arXiv subjects

Liqin Ke

Publications and source records attributed to Liqin Ke.

At least 55 records · Page 3Linked to original sources

arXiv2021

Self-consistently renormailzed spin-wave theory of layered ferromagnets on honeycomb lattice

We develop a self-consistently renormalized spin-wave theory, within a mean-field approximation, for the two-dimensional Heisenberg ferromagnet with perpendicular easy-axis anisotropy on the honeycomb lattice, as well as its few-layer and bulk extensions. In this method, the magnetization dependence on temperature is found as the solution of the self-consistency equation. Furthermore, we account for the physical difference of surface and bulk layers by treating the layers as separate sublattices. Thus, the method can be readily generalized to study various magnetic phenomena in a broad range of systems, including those comprising magnetically inequivalent sublattices. Using our theory, we calculate the temperature-dependent magnetization for two chromium-based layered van der Waals insulating magnets, Cr$_2$Ge$_2$Te$_6$ and CrI$_3$, employing various sets of Heisenberg exchange and single-ion anisotropy values reported for these materials in the existing literature. As expected, we observe a strong dimensionality effect where the ordering temperature is reduced and its sensitivity on the anisotropy is enhanced with the decrease of dimensionality.

cond-mat.mtrl-sci↗

arXiv2021

Suppression of antiferromagnetic order and strong ferromagnetic spin fluctuations in Ni-doped CaCo2As2 single crystals

CaCo2As2 is a unique itinerant system having strong magnetic frustration. Here we report the effect of electron doping on the physical properties resulting from Ni substitutions for Co. The A-type antiferromagnetic transition temperature TN = 52 K for x = 0 decreases to 22 K with only 3 percent Ni substitution and is completely suppressed for x > 0.11. For 0.11 < x < 0.52 strong ferromagnetic (FM) fluctuations develop as revealed by magnetic susceptibility chi(T) measurements. Heat-capacity Cp(T) measurements reveal the presence of FM quantum spin fluctuations for 0.11 < x < 0.52. Our density-functional theory (DFT) calculations confirm that FM fluctuations are enhanced by Ni substitutions for Co. The Sommerfeld electronic heat-capacity coefficient is enhanced for x = 0, 0.21, and 0.42 by about a factor of two compared to DFT calculations of the bare density of states at the Fermi energy. The crystals with x > 0.52 do not exhibit FM spin fluctuations or magnetic order, which was found from the DFT calculations to arise from a Stoner transition. Neutron-diffraction studies of crystals with x = 0.11 and 0.16 found no evidence of A-type ordering as observed in CaCo2As2 or of other common magnetic structures.

cond-mat.str-el↗

arXiv2021

Defect-driven ferrimagnetism and hidden magnetization in MnBi$_2$Te$_4$

MnBi$_2$Te$_4$ (MBT) materials are promising antiferromagnetic topological insulators where field driven ferromagnetism is predicted to cause a transition between axion insulator and Weyl semimetallic states. However, the presence of antiferromagnetic coupling between Mn/Bi antisite defects and the main Mn layer can reduce the low-field magnetization, and it has been shown that such defects are more prevalent in the structurally identical trivial magnetic insulator MnSb$_2$Te$_4$ (MST). We use high-field magnetization measurements to show that the magnetization of MBT and MST occur in stages and full saturation requires fields of~$\sim$~60 Tesla. As a consequence, the low-field magnetization plateau state in MBT, where many determinations of quantum anomalous Hall state are studied, actually consists of ferrimagnetic septuple blocks containing both a uniform and staggered magnetization component.

