AbstractWhen confronted by severe geometric constraints, dislocations may respond in unforeseen ways. One example of such unexpected behavior is parallel glide in unpassivated, ultrathin (200 nm and thinner) metal films. This involves the glide of dislocations parallel to and very near the film/substrate interface, following their emission from grain boundaries. In situ transmission electron microscopy reveals that this mechanism dominates the thermomechanical behavior of ultrathin, unpassivated copper films. However, according to Schmid's law, the biaxial film stress that evolves during thermal cycling does not generate a resolved shear stress parallel to the film/substrate interface and therefore should not drive such motion. Instead, it is proposed that the observed dislocations are generated as a result of atomic diffusion into the grain boundaries. This provides experimental support for the constrained diffusional creep model of Gao et al.[1], in which they described the diffusional exchange of atoms between the unpassivated film surface and grain boundaries at high temperatures, a process that can locally relax the film stress near those boundaries. In the grains where it is observed, parallel glide can account for the plastic strain generated within a film during thermal cycling. One feature of this mechanism at the nanoscale is that, as grain size decreases, eventually a single dislocation suffices to mediate plasticity in an entire grain during thermal cycling. Parallel glide is a new example of the interactions between dislocations and the surface/interface, which are likely to increase in importance during the persistent miniaturization of thin film geometries.