Freestanding films provide a versatile platform for materials engineering thanks to additional structural motifs not found in films with a substrate. A ubiquitous example is wrinkles, yet little is known about how they can develop over as fast as a few picoseconds due to a lack of experimental probes to visualize their dynamics in real time on the nanoscopic scale. Here, we use time-resolved electron diffraction to directly observe light-activated wrinkling formation in freestanding La2/3Ca1/3MnO3 films. Via a "lock-in" analysis of oscillations in the diffraction peak position, intensity, and width, we quantitatively reconstructed how wrinkles develop on the time scale of lattice vibration. Contrary to the common assumption of fixed boundary conditions, we found that wrinkle development is associated with ultrafast delamination at the film boundaries. Our work provides a generic protocol to quantify wrinkling dynamics in freestanding films and highlights the importance of the film-substrate interaction in determining the properties of freestanding structures.
Keywords: delamination; freestanding thin film; strongly correlated oxides; ultrafast electron diffraction; wrinkle formation.