cond-mat.mtrl-sci↗

arXiv2021

Evolution of Magnetic Interactions in Sb-substituted MnBi2Te4

The Mn(Bi$_{1-x}$Sb$_x$)$_2$Te$_4$ series is purported to span from antiferromagnetic (AF) topological insulator at x = 0 to a trivial AF insulator at x = 1. Here we report on neutron diffraction and inelastic neutron scattering studies of the magnetic interactions across this series. All compounds measured possess ferromagnetic (FM) triangular layers and we find a crossover from AF to FM interlayer coupling near x = 1 for our samples. The large spin gap at x = 0 closes rapidly and the average FM exchange interactions within the triangular layer increase with Sb substitution. Similar to a previous study of MnBi$_2$Te$_4$, we find severe spectral broadening which increases dramatically across the compositional series. In addition to broadening, we observe an additional sharp magnetic excitation in MnSb$_2$Te$_4$ that may indicate the development of local magnetic modes based on recent reports of antisite disorder between Mn and Sb sublattices. The results suggest that both substitutional and antisite disorder contribute substantially to the magnetism in Mn(Bi$_{1-x}$Sb$_x$)$_2$Te$_4$.

cond-mat.str-el↗

arXiv2020

Electron correlation effects on exchange interactions and spin excitations in 2D van der Waals materials

Despite serious effort, the nature of the magnetic interactions and the role of electron-correlation effects in magnetic two-dimensional (2D) van der Waals materials remain elusive. Using CrI$_3$ as a model system, we show that the calculated electronic structure including nonlocal electron correlations yields spin excitations consistent with inelastic neutron scattering measurements. Remarkably, this approach identifies an unreported correlation-enhanced interlayer super-superexchange, which rotates the magnon Dirac lines off, and introduces a gap along, the high-symmetry $Γ$-$K$-$M$ path. This discovery provides a different perspective on the gap opening mechanism observed in CrI$_3$, which was previously associated with spin-orbit coupling through the Dzyaloshinskii-Moriya interaction or Kitaev interaction. Our observation elucidates the critical role of electron correlations on the spin ordering and spin dynamics in magnetic van der Waals materials and demonstrates the necessity of explicit treatment of electron correlations in the broad family of 2D magnetic materials.

cond-mat.mtrl-sci↗

arXiv2020

X-ray spectra in magnetic van der Waals materials Fe$_3$GeTe$_2$, CrI$_3$, and CrGeTe$_3$: a first-principles study

Using density functional theory (DFT) methods, we have calculated X-ray absorption spectroscopy (XAS) and X-ray circular dichroism (XMCD) spectra in bulk and thin films of Fe$_3$GeTe$_2$, CrI$_3$, and CrGeTe$_3$. DFT+$U$ methods are employed for better handling of correlation effects of 3$d$ electrons of transition metals. We discuss relations between the density of states, radial matrix elements, and the corresponding spectra. By comparing the calculated spectra with previously measured spectra, we discuss the reliability of DFT+$U$ methods to describe the electronic structures of these materials and determine the corresponding optimal $U$ and $J$ parameters.

cond-mat.mtrl-sci↗

arXiv2020

Exact Self-Consistent Effective Hamiltonian Theory

We propose a general variational fermionic many-body wavefunction that generates an effective Hamiltonian in a quadratic form, which can then be exactly solved. The theory can be constructed within the density functional theory framework, and a self-consistent scheme is proposed for solving the exact density functional theory. We apply the theory to structurally-disordered systems, symmetric and asymmetric Hubbard dimers, and the corresponding lattice models. The single fermion excitation spectra show a persistent gap due to the fermionic-entanglement-induced pairing condensate. For disordered systems, the density of states at the edge of the gap diverges in the thermodynamic limit, suggesting a topologically ordered phase. A sharp resonance is predicted as the gap is not dependent on the temperature of the system. For the symmetric Hubbard model, the gap for both half-filling and doped case suggests that the quantum phase transition between the antiferromagnetic and superconducting phases is continuous.

cond-mat.str-el↗

arXiv2020

Role of non-locality in exchange-correlation for magnetic 2D van der Waals materials

To obtain accurate independent-particle descriptions for ferromagnetic two-dimensional van der Waals materials, we apply the quasiparticle self-consistent $GW$ (QSGW) method to VI$_3$, CrI$_3$, CrGeTe$_3$, and Fe$_3$GeTe$_2$. QSGW provides a description of the nonlocal exchange-correlation term in the one-particle Hamiltonian. The nonlocal term is important not only as the $U$ of density functional theory (DFT)+$U$ but also for differentiating occupied and unoccupied states in semiconductors. We show the limitations of DFT+$U$ in mimicking QSGW.

