Strong Antiferromagnetic Research Articles

Geometrically frustrated Gd2Ti2O7 oxide: A comprehensive exploration of structural, magnetic, and magnetocaloric properties for cryogenic magnetic cooling applications

The magnetocaloric effect (MCE) has been extensively studied in various magnetic solids, aiming to both facilitate practical applications in magnetic cooling and deepen our understanding these materials’ intrinsic properties. This study presents a systematic investigation of Gd2Ti2O7 oxide, characterized by a geometrically frustrated magnetic structure, focusing on its structural and magnetic characteristics through experimental analysis and theoretical calculations. Emphasis is placed on its magnetic phase transition (MPT) and magnetocaloric properties, scrutinizing temperatures as low as 0.4 K and magnetic fields up to 16 T. The results reveal that Gd2Ti2O7 oxide possesses a crystalline cubic pyrochlore-type structure with an antiferromagnetic (AFM) semiconductor ground state. The material undergoes a first-order MPT in low field and low-temperature regimes, transitioning to a second-order MPT above 2 K up to 16 T. Evaluation of magnetocaloric parameters, including maximum magnetic entropy change, temperature-averaged entropy change, relative cooling power, and refrigerant capacity, indicates moderate values under low magnetic field changes, while significantly large values are achievable under high magnetic field changes. This finding suggests that potential cryogenic magnetocaloric materials (MCMs) with optimal performance should exhibit low MPT temperatures induced by magnetic frustration and possess a ground state with a sufficiently large magnetic moment induced by low magnetic fields, thus avoiding excessively strong AFM coupling. This study lays the groundwork for future cryogenic MCM design and provides valuable insights into the intrinsic properties of geometrically frustrated magnetic materials.

Crystal structure, magnetic and Mössbauer studies of DyFexMn1-xO3 multiferroic manganites

The influence of iron replacement on the structural and magnetic properties of Dysprosium manganites was studied using the series of DyFexMn1-xO3 (x = 0.0, 0.1, 0.3, 0.5, 0.7, 0.9, and 1.0) compounds. All samples were fabricated by means of the modified auto-combustion sol-gel method, followed by the ball milling technique. Orthorhombic structure (Pnma space group) with high phase purity and crystallinity featured all samples, according to X-ray diffraction analysis. The temperature dependence of magnetization curves indicated antiferromagnetic (AFM) to paramagnetic (PM) transition with the increase in temperature. The Néel temperature (TN) was observed to shift to higher temperatures, whereas the spin reorientation transition temperature (TSR) reduced as Fe3+ content increased. Cusps in the zero-field-cooled (ZFC) curves were detected at low temperatures (around 4 K) as an indication of the ordering of the Dy spin. 57Fe Mӧssbauer spectra in samples with low iron content were dominated by a high spin (Fe3+) paramagnetic doublet at both 295 K and 78 K, while the distribution in the hyperfine magnetic field accounted for the appearance of the broadening magnetic peaks. High iron samples revealed a magnetic sextet with fit-resolved patterns that indicated a strong AFM coupling of Fe3+ ions. The hyperfine magnetic field (Bhf) magnitude demonstrated a linear increase with the increase in iron doping.

High Efficiency and Flexible Modulation of Spintronic Terahertz Emitters in Synthetic Antiferromagnets.

Spintronic terahertz (THz) emitters based on synthetic antiferromagnets (SAFs) of FM1/Ru/FM2 (FM: ferromagnet) have shown great potential for achieving coherent superposition and significant THz power enhancement due to antiparallel magnetization alignment. However, key issues regarding the effects of interlayer exchange coupling and net magnetization on THz emissions remain unclear, which will inevitably hinder the performance improvement and practical application of THz devices. In this work, we have investigated the femtosecond laser-induced THz emission in Pt (3)/CoFe (3)/Ru (tRu = 0-3.5)/CoFe (tCoFe = 1.5-10)/Pt (3) (in units of nm) films with compensated and uncompensated magnetic moments. Antiferromagnetic (AF) coupling occurs in the Ru thickness ranges of 0.2-1.1 and 1.9-2.3 nm, with the first peak (tRu = 0.4 nm) of the AF coupling field (Hex) significantly higher than that of the second peak (2.0 nm). Rather high THz amplitude is found for the samples with strong AF coupling. Nevertheless, despite the same remanence ratio of zero, the THz amplitude for the symmetric SAF films declines significantly as the tRu decreases from 0.8 to 0.4 nm, which is mainly ascribed to the noncolinear magnetization vectors due to the increased biquadratic coupling term. Specifically, we demonstrate that an asymmetric SAF structure with a dominant FM layer is more favored than the completely compensated one, which could generate significantly enhanced THz electric field with well-controlled polarity and intensity. In addition, as the temperature decreases, the THz emission intensity increases for the SAF samples of tRu = 0.9 nm with negligible biquadratic coupling, which is contrary to the decreasing trend of the tRu = 0.4 nm sample and has been attributed to the greatly enhanced Hex.

