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Multimode Coherent Hybrid States: Ultrafast Investigation of Double Rabi Splitting between Surface Plasmons and Sulforhodamine 101 Dyes
Author(s) -
Wang Hai,
Wang HaiYu,
Wang Lei,
Chen QiDai,
Xu HuaiLiang,
Carrara Angelica,
Proietti Zaccaria Remo,
Sun HongBo,
Toma Andrea
Publication year - 2017
Publication title -
advanced optical materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.89
H-Index - 91
ISSN - 2195-1071
DOI - 10.1002/adom.201600857
Subject(s) - femtosecond , sulforhodamine b , materials science , exciton , plasmon , multi mode optical fiber , molecular physics , ultrashort pulse , femtochemistry , spectroscopy , surface plasmon , optoelectronics , laser , atomic physics , chemical physics , optics , physics , chemistry , condensed matter physics , optical fiber , biochemistry , quantum mechanics , cytotoxicity , in vitro
A multimode coherent hybrid system formed by strongly coupled surface plasmons in gold nanohole arrays and excitons in sulforhodamine 101 dyes is investigated by using both a steady‐state spectroscopic method and a femtosecond transient absorption spectra approach. A double Rabi splitting up to 255 meV and 188 meV is observed in steady‐state transmission measurements. Furthermore, the dynamics of the multimode coherent hybrid system are studied under upper band resonant excitation. It is found that the bleaching signal associated with uncoupled sulforhodamine 101 molecules completely disappears. Instead, two distinctive bleaching signals corresponding to the middle and lower bands are formed, thus highlighting the presence of coherent hybrid states. Finally, a remarkebly long lifetime for the lower band is observed, even longer than the bleaching recovery of the uncoupled dyes, in perfect agreement with the non‐Markovian regime. These peculiar features can provide new perspectives for coherent energy transfer and mode‐selective chemistry, thus enriching the tools available in the chemical reaction landscape.