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GaV4S8 is a multiferroic semiconductor hosting magnetic cycloid (Cyc) and Néel-type skyrmion lattice (SkL) phases with a broad region of thermal and magnetic stability. Here, we use timeresolved magneto-optical Kerr spectroscopy and micro-magnetic simulations to demonstrate the coherent generation of collective spin excitations in the Cyc and SkL phases driven by an opticallyinduced modulation of uniaxial anisotropy. Our results shed light on spin-dynamics in anisotropic materials hosting skyrmions and pave a new pathway for the optical control of their magnetic order.

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We have developed a single-shot terahertz time-domain spectrometer to perform optical-pump/terahertz-probe experiments in pulsed, high magnetic fields up to 30 T. The single-shot detection scheme for measuring a terahertz waveform incorporates a reflective echelon to create time-delayed beamlets across the intensity profile of the optical gate beam before it spatially and temporally overlaps with the terahertz radiation in a ZnTe detection crystal. After imaging the gate beam onto a camera, we can retrieve the terahertz time-domain waveform by analyzing the resulting image. To demonstrate the utility of our technique, we measured cyclotron resonance absorption of optically excited carriers in the terahertz frequency range in intrinsic silicon at high magnetic fields, with results that agree well with published values.

Manipulation of excitons via coherent light-matter interaction is a promising approach for quantum state engineering and ultrafast optical modulation. Various excitation pathways in the excitonic multilevel systems provide controllability more efficient than that in the two-level system. However, these control schemes have been restricted to limited control-light wavelengths and cryogenic temperatures. Here, we report that lead halide perovskites can lift these restrictions owing to their multiband structure induced by strong spin-orbit coupling. Using CsPbBr3 perovskite nanocrystals, we observe an anomalous enhancement of the exciton energy shift at room temperature with increasing control-light wavelength from the visible to near-infrared region. The enhancement occurs because the interconduction band transitions between spin-orbit split states have large dipole moments and induce a crossover from the two-level optical Stark effect to the three-level Autler-Townes effect. Our finding establishes a basis for efficient coherent optical manipulation of excitons utilizing energy states with large spin-orbit splitting.

We investigate the exciton Mott transition (EMT) by using optical pump-terahertz probe spectroscopy on GaAs, with realizing the condition of Mott's gedanken experiment by the resonant excitation of 1s excitons. We show that an anomalous metallic phase emerges on the verge of the EMT as manifested by a peculiar enhancement of the quasiparticle mass and scattering rate. From the temperature and density dependence, the observed anomaly is shown to originate from the electron-hole (e-h) correlation which becomes prominent at low temperatures, possibly suggesting a precursor of e-h Cooper pairing.

Halide perovskite nanocrystals are suitable materials for photonic devices because their highly efficient luminescence can be tuned over a wide wavelength range by changing the nanocrystal composition and size. Here, we report on the high-order harmonic generation in a solution-processed perovskite CsPbBr 3 nanocrystal film that is excited by a strong midinfrared laser. We observe harmonics up to the 13th order, which is ultraviolet light well above the band-gap energy. By using elliptically polarized laser light, we analyze the influence of the sample structure on the intensity of the 5th harmonic. It is also found that the randomness in the orientation of the nanocrystals in the film induces a reduction in the harmonic intensities due to the interference among the harmonics emitted from nanocrystals with different phases. Our observation of high-order harmonics from nanocrystal films opens a way towards the development of an intensity modulator that can be tuned simply by changing the excitation ellipticity.

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