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Two-dimensional (2D) magnetism in van der Waals (vdW) atomic crystals and moir\'e superlattices has emerged as a topic of tremendous interest in the fields of condensed matter physics and materials science within the past half-decade since its first experimental discovery in 2016 - 2017. It has not only served as a powerful platform for investigating phase transitions in the 2D limit and exploring new phases of matter, but also provided new opportunities for applications in microelectronics, spintronics, magnonics, optomagnetics, and so on. Despite the flourishing developments in 2D magnetism over this short period of time, further efforts are welcome in multiple forefronts of 2D magnetism research for achieving the ultimate goal of routinely implementing 2D magnets as quantum electronic components. In this review article, we will start with basic concepts and properties of 2D magnetism, followed by a brief overview of historical efforts in 2D magnetism research and then a comprehensive review of vdW material-based 2D magnetism. We will conclude with discussions on potential future research directions for this growing field of 2D vdW magnetism., Comment: 50 pages, 31 figures

Broken symmetries and electronic topology are nicely manifested together in the second order nonlinear optical responses from topologically nontrivial materials. While second order nonlinear optical effects from the electric dipole (ED) contribution have been extensively explored in polar Weyl semimetals (WSMs) with broken spatial inversion (SI) symmetry, they are rarely studied in centrosymmetric magnetic WSMs with broken time reversal (TR) symmetry due to complete suppression of the ED contribution. Here, we report experimental demonstration of optical second harmonic generation (SHG) in a magnetic WSM Co$_{3}$Sn$_{2}$S$_{2}$ from the electric quadrupole (EQ) contribution. By tracking the temperature dependence of the rotation anisotropy (RA) of SHG, we capture two magnetic phase transitions, with both the SHG intensity increasing and its RA pattern rotating at $T_{C,1}$=175K and $T_{C,2}$=120K subsequently. The fitted critical exponents for the SHG intensity and RA orientation near $T_{C,1}$ and $T_{C,2}$ suggest that the magnetic phase at $T_{C,1}$ is a 3D Ising-type out-of-plane ferromagnetism while the other at $T_{C,2}$ is a 3D XY-type all-in-all-out in-plane antiferromagnetism. Our results show the success of detection and exploration of EQ SHG in a centrosymmetric magnetic WSM, and hence open the pathway towards the future investigation of its tie to the band topology., Comment: 19 pages, 4 figures

In this work, we study Metal-Insulator transition in a holographic model containing an interaction between the order parameter and charge-carrier density. It turns out that the impurity density of this model can drive the phase transition whose ordered phase corresponds to the insulating phase. The temperature behavior of DC conductivity distinguishes the insulating phase from the metal phase. We confirm this behavior by a numerical method and an analytic calculation. As a byproduct, we show the existence of a `quantum phase transition' supported by the Breitenlohner-Freedman bound argument., Comment: 22 pages, 21 figures

The interplay between a multitude of electronic, spin, and lattice degrees of freedom underlies the complex phase diagrams of quantum materials. Layer stacking in van der Waals (vdW) heterostructures is responsible for exotic electronic and magnetic properties, which inspires stacking control of two-dimensional magnetism. Beyond the interplay between stacking order and interlayer magnetism, we discover a spin-shear coupling mechanism in which a subtle shear of the atomic layers can have a profound effect on the intralayer magnetic order in a family of vdW antiferromagnets. Using time-resolved x-ray diffraction and optical linear dichroism measurements, interlayer shear is identified as the primary structural degree of freedom that couples with magnetic order. The recovery times of both shear and magnetic order upon optical excitation diverge at the magnetic ordering temperature with the same critical exponent. The time-dependent Ginzburg-Landau theory shows that this concurrent critical slowing down arises from a linear coupling of the interlayer shear to the magnetic order, which is dictated by the broken mirror symmetry intrinsic to the monoclinic stacking. Our results highlight the importance of interlayer shear in ultrafast control of magnetic order via spin-mechanical coupling.

Above-bandgap femtosecond optical excitation of a ferroelectric/dielectric BaTiO3/CaTiO3 superlattice leads to structural responses that are a consequence of the screening of the strong electrostatic coupling between the component layers. Time-resolved x-ray free-electron laser diffraction shows that the structural response to optical excitation includes a net lattice expansion of the superlattice consistent with depolarization-field screening driven by the photoexcited charge carriers. The depolarization-field-screening-driven expansion is separate from a photoacoustic pulse launched from the bottom electrode on which the superlattice was epitaxially grown. The distribution of diffracted intensity of superlattice x-ray reflections indicates that the depolarization-field-screening-induced strain includes a photoinduced expansion in the ferroelectric BaTiO3 and a contraction in CaTiO3. The magnitude of expansion in BaTiO3 layers is larger than the contraction in CaTiO3. The difference in the magnitude of depolarization-field-screening-driven strain in the BaTiO3 and CaTiO3 components can arise from the contribution of the oxygen octahedral rotation patterns at the BaTiO3/CaTiO3 interfaces to the polarization of CaTiO3. The depolarization-field-screening-driven polarization reduction in the CaTiO3 layers points to a new direction for the manipulation of polarization in the component layers of a strongly coupled ferroelectric/dielectric superlattice.

