Commensurate Antiferromagnetic Research Articles

Multiferroic quantum material Ba2Cu1−xMnxGe2O7 (0 ≤ x ≤ 1) as a potential candidate for frustrated Heisenberg antiferromagnet

Multiferroic Ba2CuGe2O7 was anticipated as a potential member of the exciting group of materials hosting a skyrmion or vortex lattice because of its profound Dzyaloshinskii–Moriya interaction (DMI) and the absence of single ion anisotropy (SIA). This phase, however, could not be evidenced and instead, it exhibits a complex incommensurate antiferromagnetic (AFM) cycloidal structure. Its sister compound Ba2MnGe2O7, in contrast, is characterized by a relatively strong in-plane exchange interaction that competes with a non-vanishing SIA and the weak DMI, resulting in a quasi-two-dimensional commensurate AFM structure. Considering this versatility in the magnetic interactions, a mixed solid solution of Cu and Mn in Ba2Cu1−xMnxGe2O7 can hold an interesting playground for its interactive DMI and SIA depending on the mixed spin states of the transition metal ions towards the skyrmion physics. Here, we present a detailed study of the micro- and macroscopic spin structure of the Ba2Cu1−xMnxGe2O7 solid solution series using high-resolution neutron powder diffraction techniques. We have developed a remarkably rich magnetic phase diagram as a function of the applied magnetic field and x, which consists of two end-line phases separated by a potentially quantum-critical phase at x = 0.57. An AFM conical structure at zero magnetic field is demonstrated to persist up to x = 0.50. Our results provide crucial information on the spin structure and magnetic properties, which are necessary for the general understanding and theoretical developments on multiferroicity in the frame of skyrmion type or frustrated AFM lattice where DMI and SIA play an important role.

Magnetic exchange interactions and non-Debye relaxation in spin-3/2 frustrated Kagomé magnet Co3V2O8

We report the experimental determination of the magnetic exchange parameter ( J/kB = 2.88 ± 0.02 K) for the Spin-3/2 ferromagnetic (FM) Kagomé lattice system: Co3V2O8 using the temperature dependence of dc-magnetic susceptibility χ(T) data by employing the fundamental Heisenberg linear chain model. Our results are quite consistent with the theoretically reported nearest neighbor dominant FM exchange coupling strength Jex−NN∼ 2.45 K. Five different magnetic phase transitions (6.2–11.2 K) and spin-flip transitions (9.6–7.7 kOe) have been probed using the ∂ ( χT )/ ∂T vs. T, heat capacity (CP -T) and differential isothermal magnetization curves. Among such sequence of transitions, the prominent ones being incommensurate antiferromagnetic (AFM) state at 11.2 K, commensurate AFM state at 8.8 K, and commensurate FM state across 6.2 K. All the successive magnetic phase transitions have been mapped onto a single H-T plane through which one can easily distinguish the above-mentioned different phases. The magnetic contribution of the CP -T near TN (11.2 K) has been analyzed using the power-law expression CM = A|T — TN|−α resulting in the critical exponent α = 0.18 ± 0.01 (0.15 ± 0.003) for T < TN (T > TN ), respectively for the Co3V2O8. It is interesting to note that non-Debye type dipole relaxation is quite prominent in Co3V2O8 and was evident from the Kohlrausch–Williams–Watts analysis of complex modulus and impedance spectra (0 ⩽β⩽ 1). Mott’s variable-range hopping of charge carriers process is evident through the resistivity analysis ( ρac -T −1/4 ) in the temperature range 275 ∘C–350 ∘C. Moreover, the frequency-dependent analysis of σac (ω) follows Jonscher’s power law yielding two distinct activation energies ( Ea∼ 0.37 and 2.29 eV) between the temperature range 39 ∘C–99 ∘C and 240 ∘C–321 ∘C.

