We demonstrate that complex supercontinuum and few-cycle ultrashort laser pulses can be fully characterized by using a cross-correlation frequency-resolved optical gating with molecular alignment induced birefringence functioned as a gate. The temporal envelope and phase of the broadband supercontinuum pulse are retrieved by the principal component generalized projection algorithm. This technique shows advantages without phase-matching constraint that may limit the measurable spectral bandwidth, experimental robustness in operating through the whole transparent spectral region of the molecular gases, and intensity sensitivity to measure weak pulses which is inherited from the intrinsic linear process in recording the molecular birefringence induced polarization spectroscopy. Experimental measurements of a few-cycle pulse in the visible region of 525-725 nm confirm that the molecular alignment gating supports a full field characterization of the ultrashort pulse around 10 fs in duration.

We experimentally demonstrate a molecular-alignment-based cross-correlation frequency-resolved optical gating technique for ultraviolet femtosecond pulse measurement, which use laser-induced impulsive alignment of gaseous molecules as the gate function instead of the phase-matched frequency mixing process in a nonlinear crystal. The spectrogram measurements and retrieving results of the intensity and phase of the second and third harmonic pulses centered at 400 and 267 nm are presented.

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The polarization-resolved laser-induced breakdown spectroscopy (PRLIBS) technique, which can significantly reduce the polarized emission from laser plasma by placing a polarizer in front of the detector, is a powerful tool to improve the line-to-continuum ratio in LIBS applications. It is shown that the continuum emission from the plasma produced through ablating an Al sample by nanosecond laser pulses is much more polarized than the discrete line emission with the single-pulse PRLIBS technique. The effects of laser fluence and detection angle on the Al polarization spectrum are systematically explored experimentally. The calculated result of the polarization spectrum as a function of laser fluence shows that it is in agreement with the experimental observations.