It remains unclear how the collective strong coupling of cavity-confined photons to the electronic transitions of molecular chromophore leverages the distinct properties of the polaritonic constituents for future technologies. In this study, we design, fabricate, and characterize multiple types of Fabry-Pérot (FP) mirco-resonators containing copper(II) tetraphenyl porphyrin (CuTPP) to show how cavity polariton formation affects radiative relaxation processes in the presence of substantial non-Condon vibronic coupling between two of this molecule’s excited electronic states. Unlike the prototypical enhancement of Q state radiative relaxation of CuTPP in a FP resonator incapable of forming polaritons, we find the light emission processes in multimode cavity polariton samples become enhanced for cavity-exciton energy differences near those of vibrations known to mediate non-Condon vibronic coupling. We propose the value of this detuning is consistent with radiative relaxation of Herzberg-Teller polaritons into collective molecular states coupled to the cavity photon coherently. We contrast the feature stemming from light emission from the HT polariton state with those that occur due to polariton-enhanced light absorption. Our results demonstrate the landscape of molecular and photonic interactions enabled by cavity polariton formation using complex chromophores and how researchers can design resonators to leverage these interactions to characterize and control polaritonic properties.
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This content will become publicly available on December 20, 2024
Terahertz Cavity Magnon Polaritons
Hybrid light–matter coupled states, or polaritons, in magnetic materials have attracted significant attention due to their potential for enabling novel applications in spintronics and quantum information processing. However, most magnon‐polariton studies in the strong coupling regime to date have been carried out for ferromagnetic materials with magnon excitations at gigahertz frequencies. Here, strong resonant photon–magnon coupling at frequencies above 1 terahertz is investigated for the first time in a prototypical room‐temperature antiferromagnetic insulator, NiO, inside a Fabry–Pérot cavity. The cavity is formed by the crystal itself with a thickness adjusted to an optimal value. Terahertz time‐domain spectroscopy measurements in magnetic fields up to 25 T reveal the evolution of the magnon frequency through Fabry–Pérot cavity modes with photon–magnon anticrossing behavior, demonstrating clear vacuum Rabi splittings exceeding the polariton linewidths. These results show that NiO is a promising platform for exploring antiferromagnetic spintronics and cavity magnonics in the terahertz frequency range.
more » « less- Award ID(s):
- 1810541
- PAR ID:
- 10481095
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Optical Materials
- ISSN:
- 2195-1071
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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