Domain walls are ubiquitous in materials that undergo phase transitions driven by spontaneous symmetry breaking. Domain walls in ferroics and multiferroics have received tremendous attention recently due to their emergent properties distinct from their domain counterparts, for example, their high mobility and controllability, as well as their potential applications in nanoelectronics. However, it is extremely challenging to detect, visualize and study the ferro-rotational (FR) domain walls because the FR order, in contrast to ferromagnetism (FM) and ferroelectricity (FE), is invariant under both the spatial-inversion and the time-reversal operations and thus hardly couple with conventional experimental probes. Here, an FR candidate $\mathrm{NiTiO_{3}}$ is investigated by ultrasensitive electric quadrupole (EQ) second harmonic generation rotational anisotropy (SHG RA) to probe the point symmetries of the two degenerate FR domain states, showing their relation by the vertical mirror operations that are broken below the FR critical temperature. We then visualize the real-space FR domains by scanning EQ SHG microscopy, and further resolve the FR domain walls by revealing a suppressed SHG intensity at domain walls. By taking local EQ SHG RA measurements, we show the restoration of the mirror symmetry at FR domain walls and prove their unconventional nonpolar nature. Our findings not only provide a comprehensive insight into FR domain walls, but also demonstrate a unique and powerful tool for future studies on domain walls of unconventional ferroics, both of which pave the way towards future manipulations and applications of FR domain walls.

Weakly coupled ferroelectric/dielectric superlattice thin film heterostructures exhibit complex nanoscale polarization configurations that arise from a balance of competing electrostatic, elastic, and domain-wall contributions to the free energy. A key feature of these configurations is that the polarization can locally have a significant component that is not along the thin-film surface normal direction, while maintaining zero net in-plane polarization. PbTiO3/SrTiO3 thin-film superlattice heterostructures on a conducting SrRuO3 bottom electrode on SrTiO3 have a room-temperature stripe nanodomain pattern with nanometer-scale lateral period. Ultrafast time-resolved x-ray free electron laser diffraction and scattering experiments reveal that above-bandgap optical pulses induce rapidly propagating acoustic pulses and a perturbation of the domain diffuse scattering intensity arising from the nanoscale stripe domain configuration. With 400 nm optical excitation, two separate acoustic pulses are observed: a high-amplitude pulse resulting from strong optical absorption in the bottom electrode and a weaker pulse arising from the depolarization field screening effect due to absorption directly within the superlattice. The picosecond scale variation of the nanodomain diffuse scattering intensity is consistent with a larger polarization change than would be expected due to the polarization-tetragonality coupling of uniformly polarized ferroelectrics. The polarization change is consistent instead with polarization rotation facilitated by the reorientation of the in-plane component of the polarization at the domain boundaries of the striped polarization structure. The complex steady-state configuration within these ferroelectric heterostructures leads to polarization rotation phenomena that have been previously available only through the selection of bulk crystal composition.

The collective dynamics of topological structures have been of great interest from both fundamental and applied perspectives. For example, the studies of dynamical properties of magnetic vortices and skyrmions not only deepened the understanding of many-body physics but also led to potential applications in data processing and storage. Topological structures constructed from electrical polarization rather than spin have recently been realized in ferroelectric superlattices, promising for ultrafast electric-field control of topological orders. However, little is known about the dynamics of such complex extended nanostructures which in turn underlies their functionalities. Using terahertz-field excitation and femtosecond x-ray diffraction measurements, we observe ultrafast collective polarization dynamics that are unique to polar vortices, with orders of magnitude higher frequencies and smaller lateral size than those of experimentally realized magnetic vortices. A previously unseen soft mode, hereafter referred to as a vortexon, emerges as transient arrays of nanoscale circular patterns of atomic displacements, which reverse their vorticity on picosecond time scales. Its frequency is significantly reduced at a critical strain, indicating a condensation of structural dynamics. First-principles-based atomistic calculations and phase-field modeling reveal the microscopic atomic arrangements and frequencies of the vortex modes. The discovery of subterahertz collective dynamics in polar vortices opens up opportunities for applications of electric-field driven data processing in topological structures with ultrahigh speed and density.

Optical excitation perturbs the balance of phenomena selecting the tilt orientation of domain walls within ferroelectric thin films. The high carrier density induced in a low-strain BaTiO3 thin film by an above-bandgap ultrafast optical pulse changes the tilt angle that 90{\deg} a/c domain walls form with respect to the substrate-film interface. The dynamics of the changes are apparent in time-resolved synchrotron x-ray scattering studies of the domain diffuse scattering. Tilting occurs at 298 K, a temperature at which the a/b and a/c domain phases coexist but is absent at 343 K in the better ordered single-phase a/c regime. Phase coexistence at 298 K leads to increased domain-wall charge density, and thus a larger screening effect than in the single-phase regime. The screening mechanism points to new directions for the manipulation of nanoscale ferroelectricity.

