Hybrid improper ferroelectricity (HIF) has received increasing scientific attention since it provides great potential for realizing single phase room temperature multiferroicity with strong magnetoelectric coupling, and Ruddlesden–Popper (R–P) compounds AO(ABO3)n with even n are the most important candidates for HIFs. However, the modulation of ferroelectric polarization is recognized as a challenging issue. Here, Sr3−xBaxSn2O7 ceramics with a large remanent polarization with respect to other R–P HIFs (∼1.0 μC/cm2) combined with a reduced coercive field are reported. The polarization increases obviously with the increasing tolerance factor, inconsistent with the previous understanding. This is because the amplitude of tilt increases and rotation decreases, which results in the increased distortion of SnO6 octahedra. That is, the polarization of R–P compounds should be determined by the combined effects of tilting and rotation and not be simply evaluated by the tolerance factor.

Hybrid improper ferroelectricity has been extensively studied in double-layer Ruddlesden–Popper oxides in recent years. Although the hybrid improper ferroelectricity could be created among triple-layer Ruddlesden–Popper oxides with an ordered A-site cation predicted by the first-principles calculations, no experimental result has been reported yet. In the present work, the room-temperature ferroelectricity has been observed in Li2La2Ti3O10 ceramics with an A-site cation ordered triple-layer Ruddlesden–Popper structure. The polar phase P21ab has been determined by combining the first-principles calculation and the powder diffraction analysis at room temperature. The hybrid improper ferroelectricity was induced by the triple-coupled irreps including the A-site cation ordering. The variable temperature differential scanning calorimetry measurements and dielectric responses indicate no evidence of phase transition over the temperature range of 200–1080 K. The present work sheds light on designing the hybrid improper ferroelectrics in A-site ordered triple-layer Ruddlesden–Popper compounds.

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Ferroelectric materials have attracted a lot of attention for several decades due to wide applications such as non-volatile random-access memories and large piezoelectric responses for sensors and transducers. [1][2][3] However, the proper ferroelectrics have been restricted to a relatively narrow range of compositions where the ferroelectric state emerges from the specific electronic configurations for orbital hybridization or the second-order Jahn-Teller ions to break the space-inversion

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