Static and dynamic magnetic properties of the spin- triangle lattice antiferromagnet Na3Fe(PO4)2 studied by 31P NMR

31P nuclear magnetic resonance (NMR) measurements have been carried out to investigate the magnetic properties and spin dynamics of Fe3+ (S = 5/2) spins in the two-dimensional triangular lattice (TL) compound Na3Fe(PO4)2. The temperature (T) dependence of nuclear spin-lattice relaxation rates () shows a clear peak around Néel temperature, K, corresponding to an antiferromagnetic (AFM) transition. From the temperature dependence of NMR shift (K) above , an exchange coupling between Fe3+ spins was estimated to be K using the spin-5/2 Heisenberg isotropic-TL model. The temperature dependence of divided by the magnetic susceptibility (χ), , above proves the AFM nature of spin fluctuations below in the paramagnetic state. In the magnetically ordered state below , the characteristic rectangular shape of the NMR spectra is observed, indicative of a commensurate AFM state in its ground state. The strong temperature dependence of 1/T 1 in the AFM state is well explained by the two-magnon (Raman) process of the spin waves in a 3D antiferromagnet with a spin-anisotropy energy gap of 5.7 K. The temperature dependence of sublattice magnetization is also well reproduced by the spin waves. Those results indicate that the magnetically ordered state of Na3Fe(PO4)2 is a conventional 3D AFM state, and no obvious spin frustration effects were detected in its ground state.

Antiferromagnetic ordering of organic Mott insulator λ−(BEDSe-TTF)2GaCl4

The band structure and magnetic properties of organic charge-transfer salt $\ensuremath{\lambda}\text{\ensuremath{-}}{(\text{BEDSe-TTF})}_{2}{\mathrm{GaCl}}_{4}$ [BEDSe-TTF: bis(ethylenediseleno)tetrathiafulvalene; abbreviated as $\ensuremath{\lambda}$-BEDSe] are investigated. The reported crystal structure is confirmed using x-ray diffraction measurements, and the transfer integrals are calculated. The degree of electron correlation $U/W$ ($U$: on-site Coulomb repulsion, $W$: bandwidth) of $\ensuremath{\lambda}$-BEDSe is larger than one and comparable to that of the isostructural Mott insulator $\ensuremath{\lambda}\ensuremath{-}({\mathrm{ET})}_{2}{\mathrm{GaCl}}_{4}$ (ET: bis(ethylenedithio)tetrathiafulvalene, abbreviated as $\ensuremath{\lambda}$-ET), whereas the $U/W$ of the superconducting salt $\ensuremath{\lambda}\ensuremath{-}({\mathrm{BETS})}_{2}{\mathrm{GaCl}}_{4}$ [BETS: bis(ethylenedithio)tetraselenafulvalene] is smaller than one. $^{13}\mathrm{C}$-NMR and $\ensuremath{\mu}\mathrm{SR}$ measurements revealed that $\ensuremath{\lambda}$-BEDSe undergoes an antiferromagnetic (AF) ordering below ${T}_{\mathrm{N}}=22$ K. In the AF state, discrete $^{13}\mathrm{C}$-NMR spectra with a remaining central peak are observed, indicating the commensurate AF spin structure also observed in $\ensuremath{\lambda}$-ET. The similarity of the structural and magnetic properties between $\ensuremath{\lambda}$-BEDSe and $\ensuremath{\lambda}$-ET suggests that both salts are in the same electronic phase, i.e., the physical properties of $\ensuremath{\lambda}$-BEDSe can be understood by the universal phase diagram of bandwidth-controlled $\ensuremath{\lambda}$-type organic conductors obtained by donor molecule substitution.

Magnetic order and disorder environments in superantiferromagnetic hbox {NdCu}_{mathbf{2}} nanoparticles

Magnetic nanoparticles exhibit two different local symmetry environments, one ascribed to the core and one corresponding to the nanoparticle surface. This implies the existence of a dual spin dynamics, leading to the presence of two different magnetic arrangements governed by different correlation lengths. In this work, two ensembles of hbox {NdCu}_{2} nanoparticles with mean sizes of 18 nm and 13 nm have been produced to unravel the magnetic couplings established among the magnetic moments located within the core and at the nanoparticle surface. To this end, we have combined neutron diffraction measurements, appropriate to investigate magnetically-ordered spin arrangements, with time-dependent macroscopic AC susceptibility measurements to reveal memory and aging effects. The observation of the latter phenomena are indicative of magnetically-frustrated states. The obtained results indicate that, while the hbox {Nd}^{3{+}} magnetic moments located within the nanoparticle core keep the bulk antiferromagnetic commensurate structure in the whole magnetic state, the correlations among the surface spins give rise to a collective frustrated spin-glass phase. The interpretation of the magnetic structure of the nanoparticles is complemented by specific-heat measurements, which further support the lack of incommensurability in the nanoparticle state.

