arXiv subjects

N. S. Sangeetha

Publications and source records attributed to N. S. Sangeetha.

At least 19 recordsLinked to original sources

arXiv2025

Spin dynamics in itinerant antiferromagnet SrCr$_2$As$_2$

SrCr$_2$As$_2$ is an itinerant antiferromagnet in the same structural family as the SrFe$_2$As$_2$ high-temperature superconductors. We report our calculations of exchange-coupling parameters $J_{ij}$ for SrCr$_2$As$_2$ using a static linear-response method based on first-principles electronic-structure calculations. We find that the dominant nearest-neighbor exchange coupling $J_{\rm{1}} > 0$ is antiferromagnetic whereas the next-nearest-neighbor interaction $J_{\rm{2}} < 0$ is ferromagnetic with $J_{\rm{2}}$/$J_{\rm{1}}$~=~$-0.68$, reinforcing the checkerboard in-plane magnetic structure. Thus, unlike other transition-metal arsenides based on Mn, Fe, or Co, we find no competing magnetic interactions in SrCr$_2$As$_2$, which aligns with experimental findings. Moreover, the orbital resolution of exchange interactions shows that $J_1$ and $J_2$ are dominated by direct exchange mediated by the Cr $d$ orbitals. To validate the calculations we conduct inelastic neutron-scattering measurements on powder samples that show steeply dispersive magnetic excitations arising from the magnetic $Γ$ points and persisting up to energies of at least 175 meV. The spin-wave spectra are then modeled using the Heisenberg Hamiltonian with the theoretically-calculated exchange couplings. The calculated neutron-scattering spectra are in good agreement with the experimental data.

cond-mat.supr-con↗

arXiv2024

Europium $c$-axis ferromagnetism in Eu(Co$_{1-x}$Ni$_{x}$)$_{2-y}$As$_{2}$: A single-crystal neutron diffraction study

We report neutron diffraction results for the body-centered-tetragonal series Eu(Co$_{1-x}$Ni$_x$)$_{2-y}$As$_2$, $x=0.10$, $0.20$, $0.42$, and $0.82$, $y\leq0.10$, that detail changes to the magnetic ordering with nominal hole doping. We report the antiferromagnetic (AFM) propagation vectors, magnetic transition temperatures, and the ordered magnetic moments. We find a nonmonotonic change of the AFM propagation vector with $x$, with a minimum occurring at the tetragonal to collapsed-tetragonal phase crossover. For $x=0.10$ and $0.82$ we find $c$-axis helix ordering of the Eu magnetic moments (spins) similar to $x=0$ and $1$, with the spins oriented within the $ab$-plane. For $x=0.20$ and $0.42$ we find higher-temperature $c$-axis FM order and lower-temperature $c$-axis cone order. Using the extinction conditions for the space group, we discovered that the Eu spins are ordered in the higher-temperature $c$-axis FM phase for intermediate values of $x$, contrary to a previous report suggesting only Co/Ni spin ordering. Although we cannot directly confirm that the Co/Ni spins are also ordered, we suggest that $c$-axis itinerant-FM ordering of the Co/Ni spins could provide a molecular field that drives FM ordering of the Eu spins, which in turn provides the anisotropy for the lower-temperature $c$-axis cone order.

cond-mat.str-el↗

arXiv2022

Frustrated Magnetic Cycloidal Structure and Emergent Potts Nematicity in CaMn$_2$P$_2$

We report neutron-diffraction results on single-crystal CaMn$_2$P$_2$ containing corrugated Mn honeycomb layers and determine its ground-state magnetic structure. The diffraction patterns consist of prominent (1/6, 1/6, $L$) reciprocal lattice unit (r.l.u.; $L$ = integer) magnetic Bragg reflections, whose temperature-dependent intensities are consistent with a first-order antiferromagnetic phase transition at the Néel temperature $T_{\rm N} = 70(1)$ K. Our analysis of the diffraction patterns reveals an in-plane $6\times6$ magnetic unit cell with ordered spins that in the principal-axis directions rotate by 60-degree steps between nearest neighbors on each sublattice that forms the honeycomb structure, consistent with the $P_Ac$ magnetic space group. We find that a few other magnetic subgroup symmetries ($P_A2/c$, $P_C2/m$, $P_S\bar{1}, P_C2, P_Cm, P_S1$) of the paramagnetic $P\bar{3}m11^\prime$ crystal symmetry are consistent with the observed diffraction pattern. We relate our findings to frustrated $J_1$-$J_2$-$J_3$ Heisenberg honeycomb antiferromagnets with single-ion anisotropy and the emergence of Potts nematicity

cond-mat.str-el↗

arXiv2022

Itinerant G-type antiferromagnet SrCr2As2 studied by magnetization, heat capacity, electrical resistivity, and NMR measurements

