Motoaki Bamba

The interaction of an ensemble of two-level atoms and a quantized electromagnetic field, described by the Dicke Hamiltonian, is an extensively studied problem in quantum optics. However, experimental efforts to explore similar physics in condensed matter typically employ bosonic matter modes (e.g., phonons, magnons, and plasmons) that are describable as simple harmonic oscillators, i.e., an infinite ladder of equally spaced energy levels. Here, we examine ultrastrong coupling between a coherent light mode and an ensemble of paramagnetic spins, a finite-multilevel system, in Gd₃Ga₅O₁₂. The electron paramagnetic resonance of Gd³⁺ ions is tuned by a magnetic field into resonance with a Fabry–Pérot cavity mode, resulting in the formation of spin–photon hybrid states, or Zeeman polaritons. We observe that the light–matter coupling strength, measured through the vacuum Rabi splitting, decreases with increasing temperature, which can be explained by the temperature-dependent population difference between the lower and higher-energy states, a trait of a finite-level system. This finding demonstrates that a spin–boson system is more compatible with the Dicke model and has advantages over boson–boson systems for pursuing experimental realizations of phenomena predicted for ultrastrongly coupled light–matter hybrids.

Although one-dimensional classical spin chains do not exhibit phase transitions, we found that a phase transition does occur when they are coupled to a cavity photon mode. This provides the simplest exactly solvable examples demonstrating that finite-temperature superradiant phase transitions can emerge from long-range fully connected interactions mediated by photons and interactions within the material.

The multimode ultrastrong coupling (USC) regime has emerged as a novel platform for accessing previously inaccessible phenomena in cavity quantum electrodynamics. Of particular interest are cavity‐mediated correlations between local and nonlocal excitations, or equivalently, between modes at zero and finite in‐plane momentum, which offer new opportunities for controlling light–matter interactions across space. However, direct experimental evidence of such interactions has remained elusive. Here, we demonstrate nonlocal multimode coupling in a Landau polariton system, where cavity photons simultaneously interact with the zero‐momentum cyclotron resonance and finite‐momentum magnetoplasmons of GaAs two‐dimensional electron gas. Our slot cavities, with their subwavelength mode volumes, supply in‐plane momentum components that enable the excitation of finite‐momentum matter modes. Terahertz time‐domain magnetospectroscopy measurements reveal a clear splitting of the upper‐polariton branch, arising from hybridization between magnetoplasmon modes and the cavity–cyclotron‐resonance hybrids. Extracted coupling strengths confirm USC of the cyclotron resonance and strong coupling of the magnetoplasmon modes to the cavity field, respectively. The experimental results are well captured by the multimode Hopfield model and finite‐element simulations. These findings establish a pathway for engineering multimode light–matter interactions involving zero‐ and finite‐momentum matter modes in the USC regime.

Two-level atoms ultrastrongly coupled with single-mode cavity photons are predicted to exhibit a quantum phase transition, entering a phase in which both the atomic polarization and the photonic field are finite even without external driving. However, this phenomenon, the superradiant phase transition (SRPT), is forbidden by a no-go theorem due to the existence of the diamagnetic term. Here, we present spectroscopic evidence for a magnonic SRPT in ErFeO ₃ , where the role of the photonic mode (two-level atoms) in the photonic SRPT is played by an Fe ³⁺ magnon mode (Er ³⁺ spins). The absence of the diamagnetic term in the Fe ³⁺ -Er ³⁺ exchange coupling ensures that the no-go theorem does not apply. Ultrabroadband terahertz and gigahertz magnetospectroscopy experiments revealed the signatures of the SRPT in thermal equilibrium, a kink and a softening, respectively, of two spin-magnon hybridized modes at the critical point. Systems near this phase are expected to harbor large-scale squeezing, which will potentially provide a route to next-generation quantum technologies.

