The lattice dynamic properties and spin-phonon coupling in DyMn$_2$O$_5$ are studied by using the density-functional theory. The calculated phonon frequencies are in very good agreement with experiments. We then compare the phonon modes calculated from different spin configurations. The results show that the phonon frequencies change substantially in different spin configurations, suggesting that the spin-phonon coupling in this material is very strong. Especially, the short range spin ordering has drastic effects on the highest Raman and IR phonon modes that might be responsible for the observed phonon anomalies near and above the magnetic phase transitions.
A novel general method of describing the spin-lattice interactions in magnetic solids was proposed in terms of first principles calculations. The spin exchange and Dzyaloshinskii-Moriya interactions as well as their derivatives with respect to atomic displacements can be evaluated efficiently on the basis of density functional calculations for four ordered spin states. By taking into consideration the spin-spin interactions, the phonons, and the coupling between them, we show that the ground state structure of a representative spin-frustrated spinel, MgCr2 O4, is tetragonally distorted, in agr…
On the basis of first-principles calculations we show that the M-type hexaferrite BaFe12O19 exhibits frustrated antiferroelectricity associated with its trigonal bipyramidal Fe3+ sites. The ferroelectric (FE) state of BaFe12O19, reachable by applying an external electric field to the antiferroelectric (AFE) state, can be made stable at room temperature by appropriate element substitution or strain engineering. Thus M-type hexaferrite, as a new type of multiferoic with coexistence of antiferroelectricity and ferrimagnetism, provide a basis for studying the phenomenon of frustrated antiferroelec…
We have studied the influence of magnetic order on the optical phonons of the geometrically frustrated spinel ZnCr$_2$O$_4$ from first-principles. By mapping the first-principles phonon calculations onto a Heisenberg-like model, we developed a method to calculate exchange derivatives and subsequently the spin-phonon couping parameter from first-principles. All calculations were performed within LSDA+U.
In this article, we report negative thermal expansion and spin frustration in hexagonal GdInO$_{3}$. Rietveld refinement of the XRD patterns reveal that the negative thermal expansion in the temperature range of 50-100K stems from the triangular lattice of Gd$^{3+}$ ions. At low temperature, the downward deviation of the inverse susceptibility ($χ^{-1}$) vs. $T$ plot from the Curie-Weiss law indicates spin frustration which inhibits long-range magnetic ordering down to 2K. Magnetostriction measurements clearly demonstrate a strong spin-lattice coupling. Low temperature anomalous phonon softeni…
Magnetism in single-side hydrogenated (C$_2$H) and fluorinated (C$_2$F) graphene is analyzed in terms of the Heisenberg model with parameters determined from first principles. We predict a frustrated ground state for both systems, which means the instability of collinear spin structures and sheds light on the absence of a conventional magnetic ordering in defective graphene demonstrated in recent experiments. Moreover, our findings suggest a highly correlated magnetic behavior at low temperatures offering the possibility of a spin-liquid state.
Frustrated magnets are one class of fascinating materials that host many intriguing phases such as spin ice, spin liquid and complex long-range magnetic orderings at low temperatures. In this work we use first-principles calculations to find that in a wide range of magnetically frustrated oxides, at zero temperature a number of non-collinear magnetic orderings are more stable than the type-I collinear ordering that is observed at finite temperatures. The emergence of non-collinear orderings in those complex oxides is due to higher-order exchange interactions that originate from second-row and …
Weyl semimetal is a topologically non-trivial phase of matter with pairs of Weyl nodes in the k-space, which act as monopole and anti-monopole pairs of Berry curvature. Two hallmarks of the Weyl metallic state are the topological surface state called the Fermi arc and the chiral anomaly. It is known that the chiral anomaly yields anomalous magneto-transport phenomena. In this study, we report the emergence of the type-II Weyl semimetallic state in the geometrically frustrated non-collinear antiferromagnetic Shastry-Sutherland lattice (SSL) GdB4 crystal. When we apply magnetic fields perpendicu…