Probing the incoherent admixture of low and high-spin states of Co in (LaPr)CoO3 perovskite: focus on structural phase transitions

We report the mixed valence and intermediate spin-state (IS) transitions in Pr substituted LaCoO3 perovskites in the form of bulk and nanostructures. Various compositions (x) of La1−x Pr x CoO3 (0 ⩽ x⩽ 0.9) were synthesized using the sol–gel process under moderate heat treatment conditions (600 °C). The structural analysis of these compounds reveals a phase crossover from the monoclinic phase (space group, s.g.: I2/a) to an orthorhombic one (s.g.: Pbnm), and a rhombohedral phase (s.g.: R-3c) to an orthorhombic one (s.g.: Pnma) in the bulk and nanostructures, respectively, for the composition range 0 ⩽ x⩽ 0.6. Such a structural transformation remarkably reduces the Jahn–Teller distortion factor ΔJT: 0.374 → 0.0016 signifying the dominant role of the IS state (S Avg = 1) of trivalent Co ions in the investigated system. Magnetization measurements reveal the ferromagnetic (FM) nature of bulk LaCoO3 along with a weak antiferromagnetic (AFM) component coexisting with an FM component. This coexistence results in a weak loop-asymmetry (zero-field exchange-bias effect ∼134 Oe) at low temperatures. Here the FM ordering occurs due to the double-exchange interaction (J EX /k B∼ 11.25 K) between the tetravalent and trivalent Co ions. Significant decrease in the ordering temperatures was noticed in the nanostructures (T C ∼ 50 K) as compared to the bulk counterpart (∼90 K) due to the finite size/surface effects in the pristine compound. However, the incorporation of Pr leads to the development of a strong AFM component (J EX/k B ∼ 18.2 K) and enhances the ordering temperatures (∼145 K for x = 0.9) with negligible FM correlations in both bulk and nanostructures of LaPrCoO3 due to the dominant super-exchange interaction: Co3+/4+‒O‒Co3+/4+. Further evidence of the incoherent mixture of low-spin (LS) and high-spin (HS) states comes from the M–H measurements which yields a saturation magnetization of M S ∼ 275 emu mol−1 (under the limit of 1/H → 0) consistent with the theoretical value of 279 emu mol−1 corresponding to the spin admixture: 65% LS + 10% IS of trivalent Co along with 25% of LS Co4+ in the bulk pristine compound. A similar analysis yields: Co3+ [30% LS + 20% IS] + Co4+ [50% of LS] for the nanostructures of LaCoO3, yet the Pr substitution decreases the spin admixture configuration. The Kubelka–Munk analysis of the optical absorbance results in a significant decrease in the optical energy band gap (E g:1.86 → 1.80 eV) with the incorporation of Pr in LaCoO3 which corroborates the above results.

Interrelationships between nematicity, antiferromagnetic spin fluctuations, and superconductivity: Role of hotspots in FeSe1−xSx revealed by high pressure Se77 NMR study

