Van der Waals interfaces can be formed by layer stacking without regard to lattice constants or symmetries of individual building blocks. We engineered the symmetry of a van der Waals interface of tungsten selenide and black phosphorus and realized in-plane electronic polarization that led to the emergence of a spontaneous photovoltaic effect. Spontaneous photocurrent was observed along the polar direction and was absent in the direction perpendicular to it. The observed spontaneous photocurrent was explained by a quantum-mechanical shift current that reflects the geometrical and topological electronic nature of this emergent interface. The present results offer a simple guideline for symmetry engineering that is applicable to a variety of van der Waals interfaces.
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