Anisotropic achiral surfaces respond differently to left-and right-hand circularly polarized light. This occurs when the orientation of the surface with respect to an otherwise achiral experimental setup makes the total geometry chiral. Such optical activity is demonstrated in second-harmonic generation from an anisotropic thin molecular film. The circular-difference response reverses sign as the handedness of the geometry is reversed and vanishes when the setup possesses a mirror plane. The results are explained within the electric-dipole-allowed second-order surface nonlinearity. [S0031-9007(96)00778-8] PACS numbers: 33.55.Ad, 42.65.Ky, Optical-activity effects, e.g., circular dichroism and optical rotation, are usually associated with chiral (enantiomorphous) materials [1]. Such materials possess no mirror planes and occur in two enantiomers that are mirror images of each other. Optical activity arises from the different interaction of chiral materials with left-and righthand circularly polarized light and reverses sign between the enantiomers. For isotropic chiral solutions, optical activity arises from the interference between the electricdipole and magnetic-dipole contributions to the optical properties of the material [1]. However, for surface geometries with only two-dimensional rotational symmetry, chiral effects can also be allowed in the electric-dipole approximation [2].On a more general level, the term optical activity is used to refer to circular-difference and optical-rotation effects that occur beyond (linear) birefringence. Such effects can occur also in achiral materials. This is possible if the experimental arrangement is chiral, i.e., it possesses a definite handedness and is described by three noncoplanar unit vectors [3]. For example, photoelectron emission from oriented linear molecules exhibits optical activity if the direction of propagation of the incident photon and the photoelectron and the axis of the molecule are not coplanar [3]. In addition, optical rotation can occur in certain nonenantiomorphous crystals [4] and oriented molecular systems [5] such as nematic liquid crystals [6,7]. However, these cases involve light propagation in a bulk sample and, consequently, separation between optical activity and linear birefringence may be very difficult [8]. Optical activity has also been observed in secondharmonic generation from an isotropic and achiral surface [9]. In this case the chirality of the experiment was not associated with the orientation of the sample but arose from the (mis)alignment of the polarizer that was used to analyze the second-harmonic light.In this Letter, we report the first observation of optical activity of achiral anisotropic surfaces. We use the alloptical technique of surface second-harmonic generation [10], which simplifies the experiment considerably compared to photoelectron emission experiments. Secondharmonic generation has already been shown to be a sensitive probe of chiral isotropic surfaces [11]. Our surface consists of a thin film of oriented molecu...