The sulfur-substituted FeSe, FeSe$_{1-x}$S$_{x} $, is one of the unique systems that provides an independent tunability of nematicity, antiferromagnetism and superconductivity under pressure ($p$). Recently Rana et al. [Phys. Rev. B 101, 180503(R) (2020)] reported, from $^{77}$Se nuclear magnetic resonance (NMR) measurements on FeSe$_{0.91}$S$_{0.09}$ under pressure, that there exists a clear role of nematicity on the relationship between antiferromagnetic (AFM) spin fluctuations and superconducting transition temperature ($T_{\rm c}$) where the AFM spin fluctuations are more effective in enhancing $T_{\rm c}$ in the absence of nematicity than with nematicity. Motivated by the work, we carried out $^{77}$Se NMR measurements on FeSe$_{1-x}$S$_{x}$ with $x$= 0.15 and 0.29 under pressure up to 2.10 GPa to investigate the relationship in a wide range of $x$ in the FeSe$_{1-x}$S$_x$ system. Based on the new results together with the previously reported data for $x$=0 [P. Wiecki et al., Phys. Rev. B 96, 180502(R) (2017)] and 0.09 [K. Rana et al. Phys. Rev. B 101, 180503(R) (2020)], we established a $p$ - $x$ - temperature ($T$) phase diagram exhibiting the evolution of AFM spin fluctuations. From the systematic analysis of the NMR data, we found that the superconducting (SC) state in nematic state arises from a non Fermi liquid state with strong stripe-type AFM spin fluctuations while the SC state without nematicity comes from a Fermi liquid state with mild stripe-type AFM spin fluctuations. Furthermore, we show that the previously reported impact of nematicity on the relationship between AFM fluctuations and superconductivity holds throughout the wide range of $x$ from $x$ = 0 to 0.29 in FeSe$_{1-x}$S$_{x}$ under pressure. We discuss the origin of the role of nematicity in terms of the different numbers of hotspots on Fermi surfaces with and without nematicity.

Perpendicular magnetic anisotropy induced by antiferromagnetic Mn-Pd alloy films: Dual effects of exchange and spin-orbit coupling

Ferromagnetic (FM) films with perpendicular magnetic anisotropy (PMA) are crucial building blocks of state-of-the-art perpendicular magnetic devices. This study investigated the effects of triggering PMA in FM thin films by applying ${\mathrm{Mn}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x}$-based antiferromagnetic (AFM) thin films with strong AFM exchange coupling from Mn and high spin-orbit coupling from Pd atoms. Our results reveal that ${\mathrm{Mn}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x}$ films can trigger PMA in Co/Ni films with weak in-plane magnetic anisotropy at room temperature through either ${\mathrm{Mn}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x}$-facilitated interfacial perpendicular crystalline anisotropy (spin-orbit coupling, $x \ensuremath{\ge}10%$) or incorporation of them with antiferromagnet-induced exchange coupling ($x \ensuremath{\le}10%$). In Co/Fe films with strong in-plane magnetic anisotropy, Mn-rich ${\mathrm{Mn}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x}$ films ($x \ensuremath{\le}10%$) can induce stable PMA at low temperatures through concurrently enhanced spin-orbit coupling and antiferromagnet-induced exchange coupling across the AFM--FM interface. Our research clarifies the dual effects of exchange and spin-orbit coupling in ${\mathrm{Mn}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x}$ films, which trigger the PMA of adjacent FM films. This indicates that ${\mathrm{Mn}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x}$ films are promising candidates for achieving controllable PMA.

Role of Magnetic Defects in Tuning Ground States of Magnetic Topological Insulators.

Magnetic defects play an important, but poorly understood, role in magnetic topological insulators (TIs). For example, topological surface transport and bulk magnetic properties are controlled by magnetic defects in Bi2 Se3 -based dilute ferromagnetic (FM) TIs and MnBi2 Te4 (MBT)-based antiferromagnetic (AFM) TIs. Despite its nascent ferromagnetism, the inelastic neutron scattering data show that a fraction of the Mn defects in Sb2 Te3 form strong AFM dimer singlets within a quintuple block. The AFM superexchange coupling occurs via Mn-Te-Mn linear bonds and is identical to the AFM coupling between antisite defects and the FM Mn layer in MBT, establishing common interactions in the two materials classes. It is also found that the FM correlations in (Sb1-x Mnx )2 Te3 are likely driven by magnetic defects in adjacent quintuple blocks across the van der Waals gap. In addition to providing answers to long-standing questions about the evolution of FM order in dilute TI, these results also show that the evolution of global magnetic order from AFM to FM in Sb-substituted MBT is controlled by defect engineering of the intrablock and interblockcoupling.

