An algorithm is introduced for the molecular simulation of constant-pressure plastic deformation in amorphous solids at zero temperature. This allows to directly study the volume changes associated with plastic deformation (dilatancy) in glassy solids. In particular, the dilatancy of polymer glasses is an important aspect of their mechanical behavior. The new method is closely related to Berendsen's barostat, which is widely used for molecular dynamics simulations at constant pressure. The new algorithm is applied to plane strain compression of a binary Lennard-Jones glass. Conditions of constant volume lead to an increase of pressure with strain, and to a concommitant increase in shear stress. At constant (zero) pressure, by contrast, the shear stress remains constant up to the largest strains investigated (epsilon = 1), while the system density decreases linearly with strain. The linearity of this decrease suggests that each elementary shear relaxation event brings about an increase in volume which is proportional to the amount of shear. In contrast to the stress-strain behavior, the strain-induced structural relaxation, as measured by the self-part of the intermediate structure factor, was found to be the same in both cases. This suggests that the energy barriers that must be overcome for their nucleation continually grow in the case of constant-volume deformation, but remain the same if the deformation is carried out at constant pressure. (C) 2004 Wiley Periodicals, Inc.