We demonstrated that ultraviolet Raman spectroscopy is an effective technique to measure the transition temperature (Tc) in ferroelectric ultrathin films and superlattices. We showed that one-unit-cell-thick BaTiO3 layers in BaTiO3/SrTiO3 superlattices are not only ferroelectric (with Tc as high as 250 kelvin) but also polarize the quantum paraelectric SrTiO3 layers adjacent to them. Tc was tuned by ∼500 kelvin by varying the thicknesses of the BaTiO3 and SrTiO3 layers, revealing the essential roles of electrical and mechanical boundary conditions for nanoscale ferroelectricity.

http://absimage.aps.org/image/MAR07/MWS_MAR07-2006-002268.pdf

Probing nanoscale ferroelectricity by ultraviolet Raman spectroscopy

Effects of the alkaline solution concentration and deposition temperature on film thickness, crystal structure and ferroelectric properties of epitaxial PbTiO&lt;sub&gt;3&lt;/sub&gt; films grown by hydrothermal method

Abstract Lead based bulk piezoelectric materials, e.g., PbZr x Ti 1‐x O 3 (PZT), are widely used in electromechanical applications, sensors, and transducers, for which optimally performing thin films are needed. The results of a multi‐domain Landau–Ginzberg‐Devonshire model applicable to clamped ferroelectric thin films are used to predict the lattice symmetry and properties of clamped PZT thin films on different substrates. Guided by the thermal strain phase diagrams that are produced by this model, experimentally structural transitions are observed. These can be related to changes of the piezoelectric properties in PZT(x = 0.6) thin films that are grown on CaF 2 , SrTiO 3 (STO) and 70% PbMg 1/3 Nb 2/3 O 3 ‐30% PbTiO 3 (PMN‐PT) substrates by pulsed laser deposition. Through temperature en field dependent in situ X‐ray reciprocal space mapping (RSMs) and piezoelectric force microscopy (PFM), the low symmetry monoclinic phase and polarization rotation are observed in the film on STO and can be linked to the measured enhanced properties. The study identifies a monoclinic ‐rhombohedral M C ‐ M A ‐ R crystal symmetry path as the polarization rotation mechanism. The films on CaF 2 and PMN‐PT remain in the same symmetry phase up to the ferroelectric‐paraelectric phase transition, as predicted. These results support the validity of the multi‐domain model which provides the possibility to predict the behavior of clamped, piezoelectric PZT thin films, and design films with enhanced properties. 

Enhanced Piezoelectricity by Polarization Rotation through Thermal Strain Manipulation in PbZr0.6Ti0.4O3 Thin Films

Electrode dependence of polydomain stability in ferroelectric thin films

We report the thermodynamic potential for single-domain (110) thin films epitaxially grown on dissimilar cubic substrates. Using different sets of paraelectric phase elastic compliance coefficients of ${\mathrm{PbTiO}}_{3}$ single crystal, calculated from the experimental room-temperature values, we predict rotational phases similar to those observed in (001) thin films under anisotropic biaxial misfit strain. The new sets of elastic compliance coefficients also predict a triclinic phase that could potentially lead to the enhancement of both dielectric and piezoelectric properties. We also conducted experimental studies on highly tetragonal monocrystalline ${\mathrm{PbZr}}_{0.05}{\mathrm{Ti}}_{0.95}{\mathrm{O}}_{3}$ thin films of different thicknesses, epitaxially grown on (110) ${\mathrm{SrTiO}}_{3}$ substrate by pulsed laser deposition technique. Piezoresponse force microscopy measurements showed that the as-grown films were single domain with the ${a}_{2}c$ phase, which corroborates with the prediction of the theory. Moreover, the ${T}_{c}$ values of both thin and thick films (17--90 nm) also fell within the predicted range $(540--600\phantom{\rule{0.16em}{0ex}}{}^{\ensuremath{\circ}}\mathrm{C})$. The measured remanet polarization of $57\ensuremath{\mu}\mathrm{C}/{\mathrm{cm}}^{2}$ was in good agreement with the theoretical values of $55--58\ensuremath{\mu}\mathrm{C}/{\mathrm{cm}}^{2}$. Small-signal piezoelectric response measurements gave a piezoelectric coefficient of 40 pm/V, which is also in good agreement with the numerically calculated values of 38--42 pm/V.

/pdf/single-domain-110-pbtio-3-thin-films-thermodynamic-theory-2arjdhy78v.pdf

Single-domain (110) PbTiO 3 thin films: Thermodynamic theory and experiments

Phase transitions and domain state transformations in a 250 nm thick PbTiO3/SrTiO3 film with c/a/c/a domain structure were investigated by temperature-dependent x-ray diffraction and Raman spectroscopy. Both techniques provide evidence that the film remains tetragonal up to 650 °C, while the bulk sample becomes cubic at 490 °C. Small anomalies in the width of both Bragg peaks and in Raman modes suggest a subtle structural rearrangement around 500 °C.

/pdf/stability-of-the-polydomain-state-in-epitaxial-ferroelectric-1ozatzvzft.pdf

Stability of the polydomain state in epitaxial ferroelectric PbTiO3 films

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Stability of the polydomain state in epitaxial ferroelectric PbTiO3 films