Study of Interacting Heisenberg Antiferromagnet Spin-1/2 and 1 Chains

Haldane conjectures the fundamental difference in the energy spectrum of the Heisenberg antiferromagnetic (HAF) of the spin S chain is that the half-integer and the integer S chain have gapless and gapped energy spectrums, respectively. The ground state (gs) of the HAF spin-1/2 and spin-1 chains have a quasi-long-range and short-range correlation, respectively. We study the effect of the exchange interaction between an HAF spin-1/2 and an HAF spin-1 chain forming a normal ladder system and its gs properties. The inter-chain exchange interaction J⊥ can be either ferromagnetic (FM) or antiferromagnetic (AFM). Using the density matrix renormalization group method, we show that in the weak AFM/FM coupling limit of J⊥, the system behaves like two decoupled chains. However, in the large AFM J⊥ limit, the whole system can be visualized as weakly coupled spin-1/2 and spin-1 pairs which behave like an effective spin-1/2 HAF chain. In the large FM J⊥ limit, coupled spin-1/2 and spin-1 pairs can form pseudo spin-3/2 and the whole system behaves like an effective spin-3/2 HAF chain. We also derive the effective model Hamiltonian in both strong FM and AFM rung exchange coupling limits.

Interfacial antiferromagnetic phase induced two-step magnetization reversal in PbZr0.52Ti0.48O3/La0.67Sr0.33MnO3 superlattices

Artificial multiferroic heterostructures have recently attracted much interests due to the demonstrated magnetoelectric coupling (MEC) and unique functionalities, promising a tantalizing perspective of novel applications in next-generation electronic, memory, sensor, and energy harvesting technologies. Herein, we report a two-step magnetization reversal in PbZr0.52Ti0.48O3/La0.67Sr0.33MnO3 (PZT/LSMO) superlattices, which originates from the strongly entangled strain-, ferroelectric (FE)-polarization-, and exchange-dependent effects. Specifically, the preferential occupancy of the in-plane Mn dx2−y2 orbitals is triggered via the collective effects of the large tensile strain and FE polarization, giving rise to an interfacial antiferromagnetic (AFM) layer with strong AFM anisotropy. The strong spin exchange coupling between the AFM layer and the adjacent ferromagnetic (FM) layer facilitates the magnetic stratification of the FM layer, leading to two coercivities, i.e., two-step magnetization reversal. Meanwhile, a sizeable exchange bias (EB) field is induced. The emerged two-step magnetization reversal concomitant with the pronounced EB phenomenon should be a signature of an enhanced MEC in PZT/LSMO superlattices. Our results will stimulate further interests in multiferroic superlattices in applications of multiferroic-based devices.

Structural and magnetic phase transitions in quasi-two-dimensional VBr3

We present a systematic study on the structural and magnetic phase transitions in quasi-two-dimensional (2D) material ${\mathrm{VBr}}_{3}$ through various experimental techniques. With decreasing the temperature, ${\mathrm{VBr}}_{3}$ first undergoes a structural phase transition at around 90 K and then changes into the antiferromagnetic (AFM) state below 26.5 K. Interestingly, in addition to the strong AFM coupling background below 26.5 K, our ${\mathrm{VBr}}_{3}$ single crystals also exhibit robust hysteresis loops with coercive field about 1.5 T at 2 K for $H//c$, but none for $H//ab$. This is a typical feature of canted AFM and should not originate from a possible ferromagnetic (FM) impurities phase, because FM materials such as ${\mathrm{VI}}_{3}$ always have clear hysteresis loops in all magnetic field directions. Magnetization measurements of angle for rotation in both $ab$ and $ac$ planes also suggest ${\mathrm{VBr}}_{3}$ as a canted AFM with easy axis slightly off the $c$ axis. Furthermore, detailed Raman spectroscopy measurements also reveal the structural phase transition at 90 K. More importantly, splitting of a doubly degenerated ${E}_{\mathrm{g}}$ mode is observed, which demonstrates threefold rotational symmetry breaking in the low-temperature phase. Considering the similar structural phase transition of isostructural materials, we conclude that ${\mathrm{VBr}}_{3}$ changes from $R\overline{3}$ structure to $C2/m$ structure with stacking order change as temperature decreases.

Magnetic properties and Mössbauer study of perovskite LaMn0.5Fe0.5O3

The wide application of LaMn0.5Fe0.5O3 perovskite is due to its very complex magnetic and structural properties. Orthorhombic perovskite structure samples were prepared by sol-gel method. The system has a special spin glass state (Néel temperature below freezing temperature). Therefore, there is a transition for the main magnetic phase from strong antiferromagnetism to ferrimagnetism and finally to superparamagnetism as the temperature increases. The typical ferromagnetic and antiferromagnetic competing exchange bias phenomenon appears in the M − H curve at 5 K. We have simulated the thermal and magnetic characteristics of the system through the XYZ model and particle swarm optimization and obtained accurate anisotropy parameters. The transitions of the Mössbauer spectra at different temperatures reflect the changes in the macroscopic magnetic properties of the system. Finally, we can explain the relaxation peak behavior of Mössbauer spectra well by the relationship between the relaxation hyperfine field and temperature. This study will provide a good illustration and reference for the magnetic nature of strongly magnetic disordered LaMn0.5Fe0.5O3 systems.

