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The anomalous Hall effect (AHE), a hallmark of time-reversal symmetry breaking, has been reported in rutile RuO2, a debated metallic altermagnetic candidate. Previously, AHE in RuO2 was observed only in strain-relaxed thick films under extremely high magnetic fields (~50 T). Yet, in ultrathin strained films with distinctive anisotropic electronic structures, there are no reports, likely due to disorder and defects suppressing metallicity thus hindering its detection. Here, we demonstrate that ultrathin, fully-strained 2 nm TiO2/t nm RuO2/TiO2 (110) heterostructures, grown by hybrid molecular beam epitaxy, retain metallicity and exhibit a sizeable AHE at a significantly lower magnetic field (< 9 T). Density functional theory calculations reveal that epitaxial strain stabilizes a non-compensated magnetic ground state and reconfigures magnetic ordering in RuO2 (110) thin films. These findings establish ultrathin RuO2 as a platform for strain-engineered magnetism and underscore the transformative potential of epitaxial design in advancing spintronic technologies., Comment: 23 pages

Magnetic anisotropy in atomically thin correlated heterostructures is essential for exploring quantum magnetic phases for next-generation spintronics. Whereas previous studies have mostly focused on van der Waals systems, here, we investigate the impact of dimensionality of epitaxially-grown correlated oxides down to the monolayer limit on structural, magnetic, and orbital anisotropies. By designing oxide superlattices with a correlated ferromagnetic SrRuO3 and nonmagnetic SrTiO3 layers, we observed modulated ferromagnetic behavior with the change of the SrRuO3 thickness. Especially, for three-unit-cell-thick layers, we observe a significant 1,500% improvement of coercive field in the anomalous Hall effect, which cannot be solely attributed to the dimensional crossover in ferromagnetism. The atomic-scale heterostructures further reveal the systematic modulation of anisotropy for the lattice structure and orbital hybridization, explaining the enhanced magnetic anisotropy. Our findings provide valuable insights into engineering the anisotropic hybridization of synthetic magnetic crystals, offering a tunable spin order for various applications., Comment: 23 pages

Altermagnetism refers to a wide class of compensated magnetic orders featuring magnetic sublattices with opposite spins related by rotational symmetry rather than inversion or translational operations, resulting in non-trivial spin splitting and high-order multipolar orders. Here, by combining theoretical analysis, electrical transport, X-ray and optical spectroscopies, and nonlinear optical measurements, we establish a phase diagram in hybrid molecular beam epitaxy-grown RuO2/TiO2 (110) films, mapping the broken symmetries along the altermagnetic/electronic/structural phase transitions as functions of film thickness and temperature. This phase diagram features a novel altermagnetic metallic polar phase in strained 2 nm samples, extending the concept of multiferroics to altermagnetic systems. These results provide a comprehensive understanding of altermagnetism upon epitaxial heterostructure design for emergent novel phases with multifunctionalities., Comment: 15 pages

This paper presents design techniques for an energy-efficient multi-lane receiver (RX) with baud-rate clock and data recovery (CDR), which is essential for high-throughput low-latency communication in high-performance computing systems. The proposed low-power global clock distribution not only significantly reduces power consumption across multi-lane RXs but is capable of compensating for the frequency offset without any phase interpolators. To this end, a fractional divider controlled by CDR is placed close to the global phase locked loop. Moreover, in order to address the sub-optimal lock point of conventional baud-rate phase detectors, the proposed CDR employs a background eye-climbing algorithm, which optimizes the sampling phase and maximizes the vertical eye margin (VEM). Fabricated in a 28nm CMOS process, the proposed 4x32Gb/s RX shows a low integrated fractional spur of -40.4dBc at a 2500ppm frequency offset. Furthermore, it improves bit-error-rate performance by increasing the VEM by 17%. The entire RX achieves the energy efficiency of 1.8pJ/bit with the aggregate data rate of 128Gb/s.

