantum yields . In Figure a, we draw a schematic representation of the microcavity and illustrate the excitation and detection geometry that we implement here.…”

Section: Resultsmentioning

confidence: 99%

Room Temperature Broadband Polariton Lasing from a Dye‐Filled Microcavity

Sannikov

Yagafarov

Georgiou

et al. 2019

Advanced Optical Materials

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GaAs-based microcavities. [2] However, the applications of III-V and II-VI inorganic semiconductors in polaritonics are relatively limited due to the challenging growth techniques required to create wide bandgap semiconductors together with the necessity of using cryogenic temperatures to create Wannier-Mott excitons. [3,4] Organic semiconductors however comprise the broadest class of strongly coupled materials developed to date and include molecular dyes, crystalline organic molecules, oligofluorenes, and conjugated polymers. [5][6][7][8][9][10][11] Owing to the high quantum yield, large dipole moment of optical transitions and high-binding energy of excitons, organic semiconductors have permitted the physics and applications of polaritonics to be explored at room temperature. [12,13] Polariton lasing is one of the most distinctive nonlinear phenomena related to the collective behavior of exciton polaritons. In contrast to conventional photon lasers, a polariton laser does not necessitate the electronic inversion of population, but is instead driven by a stimulated relaxation to a coherent state during the process of condensation to the ground polariton state. This process has allowed polariton lasers to exhibit significantly lower thresholds compared to photon lasers that have been fabricated using the same device configuration. [14,15] Recently, we demonstrated polariton lasing in the yellow part of the spectrum in an organic microcavity containing the molecular dye bromine-substituted boron-dipyrromethene (BODIPY-Br). [5] In the present paper, we explore the incorporation of another molecular dye of the BODIPY family, namely BODIPY-G1 fluorescent dye, into a microcavity and show that by incorporating a wedged cavity-layer configuration, we can achieve strong coupling over a broad range of exciton-photon detuning conditions. Such structures allow us to controllably access different cavity lengths and thus select the energy of the ground polariton state. We then use this approach to provide evidence of polariton lasing over a broad range of wavelengths (>30 nm) utilizing a single material system.

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Section: Resultsmentioning

confidence: 99%

Room Temperature Broadband Polariton Lasing from a Dye‐Filled Microcavity

Sannikov

Yagafarov

Georgiou

et al. 2019

Advanced Optical Materials

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“…There are several widely-used technologies that ultimately base their efficiency on the rates of chemical reactions or electron transfer processes that occur in excited electronic states (e.g., sunscreens, polymers, catalysis, solar cells, OLEDs). Therefore, the ability to manipulate the rates and branching ratios of these fundamental chemical processes in a reversible manner using light-matter interaction with a vacuum field, suggests a promising route for targeted control of excited state reactivity, without exposing fragile molecular species or materials to ESC Cavity-enhanced energy transfer and conductivity in organic media [30,[137][138][139] ESC/VSC Strong coupling with biological light-harvesting systems [44,[140][141][142] ESC Cavity-modified photoisomerization and intersystem crossing [28,104,[143][144][145] ESC Strong coupling with an individual molecule in a plasmonic nanocavity [95,96,98,146] ESC Polariton-enhanced organic light emitting devices [32,35,147,148] EUSC Ultrastrong light-matter interaction with molecular ensembles [29,36,92,147,[149][150][151] VSC/VUSC Vibrational polaritons in solid phase and liquid phase Fabry-Perot cavities [38-40, 45-47, 49-54, 152] VSC Manipulation of chemical reactivity in the ground electronic state [43,55,153] ESC Cavity-controlled intramolecular electron transfer in molecular ensembles. [134,[154][155]…”

Section: A Recent Experimental Progressmentioning

confidence: 99%

Molecular polaritons for controlling chemistry with quantum optics

Herrera

Owrutsky

2020

The Journal of Chemical Physics

260

248

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This is a tutorial-style introduction to the field of molecular polaritons. We describe the basic physical principles and consequences of strong light-matter coupling common to molecular ensembles embedded in UV-visible or infrared cavities. Using a microscopic quantum electrodynamics formulation, we discuss the competition between the collective cooperative dipolar response of a molecular ensemble and local dynamical processes that molecules typically undergo, including chemical reactions. We highlight some of the observable consequences of this competition between local and collective effects in linear transmission spectroscopy, including the formal equivalence between quantum mechanical theory and the classical transfer matrix method, under specific conditions of molecular density and indistinguishability. We also overview recent experimental and theoretical developments on strong and ultrastrong coupling with electronic and vibrational transitions, with a special focus on cavity-modified chemistry and infrared spectroscopy under vibrational strong coupling. We finally suggest several opportunities for further studies that may lead to novel applications in chemical and electromagnetic sensing, energy conversion, optoelectronics, quantum control and quantum technology.

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“…To demonstrate the relevance of this new method, we investigate the energy transfer inside a resonant cavity formed by two planar mirrors separated by a half wavelength. Similar photonic cavities have received a large interest owing to their potential to confine light and to enhance light-matter interactions in either the weak [20,[34][35][36]53,54] or strong coupling regime [13][14][15][16][17][18][19]. Here, we directly map the positions and conditions leading to an enhancement of the dipole-dipole energy transfer inside the cavity.…”

Section: Introductionmentioning

confidence: 99%

Direct Imaging of the Energy-Transfer Enhancement between Two Dipoles in a Photonic Cavity

et al. 2019

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Photonic cavities are gathering a large interest to enhance the energy transfer between two dipoles, with far-reaching consequences for applications in photovoltaics, lighting sources and molecular biosensing. However, experimental difficulties in controlling the dipoles' positions, orientations and spectra have limited the earlier work in the visible part of the spectrum, and have led to inconsistent results. Here, we directly map the energy transfer of microwaves between two dipoles inside a resonant half-wavelength cavity with ultrahigh control in space and frequency. Our approach extends Förster resonance energy transfer (FRET) theory to microwave frequencies, and bridges the gap between the descriptions of FRET using quantum electrodynamics and microwave engineering. Beyond the conceptual interest, we show how this approach can be used to optimize the design of photonic cavities to enhance dipole-dipole interactions and FRET. I.

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Control over Energy Transfer between Fluorescent BODIPY Dyes in a Strongly Coupled Microcavity

Cited by 85 publications

References 29 publications

Room Temperature Broadband Polariton Lasing from a Dye‐Filled Microcavity

Room Temperature Broadband Polariton Lasing from a Dye‐Filled Microcavity

Molecular polaritons for controlling chemistry with quantum optics

Direct Imaging of the Energy-Transfer Enhancement between Two Dipoles in a Photonic Cavity

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