Spin-Orbital States and Strong Antiferromagnetism of Layered Eu2SrFe2O6 and Sr3Fe2O4Cl2.

The insulating iron compounds Eu2SrFe2O6 and Sr3Fe2O4Cl2 have high-temperature antiferromagnetic (AF) order despite their different layered structures. Here, we carry out density functional calculations and Monte Carlo simulations to study their electronic structures and magnetic properties aided with analyses of the crystal field, magnetic anisotropy, and superexchange. We find that both compounds are Mott insulators and in the high-spin (HS) Fe2+ state (S = 2) accompanied by the weakened crystal field. Although they have different local coordination and crystal fields, the Fe2+ ions have the same level sequence and ground-state configuration (3z2-r2)2(xz, yz)2(xy)1(x2-y2)1. Then, the multiorbital superexchange produces strong AF couplings, and the (3z2-r2)/(xz, yz) mixing via the spin-orbit coupling (SOC) yields a small in-plane orbital moment and anisotropy. Indeed, by tracing a set of different spin-orbital states, our density functional calculations confirm the strong AF couplings and the easy planar magnetization for both compounds. Moreover, using the derived magnetic parameters, our Monte Carlo simulations give the Néel temperature TN = 420 K (372 K) for the former (the latter), which well reproduce the experimental results. Therefore, the present study provides a unified picture for Eu2SrFe2O6 and Sr3Fe2O4Cl2 concerning their electronic and magnetic properties.

Pressure-Induced Intermetallic Charge Transfer and Semiconductor-Metal Transition in Two-Dimensional AgRuO 3

Pressure-Induced Intermetallic Charge Transfer and Semiconductor-Metal Transition in Two-Dimensional AgRuO ₃

Magnetic frustration in the cubic double perovskite Ba2NiIrO6

Hybrid transition metal oxides continue to attract attention due to their multiple degrees of freedom ($e.g.$, lattice, charge, spin, and orbital) and versatile properties. Here we investigate the magnetic and electronic properties of the newly synthesized double perovskite Ba$_2$NiIrO$_6$, using crystal field theory, superexchange model analysis, density functional calculations, and parallel tempering Monte Carlo (PTMC) simulations. Our results indicate that Ba$_2$NiIrO$_6$ has the Ni$^{2+}$ ($t_{2g}^{6}e_{g}^{2}$)-Ir$^{6+}$ ($t_{2g}^{3}$) charge states. The first nearest-neighboring (1NN) Ni$^{2+}$-Ir$^{6+}$ ions prefer a ferromagnetic (FM) coupling as expected from the Goodenough-Kanamori-Anderson rules, which contradicts the experimental antiferromagnetic (AF) order in Ba$_2$NiIrO$_6$. We find that the strong 2NN AF couplings are frustrated in the fcc sublattices, and they play a major role in determining the observed AF ground state. We also prove that the $J_{\rm eff}$ = 3/2 and $J_{\rm eff}$ = 1/2 states induced by spin-orbit coupling, which would be manifested in low-dimensional (e.g., layered) iridates, are however not the case for cubic Ba$_2$NiIrO$_6$. Our PTMC simulations show that when the long-range (2NN and 3NN) AF interactions are included, an AF transition with $T_{\rm N}$ = 66 K would be obtained and it is well comparable with the experimental 51 K. Meanwhile, we propose a possible 2$\times$2$\times$2 noncollinear AF structure for Ba$_2$NiIrO$_6$.

Endohedral σ-Diradical Nitrogen-Vacancy Diamond Nanoclusters with a Confined Magnetic Space and Strong Electronic Spin Couplings.

