Simultaneously achieving high energy density and responsivity in submicron BaTiO_(3) film capacitors integrated on Si

In the research field of energy storage dielectrics,the“responsivity”parameter,defined as the recyclable/recoverable energy density per unit electric field,has become critically important for a comprehensive evaluation of the energy storage capability of a dielectric.In this work,high recyclable energy density and responsivity,i.e.,W_(rec)=161.1 J·cm^(-3) and ξ=373.8 J·(kV·m^(2))^(-1),have been simultaneously achieved in a prototype perovskite dielectric,BaTiO_(3),which is integrated on Si at 500℃ in the form of a submicron thick film.This ferroelectric film features a multi-scale polar structure consisting of ferroelectric grains with different orientations and inner-grain ferroelastic domains.A LaNiO_(3) buffer layer is used to induce a{001}textured,columnar nanograin microstructure,while an elevated deposition temperature promotes lateral growth of the nanograins(in-plane diameter increases from~10-20 nm at lower temperatures to~30 nm).These preferably oriented and periodically regulated nanograins have resulted in a small remnant polarization and a delayed polarization saturation in the film’s P-E behavior,leading to a high recyclable energy density.Meanwhile,an improved polarizability/dielectric constant of the BaTiO_(3) film has produced a much larger maximum polarization than those deposited at lower temperatures at the same electric field,leading to a record-breaking responsivity for this simple perovskite.

Dielectric ultracapacitors based on columnar nano-grained ferroelectric oxide films with gradient phases along the growth direction

In this work,dielectric ultracapacitors were designed and fabricated using a combination of phase boundary and nanograin strategies.These ultracapacitors are based on submicron-thick Ba(Zr_(0.2)Ti_(0.8))O_(3) ferroelectric films sputterdeposited on Si at 500℃.With a composition near a polymorphic phase boundary(PPB),a compressive strain,and a high nucleation rate due to the lowered deposition temperature,these films exhibit a columnar nanograined microstructure with gradient phases along the growth direction.Such a microstructure presents three-dimensional polarization inhomogeneities on the nanoscale,thereby significantly delaying the saturation of the overall electric polarization.Consequently,a pseudolinear,ultraslim polarization(P)-electric field(E)hysteresis loop was obtained,featuring a high maximum applicable electric field(~5.7 MV/cm),low remnant polarization(~5.2μC/cm^(2))and high maximum polarization(~92.1μC/cm^(2)).This P-E loop corresponds to a high recyclable energy density(Wrec~208 J/cm^(3))and charge‒discharge efficiency(~88%).An indepth electron microscopy study revealed that the gradient ferroelectric phases consisted of tetragonal(T)and rhombohedral(R)polymorphs along the growth direction of the film.The T-rich phase is abundant near the bottom of the film and gradually transforms into the R-rich phase near the surface.These films also exhibited a high Curie temperature of~460℃and stable capacitive energy storage up to 200℃.These results suggest a feasible pathway for the design and fabrication of high-performance dielectric film capacitors.