The partial-dislocation-mediated processes have so far eluded high-resolution transmission electron microscopy studies in nanocrystalline ͑nc͒ Ni with nonequilibrium grain boundaries. It is revealed that the nc Ni deformed largely by twinning instead of extended partials. The underlying mechanisms including dissociated dislocations, high residual stresses, and stress concentrations near stacking faults are demonstrated and discussed. © 2006 American Institute of Physics. ͓DOI: 10.1063/1.2227639͔The mechanical properties of nanocrystalline ͑nc͒ materials are controlled by their deformation mechanisms, 1 which include partial dislocation emission from grain boundaries ͑GBs͒, 2-10 deformation twinning, 9-20 full dislocations, 3,5,7 GB sliding, 3,11-13 and grain rotation. 11,14 Basing on generalized planar fault energy ͑GPFE͒ curves, molecular dynamics ͑MD͒ simulations predicted that nc Ni prefers to deform by extended partials, rather than twinning. 5 The two energies on the GPFE curves, the unstable stacking fault energy ͑SFE͒ ␥ usf and the unstable twin fault energy ␥ utf , are believed to play critical roles in the activation of extended partials and twining. 5 However, a recent study indicates that the ␥ usf and ␥ utf values obtained from GPFE curves vary significantly with the models used for their calculation and it is not clear if these values even qualitatively agree with the real values, 21 which so far cannot be experimentally measured. A recent experimental study 22 revealed the formation of both stacking faults and deformation twins in electrodeposited Ni, which has GBs not far from equilibrium and those used in MD simulations.Nanomaterials often have nonequilibrium GBs with high densities of extrinsic ͑extra͒ dislocations. [23][24][25] This is especially true for those nc metals and alloys produced by severe plastic deformation. 26 It has been claimed that the GPFE curves are not applicable to these nc metals and alloys because partial dislocations already exist at/near nonequilibrium GBs and therefore do not need to be nucleated. 27,28 In other words, since the ␥ usf and ␥ utf only affect the nucleation process of the extended partial and the first twin partial, they should not affect the nc metals and alloys with nonequilibrium GBs. However, experimental evidence is still lacking to support such a claim.The objective of this work is to study the partialdislocation-mediated processes in nanomaterials with nonequilibrium GBs. We chose to use nc Ni produced by surface mechanical attrition treatment ͑SMAT͒ ͑Ref. 29͒ in this study because Ni has been extensively studied by MD simulations and experiments, and SMAT can produce nc Ni with impurity-free nonequilibrium GBs.A Ni plate with a purity of 99.998% was subjected to SMAT at room temperature to produce a layer of nc Ni. 30 Extensive high-resolution electron microscopy ͑HREM͒ observations revealed that at the depth of 27 m from the surface, the nc Ni has grain sizes in the range of 20-100 nm. The grain size is found to affect twinning propensity: twin...