arXiv subjects

Seongjoo Jung

Publications and source records attributed to Seongjoo Jung.

3 recordsLinked to original sources

arXiv2026

Ferroic Polarization from Nonpolar Phonons

Born effective charge, a fundamental quantity in lattice dynamics and ferroelectrics, provides a quantitative measure of linear polarization response to ionic displacements. However, it does not account for higher-order effects, which can play a significant role in certain materials, such as fluorite HfO$_2$. In this letter, we use the second-order mode effective charges defined with the second-order atomic dynamical charges as a measure of the dipole moments generated by nonpolar lattice distortions. Using first-principles calculations, we demonstrate that specific combinations of nonpolar phonons in many oxides can induce strongly aligned second-order polarizations, reaching magnitudes comparable to those of intrinsically polar modes even in the zero frequency limit, broadening the understanding of second-order effects, which have historically been emphasized for their dynamical effects at specific frequency ranges. Through a symmetry-based analysis of the charge density, we elucidate the microscopic origin of these effects, tracing them to variations in bond covalency and local electronic rearrangements. We also demonstrate large second-order mode effective charge in well-studied perovskites, highlighting the generality of these phenomena. Our results offer new insights into the design principles of next-generation ferroelectric, piezoelectric and multifunctional materials from the higher-order contribution to polarization in crystalline solids.

cond-mat.mtrl-sci↗

arXiv2026

Triggered ferroelectricity in HfO$_2$ from hybrid phonons and higher-order dynamical charges

Ferroelectric HfO$_2$ has emerged as a highly promising material for high-density nonvolatile memory and nanoscale transistor applications. However, the uncertain origin of polarization in HfO$_2$ limits our ability to fully understand and control its ferroelectricity. Ferroelectricity, the emergence of a spontaneous and switchable polarization in solids, is conventionally understood to be governed by unstable structural modes (phonons), arising either directly from an unstable polar phonon or indirectly through coupling of unstable nonpolar phonons with a polar mode. While these 'proper' and 'improper' mechanisms successfully explain ferroelectricity for most systems, they do not encompass all possible phenomena. Here, we present a novel mechanism of 'hybrid-triggered' ferroelectricity, where a polar order emerges through trilinear coupling without any structural instabilities. Our group theoretical analysis starting from a high-symmetry reference structure shows that this mechanism is realized in intensely-debated ferroelectric HfO$_2$, along with quantitative confirmation from first-principles calculations. We also show that dynamical charges in this material are highly unconventional, and a significant contribution to the total polarization arises solely from high-order couplings of nonpolar phonons. These findings underline that even simple crystal structures can host surprisingly complicated interplay between different structural orders, elucidate the origin of ferroelectricity and antiferroelectricity in fluorite-related structures, and provide foundational understanding for designing superior ferroelectric materials.

cond-mat.mtrl-sci↗

arXiv2024

Octahedral Rotation Induced, Antiferroelectric-like Double Hysteresis in Strained Perovskites

Antiferroelectrics, which host both polar and antipolar order parameters, are characterized by the double hysteresis loops which are advantageous for various applications such as high-density energy storage. In this study, we investigate the coupling between oxygen octahedral rotations and polarization in well-known perovskites, with a focus on SrTiO$_3$. Using first-principles calculations and symmetry-adapted Landau-Ginzburg-Devonshire theory, we construct an energy landscape to analyze how this coupling shapes polarization-voltage hysteresis behavior. We show that tuning the relative strength of polar and rotational instabilities by exploiting epitaxial strain and layering leads to nontrivial hysteresis behavior. Consequently, the rotation coupling with polarization leads to an expanded search space of materials exhibiting antiferroelectric-like double hysteresis.

cond-mat.mtrl-sci↗