Under ultrahigh stresses (e.g., under high strain rates or in small-volume metals) deformation twinning (DT) initiates on a very short time scale, indicating strong spatial-temporal correlations in dislocation dynamics. Using atomistic simulations, here we demonstrate that surface rebound of relativistic dislocations directly and efficiently triggers DT under a wide range of laboratory experimental conditions. Because of its stronger temporal correlation, surface rebound sustained relay of partial dislocations is shown to be dominant over the conventional mechanism of thermally activated nucleation of twinning dislocations. DOI: 10.1103/PhysRevLett.117.165501 Recent advances in small-volume materials fabrication have created a remarkable category of metallic crystals that can retain pristine crystal structures on the length scale of 10 1 − 10 2 nanometers [1][2][3][4][5][6][7]. Deformation twinning (DT) has been shown to initiate in these metals at ultrahigh stresses (∼10 −2 G, where G is shear modulus) and on a very short time scale (≪0.01 s, the typical time resolution of state-of-the-art in situ microscopy imaging techniques) [2,[4][5][6], indicating strong spatial-temporal correlations in the underlying dislocation dynamics. Such strongly correlated DT mode requires extremely stringent spatial and temporal coordination of twinning dislocations (the right type of partial dislocations on consecutive atomic planes one after another [8]). This is hardly possible by the conventional pole mechanism [9,10] due to the pristine nature of the deformation volume, nor by the generally believed thermally activated nucleation (TAN) [2,[5][6][7][11][12][13] due to possible long waiting time.In the following, we illustrate that while the first dislocation to initiate DT must come from a TAN event, subsequent twinning dislocations can be generated by dislocations running at speeds near the transverse sound speed (c t ). Specifically, twinning dislocations are generated successively on each and every consecutive atomic plane by a surfacerebound sustained (SRS) nucleation process, in a domino cascade fashion. This mechanism is highly efficient due to its strong temporal correlation; i.e., there is almost no time delay between two successive twinning partials. The SRS mechanism can thus dominate over the TAN mechanism over a wide range of experimental conditions. Atomistic simulations, reaction pathway sampling method, and the harmonic transition state theory will be combined to reveal the mechanism underlying the strongly correlated DT. Direct molecular dynamics (MD) simulations were performed to observe how dislocations behave after nucleation in highly stressed nanowires and slab configurations. The free end nudged elastic band method (FENEB) [11,14] was used to obtain the activation energy barriers for TAN of surface dislocation. The empirical potential for copper [15] based on the embedded atom method was used to describe the interatomic interactions. All simulations were performed using the LAMMPS Figure 1 shows DT ...