The Dicke model describes the cooperative interaction of an ensemble of two-level atoms with a single-mode photonic field and exhibits a quantum phase transition as a function of light–matter coupling strength. Extending this model by incorporating short-range atom–atom interactions makes the problem intractable but is expected to produce new physical phenomena and phases. Here, we simulate such an extended Dicke model using a crystal of ErFeO₃, where the role of atoms (photons) is played by Er³⁺ spins (Fe³⁺ magnons). Through terahertz spectroscopy and magnetocaloric effect measurements as a function of temperature and magnetic field, we demonstrated the existence of a novel atomically ordered phase in addition to the superradiant and normal phases that are expected from the standard Dicke model. Further, we elucidated the nature of the phase boundaries in the temperature–magnetic-field phase diagram, identifying both first-order and second-order phase transitions. These results lay the foundation for studying multiatomic quantum optics models using well-characterized many-body solid-state systems.

The Dicke model describes the cooperative interaction of an ensemble of two-level atoms with a single-mode photonic field and exhibits a quantum phase transition as a function of light--matter coupling strength. Extending this model by incorporating short-range atom--atom interactions makes the problem intractable but is expected to produce new phases. Here, we simulate such an extended Dicke model using a crystal of ErFeO$_3$, where the role of atoms (photons) is played by Er$^{3+}$ spins (Fe$^{3+}$ magnons). Through magnetocaloric effect and terahertz magnetospectroscopy measurements, we demonstrated the existence of a novel atomically ordered phase in addition to the superradiant and normal phases that are expected from the standard Dicke model. Further, we elucidated the nature of the phase boundaries in the temperature--magnetic-field phase diagram, identifying both first-order and second-order phase transitions. These results lay the foundation for studying multiatomic quantum optics models using well-characterized many-body condensed matter systems.

Intense terahertz pulses offer unique pathway to resonantly drive the correlated spin systems up to the nonlinear regime. However, detection of such nonlinear spin dynamics often suffers from the small signal amplitude that can be easily hindered by the linear background components. In order to efficiently extract the nonlinear signals, here we demonstrate that magnetooptical effect can be utilized. We excite spin precession in orthoferrite YFeO₃ by the magnetic field of intense terahertz pulse and probe its dynamics by transient transmissivity change in the near infrared. The observed waveforms contain quasi-ferromagnetic-mode magnon oscillation and its second harmonics with a comparably strong amplitude. The result can be explained by dielectric function derived from magnetorefractive Hamiltonian. We reveal that the strong second harmonic signal microscopically originates from the dynamics of the quasi-ferromagnetic mode magnon at nonlinear regime, wherein spin canting angle periodically oscillates.

Some of the most exotic properties of the quantum vacuum are predicted in ultrastrongly coupled photon–atom systems; one such property is quantum squeezing leading to suppressed quantum fluctuations of photons and atoms. This squeezing is unique because (1) it is realized in the ground state of the system and does not require external driving, and (2) the squeezing can be perfect in the sense that quantum fluctuations of certain observables are completely suppressed. Specifically, we investigate the ground state of the Dicke model, which describes atoms collectively coupled to a single photonic mode, and we found that the photon–atom fluctuation vanishes at the onset of the superradiant phase transition in the thermodynamic limit of an infinite number of atoms. Moreover, when a finite number of atoms is considered, the variance of the fluctuation around the critical point asymptotically converges to zero, as the number of atoms is increased. In contrast to the squeezed states of flying photons obtained using standard generation protocols with external driving, the squeezing obtained in the ground state of the ultrastrongly coupled photon–atom systems is resilient against unpredictable noise.

Some of the most exotic properties of the quantum vacuum are predicted in ultrastrongly coupled photon–atom systems; one such property is quantum squeezing leading to suppressed quantum fluctuations of photons and atoms. This squeezing is unique because (1) it is realized in the ground state of the system and does not require external driving, and (2) the squeezing can be perfect in the sense that quantum fluctuations of certain observables are completely suppressed. Specifically, we investigate the ground state of the Dicke model, which describes atoms collectively coupled to a single photonic mode, and we found that the photon–atom fluctuation vanishes at the onset of the superradiant phase transition in the thermodynamic limit of an infinite number of atoms. Moreover, when a finite number of atoms is considered, the variance of the fluctuation around the critical point asymptotically converges to zero, as the number of atoms is increased. In contrast to the squeezed states of flying photons obtained using standard generation protocols with external driving, the squeezing obtained in the ground state of the ultrastrongly coupled photon–atom systems is resilient against unpredictable noise.