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PreprintarXiv licencearXiv

NIR-probe transient absorption on rubrene microcavities demonstrates no changes to singlet fission by strong coupling

Abstract

Strong light-matter coupling has been proposed to control singlet-exciton fission, yet reported effects remain controversial due to the prevalence of cavity-induced optical artifacts in transient absorption measurements. Here, we investigate singlet fission in dielectric microcavities containing rubrene by probing in the near-infrared region, outside the cavity stopband, to eliminate mode-filtering artifacts. Across contrasting cavity quality factors (Q = 90 and $1150$) and a range of exciton-photon detunings (+20 to −110 meV), we find that the underlying kinetics are virtually identical to uncoupled films. Although minor spectral changes occur, transfer matrix simulations reveal these stem purely from mirror interference rather than modified photophysics. Transient electron paramagnetic resonance further confirms that high-spin triplet dynamics remain unperturbed. Together, these findings establish a widely applicable experimental framework for evaluating molecular photophysics in microcavities, revealing that singlet fission remains unaltered in strongly coupled rubrene.

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BibTeX
@misc{gordon2026nirprobe,
  title = {{NIR-probe transient absorption on rubrene microcavities demonstrates no changes to singlet fission by strong coupling}},
  author = {Robert H. Gordon and James P. Pidgeon and Rachel C. Kilbride and Tingxiang Yang and Benjamin Stewart and Yan Chen and Timothy Thornber and Peter Claronino and Graham J. Leggett and Claudia E. Tait and Marie Rider and Jenny Clark},
  howpublished = {arXiv},
  year = {2026},
  month = oct,
  doi = {10.48550/arxiv.2610.26675},
  eprint = {2610.26675},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2610.26675},
}
RIS
TY  - UNPB
TI  - NIR-probe transient absorption on rubrene microcavities demonstrates no changes to singlet fission by strong coupling
AU  - Robert H. Gordon
AU  - James P. Pidgeon
AU  - Rachel C. Kilbride
AU  - Tingxiang Yang
AU  - Benjamin Stewart
AU  - Yan Chen
AU  - Timothy Thornber
AU  - Peter Claronino
AU  - Graham J. Leggett
AU  - Claudia E. Tait
AU  - Marie Rider
AU  - Jenny Clark
PY  - 2026
DA  - 2026/10/19
PB  - arXiv
DO  - 10.48550/arxiv.2610.26675
UR  - https://arxiv.org/abs/2610.26675
AB  - Strong light-matter coupling has been proposed to control singlet-exciton fission, yet reported effects remain controversial due to the prevalence of cavity-induced optical artifacts in transient absorption measurements. Here, we investigate singlet fission in dielectric microcavities containing rubrene by probing in the near-infrared region, outside the cavity stopband, to eliminate mode-filtering artifacts. Across contrasting cavity quality factors (Q = 90 and $1150$) and a range of exciton-photon detunings (+20 to −110 meV), we find that the underlying kinetics are virtually identical to uncoupled films. Although minor spectral changes occur, transfer matrix simulations reveal these stem purely from mirror interference rather than modified photophysics. Transient electron paramagnetic resonance further confirms that high-spin triplet dynamics remain unperturbed. Together, these findings establish a widely applicable experimental framework for evaluating molecular photophysics in microcavities, revealing that singlet fission remains unaltered in strongly coupled rubrene.
ER  -