Optical frequency combs, consisting of well‐controlled equidistant frequency lines, have been widely used in precision spectroscopy and metrology. Terahertz combs have been realized in quantum cascade lasers (QCLs) by employing either an active mode‐locking or phase seeding technique, or a dispersion compensator mirror. However, it remains a challenge to achieve the passive comb formation in terahertz semiconductor lasers due to the insufficient nonlinearities of conventional saturable absorbers. Here, a passive terahertz frequency comb is demonstrated by coupling a multilayer graphene sample into a QCL compound cavity. The terahertz modes are self‐stabilized with intermode beat note linewidths down to a record of 700 Hz and the comb operation of graphene‐coupled QCLs is validated by on‐chip dual‐comb measurements. Furthermore, the optical pulse emitted from the graphene‐coupled QCL is directly measured employing a terahertz pump–probe technique. The enhanced passive frequency comb operation is attributed to the saturable absorption behavior of the graphene‐integrated saturable absorber mirror, as well as the dispersion compensation introduced by the graphene sample. The results provide a conceptually different graphene‐based approach for passive comb formation in terahertz QCLs, opening up intriguing opportunities for fast and high‐precision terahertz spectroscopy and nonlinear photonics.
Efficient forward stimulated Raman scattering (SRS) was observed along 400-nm femtosecond (fs) laser filaments in water. SRS conversion dominated over self-phase modulation induced continuum generation as the input pulse energy was above 4 μJ (∼30 Pcr), implying that plasma in the aqueous filamentation channel played an important role in compensating for the group velocity walk-off between the pump and Stokes pulses. By overlapping two synchronous fs 400-nm filaments to form plasma grating in water, significant enhancement of SRS conversion was observed. Such a SRS enhancement originated from the ultrahigh plasma density in the intersection region of the preformed plasma grating.
We present direct observation of filamentary plasma grating induced by interference between two noncollinear infrared femtosecond pulses in water by doping with gold nanoparticles. The gold nanoparticles act as scattering media in water and visualize the fine structure of local optical fields of plasma grating. By measuring the variation of local conductivity as laser undergoes filamentation in water, the generated electron density in water is qualitatively studied. Significant enhancement of local electron density is observed at the intersecting region as two laser beams form plasma grating, indicating the breakthrough of clamped intensity of a conventional filament in water.
We experimentally demonstrated that nonlinear filament interaction could spectrally modulate terahertz (THz) radiation generated from asymmetric two-color filaments. It was the spatial plasma density modulation in plasma channels that induced the THz spectral modulation. As a result of optical manipulation of electron density in the filamentary plasma gratings, the proportion of high-frequency THz spectra increased, while that of low-frequency THz spectra decreased, indicating that the increase of free electron density in the filamentary plasma grating brought about THz frequency upshifts.
Two aggregation-induced emission (AIE) macrocycles (DMP[5]-TPE and PCP[5]-TPE) were prepared by embedding Tetraphenylethene (TPE) unit into the skeletons of Dimethoxypillar[5]arene (DMP[5]) and [15]Paracyclophane ([15]PCP) at meso position, respectively. In crystal, the PCP[5]-TPE showed a distorted cavity, and the incubation of hexane inside the DMP[5]-TPE cavity caused a distinct change in the molecular conformation compared to PCP[5]-TPE. There was no complexation between PCP[5]-TPE and 1,4-dicyanobutane (DCB). UV absorption experiments showed the distorted cavity of DMP[5]-TPE hindered association with DCB.
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