The ferroelectric soft mode in a thin film was impulsively driven to a large amplitude using intense picosecond terahertz pulses. As the terahertz electric field increased, the soft-mode absorption peak exhibited blueshifting and spectral narrowing. A classical anharmonic oscillator model suggests that the induced displacement is comparable to that of the ferroelectric phase transition. The spectral narrowing indicates that the displacement exceeds that induced by any inhomogeneities in the film, demonstrating that the method can be used to explore intrinsic quartic anharmonicity.
PbTe crystals have a soft transverse optical phonon mode in the terahertz frequency range, which is known to efficiently decay into heat-carrying acoustic phonons, resulting in anomalously low thermal conductivity. Here, we studied this phonon via polarization-dependent terahertz spectroscopy. We observed softening of this mode with decreasing temperature, indicative of incipient ferroelectricity, which we explain through a model including strong anharmonicity with a quartic displacement term. In magnetic fields up to 25 T, the phonon mode splits into two modes with opposite handedness, exhibiting circular dichroism. Their frequencies display Zeeman splitting together with an overall diamagnetic shift with increasing magnetic field. Using a group-theoretical approach, we demonstrate that these observations are the result of magnetic field-induced morphic changes in the crystal symmetries through the Lorentz force exerted on the lattice ions. Thus, our Letter reveals a novel process of controlling phonon properties in a soft ionic lattice by a strong magnetic field.
Exotic quantum vacuum phenomena are predicted in cavity quantum electrodynamics systems with ultrastrong light-matter interactions. Their ground states are predicted to be vacuum squeezed states with suppressed quantum fluctuations owing to antiresonant terms in the Hamiltonian. However, such predictions have not been realized because antiresonant interactions are typically negligible compared to resonant interactions in light-matter systems. Here we report an unusual, ultrastrongly coupled matter-matter system of magnons that is analytically described by a unique Hamiltonian in which the relative importance of resonant and antiresonant interactions can be easily tuned and the latter can be made vastly dominant. We found a regime where vacuum Bloch-Siegert shifts, the hallmark of antiresonant interactions, greatly exceed analogous frequency shifts from resonant interactions. Further, we theoretically explored the system’s ground state and calculated up to 5.9 dB of quantum fluctuation suppression. These observations demonstrate that magnonic systems provide an ideal platform for exploring exotic quantum vacuum phenomena predicted in ultrastrongly coupled light-matter systems.
We have developed a femtosecond time-resolved luminescence spectroscopy by the optical Kerr-gate (OKG) method to investigate ultrafast carrier dynamics and relaxation processes of materials. Solid glasses with a high nonlinear refractive index were used as the Kerr media to obtain a subpicosecond time resolution. When a quartz plate was used as the Kerr medium, the Kerr efficiency and the instrumental response time of our spectroscopic system were 5–10 % and ∼250 fs, respectively. By employing the OKG method, we revealed the internal conversion from to state of β-carotene with a low fluorescence quantum yield and an ultrafast fluorescence decay time, and the lifetime of the state was determined to be 210 fs. An advantage of the OKG method relative to the conventional up-conversion technique is its ability to directly obtain time-resolved luminescence spectra, and thus the OKG method might be superior to the up-conversion technique to investigate ultrafast carrier dynamics and relaxation processes of materials.
Single-shot measurements of terahertz (THz) electric-field waveforms are demonstrated using a reflective echelon mirror, which produces multiple probe pulses with different time-delays. The polarization rotation of the probe pulses, due to the electro-optic effect induced by the THz electric field generated from grating-coupled , was imaged onto a two-dimensional complementary metal-oxide-semiconductor camera. A waveform with a weak peak field strength of 0.6 kV/cm was obtained with a good signal-to-noise ratio, demonstrating precise single-shot detection of the THz electric field waveform.