The electronic properties and their modulations for the nitrogen-vacancy (NV) centers in various nanoscale diamonds are of profound current interest because of their potential applications. However, although the NV centers as chromophores in diamond are the most widely studied, surprisingly, little is known about their magnetic spin coupling properties up to now. Here, we for the first time show, using the spin-polarized DFT calculations, that the NV centers can act as unique endohedral σ-diradical magnets in diamond nanoclusters and exhibit quite strong ferromagnetic (FM) or antiferromagnetic (AFM) spin coupling characteristics due to their unique endotetrahedral structures with favorable radical-radical contacts. Although the neutral NV center (NV0) in its doublet ground state exhibits quite strong AFM spin coupling among three radical C-sites (i.e., an AFM triradical center), interestingly, excess electron injection can convert it to a FM diradical magnet (i.e., the triplet ground state NV-) with almost unchanged J-coupling magnitude, and the J-coupling of the nanocluster can be noticeably enhanced by F-termination of the surface due to triradical spin delocalization mediated by excess electron. However, interior modification (one C in the endotetrahedron core is substituted by N or B or is hydrogenated) can assign the nanocluster perfect AFM diradical character. The spin coupling strength presents a quasilinear correlation with the distance between the two C radicals in the NV core for the same size of the clusters and a high linear correlation with the energy difference between two singly occupied molecular orbitals. Clearly, the FM and AFM couplings as well as their switching behavior in such NV defect diamond nanoclusters featuring the endohedral σ-diradicals are a novel type of promising magnetic material motifs. These findings open up promising spintronic application prospects of the NV diamonds and provide helpful information for the design of inorganic magnetic materials and logic devices.

Comprehensively understanding the natures of crystal structure and magnetic behavior of a radical salt with regular mixed anion-cation stacks

In this study, the ionic crystals of [TTF][Au(mnt)2] (1; mnt2− ​= ​maleonitriledithiolate) have been grown using solvent diffusion method, and characterized by microanalysis, IR and Raman spectra, TG and powder X-ray diffraction (PXRD) techniques. Crystal of 1 belongs to triclinic space P−1 with Z ​= ​1 and both planar TTF+ and [Au(mnt)2]− locate at an inversion center, respectively. Cation (C) and anion (A) form uniform … CACA … mixed stack along [1 0 0] direction, and the charge-assisted H-bonds form between neighboring mixed stacks. 1 features an S ​= ​½ Heisenberg uniform antiferromagnetic (AFM) chain with J/kB ​= ​−2.08(1) K with g ​= ​2.0085 fixed, and absent spin-Peierls transition above 1.9 ​K, however, with long-range AFM ordering below 1.9 ​K. Additionally, 1 displays different style of mixed stack from [TTF][M(mnt)2] (M ​= ​Pd or Pt; … C2A2C2A2 … manner mixed stack) owing to strong AFM couplings (−J/kB ​> ​1000 ​K) in a [M(mnt)2]22− dimer.

Incommensurate and commensurate antiferromagnetic states in CaMn2As2 and SrMn2As2 revealed by As75 NMR

We carried out $^{75}\mathrm{As}$ nuclear magnetic resonance (NMR) measurements on the trigonal $\mathrm{Ca}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ and $\mathrm{Sr}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ insulators exhibiting antiferromagnetic (AFM) ordered states below N\'eel temperatures ${T}_{\mathrm{N}}=62$ and 120 K, respectively. In the paramagnetic state above ${T}_{\mathrm{N}}$, typical quadrupolar-split $^{75}\mathrm{As}$ NMR spectra were observed for both systems. The $^{75}\mathrm{As}$ quadrupolar frequency ${\ensuremath{\nu}}_{\mathrm{Q}}$ for $\mathrm{Ca}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ decreases with decreasing temperature, while ${\ensuremath{\nu}}_{\mathrm{Q}}$ for $\mathrm{Sr}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ increases, showing an opposite temperature dependence. In the AFM state, the relatively sharp and distinct $^{75}\mathrm{As}$ NMR lines were observed in $\mathrm{Sr}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ and the NMR spectra were shifted to lower fields for both magnetic fields $H\ensuremath{\parallel}c$ axis and $H\ensuremath{\parallel}ab$ plane, suggesting that the internal fields ${B}_{\mathrm{int}}$ at the As site produced by the Mn ordered moments are nearly perpendicular to the external magnetic field direction. No obvious distribution of ${B}_{\mathrm{int}}$ was observed in $\mathrm{Sr}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$, which clearly indicates a commensurate AFM state. In sharp contrast to $\mathrm{Sr}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$, broad and complex NMR spectra were observed in $\mathrm{Ca}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ in the AFM state, which clearly shows a distribution of ${B}_{\mathrm{int}}$ at the As site, indicating an incommensurate state. From the analysis of the characteristic shape of the observed spectra, the AFM state of $\mathrm{Ca}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ was determined to be a two-dimensional incommensurate state where Mn ordered moments are aligned in the $ab$ plane. A possible origin for the different AFM states in the systems was discussed. Both $\mathrm{Ca}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ and $\mathrm{Sr}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ show very large anisotropy in the nuclear spin-lattice relaxation rate $1/{T}_{1}$ in the paramagnetic state. $1/{T}_{1}$ for $H\ensuremath{\parallel}ab$ is much larger than that for $H\ensuremath{\parallel}c$, indicating strong anisotropic AFM spin fluctuations in both compounds.

