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Hybrid‐State Dynamics of Dye Molecules and Surface Plasmon Polaritons under Ultrastrong Coupling Regime
Author(s) -
Wang Hai,
Wang HaiYu,
Chen QiDai,
Xu HuaiLiang,
Sun HongBo,
Huang Fangcheng,
Raja Waseem,
Toma Andrea,
Proietti Zaccaria Remo
Publication year - 2018
Publication title -
laser and photonics reviews
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 3.778
H-Index - 116
eISSN - 1863-8899
pISSN - 1863-8880
DOI - 10.1002/lpor.201700176
Subject(s) - coupling (piping) , surface plasmon polariton , surface plasmon , polariton , spectroscopy , plasmon , exciton , localized surface plasmon , molecular physics , absorption (acoustics) , conical surface , materials science , reflection (computer programming) , atomic physics , physics , condensed matter physics , optics , optoelectronics , quantum mechanics , computer science , metallurgy , composite material , programming language
The achievement of an ultrastrong coupling regime between surface plasmon modes generated by gold conical pits arrays and excitons associated to squaraine dye is demonstrated. Numerical and experimental steady‐state reflection measurements demonstrate a remarkable Rabi splitting of 860 meV, to date the largest reported value involving surface plasmon modes. Furthermore, the dynamics of the hybrid states under the ultrastrong coupling regime is investigated by transient absorption spectroscopy. The results show that the upper bands are too short‐lived to be detected, while the lower bands have a relatively shorter lifetime with respect to the bleaching recovery of pure squaraine dye. This result contradicts the behaviour of systems in strong coupling regimes, suggesting a different photophysics between strong and ultrastrong coupled systems.