Enhancing the Efficiency of Polariton OLEDs in and Beyond the Single‐Excitation Subspace

Advanced Optical Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 25, 2025

Abstract Organic light‐emitting diodes (OLEDs) have redefined lighting with their environment‐friendliness and flexibility. However, only 25% of the electronic states organic molecules can emit light upon electrical excitation, limiting overall efficiency OLEDs. Strong light–matter coupling, achieved by confining within OLEDs using mirrors, creates hybrid light‐matter known as polaritons, which could “activate” remaining 75% triplet states. Here, triplet‐to‐polariton transition is studied rates for both reverse inter‐system crossing triplet‐triplet annihilation are derived. In addition, how harmful singlet‐singlet be reduced strong coupling explored.

Language: Английский

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Controlling the Manifold of Polariton States Through Molecular Disorder

Advanced Optical Materials, Journal Year: 2024, Volume and Issue: 12(11)

Published: Jan. 15, 2024

Abstract Exciton polaritons, arising from the interaction of electronic transitions with confined electromagnetic fields, have emerged as a powerful tool to manipulate properties organic materials. However, standard experimental and theoretical approaches overlook significant energetic disorder present in most materials now studied. Using conjugated polymer P3HT model platform, degree is systematically tuned corresponding redistribution photonic character within polariton manifold observed. Based on these subtle spectral features, more generalized approach developed describe strong light‐matter coupling disordered systems that captures key spectroscopic observables provides description rich states intermediate between bright dark. Applied wide range systems, method challenges prevailing notions about ultrastrong whether it can be achieved broad, absorbers.

Language: Английский

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Strong coupling-induced frequency shifts of highly detuned photonic modes in multimode cavities

The Journal of Chemical Physics, Journal Year: 2024, Volume and Issue: 160(20)

Published: May 28, 2024

Strong coupling between light and molecules is a fascinating topic exploring the implications of hybridization photonic molecular states. For example, many recent experiments have explored possibility that strong vibrational modes might modify chemical reaction rates. In these experiments, reactants are introduced into planar cavity, mode bond strongly couples to one supported by cavity. Some quantify rates tracking spectral shift higher-order cavity highly detuned from reactant. Here, we show position modes, even though they detuned, can still be influenced coupling. We highlight need consider this coupling-induced frequency if avoid underestimating cavity-induced rate changes. anticipate our work will assist in re-analysis several high-profile results has for design future experiments.

Language: Английский

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Selection Bias in Strong Coupling Experiments

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(6), P. 1708 - 1710

Published: Feb. 15, 2024

The strong coupling of light and molecules offers a potential new pathway to modify the properties photonic modes molecules. There are many reasons be optimistic about prospects coupling; however, progress in this field is currently hindered by challenges reproducibility, problems associated with differentiating between other effects, lack clear theoretical model describe reported effects. Concerning question possible mechanisms when examining experimental data, here, we show how cognitive bias can lead us place undue emphasis on given interpretation unsystematic data. We hope that Viewpoint will, where appropriate, help readers plan experiments more carefully evaluate significance data obtained from them.

Language: Английский

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Cavity Controlled Upconversion in CdSe Nanoplatelet Polaritons

ACS Nano, Journal Year: 2024, Volume and Issue: 18(32), P. 21388 - 21398

Published: July 30, 2024

Exciton-polaritons provide a versatile platform for investigating quantum electrodynamics effects in chemical systems, such as polariton-altered reactivity. However, using polaritons contexts will require better understanding of their photophysical properties under ambient conditions, where chemistry is typically performed. Here, we used cavity quality factor to control strong light–matter interactions and particular the excited state dynamics colloidal CdSe nanoplatelets (NPLs) coupled Fabry–Pérot optical cavity. With increasing factor, observe significant population upper polariton (UP) state, exemplified by rare observation substantial UP photoluminescence (PL). Excitation lower (LP) states results upconverted PL emission from branch due efficient exchange between LP, reservoir dark present collectively polaritonic systems. In addition, measure time scales ∼100 ps, implying great potential NPL based systems affect photochemical reaction rates. State-of-the-art dynamical simulations show outstanding quantitative agreement with experiments, thus important insight into nanocrystal-based These findings represent step toward development practical photochemistry platforms.

Language: Английский

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More than just smoke and mirrors: Gas-phase polaritons for optical control of chemistry

The Journal of Chemical Physics, Journal Year: 2024, Volume and Issue: 161(7)

Published: Aug. 15, 2024

Gas-phase molecules are a promising platform to elucidate the mechanisms of action and scope polaritons for optical control chemistry. Polaritons arise from strong coupling dipole-allowed molecular transition with photonic mode an cavity. There is mounting evidence modified reactivity under polaritonic conditions; however, complex condensed-phase environment most experimental demonstrations impedes mechanistic understanding this phenomenon. While gas phase was playground early efforts in atomic cavity quantum electrodynamics, we have only recently demonstrated formation these conditions. Studying isolated gas-phase would eliminate solvent interactions enable state resolution reaction progress. In Perspective, contextualize recent field polariton chemistry offer practical guide design moving forward.

