Artificial Superlattices Research Articles

Engineering the Coherent Phonon Transport in Polar Ferromagnetic Oxide Superlattices.

Artificial superlattices composed of perovskite oxides serves as an essential platform for engineering coherent phonon transport by redefining the lattice periodicity, which strongly influences the lattice-coupled phase transitions in charge and spin degrees of freedom. However, previous methods of manipulating phonons have been limited to controlling the periodicity of superlattice, rather than utilizing complex mutual interactions that are prominent in transition metal oxides. In this study onoxide superlattices composed of ferromagnetic metallic SrRuO3 and quantum paraelectric SrTiO3, phonon modulation by controlling the geometry of superlattice in atomic-scale precision is realized, demonstrating the coherent phonon engineering using structural and magnetic phase transitions. By modulating the interface density, coherent-incoherent crossover of the phonon transport at room temperature is observed, which is coupled with a change in interfacial structural continuity. Upon cooling, the close relation between phonon transport and multiple phase transitions is identified. In particular, the enhancement of the polar state in SrTiO3 layer at ≈200K leads to the weakening of phonon coherence and a further reduction of thermal conductivity in superlattices compared to the bulk limit. These findings provide a guide to developing future thermoelectric nanodevices by engineering the coherence of phonons via the design of complex oxide heterostructures.

Enhancing 2D Photonics and Optoelectronics with Artificial Microstructures.

By modulating subwavelength structures and integrating functional materials, 2D artificial microstructures (2D AMs), including heterostructures, superlattices, metasurfaces and microcavities, offer a powerful platform for significant manipulation of light fields and functions. These structures hold great promise in high-performance and highly integrated optoelectronic devices. However, a comprehensive summary of 2D AMs remains elusive for photonics and optoelectronics. This review focuses on the latest breakthroughs in 2D AM devices, categorized into electronic devices, photonic devices, and optoelectronic devices. The control of electronic and optical properties through tuning twisted angles is discussed. Some typical strategies that enhance light-matter interactions are introduced, covering the integration of 2D materials with external photonic structures and intrinsic polaritonic resonances. Additionally, the influences of external stimuli, such as vertical electric fields, enhanced optical fields and plasmonic confinements, on optoelectronic properties is analysed. The integrations of these devices are also thoroughly addressed. Challenges and future perspectives are summarized to stimulate research and development of 2D AMs for future photonics and optoelectronics.

Engineering optoelectronic properties of [formula omitted] superlattices using first principles method

Recent advancements in thin-film growth techniques have opened doors for engineering innovative heterostructures with ultra-thin layers. These artificial superlattices hold promise for novel optoelectronic devices. However, a complete understanding of their properties is crucial for optimal design. In this study, we employ the full-potential linearized augmented plane wave (FP−LAPW) approach based on density functional theory (DFT) to engineer the optoelectronic properties of (HgSe)n/(ZnTe)n superlattices by controlling the number of layers (n) in SLs; The exchange-correlation potential was calculated by the generalized gradient GGA approximation and the optoelectronics properties has adjusted by the Tran-Blaha modified Becke-Johnson (TB−mBJ) correction of GGA approximation. Our findings shed light on the significant influence of stacking periodicity on the optoelectronic properties of HgTe/ZnTe SLs. We demonstrate that manipulating layer count is a viable strategy for engineering their optoelectronic characteristics. Additionally, the predicted near-infrared absorption makes these SLs promising candidates for near-infrared detector applications.

Real-time dynamics of angular momentum transfer from spin to acoustic chiral phonon in oxide heterostructures.

Chiral phonons have recently been explored as a novel degree of freedom in quantum materials. The angular momentum carried by these quasiparticles is generated by the breaking of chiral degeneracy of phonons, owing to the chiral lattice structure or the rotational motion of ions of the material. In ferromagnets, a mechanism for generating non-equilibrium chiral phonons has been suggested, but their temporal evolution, which obeys Bose-Einstein statistics, remains unclear. Here we report the real-time dynamics of thermalized chiral phonons in an artificial superlattice composed of ferromagnetic metallic SrRuO3 and non-magnetic insulating SrTiO3. Following the photo-induced ultrafast demagnetization in the SrRuO3 layer, we observed the appearance of a magneto-optic signal in the superlattice, which is absent in the SrRuO3 single films. This magneto-optic signal exhibits thermally driven dynamic properties and a clear correlation with the thickness of the non-magnetic SrTiO3 layer, implying that it originates from thermalized chiral phonons. We use numerical calculations considering the magneto-elastic coupling in SrRuO3 to validate our experimental observations and the angular momentum transfer mechanism between the lattice and spin systems in ferromagnetic systems and also to the non-magnetic system.

