Polarization anomaly in high harmonics in the crossover region between perturbative and extreme nonlinearity in GaAs

We investigate the characteristics of high harmonics (HHs) unique to the nonperturbative nonlinear regime. We show that the polarization state of HHs generated from GaAs changes drastically across the crossover from the weak-field perturbative regime to the strong-field extreme nonlinear regime, while the linearly polarized infrared excitation field (Eexc) is fixed to a particular crystal direction. The dependence on the Eexc-field strength reveals that multiple emission processes with different nonlinear orders and temporal phases contribute to each order HH, and the interference among them plays a pivotal role. This interference manifests itself as a unique phenomenon: a large HH ellipticity emerges in the course of crossover, despite the fact that GaAs hosts no magnetization or linear birefringence. These results demonstrate that not only the material's symmetry but also the ultrafast nonlinear dynamics largely affects the HH polarization, and hence, HH polarization and its Eexc-field dependence provide a useful experimental tool to probe ultrafast coherent dynamics in light-driven solid-state materials

Electron-Hole Correlation around Exciton Mott Transition Investigated by Terahertz Spectroscopy

学位の種別: 課程博士審査委員会委員 : （主査）東京大学教授 長谷川 修司, 東京大学教授 小形 正男, 東京大学教授 湯本 潤司, 東京大学教授 髙木 英典, 東京大学准教授 村川 智University of Tokyo(東京大学

Generation of wavelength-tunable few-cycle pulses in the mid-infrared at repetition rates up to 10 kHz

We demonstrate a compact and tunable mid-infrared light source that provides carrier-envelope-phase (CEP)-locked pulses at repetition rates from 500 Hz to 10 kHz. The seed pulses were generated by intra-pulse difference frequency mixing of the output of an Yb:KGW regenerative amplifier that had been spectrally broadened by continuum generation using multiple plates. Then, a two-stage optical parametric amplifier was used to obtain output energies of about 100 µJ/pulse for center wavelengths between 2.8 and 3.5 µm. Owing to the intense pulse energies, it was possible to compress the multi-cycle pulses down to two-cycle pulses using YAG and Si plates

Strong spin-orbit coupling inducing Autler-Townes effect in lead halide perovskite nanocrystals

ペロブスカイトナノ粒子において近赤外光による大きな超高速光変調を室温で実現 --光通信帯における新たな超高速光スイッチング技術の開発に期待--. 京都大学プレスリリース. 2021-05-24.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

Enhancing the Hot-Phonon Bottleneck Effect in a Metal Halide Perovskite by Terahertz Phonon Excitation

ハライドペロブスカイト半導体においてテラヘルツ励起によるホットキャリアの長寿命化を実現 --太陽電池材料のフォノン操作による高効率化への新たな指針--. 京都大学プレスリリース. 2021-02-19.We investigate the impact of phonon excitations on the photoexcited carrier dynamics in a lead-halide perovskite CH3NH3PbI3, which hosts unique low-energy phonons that can be directly excited by terahertz pulses. Our time-resolved photoluminescence measurements reveal that strong terahertz excitation prolongs the cooling time of hot carriers, providing direct evidence for the hot-phonon bottleneck effect. In contrast to the previous studies where phonons are treated as a passive heat bath, our results demonstrate that phonon excitation can significantly perturb the carrier relaxation dynamics in halide perovskites through the coupling between transverse- and longitudinal-optical phonons

Ultrastrong coupling between THz phonons and photons caused by an enhanced vacuum electric field

テラヘルツ周波数帯の真空量子揺らぎと格子振動の超強結合状態の実現 --量子光を駆動力とする新規物性制御への挑戦--. 京都大学プレスリリース. 2021-07-30.Ultrastrong coupling (USC) between phonons and vacuum photons can result in fascinating quantum phenomena, though it is difficult to achieve due to the small dipole moments of phonons in solids. Here, we investigate the vacuum Rabi splitting by coupling phonons in perovskite CH₃NH₃PbI₃ films with photons in split ring resonators. As the gap size of the resonator decreases, the coupling strength η increases due to the enhanced vacuum field in the gap, reaching the USC regime (η∼0.24) at a gap size of 100 nm. Our results show that nanoresonators are an excellent platform for studies of vacuum-dressed phonon properties

Interference effects in high-order harmonics from colloidal perovskite nanocrystals excited by an elliptically polarized laser

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 CsPbBr₃ 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

Slowdown of photoexcited spin dynamics in the non-collinear spin-ordered phases in skyrmion host GaV4S8

Formation of magnetic order alters the character of spin excitations, which then affects transport properties. We investigate the photoexcited ultrafast spin dynamics in different magnetic phases in Néel-type skyrmion host GaV(4)S(8) with time-resolved magneto-optical Kerr effect experiments. The coherent spin precession, whose amplitude is enhanced in the skyrmion-lattice phase, shows a signature of phase coexistence across the magnetic phase transitions. The incoherent spin relaxation dynamics slows down by a factor of two in the skyrmion-lattice/cycloid phases, indicating significant decrease in thermal conductivity triggered by a small change of magnetic field. The slow heat diffusion in the skyrmion-lattice/cycloid phases is attributed to the stronger magnon scattering off the domain walls formed in abundance in the skyrmion-lattice/cycloid phase. These results highlight the impact of spatial spin structure on the ultrafast heat transport in spin systems, providing a useful insight for the step toward ultrafast photocontrol of the magnets with novel spin orders

Generation of third-harmonic spin oscillation from strong spin precession induced by terahertz magnetic near fields

The ability to drive a spin system to state far from the equilibrium is indispensable for investigating spin structures of antiferromagnets and their functional nonlinearities for spintronics. While optical methods have been considered for spin excitation, terahertz (THz) pulses appear to be a more convenient means of direct spin excitation without requiring coupling between spins and orbitals or phonons. However, room-temperature responses are usually limited to small deviations from the equilibrium state because of the relatively weak THz magnetic fields in common approaches. Here, we studied the magnetization dynamics in a HoFeO3 crystal at room temperature. A custom-made spiral-shaped microstructure was used to locally generate a strong multicycle THz magnetic near field perpendicular to the crystal surface; the maximum magnetic field amplitude of about 2 T was achieved. The observed time-resolved change in the Faraday ellipticity clearly showed second- and third-order harmonics of the magnetization oscillation and an asymmetric oscillation behaviour. Not only the ferromagnetic vector M but also the antiferromagnetic vector L plays an important role in the nonlinear dynamics of spin systems far from equilibrium