Language: Английский

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Enwrapped Perylene Bisimide Enables Room Temperature Polariton Lasing and Photonic Lattices

Advanced Optical Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 8, 2025

Abstract Perylene bisimides (PBIs) are organic dyes with photoluminescence quantum yields (PLQY) close to unity in solution and great thermal photo‐chemical stability. These features alongside the tunability of their solid‐state packing arrangement via chemical functionalization make this material class an excellent candidate for exciton‐polariton lasing at room temperature. Polariton is well understood III–V semiconductors cryogenic temperatures, however, search emitter materials robust versatile room‐temperature applications ongoing. While, e.g., perovskites several identified support polariton lasing, many these lack long‐term stability under ambient conditions. Here, optical microcavities fabricated using a strongly enwrapped PBI chromophore prevailing monomer‐like absorption emission properties solid state. Voluminous bay‐substituents prevent π‐π‐stacking induced PLQY‐quenching, thereby enabling Additionally, photonic confinement single hemispheric resonators demonstrated leading localized polaritonic modes discrete energies, as lattices revealing distinct band‐structures. Due possibility tunable by precise control emitters, results pave way polarization‐dependent light‐matter coupling, including topological effects within oriented crystalline thin‐film microcavity structures.

Language: Английский

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Continuously Tuning Strong Exciton–Photon Coupling via Molecular Orientation in Organic Microcavities

Advanced Optical Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 11, 2025

Abstract Exciton‐polaritons in organic microcavities are applied devices including lasers, light‐emitting devices, and photodetectors, as well structures capable of tuning exciton kinetics energy transfer. To enable a broader tailoring polariton properties, it is important to develop means better control molecular orientation tune the intensity exciton–photon interaction. Vapor‐processed, glassy thin films previously shown have tunable evidenced by phenomena birefringence transition dipole moment (TDM) alignment. Here, this tunability TDM with film processing conditions exploited continuously vary interaction between confined cavity photon mode. By embedding 4,4′‐bis[(N‐carbazole)styryl]biphenyl (BSB‐Cz) metal‐reflector microcavity, ultrastrong coupling hybridization multiple electronic transitions BSB‐Cz demonstrated common Increasing temperature during deposition tunes from predominantly in‐plane random slightly vertical. This leads corresponding ≈30% variation associated Rabi splitting, consistent theoretical predictions. work demonstrates strength materials perspective while also providing handle disorder film.

Language: Английский

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Role of Vibrational-Assisted Scattering and Surface-Enhanced Raman Scattering in Colloidal Plexcitonic Materials

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: April 16, 2025

Strong coupling between excitons and an electromagnetic mode leads to the formation of polaritonic materials. These half-light half-matter states obey Bose-Einstein statistics have therefore promised a route toward room temperature condensates low-threshold polariton lasers. However, our understanding how enhance rate relaxation lowest energy excited state must be greatly enhanced for electrically driven organic lasers realized. Here, mechanism excited-state in colloidal plexcitonic materials (CPMs) is explored. CPMs are subgroup formed when exciton interacts strongly with plasmonic resonance nanoparticle. Based on current systems, which based experiments done using Fabry-Pérot cavities, expected high rates through vibrationally assisted scattering (VAS) mechanism. so far, it has been unclear whether we can transfer knowledge gained from cavities cavities. Our results indicate that not only VAS but also surface-enhanced Raman (SERS) active predominant depends excitation occurs. Therefore, caution exercised interpreting emission theories obtained prepared Additionally, found provide enhancement both part SERS, increasing its factor allowing tuning sensitivity specific vibrations.

Language: Английский

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Near-UV Tunable Polaritons from Magic-Size Clusters

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: April 22, 2025

Stronglight-matter coupling to form polaritons has gained significant attention for its applications in materials engineering, optoelectronics, and beyond. The combined properties of their underlying states allow numerous advantages such as delocalization over long distances, room-temperature Bose-Einstein condensation, tunability energy states. Few exciton-polariton systems, however, reach into the UV, identifying ideal that possess large oscillator strengths, exciton binding energies, ease processing, are stable device integration proven challenging. Here, we demonstrate CdS magic-size clusters (MSCs) combine all these traits. Simple solution processing metallic Fabry-Perot (FP) cavities enables MSCs exhibit strong coupling, demonstrated by square root dependence Rabi splitting on chromophore concentration. 390 meV can be achieved, with emission from polariton spanning 3.07 eV (403 nm) 3.64 (340 nm). When splittings normalized excitonic line width, this system is comparable high-performing systems visible range surpasses reported UV systems. absorption establishes a platform develop polaritonic devices across near-UV.

Language: Английский

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