Direct writing with tilted-front femtosecond pulses

Shaping light fields in both space and time provides new degrees of freedom to manipulate light-matter interaction on the ultrafast timescale. Through this exploitation of the light field, a greater appreciation of spatio-temporal couplings in focusing has been gained, shedding light on previously unexplored parameters of the femtosecond light pulse, including pulse front tilt and wavefront rotation. Here, we directly investigate the effect of major spatio-temporal couplings on light-matter interaction and reveal unambiguously that in transparent media, pulse front tilt gives rise to the directional asymmetry of the ultrafast laser writing. We demonstrate that the laser pulse with a tilted intensity front deposits energy more efficiently when writing along the tilt than when writing against, producing either an isotropic damage-like or a birefringent nanograting structure. The directional asymmetry in the ultrafast laser writing is qualitatively described in terms of the interaction of a void trapped within the focal volume by the gradient force from the tilted intensity front and the thermocapillary force caused by the gradient of temperature. The observed instantaneous transition from the damage-like to nanograting modification after a finite writing length in a transparent dielectric is phenomenologically described in terms of the first-order phase transition