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Sankalpa Hazra

Publications and source records attributed to Sankalpa Hazra.

9 recordsLinked to original sources

Strain-Induced Relaxor Multiferroicity at Room Temperature in Hexaferrite BaFe12O19 Thin Films

Multiferroic materials that combine magnetic and electric order at room temperature are rare. Here, we demonstrate strain-induced room-temperature polar order in the ferrimagnetic hexaferrite BaFe12O19. First-principles calculations reveal a strain-tunable energy landscape with multiple competing dipolar configurations and predict that compressive strain favors polar distortions. Using an isostructural Sr1.03Ga10.81Mg0.58Zr0.58O19 substrate, we grow coherently strained BaFe12O19 films with 1.1% in-plane biaxial compression. Second-harmonic generation measurements demonstrate inversion-symmetry breaking and establish a strain-stabilized polar phase that persists to at least 1000 K. Multislice electron ptychography directly reveals enhanced off-centering of Fe3+ ions within the trigonal-bipyramidal sites of the strained films and spatially varying local polarization, demonstrating the formation of polar nanoregions. Path-integral Monte Carlo simulations further show that compressive strain suppresses quantum fluctuations and stabilizes these local polar distortions. Together, these results establish strain-engineered BaFe12O19 as a room-temperature relaxor multiferroic, in which robust ferrimagnetism coexists with nanoscale polar order. Our work demonstrates a route for transforming an incipient ferroelectric ferrimagnetic into a polar magnetic material through epitaxial strain.

cond-mat.mtrl-sci↗

Quantum Saturation of the Electro-Optic Effect

Future quantum computing architectures require electro-optic materials that maintain a strong, stable performance at cryogenic temperatures. In conventional electro-optic materials, large electro-optic coefficients are often confined to narrow temperature windows near structural phase transitions, where small changes in temperature lead to large changes in the electro-optic response. Using thermodynamic analysis, phase-field simulations, experimental growth and cryogenic optical measurements we show that quantum fluctuations can be harnessed to overcome this trade-off. By tuning the ferroelectric phase boundaries down to 0 K, quantum fluctuations induce a saturation regime in which a large electro-optic response becomes nearly temperature-independent below 25 K. We demonstrate that the phase boundaries can be tuned through either strain in BaTiO3 or through chemical composition in Ba1-xCaxTiO3, leading to a large, temperature insensitive, cryogenic electro-optic effect comparable to bulk BaTiO3 at room temperature; the performance exceeds BaTiO3-on-Si by over an order of magnitude. These findings establish a general design principle for engineering high-performance electro-optic materials for cryogenic applications.

cond-mat.mtrl-sci↗

Above Room Temperature Ferroelectricity in Epitaxially Strained KTaO3

Epitaxial strain is a powerful means to engineer emergent phenomena in thin films and heterostructures. Here, we demonstrate that KTaO3, a cubic perovskite in bulk form, can be epitaxially strained into a highly tunable ferroelectric. KTaO3 films grown commensurate to SrTiO3 (001) substrates experience an in-plane strain of -2.1 % that transforms the cubic structure into a tetragonal polar phase with transition temperature of 475 K, consistent with our thermodynamic calculations. We show that the Curie temperature and the spontaneous electric polarization can be system- atically controlled with epitaxial strain. Scanning transmission electron microscopy reveals cooperative polar displacements of the potassium columns with respect to the neighboring tantalum columns at room temperature. Optical second-harmonic generation results are described by a tetragonal polar point group (4mm), indicating the emergence of a global polar ground state. We observe a ferroelectric hysteresis response, using metal-insulator-metal capacitor test structures. The results demon- strate a robust intrinsic ferroelectric state in epitaxially strained KTaO3 thin films.

cond-mat.mtrl-sci↗

Colossal Cryogenic Electro-Optic Response Through Metastability in Strained BaTiO$_{3}$ Thin Films

