arXiv subjects

N. Setter

Publications and source records attributed to N. Setter.

12 recordsLinked to original sources

arXiv2014

Lattice dynamics and antiferroelectricity in PbZrO$_3$ tested by X-ray and Brillouin light scattering

We report the results of comprehensive study of the critical dynamics of the prototype perovskite antiferroelectric PbZrO$_3$. The combination of inelastic X-ray and diffuse X-ray scattering techniques and Brillouin light scattering was used. It is found that the dispersion of the TA phonons is strongly anisotropic. The dispersion curve of the in-plane polarized TA phonons propagating in [1 1 0] direction demonstrates pronounced softening. Slowing down of the excitations at R-point is found, it is manifested in growing of the central peak. This slowing down is too weak to be considered as a primary origin of the corresponding order parameter. Obtained results are treated in terms of TA--TO flexoelectric mode coupling. It is demonstrated that the structural phase transformation in PbZrO$_3$ can be considered as the result of the only intrinsic instability associated with the ferroelectric soft mode.

cond-mat.mtrl-sci↗

arXiv2014

Close-circuit domain quadruplets in BaTiO$_3$ nanorods embedded in SrTiO$_3$ film

Cylindrical BaTiO3 nanorods embedded in (100)-oriented SrTiO3 epitaxial film in a brush-like configuration are investigated in the framework of the Ginzburg-Landau-Devonshire model. It is shown that strain compatibility at BaTiO3/SrTiO3 interfaces keeps BaTiO3 nanorods in the rhombohedral phase even at room temperature. Depolarization field at the BaTiO3/SrTiO3 interfaces is reduced by an emission of the 109-degree or 71-degree domain boundaries. In case of nanorods of about 10-80 nm diameter, the ferroelectric domains are found to form a quadruplet with a robust flux-closure arrangement of the in-plane components of the spontaneous polarization. The out-of-plane components of the polarization are either balanced or oriented up or down along the nanorod axis. Switching of the out-of-plane polarization with coercive field of about $5.10^6$ V/m occurs as a collapse of a 71-degree cylindrical domain boundary formed at the curved circumference surface of the nanorod. The remnant domain quadruplet configuration is chiral, with the $C_4$ macroscopic symmetry. More complex stable domain configurations with coexisting clockwise and anticlockwise quadruplets contain interesting arrangement of strongly curved 71-degree boundaries.

cond-mat.mtrl-sci↗

arXiv2012

Bichiral structure of feroelectric domain wall driven by flexoelectricity

The influence of flexoelectric coupling on the internal structure of neutral domain walls in tetragonal phase of perovskite ferroelectrics is studied. The effect is shown to lower the symmetry of 180-degree walls which are oblique with respect to the cubic crystallographic axes, while {100} and {110} walls stay "untouched". Being of the Ising type in the absence of the flexoelectric interaction, the oblique domain walls acquire a new polarization component with a structure qualitatively different from the classical Bloch-wall structure. In contrast to the Bloch-type walls, where the polarization vector draws a helix on passing from one domain to the other, in the flexoeffect-affected wall, the polarization rotates in opposite directions on the two sides of the wall and passes through zero in its center. Since the resulting polarization profile is invariant upon inversion with respect to the wall center it does not brake the wall symmetry in contrast to the classical Bloch-type walls. The flexoelectric coupling lower the domain wall energy and gives rise to its additional anisotropy that is comparable to that conditioned by the elastic anisotropy. The atomic orderof- magnitude estimates shows that the new polarization component P2 may be comparable with spontaneous polarization Ps, thus suggesting that, in general, the flexoelectric coupling should be mandatory included in domain wall simulations in ferroelectrics. Calculations performed for barium titanate yields the maximal value of the P2, which is much smaller than that of the spontaneous polarization. This smallness is attributed to an anomalously small value of a component of the "strain-polarization" elecrostictive tensor in this material.

cond-mat.mtrl-sci↗

arXiv2009

Polar phonons in some compressively stressed epitaxial and polycrystalline SrTiO3 thin films

Several SrTiO3 (STO) thin films without electrodes processed by pulsed laser deposition, of thicknesses down to 40 nm, were studied using infrared transmission and reflection spectroscopy. The complex dielectric responses of polar phonon modes, particularly ferroelectric soft mode, in the films were determined quantitatively. The compressed epitaxial STO films on (100) La0.18Sr0.82Al0.59-Ta0.41O3 substrates (strain 0.9%) show strongly stiffened phonon responses, whereas the soft mode in polycrystalline film on (0001) sapphire substrate shows a strong broadening due to grain boundaries and/or other inhomogeneities and defects. The stiffened soft mode is responsible for a much lower static permittivity in the plane of the compressed film than in the bulk samples.