We report a detailed examination the magnetic structure of anhydrous cupric chloride CuCl2 carried out by powder neutron diffraction, magnetic susceptibility and specific heat measurements on polycrystalline and single crystal samples as well as an evaluation of the spin exchange interactions by first principles density functional theory (DFT) calculations. Anhydrous CuCl2 shows one dimensional antiferromagnetic behavior and long range antiferromagnetic ordering below a Neel temperature of 23.9 K. Neutron powder and single crystal diffraction reveal that, below 23.9K, CuCl2 undergoes a phase t…
Absence of magnetic ordering in Bi$_3$Mn$_4$O$_{12}$(NO$_3$), (BMNO) which has a magnetic subsystem that consists of honeycomb bi-layers of Mn$^{4+}$ ions with spin S=3/2, has raised the expectation that its ground state is strongly frustrated due to longer-range antiferromagnetic interactions. We calculate the magnetic exchange coupling constants of the BMNO complex within a density functional approach and find that the dominating interactions between Mn spins are the antiferromagnetic nearest-neighbor $J_1$ and interlayer interaction $J_c$. The largest interaction is $J_c$, which substantial…
By using a fully relativistic embedded cluster Green's function technique we investigated the magnetic anisotropy properties of four different compact Cr trimers (equilateral triangles) and Cr mono-layers deposited on Au(111) surface in both fcc and hcp stackings. For all trimers the magnetic ground state was found a frustrated 120$^\circ$ Néel configuration. Applying global spin rotations to the magnetic ground state, the predictions of an appropriate second order spin Hamiltonian were reproduced with high accuracy by the first principles calculations. For the Cr trimers with adjacent Au atom…
Kagome-net, appearing in areas of fundamental physics, materials, photonic and cold-atom systems, hosts frustrated fermionic and bosonic excitations. However, it is extremely rare to find a system to study both fermionic and bosonic modes to gain insights into their many-body interplay. Here we use state-of-the-art scanning tunneling microscopy and spectroscopy to discover unusual electronic coupling to flat-band phonons in a layered kagome paramagnet. Our results reveal the kagome structure with unprecedented atomic resolution and observe the striking bosonic mode interacting with dispersive …
A description of non-collinear magnetism in the framework of spin-density functional theory is presented for the exact exchange energy functional which depends explicitly on two-component spinor orbitals. The equations for the effective Kohn-Sham scalar potential and magnetic field are derived within the optimized effective potential (OEP) framework. With the example of a magnetically frustrated Cr monolayer it is shown that the resulting magnetization density exhibits much more non-collinear structure than standard calculations. Furthermore, a time-dependent generalization of the non-collinea…
Intrinsic magnetic van der Waals (vdW) materials have attracted much attention, especially Fe$_{3}$GeTe$_{2}$ (FGT), which exhibits highly tunable properties. However, despite vast efforts, there are still several challenging issues to be resolved. Here using a first-principles linear-response approach, we carry out comprehensive investigation of both bulk and monolayer FGT. We find that although the magnetic exchange interactions in FGT are frustrated, our Monte Carlo simulations agree with the total energy calculations, confirming that the ground state of bulk FGT is indeed ferromagnetic (FM…
Coexistence of static order and spin dynamics in an S = 5/2 frustrated triangular antiferromagnet
Indian Institute of Technology Madras（马德拉斯理工学院）；Jožef Stefan Institute（约热·斯特凡研究所）；University of Ljubljana（卢布尔雅那大学）；ISIS Neutron and Muon Source, Rutherford Appleton Laboratory（卢瑟福阿普尔顿实验室 ISIS 中子与缪子源）；R. B. College (A Constituent Unit of Lalit Narayan Mithila University, Darbhanga)（R.B.学院（拉尔纳拉扬·米提拉大学达布汉加附属单位））
We present a first-principles investigation of the spin-ice state in Dy$_2$Ti$_2$O$_7$ using a magnetic source-free exchange and correlation functional, implemented in the Castep electronic-structure code. By comparing results from the conventional local spin-density approximation, we show that a spin-ice state in Dy$_2$Ti$_2$O$_7$ can be reliably obtained by removing the magnetic sources from the exchange and correlation contributions to the potential, and we contrast this against the computed ground states of other frustrated pyrochlore magnets.