The search for thin film electro-optic (EO) materials that can retain superior performance under cryogenic conditions has become critical for quantum computing. Barium titanate thin films show large linear EO coefficients in the tetragonal phase at room temperature, which is severely degraded down to ~200 pm V$^{-1}$ in the rhombohedral phase at cryogenic temperatures. There is immense interest in manipulating these phase transformations and retaining superior EO properties down to liquid helium temperature. Utilizing the thermodynamic theory of optical properties, a large low-temperature EO response is designed by engineering the energetic competition between different ferroelectric phases, leading to a low-symmetry monoclinic phase with a massive EO response. The existence of this phase is demonstrated in a strain-tuned BaTiO$_{3}$ thin film that exhibits a linear EO coefficient of 2516 +/- 100 pm V$^{-1}$ at 5 K, which is an order of magnitude higher than the best reported performance thus far. Importantly, the EO coefficient increases by 100x during cooling, unlike the conventional films, where it degrades. Further, at the lowest temperature, significant higher order EO responses also emerge. These results represent a new framework for designing materials with property enhancements by stabilizing highly tunable metastable phases with strain. Copyright 2025 The Author(s). Advanced Materials published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. (A. Suceava, S. Hazra, A. Ross, et al. "Colossal Cryogenic Electro-Optic Response Through Metastability in Strained BaTiO3 Thin Films." Adv. Mater. (2025): e07564. https://doi.org/10.1002/adma.202507564)

cond-mat.mtrl-sci↗

Quantitative Nonlinear Optical Polarimetry with High Spatial Resolution

Nonlinear optical microscopy such as in the optical second-harmonic generation (SHG) modality has become a popular tool today for probing materials in the physical and biological sciences. While imaging and spectroscopy are widely used in the microscopy mode, nonlinear polarimetry, which can shed light on materials' symmetry and microstructure, is relatively underdeveloped. This is partly because quantitative analytical modeling of the optical SHG response for anisotropic crystals and films largely assumes low-numerical aperture (NA) focusing of light, where the plane-wave approximation is sufficient. Tight focusing provides unique benefits in revealing out-of-plane polarization responses, which cannot be detected by near-plane-wave illumination at normal incidence. Here, we outline a method for quantitatively analyzing SHG polarimetry measurements obtained under high-NA focusing within a microscope geometry. Experiments and simulations of a variety of standard samples, from single crystals to thin films, are in good agreement, including measured and simulated spatial SHG maps of ferroelectric domains. A solution to the inverse problem is demonstrated, where the spatial distribution of an SHG tensor with unknown tensor coefficient magnitudes is determined by experimentally measured polarimetry. The ability to extract the out-of-plane component of the nonlinear polarization in normal incidence is demonstrated, which can be valuable for high-resolution polarimetry of 2D materials, thin films, heterostructures, and uniaxial crystals with a strong out-of-plane response. Copyright 2025 Optica Publishing Group. Users may use, reuse, and build upon the article, or use the article for text or data mining, so long as such uses are for non-commercial purposes and appropriate attribution is maintained. All other rights are reserved. https://doi.org/10.1364/OPTICA.559060

cond-mat.mtrl-sci↗

Improper Ferroelectricity at the Monolayer Limit

Ultrathin ferroelectric films with out-of-plane polarization and high Curie temperatures are key to miniaturizing electronic devices. Most ferroelectrics employed in devices are proper ferroelectrics, where spontaneous polarization is the primary order parameter. Unfortunately, the Curie temperature of proper ferroelectrics is drastically reduced as the ferroelectric becomes thin; nearly all proper ferroelectrics need to be thicker than several unit cells. The absence of an ultrathin limit has been predicted, but not verified for improper ferroelectrics. These are ferroelectrics where the polarization emerges secondary to the primary order parameter, such as a structural distortion. Here we report improper ferroelectricity with an undiminished Curie temperature in a 0.75-unit-cell-thick hexagonal LuFeO3 (h-LuFeO3) film grown on a SrCo2Ru4O11 bottom electrode with an atomically engineered monolayer bridging layer. Our results demonstrate the absence of a critical thickness for improper ferroelectricity and provide a methodology for creating ultrathin improper ferroelectrics by stabilizing their primary order parameters.