This paper presents an I/O interface with Xtalk Minimizing Affine Signaling (XMAS), which is designed to support high-speed data transmission in die-to-die communication over silicon interposers or similar high-density interconnects susceptible to crosstalk. The operating principles of XMAS are elucidated through rigorous analyses, and its advantages over existing signaling are validated through numerical experiments. XMAS not only demonstrates exceptional crosstalk removing capabilities but also exhibits robustness against noise, especially simultaneous switching noise. Fabricated in a 28-nm CMOS process, the prototype XMAS transceiver achieves an edge density of 3.6TB/s/mm and an energy efficiency of 0.65pJ/b. Compared to the single-ended signaling, the crosstalk-induced peak-to-peak jitter of the received eye with XMAS is reduced by 75% at 10GS/s/pin data rate, and the horizontal eye opening extends to 0.2UI at a bit error rate < 10$^{-12}$.

Graphene, with spin and valley degrees of freedom, fosters unexpected physical and chemical properties for the realization of next-generation quantum devices. However, the spin symmetry of graphene is rather robustly protected, hampering manipulation of the spin degrees of freedom for the application of spintronic devices such as electric gate tunable spin filters. We demonstrate that a hybrid heterostructure composed of graphene and LaCoO3 epitaxial thin film exhibits an electrically tunable spin exchange splitting. The large and adjustable spin exchange splitting of 155.9 - 306.5 meV was obtained by the characteristic shifts in both the spin symmetry broken quantum Hall states and the Shubnikov-de-Haas oscillations. Strong hybridization induced charge transfer across the hybrid heterointerface has been identified for the observed spin exchange splitting. The substantial and facile controllability of the spin exchange splitting provides an opportunity for spintronics applications with the electrically-tunable spin polarization in hybrid heterostructures., Comment: 20 pages, 5 figures, 1 table

This paper presents Flash, an optimized private inference (PI) hybrid protocol utilizing both homomorphic encryption (HE) and secure two-party computation (2PC), which can reduce the end-to-end PI latency for deep CNN models less than 1 minute with CPU. To this end, first, Flash proposes a low-latency convolution algorithm built upon a fast slot rotation operation and a novel data encoding scheme, which results in 4-94x performance gain over the state-of-the-art. Second, to minimize the communication cost introduced by the standard nonlinear activation function ReLU, Flash replaces the entire ReLUs with the polynomial $x^2+x$ and trains deep CNN models with the new training strategy. The trained models improve the inference accuracy for CIFAR-10/100 and TinyImageNet by 16% on average (up to 40% for ResNet-32) compared to prior art. Last, Flash proposes an efficient 2PC-based $x^2+x$ evaluation protocol that does not require any offline communication and that reduces the total communication cost to process the activation layer by 84-196x over the state-of-the-art. As a result, the end-to-end PI latency of Flash implemented on CPU is 0.02 minute for CIFAR-100 and 0.57 minute for TinyImageNet classification, while the total data communication is 0.07GB for CIFAR-100 and 0.22GB for TinyImageNet. Flash improves the state-of-the-art PI by 16-45x in latency and 84-196x in communication cost. Moreover, even for ImageNet, Flash can deliver the latency less than 1 minute on CPU with the total communication less than 1GB.

4d transition metal perovskite oxides serve as suitable testbeds for the study of strongly correlated metallic properties. Among these, $SrMoO_{3}$ (SMO) exhibits remarkable electrical conductivity at room temperature. The temperature-dependent resistivity $(\rho(T))$ exhibits a Fermi-liquid behavior below the transition temperature $T^{*}$, reflecting the dominant electron-electron interaction. Above $T^{*}$, electron-phonon interaction becomes more appreciable. In this study, we employed the power-law scaling of $\rho(T)$ to rigorously determine the $T^{*}$. We further demonstrate that the $T^{*}$ can be modified substantially by ~40 K in epitaxial thin films. It turns out that the structural quality determines $T^{*}$. Whereas the plasma frequency could be tuned by the change in the electron-electron interaction via the effective mass enhancement, we show that the plasmonic properties are more directly governed by the electron-impurity scattering. The facile control of the electron scattering mechanism through structural quality modulation can be useful for plasmonic sensing applications in the visible region.

