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  1. Persistent structural distortion for anticipated improper ferroelectricity in ultrathin h-Lu1−xCaxMnO3 films

    Improper ferroelectricity in hexagonal rare-earth manganites (h-RMnO3, R = Ho–Lu, Y, Sc) arises from a geometric distortion as the primary order parameter, resilient to depolarizing fields and promising for ultrathin ferroelectric devices. However, the substrate-induced interface clamping effect, which suppresses the geometric distortion in the sub-nanometer regime, has thus far hindered the realization of two-dimensional improper ferroelectrics. This study demonstrates that doping with calcium can enhance ferroelectric structural distortion in h-LuMnO3 thin films. Compressively strained h-Lu1−xCaxMnO3 (x = 0.1, 0.2, 0.3, 0.4, 0.5) epitaxial thin films were stabilized on sapphire substrates using an h-ScFeO3 buffer layer. We have found thatmore » the interface clamping effect is entirely overcome when the doping concentration reaches x ⩾ 0.2, establishing a potential quasi-2D ferroelectric system with a remarkably high estimated structural transition temperature of larger than 1200 K inferred indirectly from temperature-resolved reflection high-energy electron diffraction. This finding suggests a general strain engineering strategy to enhance improper ferroelectricity in hexagonal manganites.« less
  2. Enhanced magnetic and optical properties of Y3Fe5O12 (YIG) films with Au nanoinclusions

    Y3Fe5O12 (YIG) thin films are well known for their ferrimagnetic insulating property and low Gilbert damping coefficient (α), allowing them to be used for various spintronic applications and as magneto-optical isolators for photonic devices. Instead of doping, incorporation of plasmonic metals as nanoinclusions could be a promising route for improved magneto-optical coupling properties. In this work, YIG–Au nanocomposites have been deposited with ferrimagnetic insulating YIG as the matrix and Au nanoinclusions which introduce plasmonic absorption, optical anisotropy, and hyperbolic properties. Films with varying Au nanoinclusion densities have been processed and annealed to compare with the as-deposited ones. The films thatmore » had low Au nanoinclusion density and were annealed presented a lower magnetic damping coefficient of 2.84 × 10−4 than the pure YIG film (9.66 × 10−4). The as-deposited film with the highest Au density shows the strongest hyperbolic properties among all samples. These results demonstrate that both magnetic damping and optical properties can be tuned through deposition conditions in YIG–Au nanocomposite thin films, allowing for a balance of both properties. This YIG–Au nanocomposite system presents promising potential in next-generation opto-spintronic devices.« less
  3. Future of condensed matter physics for the next 10 years

    This perspective outlines a selection of research directions that members of the JPCM editorial board anticipate may shape the frontier of condensed matter physics over the next decade. Rather than a comprehensive review or formal roadmap, this perspective reflects a set of informed views drawn from diverse areas of expertise. Our intention is to spark curiosity, provoke discussion, and encourage readers to imagine—and pursue—the exciting possibilities that lie ahead.
  4. Dual Mechanism for Transient Capacitance Anomaly in Improper Ferroelectrics

    Negative capacitance (NC) effects in ferroelectrics can potentially break fundamental limits of power dissipation known as “Boltzmann tyranny.” However, the origin of transient NC of ferroelectrics, which is attributed to two different mechanisms involving free-energy landscape and nucleation, is under intense debate. Here, we report the coexistence of transient NC and an S-shaped anomaly during the switching of ferroelectric hexagonal ferrites capacitor in an RC circuit. The early-stage NC arises from the nucleation process, while the late-stage S-shaped anomaly corresponds to a nascent NC associated with the free-energy landscape. The entire waveform can be reproduced using a hybrid model thatmore » simultaneously incorporates these two mechanisms. These results highlight the multivariable free-energy landscape of hexagonal ferrites that enables an abrupt change of the internal field and demonstrate that the two mechanisms are not mutually exclusive, resolving the long-standing debate. In conclusion, the behavior of the S-shaped anomaly also provides a pathway to extract parameters of free-energy landscape and switching dynamics.« less
  5. Microstructural Underpinnings of Giant Intrinsic Exchange Bias in Epitaxial NiCo2O4 Thin Films

    Understanding intrinsic exchange bias in nominally single-component ferromagnetic or ferrimagnetic materials is crucial for simplifying related device architectures. However, the mechanisms behind this phenomenon and its tunability remain elusive, which hinders the efforts to achieve unidirectional magnetization for widespread applications. Inspired by the high tunability of ferrimagnetic inverse spinel NiCo2O4, the origin of intrinsic exchange bias in NiCo2O4 (111) films deposited on Al2O3 (0001) substrates are investigated. The comprehensive characterizations, including electron diffraction, X-ray reflectometry and spectroscopy, and polarized neutron reflectometry, reveal that intrinsic exchange bias in NiCo2O4 (111)/Al2O3 (0001) arises from a reconstructed antiferromagnetic rock-salt NixCo1-xO layer at themore » interface between the film and the substrate due to a significant structural mismatch. Remarkably, by engineering the interfacial structure under optimal growth conditions, it can achieve exchange bias larger than coercivity, leading to unidirectional magnetization. Such giant intrinsic exchange bias can be utilized for realistic device applications. This work establishes a new material platform based on NiCo2O4, an emergent spintronics material, to study tunable interfacial magnetic and spintronic properties.« less
  6. Intrinsic exchange bias from interfacial reconstruction in an epitaxial NixCoyFe3–xyO4(111)/α-Al2O3(0001) thin film family