First-order antiferromagnetic transitions of SrMn2P2 and CaMn2P2 single crystals containing corrugated-honeycomb Mn sublattices

SrMn2P2 and CaMn2P2 are insulators that adopt the trigonal CaAl2Si2-type structure containing corrugated Mn honeycomb layers. Magnetic susceptibility χ and heat capacity versus temperature T data reveal a weak first-order antiferromagnetic (AFM) transition at the Néel temperature [Formula: see text] K for SrMn2P2 and a strong first-order AFM transition at [Formula: see text] K for CaMn2P2 Both compounds exhibit isotropic and nearly T-independent [Formula: see text], suggesting magnetic structures in which nearest-neighbor moments are aligned at [Formula: see text] to each other. The 31P NMR measurements confirm the strong first-order transition in CaMn2P2 but show critical slowing down above [Formula: see text] for SrMn2P2, thus also evidencing second-order character. The 31P NMR measurements indicate that the AFM structure of CaMn2P2 is commensurate with the lattice whereas that of SrMn2P2 is incommensurate. These first-order AFM transitions are unique among the class of (Ca, Sr, Ba)Mn2 (P, As, Sb, Bi)2 compounds that otherwise exhibit second-order AFM transitions. This result challenges our understanding of the circumstances under which first-order AFM transitions occur.

Phase diagrams of the antiferromagnetic XY model on a triangular lattice with higher-order interactions.

We study the effects of higher-order antinematic interactions on the critical behavior of the antiferromagnetic (AFM) XY model on a triangular lattice using Monte Carlo simulations. The parameter q of the generalized antinematic (ANq) interaction is found to have a pronounced effect on the phase diagram topology by inducing new quasi-long-range ordered phases due to competition with the conventional AFM interaction as well as geometrical frustration. For values of q divisible by 3, the ground-state competition between the two interactions results in a frustrated canted AFM phase appearing at low temperatures wedged between the AFM and ANq phases. For q nondivisible by 3, with the increase of q one can observe the evolution of the phase diagram topology featuring two (q=2), three (q=4,5), and four (q≥7) ordered phases. In addition to the two phases previously found for q=2, the first new phase with solely AFM ordering arises for q=4 in the limit of strong AFM coupling and higher temperatures by separating from the phase with the coexisting AFM and ANq orderings. For q=7, another phase with AFM ordering but multimodal spin distribution in each sublattice appears at intermediate temperatures. All these algebraic phases also display standard and generalized chiral long-range orderings, which decouple at higher temperatures in the regime of dominant ANq (AFM) interaction for q≥4 (q≥7) preserving only the generalized (standard) chiral ordering.

Pressure-induced reconstitution of Fermi surfaces and spin fluctuations in S-substituted FeSe

FeSe is a unique high-T_c iron-based superconductor in which nematicity, superconductivity, and magnetism are entangled with each other in the P-T phase diagram. We performed ^{77}Se-nuclear magnetic resonance measurements under pressures of up to 3.9 GPa on 12% S-substituted FeSe, in which the complex overlap between the nematicity and magnetism are resolved. A pressure-induced Lifshitz transition was observed at 1.0 GPa as an anomaly of the density of states and as double superconducting (SC) domes accompanied by different types of antiferromagnetic (AF) fluctuations. The low-T_{mathrm{c}} SC dome below 1 GPa is accompanied by strong AF fluctuations, whereas the high-T_{mathrm{c}} SC dome develops above 1 GPa, where AF fluctuations are fairly weak. These results suggest the importance of the d_{xy} orbital and its intra-orbital coupling for the high-T_{mathrm{c}} superconductivity.