Among currently available optical spectroscopic methods, Raman spectroscopy has versatile application to investigation of dynamical processes of molecules leading to chemical changes in the gas and liquid phases. However, it is still a challenge to realize an ideal standoff coherent Raman spectrometer with which both high temporal resolution and high-frequency resolution can be achieved, so that one can remotely probe chemical species in real time with high temporal resolution while monitoring the populations in their respective rovibronic levels in the frequency domain with sufficiently high spectral resolution. In the present study, we construct an air-laser-based Raman spectrometer, in which near-infrared femtosecond (fs) laser pulses at 800 nm and cavity-free picosecond N2+ air-laser pulses at 391 nm generated by the filamentation induced by the fs laser pulses are simultaneously used, enabling us to generate a hybrid ps/fs laser source at a desired standoff position for standoff surveillance of chemical and biochemical species. With this prototype Raman spectrometer, we demonstrate that the temporal evolution of the electronic, vibrational, and rotational states of N2+ and the coupling processes of the rovibrational wave packet of N2 molecules can be probed.

Chirp-free solitons have been mainly achieved with anomalous-dispersion fiber lasers by the balance of dispersive and nonlinear effects, and the single-pulse energy is constrained within a relatively small range. Here, we report a class of chirp-free pulse in normal-dispersion erbium-doped fiber lasers, termed birefringence-managed soliton, in which the birefringence-related phase-matching effect dominates the soliton evolution. Controllable harmonic mode locking from 5 order to 85 order is obtained at the same pump level of ~10 mW with soliton energy fully tunable beyond ten times, which indicates a new birefringence-related soliton energy law, which fundamentally differs from the conventional soliton energy theorem. The unique transformation behavior between birefringence-managed solitons and dissipative solitons is directly visualized via the single-shot spectroscopy. The results demonstrate a novel approach of engineering fiber birefringence to create energy-tunable chirp-free solitons in normal-dispersion regime and open new research directions in fields of optical solitons, ultrafast lasers, and their applications.

We proposed a simple method based on the seeded free-electron laser (FEL) to generate fully coherent X-ray pulses with durations at dozens of attosecond level. The echo-enabled harmonic generation technique is utilized to generate the fully coherent laser pulse covering the water-window range. A wavefront rotation laser is adopted as the seed to tailor the longitudinal contour of the radiation pulse. Due to the sensitivity of seeded FEL to external lasers, this method can effectively inhibit the bunching of the adjacent regions while preserving an isolated bunching in the middle. Sending such an electron beam into a short undulator, simulation results show that ultrashort X-ray pulses with peak power of GW level and pulse duration as short as 86 attoseconds can be generated. The proposed scheme can make it possible to study the electronic dynamic of the valence electrons of which the time scale is about 100 attoseconds and may open up a new frontier of ultrafast science.