Unexpected, yet useful functionalities emerge when two or more materials merge coherently. Artificial oxide superlattices realize atomic and crystal structures that are not available in nature, thus providing controllable correlated quantum phenomena. This review focuses on 4d and 5d oxide superlattices, in which the spin-orbit coupling plays a significant role compared with conventional 3d oxide superlattices. Modulations in crystal structures with octahedral distortion, phonon engineering, electronic structures, spin orderings, and dimensionality control are discussed for 4d oxide superlattices. Atomic and magnetic structures, Jeff = 1/2 pseudospin and charge fluctuations, and the integration of topology and correlation are discussed for 5d oxide superlattices. This review provides insights into how correlated quantum phenomena arise from the deliberate design of superlattice structures that give birth to novel functionalities., Comment: 68 pages

Processing convolution layers remains a huge bottleneck for private deep convolutional neural network (CNN) inference for large datasets. To solve this issue, this paper presents a novel homomorphic convolution algorithm that provides speedup, communication cost, and storage saving. We first note that padded convolution provides the advantage of model storage saving, but it does not support channel packing, thereby increasing the amount of computation and communication. We address this limitation by proposing a novel plaintext multiplication algorithm using the Walsh-Hadamard matrix. Furthermore, we propose the optimization techniques to significantly reduce the latency of the proposed convolution by selecting the optimal encryption parameters and applying lazy reduction. It achieves 1.6-3.8x speedup and reduces the weight storage by 2000-8000x compared to the conventional convolution. When the proposed convolution is employed for CNNs like VGG-16, ResNet-20, and MobileNetV1 on ImageNet, it reduces the end-to-end latency by 1.3-2.6x, the memory usage by 2.1-7.9x and communication cost by 1.7-2.0x compared to conventional method.

The magnetic anisotropy of low-dimensional Mott systems exhibits unexpected magnetotransport behavior useful for spin-based quantum electronics. Yet, the anisotropy of natural materials is inherently determined by the crystal structure, highly limiting its engineering. We demonstrate the magnetic anisotropy modulation near a digitized dimensional Mott boundary in artificial superlattices composed of a correlated magnetic monolayer SrRuO3 and nonmagnetic SrTiO3. The magnetic anisotropy is initially engineered by modulating the interlayer coupling strength between the magnetic monolayers. Interestingly, when the interlayer coupling strength is maximized, a nearly degenerate state is realized, in which the anisotropic magnetotransport is strongly influenced by both the thermal and magnetic energy scales. Our results offer a new digitized control for magnetic anisotropy in low-dimensional Mott systems, inspiring promising integration of Mottronics and spintronics., Comment: 30 pages

With the growing demand for high-bandwidth applications like video streaming and cloud services, the data transfer rates required for wireline communication keeps increasing, making the channel loss a major obstacle in achieving low bit error rate (BER). Equalization techniques such as feed-forward equalizer (FFE) and decision feedback equalizer (DFE) are commonly used to compensate for channel loss in wireline communication, but they have limitations in terms of noise boosting and timing constraints. On the other hand, the forward-backward algorithm can achieve better BER performance, but its high complexity makes it impractical for wireline communication. In this work, we propose a novel neural network, NeuralEQ, that effectively mimics the forward-backward algorithm and performs better than FFE and DFE while reducing complexity of the forward-backward algorithm. Performance of NeuralEQ is verified through simulations using real channels.

Understanding epitaxial strain relaxation is one of the key challenges in functional thin films with strong structure-property relation. Herein, we employ an emerging data analytics approach to quantitatively evaluate the underlying relationships between critical thickness (hc) of strain relaxation and various physical and chemical features, despite the sporadic experimental data points available. First, we have collected and refined reported hc of perovskite oxide thin film/substrate system to construct a consistent sub-dataset which captures a common trend among the varying experimental details. Then, we employ correlation analyses and feature engineering to find the most relevant feature set which include Poisson's ratio and lattice mismatch. With the insight offered by correlation analyses and feature engineering, machine learning (ML) models have been trained to deduce a decent accuracy, which has been further validated experimentally. the demonstrated framework is expected to be efficiently extended to the other classes of thin films in understanding hc., Comment: 24 pages, 5 figures