cond-mat.mtrl-sci↗

Peculiar magnetic and magneto-transport properties in a non-centrosymmetric self-intercalated van der Waals ferromagnet Cr5Te8

Trigonal Cr$_5$Te$_8$, a self-intercalated van der Waals ferromagnet with an out-of-plane magnetic anisotropy, has long been known to crystallize in a centrosymmetric structure. However, optical second harmonic generation experiments, together with comprehensive structural analysis, indicate that this compound rather adopts a non-centrosymmetric structure. Lorentz transmission electron microscopy reveals the presence of Néel-type skyrmions, consistent with its non-centrosymmetric structure. A large anomalous Hall conductivity of 102 ohm$^{-1}$cm$^{-1}$ at low temperature stems from intrinsic origin, which is larger than any previously reported values in the bulk Cr-Te system. Notably, spontaneous topological Hall resistivity arising from the skyrmionic phase has been observed. Our findings not only elucidate the unique magnetic and magneto-transport properties of non-centrosymmetric trigonal Cr$_5$Te$_8$, but also open new avenues for investigating the effects of broken inversion symmetry on material properties and their potential applications.

cond-mat.mtrl-sci↗

Quantum fluctuations lead to glassy electron dynamics in the good metal regime of electron doped KTaO3

One of the central challenges in condensed matter physics is to comprehend systems that have strong disorder and strong interactions. In the strongly localized regime, their subtle competition leads to glassy electron dynamics which ceases to exist well before the insulator-to-metal transition is approached as a function of doping. Here, we report on the discovery of glassy electron dynamics deep inside the good metal regime of an electron-doped quantum paraelectric system: KTaO$_3$. We reveal that upon excitation of electrons from defect states to the conduction band, the excess injected carriers in the conduction band relax in a stretched exponential manner with a large relaxation time, and the system evinces simple aging phenomena - a telltale sign of glassy dynamics. Most significantly, we observe a critical slowing down of carrier dynamics below 35 K, concomitant with the onset of quantum paraelectricity in the undoped KTaO$_3$. Our combined investigation using second harmonic generation technique, density functional theory and phenomenological modeling demonstrates quantum fluctuation-stabilized soft polar modes as the impetus for the glassy behavior. This study addresses one of the most fundamental questions regarding the potential promotion of glassiness by quantum fluctuations and opens a route for exploring glassy dynamics of electrons in a well-delocalized regime.

cond-mat.str-el↗

Electron trapping and detrapping in an oxide two-dimensional electron gas: The role of ferroelastic twin walls

The choice of electrostatic gating over the conventional chemical doping for phase engineering of quantum materials is attributed to the fact that the former can reversibly tune the carrier density without affecting the system's level of disorder. However, this proposition seems to break down in field-effect transistors involving SrTiO$_3$ (STO) based two-dimensional electron gases. Such peculiar behavior is associated with the electron trapping under an external electric field. However, the microscopic nature of trapping centers remains an open question. In this paper, we investigate electric field-induced charge trapping/detrapping phenomena at the conducting interface between band insulators $γ$-Al$_2$O$_3$ and STO. Our transport measurements reveal that the charge trapping under +ve back gate voltage ($V_g$) above the tetragonal to cubic structural transition temperature ($T_c$) of STO is contributed by the electric field-assisted thermal escape of electrons from the quantum well, and the clustering of oxygen vacancies (OVs) as well. We observe an additional source of trapping below the $T_c$, which arises from the trapping of free carriers at the ferroelastic twin walls of STO. Application of -ve $V_g$ results in a charge detrapping, which vanishes above $T_c$ also. This feature demonstrates the crucial role of structural domain walls in the electrical transport properties of STO based heterostructures. The number of trapped (detrapped) charges at (from) the twin wall is controlled by the net polarity of the wall and is completely reversible with the sweep of $V_g$.

cond-mat.mes-hall↗