Evolution of Bonding and Magnetism via Changes in Valence Electron Count in CuFe2–xCoxGe2

A series of solid solutions, CuFe2-xCoxGe2 (x = 0, 0.2, 0.4, 0.8, and 1.0), have been synthesized by arc-melting and characterized by powder X-ray and neutron diffraction, magnetic measurements, Mössbauer spectroscopy, and electronic band structure calculations. All compounds crystallize in the CuFe2Ge2 structure type, which can be considered as a three-dimensional framework built of fused MGe6 octahedra and MGe5 trigonal bipyramids (M = Fe and Co), with channels filled by rows of Cu atoms. As the Co content (x) increases, the unit cell volume decreases in an anisotropic fashion: the b and c lattice parameters decrease while the a parameter increases. The changes in all the parameters are nearly linear, thus following Vegard's law. CuFe2Ge2 exhibits two successive antiferromagnetic (AFM) orderings, corresponding to the formation of a commensurate AFM structure, followed by an incommensurate AFM structure observed at lower temperatures. As the Co content increases, the AFM ordering temperature (TN) gradually decreases, and only one AFM transition is observed for x ≥ 0.2. The magnetic behavior of unsubstituted CuFe2Ge2 was found to be sensitive to the preparation method. The temperature-dependent zero-field 57Fe Mössbauer spectra reveal two hyperfine split components that evolve in agreement with the two consecutive AFM orderings observed in magnetic measurements. In contrast, the field-dependent spectra obtained for fields ≥2 T reveal a parallel arrangement of the moments associated with the two crystallographically unique metal sites. Electronic band structure calculations and chemical bonding analysis reveal a mix of strong M-M antibonding and non-bonding states at the Fermi level, in support of the overall AFM ordering observed in zero field. The substitution of Co for Fe reduces the population of the M-M antibonding states and the overall density of states at the Fermi level, thus suppressing the TN value.

Magnetic phase transitions in the LiNi0.9 M 0.1PO4 (M = Mn, Co) single crystals

The LiNiPO4, LiNi0.9Mn0.1PO4, and LiNi0.9Co0.1PO4 single crystals are studied with heat capacity and neutron diffraction measurements over the temperature interval (10–30) K. Two peaks are observed on the temperature dependence of heat capacity for LiNiPO4, and LiNi0.9Co0.1PO4 samples. One peak indicates the first order phase transition from an antiferromagnetic commensurate (C) structure to an incommensurate (IC) one upon heating. According to neutron diffraction, in LiNiPO4 the IC ordering is described by the propagation vector k = 2π/b(0, 0.080, 0) at the Néel temperature T N = 20.8 K, and k = 2π/b(0, 0.098, 0) at T N = 20.2(1) K for LiNi0.9Co0.1PO4. A further increase in temperature leads to the second order phase transition to a paramagnetic state at critical temperature T IC = 21.7 K and 21.1 K for LiNiPO4 and LiNi0.9Co0.1PO4, respectively. The C and IC phases coexist over the temperature interval (20.6–20.8) K and (20.2–21.2) K in LiNiPO4 and LiNi0.9Co0.1PO4, respectively. In the LiNi0.9Mn0.1PO4 the magnetic phase transition occurs at T N = 22.7 K, but a magnetic scattering is observed up to 24.6 K.

Low-temperature domain-wall freezing and nonequilibrium dynamics in the transverse-field Ising model material CoNb2O6

${\mathrm{CoNb}}_{2}{\mathrm{O}}_{6}$ is a rare realization of the transverse-field Ising model, making it a useful tool for studying both equilibrium and nonequilibrium many-body quantum physics. Despite a large body of work dedicated to characterizing this material, details of the ordered states in the presence of relatively weak transverse fields have not been discussed in detail. Here, we present a detailed study of ${\mathrm{CoNb}}_{2}{\mathrm{O}}_{6}$ via ac susceptibility measurements in order to further characterize its low-temperature behavior in the presence of a transverse field. Specifically, we call attention to an unconventional freezing transition in zero field below ${T}_{F}=1.2$ K, occurring within the well-known commensurate antiferromagnetic (CAFM) state that onsets at ${T}_{N2}=1.9$ K. We performed a series of transverse-field quenches into this frozen state, which resulted in a slowly relaxing susceptibility, ${\ensuremath{\chi}}^{\ensuremath{'}}(t)$, that followed a logarithmic decay within the time range measured. We discuss the frozen state in the context of the freezing of previously discussed ``free'' chains arising from domain walls between the four degenerate sublattices of the CAFM state. We also attempted to observe Kibble-Zurek scaling by quenching the transverse field into the frozen state at different rates. This produced a null result; the behavior can be fully explained by coarsening of domains over the time scale of the quenches. The absence of a clear Kibble-Zurek scaling is itself surprising, given the proposed ubiquity of the phenomenon for general second-order phase transitions.