Anomalous behavior of critical current in a superconducting film triggered by DC plus terahertz current

The critical current in a superconductor (SC) determines the performance of many SC devices, including SC diodes which have attracted recent attention. Hitherto, studies of SC diodes are limited in the DC-field measurements, and their performance under a high-frequency current remains unexplored. Here, we conduct the first investigation on the interaction between the DC and terahertz (THz) current in a SC artificial superlattice. We found that the DC critical current is sensitively modified by THz pulse excitations in a nontrivial manner. In particular, at low-frequency THz excitations below the SC gap, the critical current becomes sensitive to the THz-field polarization direction. Furthermore, we observed anomalous behavior in which a supercurrent flows with an amplitude larger than the modified critical current. Assuming that vortex depinning determines the critical current, we show that the THz-current-driven vortex dynamics reproduce the observed behavior. While the delicate nonreciprocity in the critical current is obscured by the THz pulse excitations, the interplay between the DC and THz current causes a non-monotonic SC/normal-state switching with current amplitude, which can pave a pathway to developing SC devices with novel functionalities.

Disruption of polar order in lead zirconate titanate by composition-modulated artificial superlattice

Lead zirconate titanate (Pb (Zrx, Ti1−x)O3: PZT) is a well-known ferroelectric compound, in which long-range polar order is usually developed. In the present study, it was clarified by distortion-corrected atomic-scale scanning transmission electron microscopy imaging that long-range polar order is disrupted in PZT by utilizing composition-modulated superlattice. Shape of unit cell was unusual both in the Pb(Zr0.65Ti0.35)O3 (PZT65) and Pb(Zr0.30Ti0.70)O3 (PZT30) layers, which was due to mutual in-plane lattice constraint. By taking account of this, first-principles calculations clarified that multiple directions can be energetically favorable for lead-ion displacement, which explains a reason why long-range polar order was disrupted.

Novel Route for Enhancing Piezoelectricity of Ferroelectric Films: Controlling Nontrivial Polarization States in Pb(Zr, Ti)O3 Monodomain Superlattice Structure.

Artificial superlattice films made of Pb(Zr0.4Ti0.6)O3 and Pb(Zr0.6Ti0.4)O3 were investigated for their polarization states and piezoelectric properties theoretically and experimentally in this study. The developed theory predicts nontrivial polarization along neither [001] nor [111] directions in (111)-epitaxial monodomain superlattice films with uniform compressive strain. Such films were achieved via pulsed laser deposition. When the layer thickness is reduced to 3 nm, d33 becomes 128 ± 3.8 pm/V at 100 kV/cm and 71.3 ± 2.83 pm/V at 600 kV/cm, comparable to that of (111)-oriented Pb(Zr0.4Ti0.6)O3 or Pb(Zr0.6Ti0.4)O3 bulks and clearly exceeding that of the typical clamped films. The measurement agrees with the theoretical analysis, which reveals that the enhanced piezoelectricity is due to rotation of the nontrivial polarization. Furthermore, the theoretical study predicts an even larger d33 exceeding 300 pm/V for specific parameters in superlattice films with uniform tensile strain, which is promising for applications of microelectromechanical systems.

Controllable van der Waals gaps by water adsorption.

Van der Waals (vdW) gaps with ångström-scale heights can confine molecules or ions to an ultimately small scale, providing an alternative way to tune material properties and explore microscopic phenomena. Modulation of the height of vdW gaps between two-dimensional (2D) materials is challenging due to the vdW interaction. Here we report a general approach to control the vdW gap by preadsorption of water molecules on the material surface. By controlling the saturation vapour pressure of water vapour, we can precisely control the adsorption level of water molecules and vary the height of the vdW gaps of MoS2 homojunctions from 5.5 Å to 53.6 Å. This technique can be further applied to other homo- and heterojunctions, constructing controlled vdW gaps in 2D artificial superlattices and in 2D/3D and 3D/3D heterojunctions. Engineering the vdW gap has great practical potential to modulate the device performance, as evidenced by the vdW-gap-dependent diode characteristics of the MoS2/gap/MoS2 junction. Our work introduces a general strategy of molecular preadsorption that can extend to various precursors, creating more tunability and variability in vdW material systems.