Atomic-scale precision epitaxy of perovskite oxide superlattices provides unique opportunities for controlling the correlated electronic structures, activating effective control knobs for intriguing functionalities including electromagnetic, thermoelectric, and electrocatalytic behaviors. In this study, we investigated the close interplay between the atomic and electronic structures of correlated superlattices synthesized by atomic-scale precision epitaxy. In particular, we employ superlattices composed of correlated magnetic SrRuO3 (SRO) and quantum paraelectric SrTiO3 (STO) layers. In those superlattices, RuO6 octahedral distortion is systematically controlled from 167 to 175 degrees depending on the thickness of the STO layers, also affecting the TiO6 octahedral distortion within the STO layer. Customized octahedral distortion within SRO/STO superlattices in turn modifies the electronic structures of both the Ti and Ru compounds, observed by X-ray absorption spectroscopy. Our results identify the close correlation between atomic lattice and electronic structures enabled by the facile controllability of atomic-scale epitaxy, which would be useful for designing future correlated oxide devices., Comment: 14 pages

Atomic-scale precision control of magnetic interactions facilitates a synthetic spin order useful for spintronics, including advanced memory and quantum logic devices. Conventional modulation of synthetic spin order has been limited to metallic heterostructures that exploit RKKY interaction through a nonmagnetic metallic spacer; however, they face problems arising from Joule heating and/or electric breakdown. The practical realization and observation of a synthetic spin order across a nonmagnetic insulating spacer would lead to the development of spin-related devices with a completely different concept. Herein, we report the atomic-scale modulation of the synthetic spiral spin order in oxide superlattices composed of ferromagnetic metal and nonmagnetic insulator layers. The atomically controlled superlattice exhibit an oscillatory magnetic behavior, representing the existence of a spiral spin structure. Depth-sensitive polarized neutron reflectometry evidences modulated spiral spin structures as a function of the nonmagnetic insulator layer thickness. Atomic-scale customization of the spin state could lead the field one step further to actual spintronic applications., Comment: 18 pages

Ferromagnetic insulators play a crucial role in the development of low-dissipation quantum magnetic devices for spintronics. Epitaxial LaCoO3 thin film is a prominent ferromagnetic insulator, in which the robust ferromagnetic ordering emerges owing to epitaxial strain. Whereas it is evident that strong spin-lattice coupling induces ferromagnetism, the reported ferromagnetic properties of epitaxially strained LaCoO3 thin films were highly consistent. For example, even under largely modulated degree of strain, the reported Curie temperatures of epitaxially strained LaCoO3 thin films lie within 80-85 K, without much deviation. In this study, substantial enhancement (~18%) in the Curie temperature of epitaxial LaCoO3 thin films is demonstrated via crystallographic orientation dependence. By changing the crystallographic orientation of the films from (111) to (110), the crystal-field energy was reduced and the charge transfer between the Co and O orbitals was enhanced. These modifications led to a considerable enhancement of the ferromagnetic properties (including the Curie temperature and magnetization), despite the identical nominal degree of epitaxial strain. The findings of this study provide insights into facile tunability of ferromagnetic properties via structural symmetry control in LaCoO3., Comment: 17 pages, 4 Figures, 2 Tables

This paper proposes Impala, a new cryptographic protocol for private inference in the client-cloud setting. Impala builds upon recent solutions that combine the complementary strengths of homomorphic encryption (HE) and secure multi-party computation (MPC). A series of protocol optimizations are developed to reduce both communication and performance bottlenecks. First, we remove MPC's overwhelmingly high communication cost from the client by introducing a proxy server and developing a low-overhead key switching technique. Key switching reduces the clients bandwidth by multiple orders of magnitude, however the communication between the proxy and cloud is still excessive. Second, to we develop an optimized garbled circuit that leverages truncated secret shares for faster evaluation and less proxy-cloud communication. Finally, we propose sparse HE convolution to reduce the computational bottleneck of using HE. Compared to the state-of-the-art, these optimizations provide a bandwidth savings of over 3X and speedup of 4X for private deep learning inference.

