Quantitative evaluation of light–matter interaction parameters in organic single-crystal microcavities

Nishimura, Takumi; Yamashita, Ken; Takahashi, Shogo; Yamao, Takeshi; Hotta, Shu; Yanagi, Hisao; Nakayama, Masaaki

doi:10.1364/ol.43.001047

Cited by 10 publications

(5 citation statements)

References 29 publications

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“…While the upper polariton branches (UPB n ) are unobservable in both the PL and transmission measurements, probably due to the ultrafast energy relaxation and the strong absorption by the continuous band at E > ∼2.7 eV, respectively, the dispersion of LPB n can be accounted for by the coupled oscillator model (see also Figure S5 in the Supporting Information). The Rabi splitting energy ℏω Rabi estimated to be ∼188 meV (see Figure 2c) is consistent with the recent results 31,33 and would be moderate for room-temperature polariton studies. 11−15 The polariton lifetimes evaluated from the spectral line widths of transmission peaks are in a range of 550−650 fs (see Figure S4 in the Supporting Information).…”

Section: ■ Results and Discussionsupporting

confidence: 91%

“…The reflection bands of the bottom and top DBRs cover the exciton energy (E ex ≈ 2.7 eV) and almost the whole emission band (see Figure S2 in the Supporting Information). In recent studies, 31,33 we have already confirmed that the BP1T-CN crystal microcavities are in the strong coupling regime that is due to the large transition dipole moment and the strong in-plane molecular polarization.…”

Section: ■ Results and Discussionmentioning

confidence: 58%

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Ultrafast Dynamics of Polariton Cooling and Renormalization in an Organic Single-Crystal Microcavity under Nonresonant Pumping

et al. 2018

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Microcavity systems with organic luminescent materials have a hot prospect for room-temperature cavity-polariton devices. The polariton dispersion relation of organic microcavities is significantly different from that of inorganic microcavities due to the strong localization of Frenkel excitons. Also photoexcited particles will undergo a different cooling mechanism until they reach the polariton ground state. In the characterization of efficient polariton condensates, therefore, the polariton cooling dynamics as well as the kinetics of the polariton eigenstate should be measured. Here we present experimental studies on ultrafast dynamics of cavity polaritons in an organic singlecrystal microcavity under nonresonant pumping. In time-resolved photoluminescence measurements we observed, for the first time, an ultrafast dynamics of stimulated cooling of the organic cavity polariton. Transient transmission measurement enabled us to investigate the detailed renormalization dynamics of the polariton eigenstate. The results clearly demonstrated the prospect of organic microcavities for room-temperature polaritonic devices.

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Section: ■ Results and Discussionsupporting

confidence: 91%

Section: ■ Results and Discussionmentioning

confidence: 58%

Ultrafast Dynamics of Polariton Cooling and Renormalization in an Organic Single-Crystal Microcavity under Nonresonant Pumping

et al. 2018

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“…The Q value is estimated to be ≈97 from the refractive index of the BP1T‐CN crystal and the reflectivity of the DBR mirror in the present half‐VCSEL. Although this Q value is larger than 2ℏω/ℏΩ (≈50) satisfying the criterion of Equation , there is much room for improving the strong coupling conditions to increase Q , for example, by introducing a full‐VCSEL structure …”

Section: Polaritonic Emission From Microcavity Structures With Tpco Cmentioning

confidence: 99%

Cooperative Behaviors in Amplified Emission from Single Microcrystals of Thiophene/Phenylene Co‐Oligomers toward Organic Polariton Laser

Yanagi

Sasaki

Yamashita

2019

Advanced Optical Materials

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After successful commercialization of organic light‐emitting diodes (OLEDs), organic semiconductor lasers have become a practical research target for versatile optoelectronic applications. Realization of electrically pumped lasing with molecular materials faces critical issues such as exciton quenching by injected carriers, nonradiative triplet states, and difficulties in introduction of resonators. One of potential routes to overcome them is to utilize polaritonic emission based on cooperative coupling of photons with excitons and/or phonons in molecular crystals. This report overviews cooperative behaviors observed in amplified emissions from single‐crystal thiophene/phenylene co‐oligomers (TPCOs) and discusses their expected potential toward organic polariton lasers. First, amplified emission accompanied with unusual time delay, spectral splitting, and fluence dependence of lasing threshold is presented, suggesting superfluorescence from macroscopically correlated molecular excitons, not based on the conventional stimulated emission process. Second, selectively enhanced Raman scattering under off‐resonant condition is shown, which is interpreted as a result of contribution of coherent vibrations in the TPCO crystals. Then, angle‐resolved spectroscopies demonstrate a stable existence of exciton polaritons at room temperature in microcavity devices with TPCO crystals. It is concluded that all those unique behaviors are ascribed to the TPCO excitons and vibrations having large oscillator strength under the uniaxially oriented molecular alignment.

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“…Moreover, strong coupling between emissive excitons and photons in vertical-cavity surface-emitting laser (VCSEL) structures with TPCOs enables us to realize an alternative scheme of polariton lasers. [22][23][24][25][26][27] To fabricate a PN junction in OLEDs, the conduction type of TPCOs can be controlled by introduction of peripheral groups. For example, electron-donating methoxy groups at both ends of the oligomer chain increase the HOMO/LUMO energies resulting in P-type conduction.…”

Section: Introductionmentioning

confidence: 99%

Organic light-emitting diodes with a PIN structure of only thiophene/phenylene co-oligomer derivatives

Dokiya

Ishigami

Akazawa

et al. 2020

Jpn. J. Appl. Phys.

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Organic light-emitting diodes with trilayer PIN structures are fabricated using only thiophene/penylene co-oligomer derivatives: 5,5′-bis(4-biphenylyl)-2,2′-bithiophene (BP2T), 5″′-bis(4-trifluoromethylphenyl)[2,2′;5′,2″;5″,2″′]quaterthiophene (P4T-CF3), and 5,5′-bis-(4′-cyanobiphenyl-4-yl)-2,2′-bithiophene (BP2T-CN) as the P, I, and N materials, respectively. As designed from their expected frontier orbital energies, electroluminescence (EL) is obtained from the P4T-CF3 layer. When the BP2T layer is first deposited on an indium-tin-oxide (ITO) substrate, the device (Al:Li/BP2T-CN/P4T-CF3/BP2T/ITO) shows homogeneous EL. On the other hand, the device with an opposite deposition order (Au/BP2T/P4T-CF3/BP2T-CN/ITO) shows dotted EL with higher efficiency at lower bias voltages. By decreasing the deposition rate of the P4T-CF3 layer in the latter device, its morphological change results in homogeneous EL with increased density of dotted emission.

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Quantitative evaluation of light–matter interaction parameters in organic single-crystal microcavities

Cited by 10 publications

References 29 publications

Ultrafast Dynamics of Polariton Cooling and Renormalization in an Organic Single-Crystal Microcavity under Nonresonant Pumping

Ultrafast Dynamics of Polariton Cooling and Renormalization in an Organic Single-Crystal Microcavity under Nonresonant Pumping

Cooperative Behaviors in Amplified Emission from Single Microcrystals of Thiophene/Phenylene Co‐Oligomers toward Organic Polariton Laser

Organic light-emitting diodes with a PIN structure of only thiophene/phenylene co-oligomer derivatives

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