Noncentrosymmetric Triangular Magnet CaMnTeO$_6$: Strong Quantum Fluctuations and Role of s0 vs. s2 Electronic States in Competing Exchange Interactions
Xudong Huai, Emmanuel Acheampong, Erich Delles, Michał J. Winiarski, Maurice Sorolla, Lila Nassar, Mingli Liang, Caleb Ramette, Huiwen Ji, Allen Scheie, Stuart … 展开作者
Xudong Huai, Emmanuel Acheampong, Erich Delles, Michał J. Winiarski, Maurice Sorolla, Lila Nassar, Mingli Liang, Caleb Ramette, Huiwen Ji, Allen Scheie, Stuart Calder, Martin Mourigal, Thao T. Tran
非中心对称三角磁体为实现强量子涨落提供了独特平台。然而，由于在原子层面上对竞争交换相互作用的可调性存在知识空白，设计这类量子材料仍然是一个开放性挑战。在此，我们基于细致的化学和物理考量，创造了一种新的非中心对称三角 S = 3/2 磁体 CaMnTeO$_6$。该模型材料表现出竞争性磁相互作用，并具有非线性光学响应，能够产生相干光子。CaMnTeO$_6$ 的非公度磁基态具有异常大的自旋转角 127°(1)，表明各向异性层间交换作用很强，并与各向同性层间 Heisenberg 相互作用相互竞争。从低温热容和中子衍射测量中提取的磁矩为 1.39(1) $μ$B，仅为静态磁矩期望值 3 $μ$B 的 46%。这一降低表明在半整数自旋 S = 3/2 的 CaMnTeO$_6$ 磁体中存在强量子涨落，这是罕见的。通过比较 AMnTeO$_6$（A = Ca, Sr, Pb）的自旋极化能带结构、化学键合和物理性质，我们展示了量子化学解释如何能够阐明对磁交换相互作用基本原理的深入理解，为以原子级精确控制来调制自旋动力学提供了有力工具。
英文摘要：
Noncentrosymmetric triangular magnets offer a unique platform for realizing strong quantum fluctuations. However, designing these quantum materials remains an open challenge attributable to a knowledge gap in the tunability of competing exchange interactions at the atomic level. Here, we create a new noncentrosymmetric triangular S = 3/2 magnet CaMnTeO$_6$ based on careful chemical and physical considerations. The model material displays competing magnetic interactions and features nonlinear optical responses with the capability of generating coherent photons. The incommensurate magnetic ground state of CaMnTeO$_6$ with an unusually large spin rotation angle of 127 deg.(1) indicates that the anisotropic interlayer exchange is strong and competing with the isotropic interlayer Heisenberg interaction. The moment of 1.39(1) $μ$B, extracted from low-temperature heat capacity and neutron diffraction measurements, is only 46% of the expected value of the static moment 3 $μ$B. This reduction indicates the presence of strong quantum fluctuations in the half-integer spin S = 3/2 CaMnTeO$_6$ magnet, which is rare. By comparing the spin-polarized band structure, chemical bonding, and physical properties of AMnTeO$_6$ (A = Ca, Sr, Pb), we demonstrate how quantum-chemical interpretation can illuminate insights into the fundamentals of magnetic exchange interactions, providing a powerful tool for modulating spin dynamics with atomically precise control.
The Loewdin orthogonalization procedure being the well-known technique, particularly in quantum chemistry, however, gives rise to novel effects missed in earlier studies. Making use of the technique of irreducible tensorial operators we have developed a regular procedure for account of the orthogonalization effects. For illustration we address the emergence of a specific magnetoelectric coupling for noncentrosymmetric 3d or 4f ions.