Increasing demand for larger touch screen panels (TSPs) places more energy burden to mobile systems with conventional sensing methods. To mitigate this problem, taking advantage of the touch event sparsity, this paper proposes a novel TSP readout system that can obtain huge energy saving by turning off the readout circuits when none of the sensors are activated. To this end, a novel ultra-low-power always-on event and region of interest detection based on lightweight compressed sensing is proposed. Exploiting the proposed event detector, the context-aware TSP readout system, which can improve the energy efficiency by up to 42x, is presented., Comment: Accepted in IEEE TCAS-II

Due to the limitations of realizing artificial neural networks on prevalent von Neumann architectures, recent studies have presented neuromorphic systems based on spiking neural networks (SNNs) to reduce power and computational cost. However, conventional analog voltage-domain integrate-and-fire (I&F) neuron circuits, based on either current mirrors or op-amps, pose serious issues such as nonlinearity or high power consumption, thereby degrading either inference accuracy or energy efficiency of the SNN. To achieve excellent energy efficiency and high accuracy simultaneously, this paper presents a low-power highly linear time-domain I&F neuron circuit. Designed and simulated in a 28nm CMOS process, the proposed neuron leads to more than 4.3x lower error rate on the MNIST inference over the conventional current-mirror-based neurons. In addition, the power consumed by the proposed neuron circuit is simulated to be 0.230uW per neuron, which is orders of magnitude lower than the existing voltage-domain neurons., Comment: Accepted in AICAS 2022

Engineering of phonons, i.e., collective lattice vibrations in crystals, is essential for manipulating physical properties of materials such as thermal transport, electron-phonon interaction, confinement of lattice vibration, and optical polarization. Most approaches to phonon-engineering have been largely limited to the high-quality heterostructures of typical semiconductors. Yet, artificial engineering of phonons in a variety of materials with functional properties, such as complex oxides, will yield unprecedented applications of coherent tunable phonons in future quantum acoustic devices. In this study, we demonstrate artificial engineering of phonons in the atomic-scale SrRuO3/SrTiO3 superlattices, wherein tunable phonon modes were observed via confocal Raman spectroscopy. In particular, the coherent superlattices led to the backfolding of acoustic phonon dispersion, resulting in zone-folded acoustic phonons in the THz frequency domain. We could further fine-tune the frequencies from 1 to 2 THz via atomic-scale precision thickness control. In addition, we observed a polar optical phonon originating from the local inversion symmetry breaking in the artificial oxide superlattices, exhibiting emergent functionality. Our approach of atomic-scale heterostructuring of complex oxides will vastly expand material systems for quantum acoustic devices, especially with the viability of functionality integration., Comment: 23 pages

Chiral symmetry breaking of phonons plays an essential role in emergent quantum phenomena owing to its strong coupling to spin degree of freedom. However, direct experimental evidence of the chiral phonon-spin coupling is lacking. In this study, we report a chiral phonon-mediated interlayer exchange interaction in atomically controlled ferromagnetic metal (SrRuO3)-nonmagnetic insulator (SrTiO3) heterostructures. Owing to the unconventional interlayer exchange interaction, we have observed rotation of magnetic moments as a function of nonmagnetic insulating spacer thickness, resulting in a spin spiral state. The chiral phonon-spin coupling is further confirmed by phonon Zeeman effects. The existence of the chiral phonons and their interplay with spins along with our atomic-scale heterostructure approach open a window to unveil the crucial roles of chiral phonons in magnetic materials., Comment: 40 pages

Due to the fundamental limit to reducing power consumption of running deep learning models on von-Neumann architecture, research on neuromorphic computing systems based on low-power spiking neural networks using analog neurons is in the spotlight. In order to integrate a large number of neurons, neurons need to be designed to occupy a small area, but as technology scales down, analog neurons are difficult to scale, and they suffer from reduced voltage headroom/dynamic range and circuit nonlinearities. In light of this, this paper first models the nonlinear behavior of existing current-mirror-based voltage-domain neurons designed in a 28nm process, and show SNN inference accuracy can be severely degraded by the effect of neuron's nonlinearity. Then, to mitigate this problem, we propose a novel neuron, which processes incoming spikes in the time domain and greatly improves the linearity, thereby improving the inference accuracy compared to the existing voltage-domain neuron. Tested on the MNIST dataset, the inference error rate of the proposed neuron differs by less than 0.1% from that of the ideal neuron., Comment: Accepted in ISCAS 2022