The mechanism of spontaneous exchange bias (SEB) and the dominant factor of its blocking temperature are still unclear in Heusler alloys. Here, the related investigations are performed in Mn2Ni1.5Al0.5 Heusler alloys with SEB. The results of both magnetic measurements and first-principles calculations confirmed that spin frustrated and unfrustrated antiferromagnetic (AFM) states coexist there and they have different magnetic anisotropies, which are essential for SEB. Based on a series of measurement strategies, we demonstrate that the frustrated AFM state undergoes a first-order magnetic trans…
Interlocked Vortex Order in the Frustrated $A_3$V$_9$Te$_{13}$ Lattice ($A$=Cs,Rb)
New Cornerstone Science Laboratory, Center for Correlated Matter, Zhejiang University（新Cornerstone科学实验室，关联物质中心，浙江大学）；School of Physics, Zhejiang University（物理学院，浙江大学）；Institute for Advanced Study in Physics, Zhejiang University（物理学高等研究院，浙江大学）
We investigate the magnetic properties of Ru$_{2}$Mn$Z$ ($Z$ = Sn, Sb, Ge, Si) chemically ordered full Heusler compounds for zero as well as finite temperatures. Based on first principles calculations we derive the interatomic isotropic bilinear and biquadratic couplings between Mn atoms from the paramagnetic state. We find frustrated isotropic couplings for all compounds and in case of $Z$ = Si and Sb a nearest-neighbor biquadratic coupling that favors perpendicular alignment between the Mn spins. By using an extended classical Heisenberg model in combination with spin dynamics simulations we…
We have examined the effect of a c(2x2) overlayer of CO on the surface phonons of the substrate, Cu(001), by applying the density functional perturbation theory with both the local (LDA) and the generalized-gradient (GGA) density approximations, through the Hedin-Lundqvist and the Perdew-Burke-Ernzerhof functionals, respectively. Our results (GGA) trace the Rayleigh wave softening detected by helium atom scattering (HAS) experiments to changes in the force constants between the substrate surface atoms brought about by CO chemisorption, resolving an ongoing debate on the subject. The calculated…
First principles density functional theory DFT+U calculations and experimental neutron diffraction structure analyses were used to determine the low-temperature crystallographic and magnetic structure of bixbyite Mn2O3. The energies of various magnetic arrangements, calculated from first principles, were fit to a cluster-expansion model using a Bayesian method that overcomes a problem of underfitting caused by the limited number of input magnetic configurations. The model was used to predict the lowest-energy magnetic states. Experimental determination of magnetic structure benefited from opti…
We present a detailed first principles study of Fe-pnictides with particular emphasis on competing magnetic interactions, structural phase transition, giant magneto-elastic coupling and its effect on phonons. The exchange interactions $J_{i,j}(R)$ are calculated up to $\approx 12 $Å$. We find that $J_{i,j}(R)$ has an oscillatory character with an envelop decaying as $1/R^3$ along the stripe-direction while it is very short range along the diagonal direction and antiferromagnetic. A brief discussion of the neutron scattering determination of these exchange constants from a single crystal sample…
Cu(1,3-benzenedicarboxylate) [Cu(1,3-bdc)] contains structurally perfect kagomé planes formed by Cu$^{2+}$ ions without the presence of diamagnetic defects. This organometallic compound should have served as a precious platform to explore quantum frustrated magnetism, yet the experimental results so far are mysterious, leading to questions such as "Is Cu(1,3-bdc) just a trivial weak ferromagnet?". Using the the density functional theory, we have systematically studied the electronic and magnetic properties of Cu(1,3-bdc), putting forth a theoretical basis to clarify this novel material. We pre…
We present calculations of the magnetic ground states of Cr trimers in different geometries on top of a Au(111) surface. By using a least square fit method based on a fully relativistic embedded-cluster Green's function method first we determined the parameters of a classical vector-spin model consisting of second and fourth order interactions. The newly developed method requires no symmetry constraints, therefore, it is throughout applicable for small nanoparticles of arbitrary geometry. The magnetic ground states were then found by solving the Landau-Lifshitz-Gilbert equations. In all consid…