cond-mat.str-el↗

arXiv2020

Spin Dynamics in the Antiferromagnetic Oxypnictides and Fluoropnictides: LaMnAsO, LaMnSbO, and BaMnAsF

Inelastic neutron scattering (INS) from polycrystalline antiferromagnetic LaMnAsO, LaMnSbO, and BaMnAsF are analyzed using a $J_1-J_2-J_c$ Heisenberg model in the framework of the linear spin-wave theory. All three systems show clear evidence that the nearest- and next-nearest-neighbor interactions within the Mn square lattice layer ($J_1$ and $J_2$) are both antiferromagnetic (AFM). However, for all compounds studied the competing interactions have a ratio of $2J_2/J_1 < 1$, which favors the square lattice checkerboard AFM structure over the stripe AFM structure. The inter-plane coupling $J_c$ in all three systems is on the order of $\sim 3\times10^{-4}J_1$, rendering the magnetic properties of these systems with quasi-two-dimensional character. The substitution of Sb for As significantly lowers the in-plane exchange coupling, which is also reflected in the decrease of the N{é}el temperature, $T_{\rm N}$. Although BaMnAsF shares the MnAs sheets as LaMnAsO, their $J_1$ and $J_2$ values are substantially different. Using density functional theory, we calculate exchange parameters $J_{ij}$ to rationalize the differences among these systems.

cond-mat.str-el↗

arXiv2020

Deterministic strain-control of stability and current-induced motion of skyrmions in chiral magnets

External magnetic field, temperature, and spin-polarized current are usually employed to create and control nanoscale vortex-like spin configurations such as magnetic skyrmions. Although these methods have proven successful, they are not energy-efficient due to high power consumption and dissipation. Coupling between magnetic properties and mechanical deformation, the magnetoelastic (MEL) effect, offers a novel approach to energy-efficient control of magnetism at the nanoscale. It is of great interest in the context of ever-decreasing length scales of electronic and spintronic devices. Therefore, it is desirable to establish a comprehensive framework capable of predicting the effects of mechanical stress and enabling deterministic control of magnetic textures and skyrmions. In this work, using an advanced scheme of multiscale simulations and Lorentz transmission electron microscopy measurements we demonstrate deterministic control of topological magnetic textures and skyrmion creation in thin films and racetracks of chiral magnets. Our investigation considers not only uniaxial but also biaxial stress, which is ubiquitous in thin-film devices. The biaxial stress, rather than the uniaxial one, was shown to be more efficient to create or annihilate skyrmions when the MEL coefficient and strain have the same or opposite signs, respectively. It was also demonstrated to be a viable way to stabilize skyrmions and to control their current-induced motion in racetrack memory. Our results open prospects for deployment of mechanical stress to create novel topological spin textures, including merons, and in control and optimization of skyrmion-based devices.

cond-mat.mtrl-sci↗

arXiv2020

Electron irradiation effects on superconductivity in PdTe$_2$: an application of a generalized Anderson theorem

Low temperature ($\sim$ 20~K) electron irradiation with 2.5 MeV relativistic electrons was used to study the effect of controlled non-magnetic disorder on the normal and superconducting properties of the type-II Dirac semimetal PdTe$_2$. We report measurements of longitudinal and Hall resistivity, thermal conductivity and London penetration depth using tunnel-diode resonator technique for various irradiation doses. The normal state electrical resistivity follows Matthiessen rule with an increase of the residual resistivity at a rate of $\sim$0.77$ μΩ$cm/$(\textrm{C}/\textrm{cm}^2)$. London penetration depth and thermal conductivity results show that the superconducting state remains fully gapped. The superconducting transition temperature is suppressed at a non-zero rate that is about sixteen times slower than described by the Abrikosov-Gor'kov dependence, applicable to magnetic impurity scattering in isotropic, single-band $s$-wave superconductors. To gain information about the gap structure and symmetry of the pairing state, we perform a detailed analysis of these experimental results based on insight from a generalized Anderson theorem for multi-band superconductors. This imposes quantitative constraints on the gap anisotropies for each of the possible pairing candidate states. We conclude that the most likely pairing candidate is an unconventional $A_{1g}^{+-}$ state. While we cannot exclude the conventional $A_{1g}^{++}$ and the triplet $A_{1u}$, we demonstrate that these states require additional assumptions about the orbital structure of the disorder potential to be consistent with our experimental results, e.g., a ratio of inter- to intra-band scattering for the singlet state significantly larger than one. Due to the generality of our theoretical framework, we think that it will also be useful for irradiation studies in other spin-orbit-coupled multi-orbital systems.