Quantum materials (QMs) with strong correlation and non-trivial topology are indispensable to next-generation information and computing technologies. Exploitation of topological band structure is an ideal starting point to realize correlated topological QMs. Herein, we report that strain-induced symmetry modification in correlated oxide SrNbO3 thin films creates an emerging topological band structure. Dirac electrons in strained SrNbO3 films reveal ultra-high mobility (100,000 cm2/Vs), exceptionally small effective mass (0.04me), and non-zero Berry phase. More importantly, strained SrNbO3 films reach the extreme quantum limit, exhibiting a sign of fractional occupation of Landau levels and giant mass enhancement. Our results suggest that symmetry-modified SrNbO3 is a rare example of a correlated topological QM, in which strong correlation of Dirac electrons leads to the realization of fractional occupation of Landau levels., Comment: accepted in Sci. Adv

Atomistic defect engineering through the pulsed laser epitaxy of perovskite transition metal oxides offers facile control of their emergent opto-electromagnetic and energy properties. Among the various perovskite oxides, EuTiO3 exhibits a strong coupling between the lattice, electronic, and magnetic degrees of freedom. This coupling is highly susceptible to atomistic defects. In this study, we investigated the magnetic phase of EuTiO$_3$ epitaxial thin films via systematic defect engineering. A magnetic phase transition from an antiferromagnet to a ferromagnet was observed when the unit cell volume of EuTiO3 expanded due to the introduction of Eu-O vacancies. Optical spectroscopy and density functional theory calculations show that the change in the electronic structure as the ferromagnetic phase emerges can be attributed to the weakened Eu-Ti-Eu super-exchange interaction and the developed ferromagnetic Eu-O-Eu interaction. Facile defect engineering in EuTiO$_3$ thin films facilitates understanding and tailoring of their magnetic ground state.

Stochastic inhomogeneous oxidation is an inherent characteristic of copper (Cu), often hindering color tuning and bandgap engineering of oxides. Coherent control of the interface between metal and metal oxide remains unresolved. We demonstrate coherent propagation of an oxidation front in single-crystal Cu thin film to achieve a full-color spectrum for Cu by precisely controlling its oxide-layer thickness. Grain boundary-free and atomically flat films prepared by atomic-sputtering epitaxy allow tailoring of the oxide layer with an abrupt interface via heat treatment with a suppressed temperature gradient. Color tuning of nearly full-color RGB indices is realized by precise control of oxide-layer thickness; our samples covered ~50.4% of the sRGB color space. The color of copper/copper oxide is realized by the reconstruction of the quantitative yield color from oxide pigment (complex dielectric functions of Cu2O) and light-layer interference (reflectance spectra obtained from the Fresnel equations) to produce structural color. We further demonstrate laser-oxide lithography with micron-scale linewidth and depth through local phase transformation to oxides embedded in the metal, providing spacing necessary for semiconducting transport and optoelectronics functionality., Comment: 38 pages

Thin films of perovskite Ruthenates of the general formula ARuO3 (A = Ca and Sr) are versatile electrical conductors for viable oxide electronics. They are also scientifically intriguing, as they exhibit non-trivial electromagnetic ground states depending on the A-site element. Among them, realization of the cubic perovskite (3C) BaRuO3 thin film has been a challenge so far, because the 3C phase is metastable with the largest formation energy among the various polymorph phases of BaRuO3. In this study, we successfully prepared 3C BaRuO3 thin films employing epitaxial stabilization. The 3C BaRuO3 thin films show itinerant ferromagnetism with a transition temperature of ~48 K and a non-Fermi liquid phase. The epitaxial stabilization of the 3C BaRuO3 further enabled us to make a standard comparison of perovskite Ruthenates thin films, thereby establishing the importance of the Ru-O orbital hybridization in understanding the itinerant magnetic system., Comment: 24 pages