Two-Dimensional Artificial Ge Superlattice Confining in Electronic Kagome Lattice Potential Valleys.

Constructing two-dimensional (2D) artificial superlattices based on single-atom and few-atom nanoclusters is of great interest for exploring exotic physics. Here we report the realization of two types of artificial germanium (Ge) superlattice self-confined by a R25.3° superstructure of bismuth (Bi) induced electronic kagome lattice potential valleys. Scanning tunneling microscopy measurements demonstrate that Ge atoms prefer to be confined in the center of the Bi electronic kagome lattice, forming a single-atom superlattice at 120 K. In contrast, room temperature grown Ge atoms and clusters are confined in the sharing triangle corner and the center, respectively, of the kagome lattice potential valleys, forming an artificial honeycomb superlattice. First-principle calculations and Mulliken population analysis corroborate that our reported atomically thin Bi superstructure on Au(111) has a kagome surface potential valley with the center of the inner Bi hexagon and the space between the outer Bi hexagons being energetically favorable for trapping Ge atoms.

Channeling the exchanges of eg electrons by Co-implantation for magnetism enhancement in CrI3 monolayer

In recent few years, the two-dimensional (2D) magnets have emerged as one of the most important frontiers in materials physics and attracted much attention. As one of the earliest experimentally discovered 2D magnets, CrI3 shows a wealth of properties and has been extensively studied. In particular, an intriguing characteristic of the CrI3 monolayer is its octahedrally coordinated hollow within the unit-cell, which enables the implantation of a magnetic atom, thereby resulting in an artificial 2D superlattice with fertile physics to explore. In this work, using first-principles calculations, we investigate the Co-implanted CrI3 monolayer, denoted as Co-(CrI3)2, and demonstrate the vital roles of the exchange channels of eg electrons in enhancing magnetism. It is shown that the Co-(CrI3)2 monolayer has a half-metallic ferrimagnetic (FiM) ground-state with a net in-plane magnetic moment of 5.0μB/f.u. and a relatively high Curie point (TC) of ∼195 K, noting that TC of pristine CrI3 is only 45–61 K. The FiM ordering is established by the strong anti-ferromagnetic coupling in the t2g-eg exchange channels of the nearest-neighbor (NN) Cr–Co pair and the sizeable ferromagnetic coupling of the third NN Cr–Cr pair mediated by the itinerant eg electrons. In addition, an in-plane biaxial tensile strain of ∼2% may further enhance TC up to ∼210 K. This work offers unique insights into the magnetism enhancement of the CrI3 monolayer by atom-implantation, paving the way for the development of 2D magnets.

Hofstadter-like spectrum and magnetization of artificial graphene constructed with cylindrical and elliptical quantum dots

A comparative study of the electronic and magnetic properties of quasi-two-dimensional electrons in an artificial graphene-like superlattice composed of circular and elliptical quantum dots is presented. A complete orthonormal set of basis functions has been implemented for calculation of the energy dispersions, Hofstadter spectra, density of states and orbital magnetization of the considered systems. Our calculations indicate a topological change in the miniband structure due to the ellipticity of the quantum dots, and non-trivial modifications of the electron energy dispersion surfaces with the change of the magnetic flux per unite cell. The ellipticity of the quantum dots leads to an opening of a gap and considerable modifications of the Hofstadter spectrum. The orbital magnetization is shown to reveal significant oscillations with the change of the magnetic flux. The ellipticity of quantum dots has a qualitative impact on the dependencies of the magnetization on both the magnetic flux and the temperature.

The Superconducting Dome in Artificial High-Tc Superlattices Tuned at the Fano–Feshbach Resonance by Quantum Design

While the search for new high-temperature superconductors had been driven by the empirical “trials and errors” method for decades, we now report the synthesis of Artificial High-Tc Superlattices (AHTS) designed by quantum mechanics theory at the nanoscale. This discovery paves the way for engineering a new class of high-temperature superconductors, following the predictions of the Bianconi Perali Valletta (BPV) theory recently implemented in 2022 by Mazziotti et al. including Rashba spin-orbit coupling to create nanoscale AHTS composed of quantum wells. The high-Tc superconducting properties within these superlattices are controlled by a conformational parameter of the superlattice geometry, specifically, the ratio L/d which represents the thickness of La2CuO4 layers (L) relative to the superlattice period (d). Using molecular beam epitaxy, we have successfully grown numerous AHTS samples. These samples consist of initial layers of stoichiometric La2CuO4 units with a thickness L, doped by interface space charge, and intercalated with second layers of non-superconducting metallic material, La1.55Sr0.45CuO4 with thickness denoted as W = d − L. This configuration forms a quantum superlattice with periodicity d. The agreement observed between the experimental dependence Tc (the superconducting transition temperature) versus L/d ratio and the predictions of the BPV theory for AHTS in the form of the superconducting dome validates the hypothesis that the superconducting dome arises from the Fano–Feshbach or shape resonance in multigap superconductivity driven by quantum nanoscale confinement.

