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Jiri Hlinka

Publications and source records attributed to Jiri Hlinka.

8 recordsLinked to original sources
arXiv2026

Experimentally constrained modeling of the Pockels response of KNbO3 and KTaNbO3

The soft-mode of electro-optic (EO) metal-oxide perovskites plays a critical role in determining their Pockels responses. This is the case of potassium tantalate niobate (KTN), which exhibits an intrinsic Pockels response 2.5 times larger than that of state-of-the-art barium titanate (BTO), highlighting its potential for high-performance EO applications. By combining ab initio calculations at the density-functional theory level and far-IR measurements, we reveal that the harmonic approximation combined with semi-local exchange-correlation functionals fails to accurately capture the soft transverse optical (TO) Slater mode of both potassium niobate and KTN, which dominates the technologically relevant r51 Pockels coefficient. Replacing the calculated mode frequency with its measured value provides an experimentally constrained approach that substantially improves the predicted Pockels response. For that purpose, the previously unreported TO Slater-mode frequency of KTN is extracted from far-IR reflectivity measurements. The results emphasize the potential of KTN-based EO modulators as an alternative to standard lithium niobate and BTO technologies, with a potentially lower energy consumption and device footprint.

cond-mat.mtrl-sci↗
arXiv2024

BiFeO$_3$ nanoparticles at low-temperature using atomistic simulations -- surface charge distribution and terminations

This paper analyzes how the ferroelectric properties of cubic-like BiFeO$_3$ nanoparticles are affected by different terminations and charge distributions at the surface using ab-initio-based atomistic computational experiments. Our findings unveil multiple multidomain configurations and illustrate how the different order parameters evolve towards the surface. Interestingly, for neutral terminations, a non-rhombohedral phase of BiFeO$_3$ with a stripe-like polarization arrangement was stabilized. We evaluate the polarization, oxygen octahedra rotation, and volume variation for all the configurations obtained, taking advantage of the atomic-scale details provided by the methods used in this study.

cond-mat.mtrl-sci↗
arXiv2024

Fragmented charged domain wall below the tetragonal-orthorhombic phase transition in BaTiO3

Ferroelectric charged domain walls are known for their high electrical conductivity, making them promising candidates for applications in modern electronics. A remarkably high conductivity and nominal charge density has been found in the head-to-head ferroelastic domain wall of tetragonal barium titanate. Interestingly, the conductivity of this domain wall decreases by several orders of magnitude when the temperature drops down below about 5 degrees Celsius when the tetragonal phase transforms to the orthorhombic one. We thus explored the evolution of the ferroelectric charged domain walls in BaTiO3 crystals while they undergo this phase transition by in-situ optical microscopy. Our results reveal that, below the phase transition, the domains adjacent to charge domain walls become twinned and the head-to-head charged domain wall transforms into a superdomain wall, which is broken into alternating micron-scale segments with and without the excess bound charge. These observations naturally explains the observed loss of the domain wall conductivity below the phase transition because the macroscopic conductive channel along such fragmented superdomain wall is disrupted.

cond-mat.mtrl-sci↗
arXiv2021

Origin of relaxor behavior in barium-titanate based lead-free perovskites

It is well known that disordered relaxor ferroelectrics exhibit local polar correlations. The origin of localized fields that disrupt long range polar order for different substitution types, however, is unclear. Currently, it is known that substituents of the same valence as Ti4+ at the B-site of barium titanate lattice produce random disruption of Ti-O-Ti chains that induces relaxor behavior. On the other hand, investigating lattice disruption and relaxor behavior resulting from substituents of different valence at the B-site is more complex due to the simultaneous occurrence of charge imbalances and displacements of the substituent cation. The existence of an effective charge mediated mechanism for relaxor behavior appearing at low (< 10%) substituent contents in heterovalent modified barium titanate ceramics is presented in this work. These results will add credits to the current understanding of relaxor behavior in chemically modified ferroelectric materials and also acknowledge the critical role of defects (such as cation vacancies) in lattice disruption, paving the way for chemistry-based materials design in the field of dielectric and energy storage applications.

cond-mat.mtrl-sci↗
arXiv2021

Raman spectra of fine-grained materials from first principles

Raman spectroscopy is an advantageous method for studying the local structure of materials, but the interpretation of measured spectra is complicated by the presence of oblique phonons in polycrystals of polar materials. Whilst group theory considerations and standard ab initio calculations are helpful, they are often valid only for single crystals. In this paper, we introduce a method for computing Raman spectra of polycrystalline materials from first principles. We start from the standard approach based on the (Placzek) rotation invariants of the Raman tensors and extend it to include the effect of the coupling between the lattice vibrations and the induced electric field, and the electro-optic contribution, relevant for polar materials like ferroelectrics. As exemplified by applying the method to rhombohedral BaTiO3, AlN, and LiNbO3, such an extension brings the simulated Raman spectrum to a much better correspondence with the experimental one. Additional advantages of the method are that it is general, permits automation, and thus can be used in high-throughput fashion.

cond-mat.mtrl-sci↗
arXiv2018

Pinning of Ferroelectric Bloch Wall at a Paraelectric Layer

Phase-field simulations of domain walls between antiparallel ferroelectric domains in BaTiO3 - SrTiO3 crystalline superlattices suggest that a paraelectric layer with a thickness comparable to the thickness of the domain wall itself can act as an efficient pinning layer. Moreover, such layer is capable to unwind the characteristic structure of a ferroelectric Bloch wall passing through it.

cond-mat.mes-hall↗
arXiv2012

Bloch-type Domain Walls in Rhombohedral BaTiO3

Ferroelectric domain walls (FDWs) are usually considered to be of Ising type, but there have been suggestions in recent years that Bloch-type FDWs are also possible in some cases, e.g., in the rhombohedral phase of BaTiO3. The mechanically compatible and electrically neutral FDWs in rhombohedral BaTiO3 are of 71-degree, 109-degree, and 180-degree type. We have investigated these FDWs based both on first-principles calculations and on a Ginzburg-Landau-Devonshire (GLD) model [P. Marton, I. Rychetsky, and J. Hlinka, Phys. Rev. B 81, 144125 (2010)]. The results from both approaches confirm the Ising nature of the 71-degree FDW and the Bloch nature of the 180-degree FDW, and predict both Ising-type and Bloch-type FDWs are possible for the 109-degree case. Considering the relatively small rhombohedral strain in BaTiO3, the competition between the energies of Bloch and Ising FDWs can be discussed in terms of a picture in which a Bloch wall is regarded as being composed of a pair of smaller-angle Ising ones. A reduction by 40% in the parameters describing the gradient term in the GLD model brings it into better agreement with the first-principles results for detailed properties such as the energies and widths of the FDWs.

cond-mat.mtrl-sci↗