Hexagonal perovskites are an attractive group of materials due to their various polymorph phases and rich structure-property relationships. BaRuO3 (BRO) is a prototypical hexagonal perovskite, in which the electromagnetic properties are significantly modified depending on its atomic structure. Whereas thin-film epitaxy would vastly expand the application of hexagonal perovskites by epitaxially stabilizing various metastable polymorphs, the atomic structure of epitaxial hexagonal perovskites, especially at the initial growth stage, has rarely been investigated. In this study, we show that an intriguing nucleation behavior takes place during the initial stabilization of a hexagonal perovskite 9R BaRuO3 (BRO) thin film on a (111) SrTiO3 (STO) substrate. We use high-resolution high-angle annular dark field scanning transmission electron microscopy in combination with geometrical phase analysis to understand the local strain relaxation behavior. We find that nano-scale strained layers, composed of different RuO6 octahedral stacking, are initially formed at the interface, followed by a relaxed single crystal9R BRO thin film. Within the interface layer, hexagonal BROs are nucleated on the STO (111) substrate by both corner- and face-sharing. More interestingly, we find that the boundaries between the differently-stacked nucleation layers, i.e. heterostructural boundaries facilitates strain relaxation, in addition to the formation of conventional misfit dislocations evolving from homostructural boundaries. Our observations reveal an important underlying mechanism to understand the thin-film epitaxy and strain accommodation in hexagonal perovskites., Comment: 18 pages, 3 figures

Investigating the effects of the complex magnetic interactions on the formation of nontrivial magnetic phases enables a better understanding of magnetic materials. Moreover, an effective method to systematically control those interactions and phases could be extensively utilized in spintronic devices. SrRuO3 heterostructures function as a suitable material system to investigate the complex magnetic interactions and the resultant formation of topological magnetic phases, as the heterostructuring approach provides an accessible controllability to modulate the magnetic interactions. In this study, we have observed that the Hall effect of SrRuO3/SrTiO3 superlattices varies nonmonotonically with the repetition number (z). Using Monte Carlo simulations, we identify a possible origin of this experimental observation: the interplay between the Dzyaloshinskii-Moriya interaction and dipole-dipole interaction, which have differing z-dependence, might result in a z-dependent modulation of topological magnetic phases. This approach provides not only a collective understanding of the magnetic interactions in artificial heterostructures but also a facile control over the skyrmion phases., Comment: 3 figures

We report on the effect of epitaxial strain on magnetic and optical properties of perovskite LaCrO3 (LCO) single crystal thin films. Epitaxial LCO thin films are grown by pulsed laser deposition on proper choice of substrates to impose different strain states. A combined experimental and theoretical approach is used to demonstrate the direct correlation between lattice-strain and functional properties. The magnetization results show that the lattice anisotropy plays a critical role in controlling the magnetic behavior of LCO films. The strain induced tetragonality in the film lattice strongly affects the optical transitions and charge transfer gap in LCO. This study opens new possibilities to tailoring the functional properties of LCO and related materials by strain engineering in epitaxial growth.

The origin of strain-induced ferromagnetism, which is robust regardless of the type and degree of strain in LaCoO3 (LCO) thin films, is enigmatic despite intensive research efforts over the past decade. Here, by combining scanning transmission electron microscopy with ab initio density functional theory plus U calculations, we report that the ferromagnetism does not emerge directly from the strain itself, but rather from the creation of compressed structural units within ferroelastically formed twin-wall domains. The compressed structural units are magnetically active with the rocksalt-type high-spin/low-spin order. Our study highlights that the ferroelastic nature of ferromagnetic structural units is important for understanding the intriguing ferromagnetic properties in LCO thin films.

