Observation of ultrastrong-coupling regime in the Fabry–Pérot microcavities made of metal mirrors containing Lemke dye

Suzuki, Makoto; Nishiyama, Koji; Kani, Nobutaka; Yu, Xinmin; Uzumi, Keiji; Funahashi, Masahiro; Shimokawa, Fusao; Nakanishi, Shunsuke; Tsurumachi, Noriaki

doi:10.1063/1.5080623

Cited by 13 publications

(25 citation statements)

References 41 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…12 Effective refractive index for TM polarization. 13 TE-polarized energy of the bare cavity mode at normal incidence. 14 TM-polarized energy of the bare cavity mode at normal incidence.…”

Section: Resultsmentioning

confidence: 99%

See 1 more Smart Citation

Enhanced and Polarization-Dependent Coupling for Photoaligned Liquid Crystalline Conjugated Polymer Microcavities

2020

View full text Add to dashboard Cite

Here we report the fabrication and optical characterization of organic microcavities containing liquid-crystalline conjugated polymers (LCCPs): poly(9,9-dioctylfluoreneco-benzothiadiazole) (F8BT), poly(9,9-dioctylfluorene) (PFO) and poly(2,7-(9,9-dihexyl fluorene)-co-bithiophene) (F6T2) aligned on top of a thin transparent Sulfuric Dye 1 (SD1) photoalignment layer. We extract the optical constants of the aligned films using variable angle spectroscopic ellipsometry and fabricate metallic microcavities in which the ultrastrong coupling regime is manifest both for the aligned and non-aligned LCCPs. Transition dipole moment alignment enables a systematic increase in the interaction strength, with unprecedented solid-state Rabi splittings of up to 1.80 eV, the first to reach energies comparable to those in the visible spectrum. With an optical gap of 2.79 eV for F6T2 this gives the highest-to-date organic microcavity coupling ratio, 65%. We also demonstrate that the coupling strength is polarization-dependent with bright polariton photoluminescence for TE polarization parallel to the polymer

show abstract

“…12 Effective refractive index for TM polarization. 13 TE-polarized energy of the bare cavity mode at normal incidence. 14 TM-polarized energy of the bare cavity mode at normal incidence.…”

Section: Resultsmentioning

confidence: 99%

“…11 1.68 ± 0.01 1.70 ± 0.01 1.70 ± 0.01 1.87 ± 0.01 1.64 ± 0.01 1.71 ± 0.01 E c TE (0)(eV)13 3.13 ± 0.02 2.92 ± 0.02 2.54 ± 0.02 2.71 ± 0.02 2.48 ± 0.02 2.78 ± 0.02 E c TM (0)(eV)14 3.15 ± 01 Exciton oscillator 1 transition energy 2. Exciton oscillator 2 transition energy 3.…”

mentioning

confidence: 99%

Enhanced and Polarization-Dependent Coupling for Photoaligned Liquid Crystalline Conjugated Polymer Microcavities

2020

View full text Add to dashboard Cite

show abstract

“…[ 5 , 6 ] Their large oscillator strength can yield extreme Rabi splittings—a measure of the interaction strength—from 100's of meV to >1 eV. [ 7 , 8 , 9 , 10 , 11 ]…”

Section: Introductionmentioning

confidence: 99%

Tuning the Coherent Propagation of Organic Exciton‐Polaritons through Dark State Delocalization

et al. 2022

View full text Add to dashboard Cite

While there have been numerous reports of long-range polariton transport at room-temperature in organic cavities, the spatiotemporal evolution of the propagation is scarcely reported, particularly in the initial coherent sub-ps regime, where photon and exciton wavefunctions are inextricably mixed. Hence the detailed process of coherent organic exciton-polariton transport and, in particular, the role of dark states has remained poorly understood. Here, femtosecond transient absorption microscopy is used to directly image coherent polariton motion in microcavities of varying quality factor. The transport is found to be well-described by a model of band-like propagation of an initially Gaussian distribution of exciton-polaritons in real space. The velocity of the polaritons reaches values of ≈ 0.65 × 10 6 m s −1 , substantially lower than expected from the polariton dispersion. Further, it is found that the velocity is proportional to the quality factor of the microcavity. This unexpected link between the quality-factor and polariton velocity is suggested to be a result of varying admixing between delocalized dark and polariton states.

show abstract

“…In this study, to understand hot‐electron injection phenomena under strong coupling conditions with extremely high splitting energies, the so‐called ultrastrong coupling condition, we focused on the oscillator strength of the LSPR. The splitting energy ħΩ, which represents the coupling strength in light‐matter coupling, is related to the oscillator strength of the resonators as: [23]

true ℏ Ω \propto \sqrt{N f}

…”

Section: Figurementioning

confidence: 99%

Water Oxidation under Modal Ultrastrong Coupling Conditions Using Gold/Silver Alloy Nanoparticles and Fabry–Pérot Nanocavities

Suganami

Oshikiri

Shi³

et al. 2021

Angew Chem Int Ed

View full text Add to dashboard Cite

We developed a photoanode consisting of Au‐Ag alloy nanoparticles (NPs), a TiO2 thin film and a Au film (AATA) under modal strong coupling conditions with a large splitting energy of 520 meV, which can be categorized into the ultrastrong coupling regime. We fabricated a photoanode under ultrastrong coupling conditions to verify the relationship between the coupling strength and photoelectric conversion efficiency and successfully performed efficient photochemical reactions. The AATA photoanode showed a 4.0 % maximum incident photon‐to‐current efficiency (IPCE), obtained at 580 nm, and the internal quantum efficiency (IQE) was 4.1 %. These results were attributed to the high hot‐electron injection efficiency due to the larger near‐field enhancement and relatively negative potential distribution of the hot electrons. Furthermore, hybrid mode‐induced water oxidation using AATA structures was performed, with a Faraday efficiency of more than 70 % for O2 evolution.

show abstract

Observation of ultrastrong-coupling regime in the Fabry–Pérot microcavities made of metal mirrors containing Lemke dye

Cited by 13 publications

References 41 publications

Enhanced and Polarization-Dependent Coupling for Photoaligned Liquid Crystalline Conjugated Polymer Microcavities

Enhanced and Polarization-Dependent Coupling for Photoaligned Liquid Crystalline Conjugated Polymer Microcavities

Tuning the Coherent Propagation of Organic Exciton‐Polaritons through Dark State Delocalization

Water Oxidation under Modal Ultrastrong Coupling Conditions Using Gold/Silver Alloy Nanoparticles and Fabry–Pérot Nanocavities

Contact Info

Product

Resources

About