SrTiO3 (STO), a room-temperature paraelectric material in bulk form, has been a rich playground for emergent phenomena for decades. As an emerging material, great attention has been paid to freestanding 2D STO thin films. Recently, the room-temperature ferroelectricity has been unveiled in strained STO thin films; however, it remains an open question whether the strain-free freestanding 2D STO thin film is room-temperature ferroelectric or not. Here, we report the electric field-induced out-of-plane ferroelectric polarization in large-scale, freestanding, and strain-free 2D STO membranes at room temperature. High-resolution piezoresponse force microscopy measurements show that polarization in freestanding strain-free STO membranes can be switched by electric field and persist for an hour. The first-principles calculations suggest that the intrinsic defects such as oxygen vacancies could be linked to the observed spontaneous out-of-plane polarization in 2D STO membranes, which could be further enhanced by external electric field due to the induced symmetry breaking. Our work reports the unprecedented room-temperature ferroelectric polarization in strain-free freestanding 2D STO membranes, unlocking the great potential of freestanding 2D STO for the applications in novel electronic and logic-in-memory devices.

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