A strong correlation between magnetic interaction and topological symmetries leads to unconventional magneto-transport behavior. Weyl fermions induce topologically protected spin-momentum locking, which is closely related to spin-wave gap formation in magnetic crystals. Ferromagnetic SrRuO3, regarded as a strong candidate for Weyl semimetal, inherently possesses a nonzero spin-wave gap owing to its strong magnetic anisotropy. In this paper, we propose a method to control the spin-wave dynamics by nanolayer designing of the SrRuO3/SrTiO3 superlattices. In particular, the six-unit-cell-thick SrRuO3 layers within the superlattices undergo a phase transition in crystalline symmetry from orthorhombic to tetragonal, as the thickness of the SrTiO3 layers is modulated with atomic-scale precision. Consequently, the magnetic anisotropy, anomalous Hall conductivity, and spin-wave gap could be systematically manipulated. Such customization of magnetic anisotropy via nanoscale heterostructuring offers a novel control knob to tailor the magnon excitation energy for future spintronic applications, including magnon waveguides and filters. Our nanolayer approach unveils the important correlation between the tunable lattice degrees of freedom and spin dynamics in topologically non-trivial magnetic materials., Comment: 25 page

SrRuO3 (SRO) is an itinerant ferromagnet with strong coupling between the charge, spin, and lattice degrees of freedom. This strong coupling suggests that the electronic and magnetic behaviors of SRO are highly susceptible to changes in the lattice distortion. Here we show how the spin interaction and resultant magnon formation change with the modification in the crystallographic orientation. We fabricated SRO epitaxial thin films with (100), (110), and (111) surface orientations, to systematically modulate the spin interaction and spin dimensionality. The reduced spin dimensionality and enhanced exchange interaction in the (111)-oriented SRO thin film significantly suppresses magnon formation. Our study comprehensively demonstrates the facile tunability of magnon formation and spin interaction in correlated oxide thin films., Comment: 17 pages, 7 figures, 1 table, and 1 appendix

Bonding geometry engineering of metal-oxygen octahedra is a facile way of tailoring various functional properties of transition metal oxides. Several approaches, including epitaxial strain, thickness, and stoichiometry control, have been proposed to efficiently tune the rotation and tilting of the octahedra, but these approaches are inevitably accompanied by unnecessary structural modifications such as changes in thin-film lattice parameters. In this study, we propose a method to selectively engineer the octahedral bonding geometries, while maintaining other parameters that might implicitly influence the functional properties. A concept of octahedral tilt propagation engineering has been developed using atomically designed SrRuO3/SrTiO3 superlattices. In particular, the propagation of RuO6 octahedral tilting within the SrRuO3 layers having identical thicknesses was systematically controlled by varying the thickness of adjacent SrTiO3 layers. This led to a substantial modification in the electromagnetic properties of the SrRuO3 layer, significantly enhancing the magnetic moment of Ru. Our approach provides a method to selectively manipulate the bonding geometry of strongly correlated oxides, thereby enabling a better understanding and greater controllability of their functional properties., Comment: 27 pages, 4 figures, 6 supplementary figures

Alternate stacking of a highly conducting metallic layer with a magnetic triangular layer found in delafossite PdCrO2 provides an excellent platform for discovering intriguing correlated quantum phenomena. Thin film growth of the material may enable not only tuning the basic physical properties beyond what bulk materials can exhibit, but also developing novel hybrid materials by interfacing with dissimilar materials, yet this has proven to be extremely challenging. Here, we report the epitaxial growth of metallic delafossite PdCrO2 films by pulsed laser epitaxy (PLE). The fundamental role of the PLE growth conditions, epitaxial strain, and chemical and structural characteristics of the substrate is investigated by growing under various growth conditions and on various types of substrates. While strain plays a large role in improving the crystallinities, the direct growth of epitaxial PdCrO2 films without impurity phases was not successful. We attribute this difficulty to both the chemical and structural dissimilarities between the substrates and volatile nature of PdO layer, which make nucleation of the right phase difficult. This difficulty was overcome by growing CuCrO2 buffer layers before PdCrO2 were grown. Unlike PdCrO2, CuCrO2 films were rather readily grown with a relatively wide growth window. Only monolayer thick buffer layer was sufficient to grow the correct PdCrO2 phase. This result indicates that the epitaxy of Pd-based delafossites is extremely sensitive to the chemistry and structure of the interface, necessitating near perfect substrate materials. The resulting films are commensurately strained and show an antiferromagnetic transition at 40 K that persists down to as thin as 3.6 nm in thickness.