Quantum devices formed in high-electron-mobility semiconductor heterostructures provide a route through which quantum mechanical effects can be exploited on length scales accessible to lithography and integrated electronics. The electrostatic definition of quantum dots in semiconductor heterostructure devices intrinsically involves the lithographic fabrication of intricate patterns of metallic electrodes. The formation of metal/semiconductor interfaces, growth processes associated with polycrystalline metallic layers, and differential thermal expansion produce elastic distortion in the active areas of quantum devices. Understanding and controlling these distortions presents a significant challenge in quantum device development. We report synchrotron x-ray nanodiffraction measurements combined with dynamical x-ray diffraction modeling that reveal lattice tilts with a depth-averaged value up to 0.04 deg. and strain on the order of 10^-4 in the two-dimensional electron gas (2DEG) in a GaAs/AlGaAs heterostructure. Elastic distortions in GaAs/AlGaAs heterostructures modify the potential energy landscape in the 2DEG due to the generation of a deformation potential and an electric field through the piezoelectric effect. The stress induced by metal electrodes directly impacts the ability to control the positions of the potential minima where quantum dots form and the coupling between neighboring quantum dots.

As a means to support the access of massive machine-type communication devices, grant-free access and non-orthogonal multiple access (NOMA) have received great deal of attention in recent years. In the grant-free transmission, each device transmits information without the granting process so that the basestation needs to identify the active devices among all potential devices. This process, called an active user detection (AUD), is a challenging problem in the NOMA-based systems since it is difficult to identify active devices from the superimposed received signal. An aim of this paper is to put forth a new type of AUD based on deep neural network (DNN). By applying the training data in the properly designed DNN, the proposed AUD scheme learns the nonlinear mapping between the received NOMA signal and indices of active devices. As a result, the trained DNN can handle the whole AUD process, achieving an accurate detection of the active users. Numerical results demonstrate that the proposed AUD scheme outperforms the conventional approaches in both AUD success probability and computational complexity.

The spontaneously formed striped polarization nanodomain configuration of a PbTiO${_3}$/SrTiO${_3}$ superlattice transforms to a uniform polarization state under above-bandgap illumination with a time dependence varying with the intensity of optical illumination and a well-defined threshold intensity. Recovery after the end of illumination occurs over a temperature-dependent period of tens of seconds at room temperature and shorter times at elevated temperatures. A model in which the screening of the depolarization field depends on the population of trapped electrons correctly predicts the observed temperature and optical intensity dependence., Comment: This article has been accepted by Applied Physics Letter

Intense hard x-ray pulses from a free-electron laser induce irreversible structural damage in a perovskite oxide epitaxial heterostructure when pulse fluences exceed a threshold value. The intensity of x-ray diffraction from a 25-nm thick epitaxial BiFeO$_{3}$ layer on a SrTiO$_{3}$ substrate measured using a series of pulses decreases abruptly with a per-pulse fluence of 2.7 x 10$^{6}$ photons ${\mu}$m$^{-2}$ at 9.7 keV photon energy, but remains constant for 1.3 x 10$^{6}$ photons ${\mu}$m$^{-2}$ or less. The damage resulted in the destruction of the BiFeO$_{3}$ thin film within the focal spot area and the formation of a deep cavity penetrating into the STO substrate via the removal of tens of nanometers of material per pulse. The damage threshold occurs at a fluence that is insufficient to heat the absorption volume to the melting point. The morphology of the ablated sample is consistent with fracture rather than melting. Together these results indicate that the damage occurs via a non-thermal process consistent with ultrafast ionization of the absorption volume., Comment: The following article has been accepted by Applied Physics Letters

Above-bandgap optical illumination induces a transformation from tilted tetragonal-like (T-like) and rhombohedral-like (R-like) phases to an untilted T-like phase in compressively strained BiFeO3. Optical excitation leads to an out-of-plane lattice expansion in the T-like phase. The transformation proceeds in regions with boundaries between the T-like and tilted R-like and tilted T-like phases, consistent with the motion of a boundary. The optically induced transformation indicates that there are new optically driven routes towards nanosecond-scale control of phase transformations in ferroelectrics and multiferroics.

The nanodomain pattern in ferroelectric/dielectric superlattices transforms to a uniform polarization state under above-bandgap optical excitation. X-ray scattering reveals a disappearance of domain diffuse scattering and an expansion of the lattice. The reappearance of the domain pattern occurs over a period of seconds at room temperature, suggesting a transformation mechanism in which charge carriers in long-lived trap states screen the depolarization field. A Landau-Ginzburg-Devonshire model predicts changes in lattice parameter and a critical carrier concentration for the transformation.