AbstractUltrafast imaging is essential in physics and chemistry to investigate the femtosecond dynamics of nonuniform samples or of phenomena with strong spatial variations. It relies on observing the phenomena induced by an ultrashort laser pump pulse using an ultrashort probe pulse at a later time. Recent years have seen the emergence of very successful ultrafast imaging techniques of single non-reproducible events with extremely high frame rate, based on wavelength or spatial frequency encoding. However, further progress in ultrafast imaging towards high spatial resolution is hampered by the lack of characterization of weak probe beams. For pump–probe experiments realized within solids or liquids, because of the difference in group velocities between pump and probe, the determination of the absolute pump–probe delay depends on the sample position. In addition, pulse-front tilt is a widespread issue, unacceptable for ultrafast imaging, but which is conventionally very difficult to evaluate for the low-intensity probe pulses. Here we show that a pump-induced micro-grating generated from the electronic Kerr effect provides a detailed in-situ characterization of a weak probe pulse. It allows solving the two issues of absolute pump–probe delay determination and pulse-front tilt detection. Our approach is valid whatever the transparent medium with non-negligible Kerr index, whatever the probe pulse polarization and wavelength. Because it is nondestructive and fast to perform, this in-situ probe diagnostic can be repeated to calibrate experimental conditions, particularly in the case where complex wavelength, spatial frequency or polarization encoding is used. We anticipate that this technique will enable previously inaccessible spatiotemporal imaging in a number of fields of ultrafast science at the micro- and nanoscale.
Ultrafast pump-probe ellipsometry and microscopy reveal the surface dynamics of femtosecond laser ablation of aluminium and stainless steel