cond-mat.supr-con↗

arXiv2019

Mechanisms of skyrmion and skyrmion crystal formation from the conical phase

Real-space topological magnetic structures such as skyrmions and merons are promising candidates for information storage and transport. However, the microscopic mechanisms that control their formation and evolution are still not clear. Here, using in-situ Lorentz transmission electron microscopy, we demonstrate that skyrmion crystals (SkXs) can nucleate, grow, and evolve from the conical phase in the same ways that real nanocrystals form from vapors or solutions. More intriguingly, individual skyrmions can also "reproduce" by division in a mitosis-like process that allows them to annihilate SkX lattice imperfections, which is not available to crystals made of mass-conserving particles. Combined string method and micromagnetic calculations show that competition between repulsive and attractive interactions between skyrmions governs particle-like SkX growth, but non-conservative SkX growth appears to be defect-mediated. Our results provide insights towards manipulating magnetic topological states by applying established crystal growth theory, adapted to account for the new process of skyrmion mitosis.

cond-mat.mtrl-sci↗

arXiv2019

Competing magnetic interactions in the antiferromagnetic topological insulator MnBi$_{2}$Te$_{4}$

The antiferromagnetic (AF) compound MnBi$_{2}$Te$_{4}$ is suggested to be the first realization of an antiferromagnetic (AF) topological insulator. Here we report on inelastic neutron scattering studies of the magnetic interactions in MnBi$_{2}$Te$_{4}$ that possess ferromagnetic (FM) triangular layers with AF interlayer coupling. The spin waves display a large spin gap and pairwise exchange interactions within the triangular layer are frustrated due to large next-nearest neighbor AF exchange. The degree of frustration suggests proximity to a variety of magnetic phases, potentially including skyrmion phases, that could be accessed in chemically tuned compounds or upon the application of symmetry-breaking fields.

cond-mat.str-el↗

arXiv2019

Intersublattice magnetocrystalline anisotropy using a realistic tight-binding method based on maximally localized Wannier functions

Using a realistic tight-binding Hamiltonian based on maximally localized Wannier functions, we investigate the two-ion magnetocrystalline anisotropy energy (MAE) in $L1_0$ transition metal compounds. MAE contributions from throughout the Brillouin zone are obtained using magnetic force theorem calculations with and without perturbation theory. The results from either method agree with one another, and both reflect features of the Fermi surface. The intra-sublattice and inter-sublattice contributions to MAE are evaluated using a Green's function method. We find that the sign of the inter-sublattice contribution varies among compounds, and that its amplitude may be significant, suggesting MAE can not be resolved accurately in a single-ion manner. The results are further validated by scaling spin-orbit-coupling strength in density functional theory. Overall, this realistic tight-binding method provide an effective approach to evaluate and analyze MAE while retaining the accuracy of corresponding first-principles methods.

cond-mat.mtrl-sci↗

arXiv2018

On spinodal decomposition in alnico---a transmission electron microscopy and atom probe tomography study

