AbstractWe have investigated the response of the work function, W, of low-index aluminum surfaces to tangential strain by using first-principles calculations based on density functional theory. This response parameter is a central quantity in electrocapillary coupling of metal electrodes relating to the performance of porous metal actuators and surface stress based sensing devices. We find that Al surfaces exhibit a positive response for all orientations considered. By contrast, previous studies reported negative-valued response parameters for clean surfaces of several transition metals. We discuss separately the response of W to different types of strain and the impact of the strain on the Fermi energy and the surface dipole. We argue that the reason for the abnormal positive sign of the Al response parameter lies in its high valence electron density.