We experimentally disentangle the contributions of different quantum paths in high-order harmonic generation (HHG) from the spectrally and spatially resolved harmonic spectra. By adjusting the laser intensity and focusing position, we simultaneously observe the spectrum splitting, frequency shift and intensity-dependent modulation of harmonic yields both for the short and long paths. Based on the simulations, we discriminate the physical mechanisms of the intensity-dependent modulation of HHG due to the quantum path interference and macroscopic interference effects. Moreover, it is shown that the atomic dipole phases of different quantum paths are encoded in the frequency shift. In turn, it enables us to retrieve the atomic dipole phases and the temporal chirps of different quantum paths from the measured harmonic spectra. This result gives an informative mapping of spatiotemporal and spectral features of quantum paths in HHG.

Nitrogen/sulfur co-doped anatase TiO2 nanocrystals with a high specific surface area and a high percentage of {001} facets were synthesized by a solvent-thermal process followed by the calcination with thiourea at an optimum heat treatment temperature. Under current experimental conditions, the optimum heat treatment temperature was found at 300°C, which successfully introduced nitrogen and sulfur dopants into the anatase lattice to replace a small portion of oxygen atoms while preserving the geometry of these anatase TiO2 nanocrystals to maintain a high percentage of {001} facets. These nitrogen/sulfur co-doped anatase TiO2 nanocrystals demonstrated a largely enhanced light absorption in the whole visible-light range and exhibited much higher photocatalytic performance than both P25 TiO2 nanoparticles and anatase TiO2 nanocrystals with a high percentage of {001} facets under visible-light illumination.

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Molecules constituted by different isotopes are different in vibrational modes, making it possible to elucidate the mechanism of a chemical reaction via the kinetic isotope effect. However, the real-time observation of the vibrational motion of isotopic nuclei in molecules is still challenging due to its ultrashort time scale. Here we demonstrate a method to monitor the nuclear vibration of isotopic molecules with the frequency modulation of high-order harmonic generation (HHG) during the laser-molecule interaction. In the proof-of-principle experiment, we report a red shift in HHG from H2 and D2. The red shift is ascribed to dominant HHG from the stretched isotopic molecules at the trailing edge of the laser pulse. By utilizing the observed frequency shift, the laser-driven nuclear vibrations of H2 and D2 are retrieved. These findings pave an accessible route toward monitoring the ultrafast nuclear dynamics and even tracing a chemical reaction in real time.