We present a model of the lattice dynamics of the rare earth titanate pyrochlores R2Ti2O7 (R=Tb, Dy, Ho), which are important materials in the study of frustrated magnetism. The phonon modes are obtained by density functional calculations, and these predictions are verified by comparison with scattering experiments. Single crystal inelastic neutron scattering is used to measure acoustic phonons along high symmetry directions for R=Tb, Ho; single crystal inelastic x-ray scattering is used to measure numerous optical modes throughout the Brillouin zone for R=Ho; and powder inelastic neutron scat…
Designing electronic magnetoelectric matter with organic quantum spin trimers
Osaka Metropolitan University（大阪公立大学）；University of Florida（佛罗里达大学）；Shanghai Jiao Tong University（上海交通大学）；Osaka Prefecture University（大阪府立大学）；Florida State University（佛罗里达州立大学）；National High Magnetic Field Laboratory, Florida State University（佛罗里达州立大学国家高磁场实验室）
Noncollinear antiferromagnets (AFMs) have recently attracted a lot of attention owing to the potential emergence of exotic spin orders on geometrically frustrated lattices, which can be characterized by corresponding spin chiralities. By performing first-principles density functional calculations together with group-theory analysis and tight-binding modelling, here we systematically study the spin-order dependent anomalous Hall effect (AHE) and magneto-optical effect (MOE) in representative noncollinear AFMs Mn$_{3}X$N ($X$ = Ga, Zn, Ag, and Ni). The symmetry-related tensor shape of the intrin…
Rigorous extension of semilocal collinear functionals to noncollinear DFT using $SU(2)$ rotations
Helmholtz Institut Mainz（亥姆霍兹美因茨研究所）；GSI Helmholtzzentrum für Schwerionenforschung GmbH（GSI重离子研究中心有限公司）；Institut für Physik, Johannes Gutenberg-Universität Mainz（美因茨约翰内斯·古腾堡大学物理研究所）
Role of composition-tuned disorder on magnetic exchange interactions in NiRuMnGa
National Institute of Technology Andhra Pradesh（安得拉邦国立技术学院）；Indian Institute of Science Education and Research Berhampur（布兰普尔科学教育与研究所）；ENSICAEN, UNICAEN（恩西卡昂大学，卡昂大学）
We propose an atom-superposition-based method for simulating spin-polarized scanning tunneling microscopy (SP-STM) from first principles. Our approach provides bias dependent STM images in high spatial resolution, with the capability of using either constant current or constant height modes of STM. In addition, topographic and magnetic contributions can clearly be distinguished, which are directly comparable to results of SP-STM experiments in the differential magnetic mode. Advantages of the proposed method are that it is computationally cheap, it is easy to parallelize, and it can employ the…
Spin-1 antiferromagnets are abundant in nature, but few theories or results exist to understand their general properties and behavior, particularly in situations when geometric frustration is present. Here we study the $S=1$ Kagome compound Na$_2$Ti$_3$Cl$_8$ using a combination of Density Functional Theory, Exact Diagonalization, and Density Matrix Renormalization Group methods to achieve a first principles supported explanation of exotic magnetic phases in this compound. We find that the effective magnetic Hamiltonian includes essential non-Heisenberg terms that do not stem from spin-orbit c…
The origin of the spin-glass state in (Fe,Sn)4N alloys is studied on the basis of a Heisenberg Hamiltonian with parameters derived from first principles within the magnetic force theorem applied in the framework of the disordered local moments method and local spin-density approximation. We show that in the alloy concentration range where the spin-glass state is stable only one Fe sublattice is intrinsically magnetic and the interatomic exchange magnetic interactions are essentially short ranged due to effects of chemical and magnetic disorder. The magnetic Fe atoms with well-localized spin mo…
Van der Waals (VdW) materials have opened new directions in the study of low dimensional magnetism. A largely unexplored arena is the intrinsic tuning of VdW magnets toward new ground-states. The chromium trihalides provided the first such example with a change of inter-layer magnetic coupling emerging upon exfoliation. Here, we take a different approach to engineer new ground-states, not by exfoliation, but by tuning the spin-orbit coupling (SOC) of the non-magnetic ligand atoms (Cl,Br,I). We synthesize a three-halide series, CrCl$_{3-x-y}$Br$_{x}$I$_{y}$, and map their magnetic properties as…
Landau theory and symmetry considerations lead us to propose an explanation for several seemingly paradoxical behaviors of charge ordering (CO) and spin ordering (SO) in the mixed valence compound LuFe2O4. Both SO and CO are highly frustrated. We analyze a lattice gas model of CO within mean field theory and determine the magnitude of several of the phenomenological interactions. We show that the assumption of a continuous phase transition at which CO or SO develops implies that both CO and SO are incommensurate. To explain how ferroelectric fluctuations in the charge disordered phase can be c…