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.

Spin density wave in the strongly dimerized quasi-one-dimensional organic conductor (DMET-TTF) 2AuBr2

At ambient pressure, studies of resistivity, magnetic susceptibility, and carbon-13 nuclear magnetic resonance (NMR) were conducted on the quasi-one-dimensional organic conductor ${(\text{DMET-}\mathrm{TTF})}_{2}{\mathrm{AuBr}}_{2}$. Resistivity measurements showed a broad minimum at approximately 160 K, and the insulator behavior below this temperature and magnetic susceptibility results revealed a dip structure at 22 K. At the same temperature, a sharp peak in the temperature dependence of ${T}_{1}^{\ensuremath{-}1}$ associated with the antiferromagnetic (AFM). transition was found, along with drastic splitting of the NMR spectra, indicating a commensurate AFM structure. The amplitude of the magnetic moments was determined to be $0.06{\ensuremath{\mu}}_{B}$/molecule from the hyperfine coupling constant tensor and the angular dependence of the internal field in the AFM phase. The small magnetic moment signifies the AFM nesting type, i.e., commensurate spin density wave. An antiferromagnetic ordering of $(\ensuremath{\uparrow}\ensuremath{\uparrow}\ensuremath{\downarrow}\ensuremath{\downarrow})$ along the one-dimensional chain is expected from the $2{k}_{\mathrm{F}}$ instability. This behavior can be explained by the strong dimerization of the one-dimensional DMET-TTF chain.

Magnetic order and competition with superconductivity in (Ho-Er)Ni2B2C

The rare earth magnetic order in pure and doped Ho(1−x)Er x Ni2B2C (x = 0, 0.25, 0.50, 0.75, 1) single crystal samples was investigated using magnetization and neutron diffraction measurements. Superconducting quaternary borocarbides, RNi2B2C where R = Ho, Er , are magnetic intermetallic superconductors with the transition temperatures ∼10 K in which long range magnetic order develops in the same temperature range and competes with superconductivity. Depending on the rare earth composition the coupling between superconductivity and magnetism creates several phases, ranging from a near reentrant superconductor with a mixture of commensurate and incommensurate antiferromagnetism to an incommensurate antiferromagnetic spin modulation with a weak ferromagnetic component. All of these phases coexist with superconductivity. RKKY magnetic interactions are used to describe the magnetic orders in the pure compounds. However, the doping of Er on Ho sites which have two strong magnetic moments with two different easy directions creates new and complicated magnetic modulations with possible local disorder effects. One fascinating effect is the development of an induced magnetic state resembling the pure and doped R 2CuO4 cuprate with R = Nd and Pr.

Strengthening the Magnetic Interactions in Pseudobinary First-Row Transition Metal Thiocyanates, M(NCS)2.

Understanding the effect of chemical composition on the strength of magnetic interactions is key to the design of magnets with high operating temperatures. The magnetic divalent first-row transition metal (TM) thiocyanates are a class of chemically simple layered molecular frameworks. Here, we report two new members of the family, manganese(II) thiocyanate, Mn(NCS)2, and iron(II) thiocyanate, Fe(NCS)2. Using magnetic susceptibility measurements on these materials and on cobalt(II) thiocyanate and nickel(II) thiocyanate, Co(NCS)2 and Ni(NCS)2, respectively, we identify significantly stronger net antiferromagnetic interactions between the earlier TM ions-a decrease in the Weiss constant, θ, from 29 K for Ni(NCS)2 to -115 K for Mn(NCS)2-a consequence of more diffuse 3d orbitals, increased orbital overlap, and increasing numbers of unpaired t2g electrons. We elucidate the magnetic structures of these materials: Mn(NCS)2, Fe(NCS)2, and Co(NCS)2 order into the same antiferromagnetic commensurate ground state, while Ni(NCS)2 adopts a ground state structure consisting of ferromagnetically ordered layers stacked antiferromagnetically. We show that significantly stronger exchange interactions can be realized in these thiocyanate frameworks by using earlier TMs.