cond-mat.mtrl-sci↗

arXiv2008

Raman spectroscopy of (K,Na)NbO3 and ((K,Na)1-xLix)NbO3

A Raman scattering spectroscopy study is reported through all four phases of a (K0.5Na0.5)NbO3 crystal and ((K0.5Na0.5)1-xLix)NbO3 for x=0.02 and 0.03. The transitions among the ferroelectric phases in the Li-free crystal are homogeneous and strongly hysteretic, with no evidence of a mixed-phase region between the rhombohedral and orthorhombic phases. The Raman pattern in the lowest-temperature phase in the Li-doped material differs significantly from that found for x=0 and suggest a structural phase boundary exists at for a Li concentration of less than 2%.

cond-mat.mtrl-sci↗

arXiv2008

Nonvolatile ferroelectric control of ferromagnetism in (Ga,Mn)As

There is currently much interest in materials and structures that provide coupled ferroelectric and ferromagnetic responses, with a long-term goal of developing new memories and spintronic logic elements. Within the field there is a focus on composites coupled by magnetostrictive and piezoelectric strain transmitted across ferromagnetic-ferroelectric interfaces, but substrate clamping limits the response in the supported multilayer configuration favoured for devices. This constraint is avoided in a ferroelectric-ferromagnetic bilayer in which the magnetic response is modulated by the electric field of the poled ferroelectric. Here, we report the realization of such a device using a diluted magnetic semiconductor (DMS) channel and a polymer ferroelectric gate. Polarization reversal of the gate by a single voltage pulse results in a persistent modulation of the Curie temperature as large as 5%. The device demonstrates direct and quantitatively understood electric-fieldmediated coupling in a multiferroic bilayer and may provide new routes to nanostructured DMS materials and devices via ferroelectric domain nanopatterning. The successful implementation of a polymer-ferroelectric gate fieldeffect transistor (FeFET) with a DMS channel adds a new functionality to semiconductor spintronics and may be of importance for future low-voltage spintronics devices and memory structures.

cond-mat.mtrl-sci↗

arXiv2007

Dielectric relaxation and polar phonon softening in relaxor ferroelectric PbMg_(1/3)Ta_(2/3)O_3

Relaxor ferroelectric PbMg_1/3Ta_2/3O_3 ceramics and thin films were investigated by means of broad-band dielectric, time-domain terahertz (THz) and Fourier-transform infrared (IR) spectroscopy in the frequency range 100 Hz - 90 THz at temperatures 100 - 490 K, the THz and IR spectra were studied from 20 to 900K. Diffused and strongly temperature dependent peak in the complex permittivity is caused by a dielectric relaxation due to the dynamics of polar clusters. The relaxation appears below Burns temperature T_d in the THz range, slows down on cooling through the microwave and MHz range and anomalously broadens. The shortest and longest relaxation times of the distribution of relaxation times follow Arrhenius and Vogel-Fulcher law, respectively. The degree of B-site order has only a small influence on the parameters of the dielectric relaxation and almost no influence on the phonon parameters. Below T_m ~ 180K, the distribution of relaxation frequencies becomes broader than our experimental spectral range and frequency independent dielectric losses develop below 100 GHz in the spectra. Although the macroscopic crystal structure is cubic, IR spectra give evidence about the lower local symmetry which can be assigned to the presence of polar clusters below T_d. Infrared spectra above T_d still reveal more modes than predicted by selection rules in the paraelectric phase of the Fm-3m space group so that we suggest selection rules which take into account chemical inhomogeneity in the beta''-perovskite sublattice.

cond-mat.mtrl-sci↗

arXiv2007

Landau thermodynamic potential for BaTiO_3

In the paper, the description of the dielectric and ferroelectric properties of BaTiO_3 single crystals using Landau thermodynamic potential is addressed. Our results suggest that when using the sixth-power free energy expansion of the thermodynamic potential, remarkably different values of the fourth-power coefficient, β(the coefficient of P^4_i terms), are required to adequately reproduce the nonlinear dielectric behavior of the paraelectric phase and the electric field induced ferroelectric phase, respectively. In contrast, the eighth-power expansion with a common set of coefficients enables a good description for both phases at the same time. These features, together with the data available in literature, strongly attest to the necessity of the eighth-power terms in Landau thermodynamic potential of BaTiO_3. In addition, the fourth-power coefficients, βand ξ(the coefficient of P^2_i P^2_j terms), were evaluated from the nonlinear dielectric responses along [001], [011], and [111] orientations in the paraelectric phase. Appreciable temperature dependence was evidenced for both coefficients above T_C. Further analysis on the linear dielectric response of the single domain crystal in the tetragonal phase demonstrated that temperature dependent anharmonic coefficients are also necessary for an adequate description of the dielectric behavior in the ferroelectric phase. As a consequence, an eighth-power thermodynamic potential, with some of the anharmonic coefficients being temperature dependent, was proposed and compared with the existing potentials. In general, the potential proposed in this work exhibits a higher quality in reproducing the dielectric and ferroelectric properties of this prototypic ferroelectric substance.