Magnetization Control of Zero-Field Intrinsic Superconducting Diode Effect.

The superconducting diode effect (SDE), which causes a superconducting state in one direction and a normal-conducting state in another, has significant potential for developing ultralow power consumption circuits and non-volatile memory. However, the practical control of the SDE necessities the precise tuning of current, temperature, magnetic field, or magnetism. Therefore, the mechanisms of the SDE must be understood to develop novel materials and devices capable of realizing the SDE under more controlled and robust conditions. This study demonstrates an intrinsic zero-field SDE with an efficiency of up to 40% in Fe/Pt-inserted non-centrosymmetric Nb/V/Ta superconducting artificial superlattices. The polarity and magnitude of the zero-field SDE are controllable by the direction of magnetization, indicating that the effective exchange field acts on Cooper pairs. Furthermore, the first-principles calculation indicates that the SDE can be enhanced by an asymmetric configuration of proximity induced magnetic moments in superconducting layers, which induces a magnetic toroidal moment. This study has important implications regarding the development of novel materials and devices that can effectively control the SDE. Moreover, the magnetization control of the SDE is expected to aid in the designing of superconducting quantum devices and establishing a material platform for topological superconductors. This article is protected by copyright. All rights reserved.

Hybridizing Ti3C2Tx Layers with Layered Double Hydroxide Nanosheets at the Molecular Level: A Smart Electrode Material for H2O2 Monitoring in Cancer Cells.

Vertically stacked artificial 2D superlattice hybrids fabricated through molecular-level hybridization in a controlled fashion play a vital role in scientific and technological fields, but developing an alternate assembly of 2D atomic layers with strong electrostatic interactions could be much more challenging. In this study, we have constructed an alternately stacked self-assembled superlattice composite through integration of CuMgAl layered double hydroxide (LDH) nanosheets having positive charge with negatively charged Ti3C2Tx layers using well-controlled liquid-phase co-feeding protocol and electrostatic attraction and investigated its electrochemical performance in sensing early cancer biomarkers, i.e., hydrogen peroxide (H2O2). The molecular-level CuMgAl LDH/Ti3C2Tx superlattice self-assembly possesses superb conductivity and electrocatalytic properties, which are significant for obtaining a high electrochemical sensing aptitude. Electron penetration in Ti3C2Tx layers and rapid ion diffusion along 2D galleries have shortened the diffusion path and enhanced the charge transferring efficacy. The electrode modified with the CuMgAl LDH/Ti3C2Tx superlattice has demonstrated admirable electrocatalytic abilities in H2O2 detection with a wide linear concentration range and low real-time limit of detection (LOD) of 0.1 nM with signal/noise ratio (S/N) = 3. Practically, an electrochemical sensing podium based on the CuMgAl LDH/Ti3C2Tx superlattice has been effectively applied in real-time in vitro tracking of H2O2 effluxes excreted from different live cancer cells and normal cells after being encouraged by stimulation. The results exhibit that molecular-level heteroassembly holds great potential in electrochemical sensors to detect promising biomarkers.

Quantum Geometric Oscillations in Two-Dimensional Flat-Band Solids.

Two-dimensional van der Waals heterostructures can be engineered into artificial superlattices that host flat bands with significant Berry curvature and provide a favorable environment for the emergence of novel electron dynamics. In particular, the Berry curvature can induce an oscillating trajectory of an electron wave packet transverse to an applied static electric field. Though analogous to Bloch oscillations, this novel oscillatory behavior is driven entirely by quantum geometry in momentum space instead of band dispersion. While the current from Bloch oscillations can be localized by increasing field strength, the current from the geometric orbits saturates to a nonzero plateau in the strong-field limit. In nonmagnetic materials, the geometric oscillations are even under inversion of the applied field, whereas the Bloch oscillations are odd, a property that can be used to distinguish these two coexisting effects.