Magnetic phase diagram of the quantum spin chain compound SrCo2V2O8: a single-crystal neutron diffraction study

We explore magnetic order in the quantum spin chain compound SrCo2V2O8 up to 14.9 T and down to 50 mK, using single-crystal neutron diffraction. Upon cooling in zero-field, commensurate antiferromagnetic (C-AFM) order with modulation vector = (0, 0, 1) develops below TN ≃ 5.0 K. Applying an external magnetic field (H∥c axis) destabilizes this C-AFM order, leading to an order-disorder transition between TN and ∼1.5 K. Below 1.5 K, a commensurate to incommensurate (IC-AFM) transition occurs at 3.9 T, above which the magnetic reflections can be indexed by = (0, 0, 1 ± δl). The incommensurability δl scales monotonically with H until the IC-AFM order disappears around 7.0 T. Magnetic reflections modulated by emerge again at higher fields. While the characters of the C-AFM, IC-AFM and the emergent AFM order in SrCo2V2O8 appear to fit the descriptions of the Néel, longitudinal spin density wave and transverse AFM order observed in the related compound BaCo2V2O8, our results also reveal several unique signatures that are not present in the latter, highlighting the inadequacy of mean-field theory in addressing the complex magnetic order in systems of this class.

Valence transition model of the pseudogap, charge order, and superconductivity in electron-doped and hole-doped copper oxides

We present a valence transition model for electron- and hole-doped cuprates, within which there occurs a discrete jump in ionicity ${\mathrm{Cu}}^{2+}\ensuremath{\rightarrow}\phantom{\rule{4pt}{0ex}}{\mathrm{Cu}}^{1+}$ in both families upon doping, at or near optimal doping in the conventionally prepared electron-doped compounds and at the pseudogap phase transition in the hole-doped materials. In thin films of the ${\mathrm{T}}^{\ensuremath{'}}$ compounds, the valence transition has occurred already in the undoped state. The phenomenology of the valence transition is closely related to that of the neutral-to-ionic transition in mixed-stack organic charge-transfer solids. Doped cuprates have negative charge-transfer gaps, just as rare-earth nickelates and ${\mathrm{BaBiO}}_{3}$. The unusually high ionization energy of the closed shell ${\mathrm{Cu}}^{1+}$ ion, taken together with the doping-driven reduction in three-dimensional Madelung energy and gain in two-dimensional delocalization energy in the negative charge transfer gap state drives the transition in the cuprates. The combined effects of strong correlations and small $d\ensuremath{-}p$ electron hoppings ensure that the systems behave as effective 1/2-filled Cu band with the closed shell electronically inactive ${\mathrm{O}}^{2\ensuremath{-}}$ ions in the undoped state, and as correlated two-dimensional geometrically frustrated 1/4-filled oxygen hole band, now with electronically inactive closed-shell ${\mathrm{Cu}}^{1+}$ ions, in the doped state. The model thus gives microscopic justification for the two-fluid models suggested by many authors. The theory gives the simplest yet most comprehensive understanding of experiments in the normal states. The robust commensurate antiferromagnetism in the conventional ${T}^{\ensuremath{'}}$ crystals, the strong role of oxygen deficiency in driving superconductivity and charge carrier sign corresponding to holes at optimal doping are all manifestations of the same quantum state. In the hole-doped pseudogapped state, there occurs a biaxial commensurate period 4 charge density wave state consisting of ${\mathrm{O}}^{1\ensuremath{-}}\ensuremath{-}{\mathrm{Cu}}^{1+}\ensuremath{-}{\mathrm{O}}^{1\ensuremath{-}}$ spin singlets that coexists with broken rotational ${\mathrm{C}}_{4}$ symmetry due to intraunit cell oxygen inequivalence. Finite domains of this broken symmetry state will exhibit two-dimensional chirality and the polar Kerr effect. Superconductivity within the model results from a destabilization of the 1/4-filled band paired Wigner crystal [Phys. Rev. B 93, 165110 (2016) and Phys. Rev. B 93, 205111 (2016)]. We posit that a similar valence transition, ${\mathrm{Ir}}^{4+}\ensuremath{\rightarrow}\phantom{\rule{4pt}{0ex}}{\mathrm{Ir}}^{3+}$, occurs upon electron doping ${\mathrm{Sr}}_{2}{\mathrm{IrO}}_{4}$. We make testable experimental predictions in cuprates including superoxygenated ${\mathrm{La}}_{2}{\mathrm{CuO}}_{4+\ensuremath{\delta}}$ and iridates. Finally, as indirect evidence for the valence bond theory of superconductivity proposed here, we note that there exist an unusually large number of unconventional superconductors that exhibit superconductivity proximate to exotic charge ordered states, whose band fillings are universally 1/4 or 3/4, exactly where the paired Wigner crystal is most stable.

