We report on the dynamical response of single layer transition metal dichalcogenide MoS2 to intense above-bandgap photoexcitation using the nonlinear-optical second order susceptibility as a direct probe of the electronic and structural dynamics. Excitation conditions corresponding to the order of one electron-hole pair per unit cell generate unexpected increases in the second harmonic from monolayer films, occurring on few picosecond time-scales. These large amplitude changes recover on tens of picosecond time-scales and are reversible at megahertz repetition rates with no photoinduced change in lattice symmetry observed despite the extreme excitation conditions.

One-dimensional potassium niobate nanowires are of interest as building blocks in integrated piezoelectric devices, exhibiting large nonlinear optical and piezoelectric responses. Here we present femtosecond measurements of light-induced polarization dynamics within an optically trapped ferroelectric nanowire, using the second-order nonlinear susceptibility as a real-time structural probe. Large amplitude, reversible modulations of the nonlinear susceptibility are observed within single nanowires at megahertz repetition rates, developing on few-picosecond time-scales, associated with anomalous coupling of light into the nanowire.