Artificial
materials in the form of superlattices have been studied
actively in quest of new engineering methods or design rules for the
development of desired functionalities, in particular high-k ferroelectricity, ferromagnetism, and high mobility electron
gas. This work presents a controlled assembly strategy for fabricating
atomically precise interfaces of two-dimensional (2D) homologous perovskite
nanosheets (Ca2Na
m–3Nb
m
O3m+1
–; m = 3–6) to construct artificial
superlattices. The distinctive thickness of each 2D homologous perovskite
nanosheets attributed to the presence of different number of NbO6 octahedra provides an exquisite control to engineer interfacial
properties for tailored design of superior high-k properties and emergence of ferroelectricity. The higher dielectric
constant (εr = 427) and development of ferroelectricity
for (Ca2Nb3O10
–/Ca2Na2Nb5O16
–)6 superlattice indicate that superlattice films with
both odd number of NbO6 octahedra possess extended polarization
due to the potential effect of heterointerface and ferroelectric instabilities.
Furthermore, the increased discontinuities/offsets in Ca2Nb3O10
– and Ca2Na3Nb6O19
– nanosheets
band alignment results in superior insulating properties (∼1
× 10–11 A cm–2 at 1 V) for
(Ca2Nb3O10
–/Ca2Na3Nb6O19
–)6 superlattice. These findings exhibit new research opportunities
for the development of novel artificial high-k dielectric/ferroelectric
via precise control of interfaces at the atomic level and can be extended
to the large family of 2D perovskite compounds.