It is well known that if a crystal structure has no inversion symmetry, it may allow for Dzyaloshinskii-Moriya magnetic interactions, operating between different crystallographic unit cells, which in turn should lead to the formation of long-periodic spin-spiral structures. Such a behavior is anticipated for two simple perovskites PbVO3 and BiCoO3, crystallizing in the noncentrosymmetric tetragonal P4mm structure. Nevertheless, we argue that in reality PbVO3 and BiCoO3 should behave very differently. Due to the fundamental Kramers degeneracy for the odd-electron systems, PbVO3 has no single-io…
We have investigated anomalous Hall effect and magnetoresistance in a noncentrosymmetric itinerant magnet Cr$_{11}$Ge$_{19}$. While the temperature- and magnetic-field-dependent anomalous Hall conductivity is just proportional to the magnetization above 30 K, it is more enhanced in the lower temperature region. The magnitude of negative magnetoresistance begins to increase toward low temperature around 30 K. The anisotropic magnetoresistance emerges at similar temperature. Because there is no anomaly in the temperature dependence of magnetization around 30 K, the origin of these observations i…
The feasibility of a single-domain ferromagnet based on uniaxial magnetic ions was examined. For a noncentrosymmetric uniaxial magnetic ion of magnetic moment at a site of local electric dipole moment p, it is unknown to date whether the magnetic moment prefers to be parallel or antiparallel to the electric dipole moment. The nature of this magnetoelectric interaction was probed in terms of analogical reasoning based on the Rashba effect and density functional calculations. We show that the magnetic and electric dipole moments prefer an antiparallel arrangement, predict that Fe-doped CaZnOS is…
Materials containing multiple topological characteristics become more exotic when combined with noncentrosymmetric crystal structures and unusual magnetic phases such as the compensated half-metal state, which is gapped in one spin direction and conducting in the other. First principles calculations reveal these multiple topological features in the compensated half-metal Cr$_2$CoAl having neither time-reversal nor inversion symmetries. In the absence of (minor) spin-orbit coupling (SOC), there are (1) a total of twelve pairs of magnetic Weyl points, (2) three distinct sets of triple nodal poin…
We predict the phenomenon of antiferroelectric resonance (AFER), in which an ac electric field causes magnetic ions located at noncentrosymmetric positions in a multi-sublattice magnet to undergo magnetic transitions corresponding to exchange collective excitations of the system. We construct a theory of such resonances, and show that in magnets with collinear magnetic structures AFER is caused by relativistic and exchange-relativistic magnetoelectric interactions, while in the noncollinear magnets a significant contribution can also come from the exchange magnetoelectric interaction. We predi…
Multiple-$Q$ magnetic states often induce nontrivial topological spin textures, such as a skyrmion and a hedgehog. We theoretically investigate yet another multiple-$Q$ state with topological defects, a meron-antimeron crystal (MAX), represented by a periodic array of the meron and antimeron with a half-integer skyrmion number. Performing simulated annealing for an effective spin model of noncentrosymmetric itinerant magnets on a triangular lattice, we show that rectangular-shaped and triangular-shaped MAXs are stabilized by the interplay between the biquadratic interaction arising from the sp…
Analogous to the Hall effect, the Nernst effect is the generation of a transverse voltage due to a temperature gradient in the presence of a perpendicular magnetic field. The Nernst effect has promise for thermoelectric applications and as a probe of electronic structure. In magnetic materials, a so-called anomalous Nernst effect (ANE) is possible in zero magnetic field. Here we report a colossal ANE reaching 23 $μ$V/K in the ferromagnetic metal UCo$_{0.8}$Ru$_{0.2}$Al. Uranium's $5f$ electrons provide strong electronic correlations that lead to narrow bands, which are a known route to produci…
Helical-to-Fan Transitions under Magnetic Fields in the Noncentrosymmetric Tetragonal Magnet EuRhGe$_3$