Pressure-induced modifications of the magnetic order in the spin-chain compound Ca3Co2O6

The structural and magnetic properties of the $\mathrm{C}{\mathrm{a}}_{3}\mathrm{C}{\mathrm{o}}_{2}{\mathrm{O}}_{6}$ spin-chain compound have been studied by means of neutron and x-ray powder diffraction at pressures up to 6.8 and 32 GPa, respectively. A suppression of the initial spin-density wave state $({T}_{\mathrm{N}}=25\phantom{\rule{0.28em}{0ex}}\mathrm{K})$ and stabilization of the collinear commensurate antiferromagnetic (AFM) state at high pressures $({T}_{\mathrm{NC}}=26\phantom{\rule{0.28em}{0ex}}\mathrm{K}$ at $P=2.1$ GPa) were observed. The pressure behavior of the competing intra- and interchain magnetic interactions was analyzed on the basis of obtained structural data and their role in the formation of the magnetic phase diagram is discussed. The pressure behavior of the N\'eel temperature of the commensurate AFM phase was evaluated within the mean field theory approach and a good agreement with the experimental value $d{T}_{\mathrm{NC}}/dP=0.65\phantom{\rule{0.28em}{0ex}}\mathrm{K}/\mathrm{GPa}$ was obtained.

Identifying Two-Dimensional Z2 Antiferromagnetic Topological Insulators

We revisit the question of whether a two-dimensional topological insulator may arise in a commensurate Neel antiferromagnet, where staggered magnetization breaks the symmetry with respect to both elementary translation and time reversal, but retains their product as a symmetry. In contrast to the so-called Z2 topological insulators, an exhaustive characterization of antiferromagnetic topological phases with the help of topological invariants has been missing. We analyze a simple model of an antiferromagnetic topological insulator and chart its phase diagram, using a recently proposed criterion for centrosymmetric systems [13]. We then adapt two methods, originally designed for paramagnetic systems, and make antiferromagnetic topological phases manifest. The proposed methods apply far beyond the particular examples treated in this work, and admit straightforward generalization. We illustrate this by two examples of non-centrosymmetric systems, where no simple criteria have been known to identify topological phases. We also present, for some cases, an explicit construction of edge states in an antiferromagnetic topological insulator.

Thermal and electrical transport in metals and superconductors across antiferromagnetic and topological quantum transitions

We study thermal and electrical transport in metals and superconductors near a quantum phase transition where antiferromagnetic order disappears. The same theory can also be applied to quantum phase transitions involving the loss of certain classes of intrinsic topological order. For a clean superconductor, we recover and extend the well-known universal results. The heat conductivity for commensurate and incommensurate antiferromagnetism coexisting with superconductivity shows a markedly different doping dependence near the quantum critical point, thus allowing to distinguish the states. In the dirty limit, the results for the conductivities are qualitatively similar for the metal and the superconductor. In this regime, the geometric properties of the Fermi surface allow for a very good phenomenological understanding of the numerical results on the conductivities. In the simplest model, we find that the conductivities do not track the doping evolution of the Hall coefficient, in contrast to recent experimental findings. We propose a doping dependent scattering rate, possibly due to quenched short-range charge fluctuations below optimal doping, to consistently describe both the Hall data and the longitudinal conductivities.