Exotic Magnetic Anisotropy Near Digitized Dimensional Mott Boundary.

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. The magnetic anisotropy modulation near a digitized dimensional Mott boundary in artificial superlattices composed of a correlated magnetic monolayer SrRuO3 and nonmagnetic SrTiO3 , is demonstrated. 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. The results offer a new digitized control for magnetic anisotropy in low-dimensional Mott systems, inspiring promising integration of Mottronics and spintronics.

Correlated Quantum Phenomena of Spin–Orbit Coupled Perovskite Oxide Heterostructures: Cases of SrRuO3 and SrIrO3 Based Artificial Superlattices

AbstractUnexpected, 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 perovskite 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.

Engineering Natural Layered Framework for Low and Anisotropic Thermal Conductivity

AbstractThe development of nano–manufacture technology in the twenty‐first century has paved the way for artificial nanostructure constructions like man–made superlattices, providing historical breakthroughs in thermal physics and thermoelectrics by the modulation of phonons. Still, high–performance thermal insulators haven't come into operation due to the arduousness, costing and unscalability of artificiality. Herein, intentional engineering on a so–called ‘natural superlattice’ with alternating PbSe– and Bi2Se3–layer crystal structure is brought forth to recreate the mechanism of artificial superlattices and boost phonon localization. The thermal conductivity notably shows a direction–specific reduction, leading to minimum approaching and enhanced anisotropy. The modification of the natural framework and its effects have been supported by various transport and structure studies. This work sets a generalizable example for natural layered material engineering that bridges between the inflexible, changeless but self–assembled natural layered compounds, and the highly efficient, delicately tailored but unscalable artificial superlattice complexes. The methodology promises new horizons for practicable thermal management.

Engineering antiferroelectric nucleation in ferroelectric films with enhanced piezoelectricity

Tailoring ferroelectric-antiferroelectric phase transitions provides strategic advantages for potential applications in digital displacement transducers and ultrathin ferroelectric capacitors. In particular, epitaxy of artificial superlattice has been widely used and proved to be capable of creating antiferroelectric-type characteristics within intrinsic ferroelectrics. Here, we have achieved dedicatedly control of ferroelectric-antiferroelectric phase transition by introducing 2 unit-cells antiferroelectric PbZrO3 layers into the intrinsic ferroelectric BiFeO3 films, with the ultrathin PbZrO3 layers acting as the structural spacer to bridge the robust nucleation of striping phase in BiFeO3 layers. Aberration-corrected scanning transmission electron microscopy characterization revealed that the BiFeO3 layers experienced a transition to the antiferroelectric-like polymorph via interface-transferred lattice distortion of alternate cation displacement, thereby forming the periodic ferroelectric-antiferroelectric nanoscale laminas. Further piezoresponse force measurements gave the direct evidences that the modulated superlattice exhibited improved piezoelectric performance compared with typical rhombohedral BiFeO3 films. This work paves the way for engineering polarity-mismatched superlattices with enhanced piezoelectric response and enriches the fundamental of structure-functionality correlations in oxide heterosystems.

Extreme Enhanced Curie Temperature and Perpendicular Exchange Bias in Freestanding Ferromagnetic Superlattices.

Most recently, the freestanding of an epitaxial single-crystal oxide has been greatly developed to its fundamental concerns and the possibility of integration with metal, two-dimensional, and organic materials for more promising functionalities. In an artificial ferromagnetic oxide heterostructure and superlattice, the release of the substrate constraint can induce a reasonable transformation of the magnetic structure because the change of the lattice field occurs. In this study, we have comprehensively investigated the evolution of magnetic properties of (La0.7Ca0.3MnO3/SrRuO3)n [(LCMO/SRO)n] ferromagnetic superlattices while they are epitaxially on SrTiO3 and freestanding. It is found that the Curie temperature and the perpendicular exchange bias of the freestanding superlattices exhibit extreme sensitivity to the interface number and the thickness of LCMO and SRO, which can maximumly reach ∼293 K and ∼1150 Oe. These enhanced and bulk-beyond magnetic behaviors originate from the interfacial magnetic transition from ferromagnetic to antiferromagnetic via the charge reconstruction with the assistance of strain. Our study provides not only a reference for designing a high-performance flexible ferromagnetic architectural superlattice but also a deep understanding of the interfacial effect in freestanding ferromagnetic heterostructures benefiting flexible spintronics.