Hiroshima University（广岛大学）；Institute of Materials Structure Science, High Energy Accelerator Research Organization（高能加速器研究机构材料结构科学研究所）；University of the Ryukyus（琉球大学）；RIKEN Center for Emergent Matter Science（理化学研究所新兴物质科学中心）
The magnetic hedgehog lattice (HL) is a noncoplanar magnetic texture with a periodic array of magnetic monopoles and anti-monopoles. Despite phenomenological and numerical studies thus far, there remain open issues on the microscopic origin, especially with respect to the recent experimental findings of two different types of HLs even at zero magnetic field. Here, we study the stability of the HLs for an effective spin model with long-range interactions arising from itinerant nature of electrons. By variational calculations and simulated annealing, we find that the HLs are stabilized in the gr…
Switching magnetic texture via in-plane magnetic field in noncentrosymmetric dipolar magnets: From skyrmions to antiskyrmions and nontopological magnetic bubbles
We report a comprehensive study of the noncentrosymmetric superconductor Mo$_3$P. Its bulk superconductivity, with $T_c = 5.5$ K, was characterized via electrical resistivity, magnetization, and heat-capacity measurements, while its microscopic electronic properties were investigated by means of muon-spin rotation/relaxation ($μ$SR) and nuclear magnetic resonance (NMR) techniques. In the normal state, NMR relaxation data indicate an almost ideal metallic behavior, confirmed by band-structure calculations, which suggest a relatively high electron density of states, dominated by the Mo $4d$-orbi…
Magnetic skyrmion, i.e. a topologically stable swirling spin texture, appears as a particle-like object in the two-dimensional (2D) systems, and has recently attracted attention as a candidate of novel information carrier. In the real three-dimensional (3D) systems, a skyrmion is expected to form a string structure along an extra dimension, while its experimental identification has rarely been achieved. Here, we report the direct visualization of 3D shape of individual skyrmion strings, for the recently discovered room-temperature skyrmion-hosting noncentrosymmetric compound Mn1.4Pt0.9Pd0.1Sn.…
We study electric polarization and nonlinear optical effects in spin systems with broken inversion symmetry. We apply strong coupling expansion to the underlying electronic Hamiltonians, and systematically derive expressions for electric polarization in spin systems that are represented in terms of spin operators. The magnon representation of the obtained electric polarization operator allows us to compute linear and nonlinear optical responses by the standard diagrammatic method. We apply our formalism to Heisenberg model with alternating coupling constants and $J_1$-$J_2$ model with inversio…
Topological spin textures have attracted much attention both for fundamental physics and spintronics applications. Among them, antiskyrmions possess a unique spin configuration with Bloch-type and Néel-type domain walls due to anisotropic Dzyaloshinskii-Moriya interaction (DMI) in the noncentrosymmetric crystal structure. However, antiskyrmions have thus far only been observed in a few Heusler compounds with $D_{2\mathrm{d}}$ symmetry. Here, we report a new material Fe$_{1.9}$Ni$_{0.9}$Pd$_{0.2}$P in a different symmetry class ($S_4$ symmetry), where antiskyrmions exist over a wide temperature…
Low-temperature thermal conductivity measurements were performed on single crystal of PbTaSe$_2$, a noncentrosymmetric superconductor with topological bulk nodal lines in the electronic band structure. It is found that the residual linear term $κ_0/T$ is negligible in zero magnetic field. Furthermore, the field dependence of $κ_0/T$ exhibits a clear "$S$"-shape curve. These results suggest that PbTaSe$_2$ has multiple nodeless superconducting gaps. Therefore, the spin-triplet state with gap nodes does not play an important role in this noncentrosymmetric superconductor with strong spin-orbital…
The noncentrosymmetric superconductor Re$_{24}$Ti$_{5}$, a time-reversal symmetry (TRS) breaking candidate with $T_c = 6$\,K, was studied by means of muon-spin rotation/relaxation ($μ$SR) and tunnel-diode oscillator (TDO) techniques. At a macroscopic level, its bulk superconductivity was investigated via electrical resistivity, magnetic susceptibility, and heat capacity measurements. The low-temperature penetration depth, superfluid density and electronic heat capacity all evidence an $s$-wave coupling with an enhanced superconducting gap. The spontaneous magnetic fields revealed by zero-field…