    Intrinsic exchange bias is known as the unidirectional exchange anisotropy that emerges in a nominally single-component ferro-(ferri-)magnetic system. In this work, with magnetic and structural characterizations, we demonstrate that intrinsic exchange bias is a general phenomenon in (Ni, Co, Fe)-based spinel oxide films deposited on α-Al2O3(0001) substrates, due to the emergence of a rock-salt interfacial layer consisting of antiferromagnetic CoO from interfacial reconstruction. We show that in NixCoyFe3–x–yO4(111)/α-Al2O3(0001) films, intrinsic exchange bias and interfacial reconstruction have consistent dependences on Co concentration y, while the Ni and Fe concentration appears to be less important. This work establishes a family of intrinsicmore » exchange bias materials with great tunability by stoichiometry and highlights the strategy of interface engineering in controlling material functionalities.« less
  7. Spherulite-enhanced macroscopic polarization in molecular ferroelectric films from vacuum deposition

    Proton-transfer type molecular ferroelectrics hold significant promise for practical application due to their large spontaneous polarizations, high Curie temperatures, and small switching fields. However, it remains puzzling that preparation of quasi-2D films exhibiting macroscopic ferroelectric behaviors has been reported in only few molecular ferroelectrics. To address this puzzle, we studied the impact of microstructures on the macroscopic ferroelectric properties of 5,6-dichloro-2-methylbenzimidazole (DC-MBI) films grown using the low-temperature deposition followed by the restrained crystallization (LDRC) method. Our findings revealed a competition between dense spherulites and porous microstructures containing randomly oriented nanograins in the as-grown films. Post-growth annealing at moderate temperature promotesmore » the formation of spherulites, leading to macroscopic ferroelectric polarization switching. These results underscore the critical role of microstructure density in determining macroscopic ferroelectric properties, potentially resolving the puzzle for the absence of such behavior in many molecular ferroelectric films. Here, we anticipate that the approach proposed in this study to enhance microstructure density will significantly advance the fabrication of quasi-2D molecular ferroelectric films and unlock their potential in device applications.« less
  8. Hydrogen-induced tunable remanent polarization in a perovskite nickelate

    Materials with field-tunable polarization are of broad interest to condensed matter sciences and solid-state device technologies. Here, using hydrogen (H) donor doping, we modify the room temperature metallic phase of a perovskite nickelate NdNiO3 into an insulating phase with both metastable dipolar polarization and space-charge polarization. We then demonstrate transient negative differential capacitance in thin film capacitors. The space-charge polarization caused by long-range movement and trapping of protons dominates when the electric field exceeds the threshold value. First-principles calculations suggest the polarization originates from the polar structure created by H doping. We find that polarization decays within ~1 second whichmore » is an interesting temporal regime for neuromorphic computing hardware design, and we implement the transient characteristics in a neural network to demonstrate unsupervised learning. These discoveries open new avenues for designing ferroelectric materials and electrets using light-ion doping.« less
  9. Giant interfacial spin Hall angle from Rashba-Edelstein effect revealed by the spin Hall Hanle process

    The Rashba-Edelstein effect (REE), which generates interfacial spin polarization and subsequent spin current, is a compelling spin-charge conversion mechanism for spintronic applications, since it’s not limited by the elemental spin-orbit couplings. In this work we demonstrate REE at Pt/ferroelectric interfaces by showing a positive correlation between polarization and effective spin Hall angle in the recently elucidated spin Hall Hanle effects (SHHE), in which a Larmor precession of spin polarization in a diffusion process from the interface manifest as magnetoresistance and Hall effect. We show that REE leads to a large enhancement of the effective spin Hall angle of ferroelectric interfacemore » Pt/h-LuFeO3 compared with that of Pt/Al2O3, without obvious differences in the spin relaxation time. Modeling using SHHEs involving REE as an additional source of interfacial polarization suggests that REE can lead to an interfacial spin Hall angle (0.4 ± 0.1) in Pt/h-LuFeO3 that is one order of magnitude larger than the bulk value of Pt. Our results demonstrate that a ferroelectric interface can produce large spin-charge conversion and that SHHEs are a sensitive tool for characterizing interfacial spin-transport properties.« less
  10. Pressure-induced charge orders and their postulated coupling to magnetism in hexagonal multiferroic LuFe2O4

    Hexagonal LuFe2O4 is a promising charge order (CO) driven multiferroic material with high charge and spin-ordering temperatures. The coexisting charge and spin orders on Fe3+/Fe2+ sites result in magnetoelectric behaviors, but the coupling mechanism between the charge and spin orders remains elusive. Here, by tuning external pressure, we reveal three charge-ordered phases with suggested correlation to magnetic orders in LuFe2O4: (i) a centrosymmetric incommensurate three-dimensional CO with ferrimagnetism, (ii) a non-centrosymmetric incommensurate quasi-two-dimensional CO with ferrimagnetism, and (iii) a centrosymmetric commensurate CO with antiferromagnetism. Experimental in situ single-crystal X-ray diffraction and X-ray magnetic circular dichroism measurements combined with density functionalmore » theory calculations suggest that the charge density redistribution caused by pressure-induced compression in the frustrated double-layer [Fe2O4] cluster is responsible for the correlated spin-charge phase transitions. The pressure-enhanced effective Coulomb interactions among Fe-Fe bonds drive the frustrated (1/3, 1/3) CO to a less frustrated (1/4, 1/4) CO, which induces the ferrimagnetic to antiferromagnetic transition. Our results not only elucidate the coupling mechanism among charge, spin, and lattice degrees of freedom in LuFe2O4, but also provide a new way to tune the spin-charge orders in a highly controlled manner.« less
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