Alnico is a prime example of a finely tuned nanostructure whose magnetic properties are intimately connected to magnetic annealing (MA) during spinodal transformation and subsequent lower temperature annealing (draw) cycles. Using a combination of transmission electron microscopy and atom probe tomography, we show how these critical processing steps affect the local composition and nanostructure evolution with impact on magnetic properties. The nearly 2-fold increase of intrinsic coercivity ($H_\text{ci}$) during the draw cycle is not adequately explained by chemical refinement of the spinodal phases. Instead, increased Fe-Co phase ($α_1$) isolation, development of Cu-rich spheres/rods/blades and additional $α_1$ rod precipitation that occurs during the MA and draw, likely play a key role in $H_\text{ci}$ enhancement. Chemical ordering of the Al-Ni-phase ($α_2$) and formation of Ni-rich ($α_3$) may also contribute. Unraveling of the subtle effect of these nano-scaled features is crucial to understanding on how to improve shape anisotropy in alnico magnets.

cond-mat.mtrl-sci↗

arXiv2018

Origin of magnetic anisotropy in doped Ce$_2$Co$_{17}$ alloys

Magnetocrystalline anisotropy (MCA) in doped Ce$_{2}$Co$_{17}$ and other competing structures was investigated using density functional theory. We confirmed that the MCA contribution from dumbbell Co sites is very negative. Replacing Co dumbbell atoms with a pair of Fe or Mn atoms greatly enhance the uniaxial anisotropy, which agrees quantitatively with experiment, and this enhancement arises from electronic-structure features near the Fermi level, mostly associated with dumbbell sites. With Co dumbbell atoms replaced by other elements, the variation of anisotropy is generally a collective effect and contributions from other sublattices may change significantly. Moreover, we found that Zr doping promotes the formation of 1-5 structure that exhibits a large uniaxial anisotropy, such that Zr is the most effective element to enhance MCA in this system.

cond-mat.mtrl-sci↗

arXiv2017

Microstructural and magnetic property evolution with different heat-treatment conditions in an alnico alloy

Further property enhancement of alnico, an attractive near-term, non-rare-earth permanent magnet alloy system, primarily composed of Al, Ni, Co, and Fe, relies on improved morphology control and size refinement of its complex spinodally decomposed nanostructure that forms during heat-treatment. Using a combination of transmission electron microscopy and atom probe tomography techniques, this study evaluates the magnetic properties and microstructures of an isotropic 32.4Fe-38.1Co-12.9Ni-7.3Al-6.4Ti-3.0Cu (wt.$\%$) alloy in terms of processing parameters such as annealing temperature, annealing time, application of an external magnetic field, as well as low-temperature "draw" annealing. Optimal spinodal morphology and spacing is formed within a narrow temperature and time range ($\sim 840 \unicode{x2103}$ and 10 min during thermal-magnetic annealing (MA). The ideal morphology is a mosaic structure consisting of periodically arrayed $\sim 40$ nm diameter (Fe-Co)-rich rods ($α_1$ phase) embedded in an (Al-Ni)-rich ($α_2$ phase) matrix. A Cu-enriched phase with a size of $\sim$ 3-5 nm is located at the corners of two adjacent $\{110\}$ facets of the $α_1$ phase. The MA process significantly increased remanence ($B_\text{r}$) ($\sim$ 40-70 $\%$) of the alloy due to biased elongation of the $α_1$ phase along the $\langle100\rangle$ crystallographic direction, which is closest in orientation to the applied magnetic field. The optimum magnetic properties of the alloy with an intrinsic coercivity ($H_\text{cj}$) of 1845 Oe and a maximum energy product ($BH_\text{max}$) of 5.9 MGOe were attributed to the uniformity of the mosaic structure.

cond-mat.mtrl-sci↗

arXiv2017

Simulation of alnico coercivity

Micromagnetic simulations of alnico show substantial deviations from Stoner-Wohlfarth behavior due to the unique size and spatial distribution of the rod-like Fe-Co phase formed during spinodal decomposition in an external magnetic field. The maximum coercivity is limited by single-rod effects, especially deviations from ellipsoidal shape, and by interactions between the rods. Both the exchange interaction between connected rods and magnetostatic interaction between rods are considered, and the results of our calculations show good agreement with recent experiments. Unlike systems dominated by magnetocrystalline anisotropy, coercivity in alnico is highly dependent on size, shape, and geometric distribution of the Fe-Co phase, all factors that can be tuned with appropriate chemistry and thermal-magnetic annealing.

cond-mat.mtrl-sci↗