We performed $^{75}$As-NMR measurements to investigate the normal-state magnetic properties of CeRh$_2$As$_2$, a recently-discovered heavy-fermion superconductor. The magnitude and temperature dependence of the Knight shift at the As(2) site indicate easy-plane-type magnetic anisotropy in CeRh$_2$As$_2$. With regard to spin fluctuations, the temperature dependence of the nuclear spin-lattice relaxation rate $1/T_1$ arising from the 4$f$ electrons decreases from high-temperature constant behavior on cooling at $\sim$ 40~K, which is typical behavior of heavy-fermion systems. In addition, $1/T_1$…
The noncentrosymmetric NbReSi superconductor with $T_{c} \simeq 6.5$ K is characterized by the relatively large upper critical magnetic field. Its multigap features were observed experimentally. Recent studies suggested realization of P$\bar{6}$2m or Ima2 symmetry. We discuss the dynamical properties of both symmetries (e.g., phonon spectra). In this paper, using the ab initio techniques, we clarify this ambiguity, and conclude that the Ima2 symmetry is unstable, and P$\bar{6}$2m should be realized. The P$\bar{6}$2m symmetry is also stable in the presence of external hydrostatic pressure. We s…
Inelastic neutron scattering (INS) is employed to study damped spin-wave excitations in the noncentrosymmetric heavy-fermion superconductor CePt3Si along the antiferromagnetic Brillouin-zone boundary in the low-temperature magnetically ordered state. Measurements along the (1/2 1/2 L) and (H H 1/2-H) reciprocal-space directions reveal deviations in the spin-wave dispersion from the previously reported model. Broad asymmetric shape of the peaks in energy signifies strong spin-wave damping by interactions with the particle-hole continuum. Their energy width exhibits no evident anomalies as a fun…
Magnons, the spin-wave quanta, are disturbances that embody a wave propagating through a background medium formed by ordered magnetic moments. In an isotropic Heisenberg system, these disturbances vary in a continuous manner around an ordered spin structure, thus requiring infinitesimal energy as a wavevector approaches a magnetic zone centre. However, competing anisotropic interactions arising from broken symmetry can favour a distinct static and dynamic spin state causing a shift of the minimum point of the magnon dispersion to a nonreciprocal wavevector. Here we report the first direct evid…
We report a comprehensive study of the centrosymmetric Re$_3$B and noncentrosymmetric Re$_7$B$_3$ superconductors. At a macroscopic level, their bulk superconductivity (SC), with $T_c$ = 5.1 K (Re$_3$B) and 3.3 K (Re$_7$B$_3$), was characterized via electrical-resistivity, magnetization, and heat-capacity measurements, while their microscopic superconducting properties were investigated by means of muon-spin rotation/relaxation ($μ$SR). In both Re$_3$B and Re$_7$B$_3$ the low-$T$ zero-field electronic specific heat and the superfluid density (determined via tranverse-field $μ$SR) suggest a nod…
The ThIrSi superconductor, with $T_c = 6.5$ K, is expected to show unusual features in view of its noncentrosymmetric structure and the presence of heavy elements featuring a sizable spin-orbit coupling. Here, we report a comprehensive study of its electronic properties by means of local-probe techniques: muon-spin rotation and relaxation ({\textmu}SR) and nuclear magnetic resonance (NMR). Both the superfluid density $ρ_\mathrm{sc}(T)$ (determined via transverse-field {\textmu}SR) and the spin-lattice relaxation rate $T_1^{-1}(T)$ (determined via NMR) suggest a nodeless superconductivity. Furt…
We report superconductivity in the ternary half-Heusler compound LuPtBi, with Tc = 1.0 K and Hc2 = 1.6 T. The crystal structure of LuPtBi lacks inversion symmetry, hence the material is a noncentrosymmetric superconductor. Magnetotransport data show semimetallic behavior in the normal state, which is evidence for the importance of spin-orbit interaction. Theoretical calculations indicate that the strong spin-orbit interaction in LuPtBi should cause strong band inversion, making this material a promising candidate for 3D topological superconductivity.
