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8–11 This size effect is often discussed in terms of intrinsic size or depolarizing field effects arising in ultrathin dielectrics/ferroelectrics. 12,13 In conventional ferroelectrics (such as BaTiO 3, PbTiO 3, SrBi 2Ta 2O 9, and Bi 4Ti 3O 12), 14–16 the electric polarization reduces or even disappears when the film thickness reaches the deep nanoscale regime or a critical thickness. 8–11 This problem is even more pronounced in ferroelectric thin films. 7,8 For example, perovskite thin films (such as BaTiO 3 and PbTiO 3) often yield reduced ε r values that are 2–3 orders of magnitude smaller than the bulk values. 4–6 Previous studies on high- k dielectric thin films have consistently observed that the dielectric constant ( ε r) is significantly reduced as the film thickness decreases to 50 nm. 1–3 However, the so-called size effects present a formidable challenge ( Fig. For further miniaturization of electronic devices, the exploration of high- k dielectric/ferroelectric thin films with nanometer thicknesses are strongly needed. 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