Exciton dynamics can be strongly affected by lattice vibrations through electron-phonon coupling. This is rarely explored in two-dimensional magnetic semiconductors. Focusing on bilayer CrI3, we first show the presence of strong electron-phonon coupling through temperature-dependent photoluminescence and absorption spectroscopy. We then report the observation of periodic broad modes up to the 8th order in Raman spectra, attributed to the polaronic character of excitons. We establish that this polaronic character is dominated by the coupling between the charge-transfer exciton at 1.96 eV and a longitudinal optical phonon at 120.6 cm−1. We further show that the emergence of long-range magnetic order enhances the electron-phonon coupling strength by ~50% and that the transition from layered antiferromagnetic to ferromagnetic order tunes the spectral intensity of the periodic broad modes, suggesting a strong coupling among the lattice, charge and spin in two-dimensional CrI3. Our study opens opportunities for tailoring light-matter interactions in two-dimensional magnetic semiconductors.
In the superradiant phase transition (SRPT), coherent light and matter fields are expected to appear spontaneously in a coupled light–matter system in thermal equilibrium. However, such an equilibrium SRPT is forbidden in the case of charge-based light–matter coupling, known as no-go theorems. Here, we show that the low-temperature phase transition of ErFeO3at a critical temperature of approximately 4 K is an equilibrium SRPT achieved through coupling between Fe3+magnons and Er3+spins. By verifying the efficacy of our spin model using realistic parameters evaluated via terahertz magnetospectroscopy and magnetization experiments, we demonstrate that the cooperative, ultrastrong magnon–spin coupling causes the phase transition. In contrast to prior studies on laser-driven non-equilibrium SRPTs in atomic systems, the magnonic SRPT in ErFeO3occurs in thermal equilibrium in accordance with the originally envisioned SRPT, thereby yielding a unique ground state of a hybrid system in the ultrastrong coupling regime.
- Publication Date:
- NSF-PAR ID:
- 10361459
- Journal Name:
- Communications Physics
- Volume:
- 5
- Issue:
- 1
- ISSN:
- 2399-3650
- Publisher:
- Nature Publishing Group
- Sponsoring Org:
- National Science Foundation
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