The noncentrosymmetric superconductor Mo$_3$Rh$_2$N, with $T_c = 4.6$ K, adopts a $β$-Mn-type structure (space group $P$4$_1$32), similar to that of Mo$_3$Al$_2$C. Its bulk superconductivity was characterized by magnetization and heat-capacity measurements, while its microscopic electronic properties were investigated by means of muon-spin rotation and relaxation ($μ$SR). The low-temperature superfluid density, measured via transverse-field (TF)-$μ$SR, evidences a fully-gapped superconducting state with $Δ_0 = 1.73 k_\mathrm{B}T_c$, very close to 1.76 $k_\mathrm{B}T_c$ - the BCS gap value for …
Vector-field control and emergent basal-plane anisotropy of magnetic textures in noncentrosymmetric (Fe$_{0.63}$Ni$_{0.3}$Pd$_{0.07}$)$_3$P
Helmholtz-Zentrum Berlin für Materialien und Energie（柏林亥姆霍兹材料能源研究中心）；Department of Physics, Korea Advanced Institute of Science and Technology（韩国科学技术院物理系）；Center for Theoretical Physics of Complex Systems, Institute for Basic Science (IBS)（基础科学研究院复杂系统理论物理中心）；Heinz Maier-Leibnitz Zentrum (MLZ), Technische Universität München（慕尼黑工业大学海因茨·迈尔-莱布尼茨中心）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Dresden Center for Nanoanalysis, cfaed, Technical University Dresden（德累斯顿大学纳米分析中心）
SrAuSi$_3$ is a noncentrosymmetric superconductor (NCS) with $T_c$ = 1.54 K, which to date has been studied only via macroscopic techniques. By combining nuclear magnetic resonance (NMR) and muon-spin rotation ($μ$SR) measurements we investigate both the normal and the superconducting phase of SrAuSi$_3$ at a local level. In the normal phase, our data indicate a standard metallic behavior with weak electron correlations and a Korringa constant $S_\mathrm{exp} = 1.31 \times 10^{-5}$ sK. The latter, twice the theoretical value, can be justified by the Moriya theory of exchange enhancement. In th…
Mixing of spin singlet and spin triplet superconducting pairing state is expected in noncentrosymmetric superconductors (NCS) due to the inherent presence of Rashba-type antisymmetric spin-orbit coupling. Unlike low symmetry (tetragonal or monoclinic) NCS, parity is isotropicaly broken in space for cubic NCS and can additionally lead to the coexistence of magnetic and superconducting state under certain conditions. Motivated with such enriched possibility of unconventional superconducting phases in cubic NCS we are reporting successful formation of single crystalline cubic noncentrosymmetric P…
In noncentrosymmetric crystals with broken inversion symmetry $\mathcal{I}$, the $I-V$ ($I$: current, $V$: voltage) characteristic is generally expected to depend on the direction of $I$, which is known as nonreciprocal response and, for example, found in p-n junction. However, it is a highly nontrivial issue in translationally invariant systems since the time-reversal symmetry ($\mathcal{T}$) plays an essential role, where the two states at crystal momenta $k$ and $-k$ are connected in the band structure. Therefore, it has been considered that the external magnetic field ($B$) or the magnetic…
The magnetic properties of a pressure induced noncentrosymmetric heavy-fermion superconductor CeIrGe$_3$ have been investigated by muon spin relaxation ($μ$SR), powder neutron diffraction (ND) and inelastic neutron scattering (INS) techniques at ambient pressure. For completeness we have also measured the ac magnetic susceptibility $χ_{\rm ac}(T)$, dc magnetic susceptibility $χ(T)$, dc isothermal magnetization $M(H)$ and heat capacity $C_{\rm p}(T,H)$ down to 2 K. CeIrGe$_{3}$ is known to exhibit pressure induced superconductivity ($T_{\rm c}\approx 1.5$ K) at a pressure of 20 GPa and antiferr…
Strength of Rashba type antisymmetric spin orbit coupling has the crucial effect on superconducting and normal state properties in noncentrosymmetric (NCS) superconductors. This can be seen on various anisotropic properties of the system. For a system with lowered crystalline symmetry as in noncentrosymmetric crystals, the superconducting pairing state can have correlation to the normal state properties. In our earlier work we have shown that alfa-BiPd which has a monoclinic (P_21) structure with the absence of the centre of inversion exhibits bulk superconductivity at 3.8 K. In order to under…
We investigate an interplay between quantum geometrical effects and surface plasmons through surface plasmonic structures, based on an electron hydrodynamic theory. First we demonstrate that the quantum nonlinear Hall effect can be dramatically enhanced over a very broad range of frequency by utilizing plasmonic resonances and near-field effects of grating gates. Under the resonant condition, the enhancement becomes several orders of magnitude larger than the case without the nanostructures, while the peaks of high-harmonic plasmons expand broadly and emerge under the off-resonant condition, l…
