Direct atomic-scale evidence is presented for the shear-dilatation correlation in metallic glasses via molecular dynamics and first-principles calculations. A quantitative parabolic relationship is established between the atomic local shear and hydrostatic volumetric strains by carrying out statistical analysis on a deformed glass model. The correction is further verified by density functional theory. Our atomistic demonstration of shear-dilatation correlation collaborates with the experimentally observed a few percent volume change in shear bands. It brings quantitative insights into the unique correlation between shear transformation and cavitation in metallic glasses.© 2015 Elsevier Ltd. All rights reserved.Metallic glasses (MGs) are a category of promising high strength structural materials with many other superior physical and chemical properties [1]. The deformation mechanisms of such amorphous solid state are in sharp contrast with their crystalline counterparts since there are no long-range atoms packing pattern in MGs [2,3]. No conventional mechanisms, such as ordinary dislocation plasticity or deformation twinning in crystals, exist in MGs which can carry plastic deformation. Therefore MGs usually suffer from the notorious catastrophic failure with a strong strain localization (shear banding) phenomenon [4,5].Several models have been proposed to rationalize the inelastic deformation of MGs, which include free volume [6], shear transformation zone (STZ) [7][8][9], cooperative shear model (CSM) [10,11], flow unit [12], vibrational soft spot [13], shear-diffusive transformation [14,15], and our recently proposed tensile transformation zone (TTZ) [16][17][18]. All of these models are based on the local structural rearrangement of atoms via the interplay of atomic-scale shear and dilation/contraction in MGs [19][20][21][22][23][24]. Among them, Argon's STZ model involves local rearrangement of a cluster of atoms undergoing a stress-driven, and thermally activated shear distortion [25,23,24]. Whereas Spaepen's free volume model is based on a dynamic equilibrium between the stress-assisted creation and annihilation of free volume [6]. The free volume behaviors can be regarded as dilation and contraction of local atomic environments. Since both models have been successfully adopted to describe the homogeneous and inhomogeneous flows in MGs, there should be some intrinsic correlation between shear and dilatation/compaction during deformation of glasses [21,26].Generally, shear-dilatation correlation is an intrinsic nature of deformation in amorphous alloys although local compaction is also allowed [27,28]. For example, intuitively derived law between shear strain and local dilatation has been used in constitutive modelings of MGs [29]. Shear is not necessarily the only deformation mode accommodating the local atomic rearrangement. The microscopic scenario is that the STZ operations redistribute stress spatially which usually leads to the creation of free volume via atomic-scale dilatation [21,1]. So that local ...