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.
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