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Register a new userDirect Observation of Polarization vs. Thickness Relation in Ultra-Thin Ferroelectric Films
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A reduction of polarization in ultra-thin ferroelectric films appears to be fundamental to ferroelectricity at the nanoscale. For the model system PbTiO3 on SrTiO3, we report observation of the polarization vs. thickness relation. Distinct periodicity changes of ferroelectric domains obtained from x-ray diffraction and total energy calculations reveal a linear lowering of the polarization below a critical thickness of ~12 nm. Independent polarization and tetragonality measurements provide insight into the fundamental relation between polarization and tetragonality in nanoscale ferroelectrics.
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We present a segregrated strain model that describes the thickness-dependent dielectric properties of ferroelectric films. Using a phenomenological Landau approach, we present results for two specific materials, making comparison with experiment and with first-principles calculations whenever possible. We also suggest a smoking gun benchtop probe to test our elastic scenario.
We report a dielectric relaxation in ferroelectric thin films of the ABO3 family. We have compared films of different compositions with several growth modes: sputtering (with and without magnetron) and sol-gel. The relaxation was observed at cryogenic temperature (T<100K) for frequencies from 100Hz up to 10MHz. This relaxation activation energy is always lower than 200meV. It is very similar to the polaron relaxation that we reported in the parent bulk perovskites. Being independent of the materials size, morphology and texture, this relaxation can be a useful probe of defects in actual integrated capacitors with no need for specific shaping
The emergent behaviors in thin films of a multiaxial ferroelectric due to an electrochemical coupling between the rotating polarization and surface ions are explored within the framework of the 2-4 Landau-Ginzburg-Devonshire (LGD) thermodynamic potential combined with the Stephenson-Highland (SH) approach. The combined LGD-SH approach allows to describe the electrochemical switching and rotation of polarization vector in the multiaxial ferroelectric film covered by surface ions with a charge density dependent to the relative partial oxygen pressure. We calculate the phase diagrams and analyze the dependence of polarization components on the applied voltage, and discuss the peculiarities of quasi-static ferroelectric, dielectric and piezoelectric hysteresis loops in thin strained multiaxial ferroelectric films. The nonlinear surface screening by oxygen ions makes the diagrams very different from the known diagrams of e.g., strained BaTiO3 films. Quite unexpectedly we predict the appearance of the ferroelectric reentrant phases. Obtained results point on the possibility to control the appearance and features of ferroelectric, dielectric and piezoelectric hysteresis in multiaxial FE films covered by surface ions by varying their concentration via the partial oxygen pressure. The LGD-SH description of a multiaxial FE film can be further implemented within the Bayesian optimization framework, opening the pathway towards predictive materials optimization.
A thermodynamic theory is developed for dense laminar domain structures in epitaxial ferrolectric films. It is found that, at some critical misfit strain between the film and substrate, the 90 degrees c/a/c/a domain structure becomes unstable with respect to the appearance of the polarization component parallel to domain walls, which results in the formation of a heterophase structure. For PbTiO_3 and BaTiO_3 films, the stability ranges of polydomain and heterophase states are determined using misfit strain - temperature diagrams. Dielectric anomalies accompanying misfit-strain-driven structural transformations are described.
The effects of space charges on hysteresis loops and field distributions in ferroelectrics have been investigated numerically using the phenomenological Landau-Ginzburg-Devonshire theory. Cases with the ferroelectric fully and partially depleted have been considered. In general, increasing the number of charged impurities results in a lowering of the polarization and coercive field values. Squarer loops were observed in the partially depleted cases and a method was proposed to identify fully depleted samples experimentally from dielectric and polarization measurements alone. Unusual field distributions found for higher dopant concentrations have some interesting implications for leakage mechanisms and limit the range of validity of usual semiconductor equations for carrier transport.
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