Anomalous lattice compression and magnetic ordering in CuO at high pressures: A structural study and first-principles calculations

The structural and magnetic properties of multiferroic CuO have been studied by means of neutron and x-ray powder diffraction at pressures up to 11 and 38 GPa, respectively, and by first-principles theoretical calculations. Anomalous lattice compression is observed, with enlargement of the lattice parameter $a$, reaching a maximum at $P=13\phantom{\rule{0.16em}{0ex}}\mathrm{GPa}$, followed by its reduction at higher pressures. The lattice distortion of the monoclinic structure at high pressures is accompanied by a progressive change of the oxygen coordination around Cu atoms from the square fourfold towards the octahedral sixfold coordination. The pressure-induced evolution of the structural properties and electronic structure of CuO was successfully elucidated in the framework of full-electronic density functional theory calculations with range-separated HSE06, and meta--generalized gradient approximation hybrid M06 functionals. The antiferromagnetic (AFM) ground state with a propagation vector $q=(0.5,0,\ensuremath{-}0.5)$ remains stable in the studied pressure range. From the obtained structural parameters, the pressure dependencies of the principal superexchange magnetic interactions were analyzed, and the pressure behavior of the N\'eel temperature as well as the magnetic transition temperature from the intermediate incommensurate AFM multiferroic state to the commensurate AFM ground state were evaluated. The estimated upper limit of the N\'eel temperature at $P=38\phantom{\rule{0.16em}{0ex}}\mathrm{GPa}$ is about 260 K, not supporting the previously predicted existence of the multiferroic phase at room temperature and high pressure.

Structure and property correlations in FeS

For iron-sulfide (FeS), we investigate the correlation between the structural details, including its dimensionality and composition, with its magnetic and superconducting properties. We compare, theoretically and experimentally, the two-dimensional (2D) layered tetragonal (“t-FeS”) phase with the 3D hexagonal ("h-FeS") phase. X-ray diffraction reveals iron-deficient chemical compositions of t-Fe0.93(1)S and h-Fe0.84(1)S that show no low-temperature structural transitions. First-principles calculations reveal a high sensitivity of the 2D structure to the electronic and magnetic properties, predicting marginal antiferromagnetic instability for our compound (sulfur height of zS= 0.252) with an ordering energy of about 11meV/Fe, while the 3D phase is magnetically stable. Experimentally, h-Fe0.84S orders magnetically well above room temperature, while t-Fe0.93S shows coexistence of antiferromagnetism at TN= 116 and filamentary superconductivity below Tc= 4K. Low temperature neutron diffraction data reveals antiferromagnetic commensurate ordering with wave vector km=(0.25,0.25,0) and 0.46(2)µB/Fe. Additionally, neutron scattering measurements were used to find the particle size and iron vacancy arrangement of t-FeS and h-FeS. The structure of iron sulfide has a delicate relationship with the superconducting transition; while our sample with a = 3.6772(7)Å is a filamentary superconductor coexisting with an antiferromagnetic phase, previously reported samples with a > 3.68Å are bulk superconductors with no magnetism, and those with a≈3.674Å show magnetic properties.

Antiferromagnetic spin correlations and pseudogaplike behavior inCa(Fe1−xCox)2As2studied byAs75nuclear magnetic resonance and anisotropic resistivity

We report $^{75}$As nuclear magnetic resonance (NMR) measurements of single-crystalline Ca(Fe$_{1-x}$Co$_x$)$_2$As$_2$ ($x$ = 0.023, 0.028, 0.033, and 0.059) annealed at 350~$^{\circ}$C for 7 days. From the observation of a characteristic shape of $^{75}$As NMR spectra in the stripe-type antiferromagnetic (AFM) state, as in the case of $x$ = 0 ($T_{\rm N}$ = 170 K), clear evidence for the commensurate AFM phase transition with the concomitant structural phase transition is observed in $x$ = 0.023 ($T_{\rm N}$ = 106 K) and $x$ = 0.028 ($T_{\rm N}$ = 53 K). Through the temperature dependence of the Knight shifts and the nuclear spin lattice relaxation rates (1/$T_1$), although stripe-type AFM spin fluctuations are realized in the paramagnetic state as in the case of other iron pnictide superconductors, we found a gradual decrease of the AFM spin fluctuations below a crossover temperature $T^*$ which was nearly independent of Co-substitution concentration, and is attributed to a pseudogap-like behavior in the spin excitation spectra of these systems. The $T^*$ feature finds correlation with features in the temperature-dependent inter-plane resistivity, $\rho_c(T)$, but not with the in-plane resistivity $\rho _a (T)$. The temperature evolution of anisotropic stripe-type AFM spin fluctuations are tracked in the paramagnetic and pseudogap phases by the 1/$T_1$ data measured under magnetic fields parallel and perpendicular to the $c$ axis. Based on our NMR data, we have added a pseudogap-like phase to the magnetic and electronic phase diagram of Ca(Fe$_{1-x}$Co$_x$)$_2$As$_2$.