cond-mat.stat-mech↗

arXiv2007

Uniaxial-stress induced phase transitions in [001]c-poled 0.955Pb(Zn1/3Nb2/3)O3-0.045PbTiO3

First-order, rhombohedral to orthorhombic, stress-induced phase transitions have been evidenced by bulk charge-stress measurements and X-ray diffraction derived lattice strain measurements in [001]c-poled PZN-4.5PT. The transitions are induced by uniaxial, compressive loads applied either along or perpendicular to the poling direction. In each case, they occur via rotation of the polar vector in the Cm monoclinic plane and the induced lattice strain is hysteretic yet reversible. Although no depoling is observed in the transverse mode, net depolarization is observed under longitudinal stress which is important for the use of [001]c-poled PZN-PT and PMN-PT single crystals in Tonpilz-type underwater projectors.

cond-mat.mtrl-sci↗

arXiv2006

Anharmonicity of BaTiO_3 single crystals

By analyzing the dielectric non-linearity with the Landau thermodynamic expansion, we find a simple and direct way to assess the importance of the eighth order term. Following this approach, it is demonstrated that the eighth order term is essential for the adequate description of the para/ferroelectric phase transition of BaTiO_3. The temperature dependence of the quartic coefficient βis accordingly reconsidered and is strongly evidenced by the change of its sign above 165 C. All these findings attest to the strong polarization anharmonicity of this material, which is unexpected for classical displacive ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2005

Far-infrared soft mode behavior in PST thin films

Temperature dependences of the optic phonons in $\rm PbSc_{1/2}Ta_{1/2}O_3$ sol-gel films deposited on sapphire substrates were studied by means of Fourier transform far-infrared transmission spectroscopy in the temperature range 20-900\K. Four films displaying different B-site order with both ferroelectric and relaxor behavior were studied. In all cases the TO mode near 80\icm{} at 10\K{} softens on heating to $\approx$45\icm{} following the Cochran law with extrapolated critical temperature near 700\K{} (400\K{} above the temperature of dielectric maximum, $T_{\rm m}$), but above 600\K{} its frequency remains stabilized. It can be assigned to the A$_{1}$ component of the ferroelectric soft mode inside polar clusters which form below the Burns temperature near 700\K. In the ordered PST film another mode activates below T$_{m}$ in infrared spectra near 60\icm exhibiting also anomalous temperature dependence due to its coupling with the former mode. It is assigned to the A$_{1}$ component of the F$_{2g}$ Raman active mode. Central mode, which appears below the Burns temperature in the THz range, is assigned to the dynamics of polar clusters. It slows down on cooling and vanishes from our spectral range below $T_{\rm m}$. Another overdamped excitation assigned to the E component of the soft mode appears near 30\icm{} at low temperatures.

cond-mat.mtrl-sci↗

arXiv2004

Central mode and soft mode behavior in PbMg1/Nb2/3O3 relaxor ferroelectric

The relaxor ferroelectric PbMg1/Nb2/3O3 was investigated by means of broad-band dielectric and Fourier Transform Infrared (FTIR) transmission spectroscopy in the frequency range from 1 MHz to 15 THz at temperatures between 20 and 900 K using PMN films on infrared transparent sapphire substrates. While thin film relaxors display reduced dielectric permittivity at low frequencies, their high frequency intrinsic or lattice response is shown to be the same as single crystal/ceramic specemins. It was observed that in contrast to the results of inelastic neutron scattering, the optic soft mode was underdamped at all temperatures. On heating, the TO1 soft phonon followed the Cochran law with an extrapolated critical temperature equal to the Burns temperature of 670 K and softened down to 50 cm-1. Above 450 K the soft mode frequency leveled off and slightly increased above the Burns temperature. A central mode, describing the dynamics of polar nanoclusters appeared below the Burns temperature at frequencies near the optic soft mode and dramatically slowed down below 1 MHz on cooling below room temperature. It broadened on cooling, giving rise to frequency independent losses in microwave and lower frequency range below the freezing temperature of 200 K. In addition, a new heavily damped mode appeared in the FTIR spectra below the soft mode frequency at room temperature and below. The origin of this mode as well as the discrepancy between the soft mode damping in neutron and infrared spectra is discussed.

cond-mat.mtrl-sci↗