The physical properties of itinerant antiferromagnetic (AFM) SrCr$_2$As$_2$ with body-centered tetragonal ThCr$_2$Si$_2$ structure were investigated in single crystalline and polycrystalline forms by electrical resistivity $ρ$, heat capacity $C_{\rm p}$, magnetic susceptibility $χ$ versus temperature~$T$ and magnetization $M$ versus applied magnetic field $H$ isotherm measurements as well as $^{75}$As and $^{53}$Cr nuclear magnetic resonance (NMR) measurements in the wide temperature range $T$ = 1.6--900 K. From the $χ(T)$ and $^{75}$As NMR measurements, the G-type AFM state below $T_{\rm N}$ = 615(15) K has been determined, consistent with the previous neutron-diffraction measurements. Direct evidence of magnetic ordering of the Cr spins was shown by the observation of the $^{53}$Cr NMR spectrum under $H$ = 0. From the $χ(T)$ measurements on single-crystal SrCr$_2$As$_2$ under the two different magnetic field directions $H||ab$ and $H||c$ in the AFM state, the Cr ordered moments are shown to align along the $c$ axis in the G-type AFM state. The metallic state is directly evidenced by the $ρ$, $C_{\rm p}$, and NMR measurements, and the density of states at the Fermi energy ${\cal D}(E_{\rm F})$ in the AFM state is estimated to be 7.53 states/eV f.u. for both spin directions which is almost twice the bare ${\cal D}(E_{\rm F})$ estimated from first-principles calculations, suggesting an enhancement of the conduction-carrier mass by a factor of two in the AFM state. The ${\cal D}(E_{\rm F})$ is found to be nearly constant below at least 100 K and is independent of $H$. The $ρ(T)$ is found to show $T$-linear behavior above $T_{\rm N}$ and exhibits positive curvature below $T_{\rm N}$ where significant loss of spin-disorder scattering upon magnetic ordering is observed.

cond-mat.str-el↗

arXiv2021

Carrier Tuning of Stoner Ferromagnetism in ThCr$_{\mathbf{2}}$Si$_{\mathbf{2}}$-Structure Cobalt Arsenides

CaCo$_{2-y}$As$_2$ is an unusual itinerant magnet with signatures of extreme magnetic frustration. The conditions for establishing magnetic order in such itinerant frustrated magnets, either by reducing frustration or increasing electronic correlations, is an open question. Here we use results from inelastic neutron scattering and magnetic susceptibility measurements and density functional theory calculations to show that hole doping in Ca(Co$_{1-x}$Fe$_{x}$)$_{2-y}$As$_{2}$ suppresses magnetic order by quenching the magnetic moment while maintaining the same level of magnetic frustration. The suppression is due to tuning the Fermi energy away from a peak in the electronic density of states originating from a flat conduction band. This results in the complete elimination of the magnetic moment by $x\approx0.25$, providing a clear example of a Stoner-type transition.

cond-mat.str-el↗

arXiv2021

Incommensurate and commensurate antiferromagnetic states in CaMn2As2 and SrMn2As2 revealed by 75As NMR

We carried out $^{75}$As nuclear magnetic resonance (NMR) measurements on the trigonal CaMn$_2$As$_2$ and SrMn$_2$As$_2$ insulators exhibiting antiferromagnetic (AFM) ordered states below Néel temperatures $T_{\rm N}$ = 62 K and 120 K, respectively. In the paramagnetic state above $T_{\rm N}$, typical quadrupolar-split $^{75}$As-NMR spectra were observed for both systems. The $^{75}$As quadrupolar frequency $ν_{\rm Q}$ for CaMn$_2$As$_2$ decreases with decreasing temperature, while $ν_{\rm Q}$ for SrMn$_2$As$_2$ increases, showing an opposite temperature dependence.In the AFM state, the relatively sharp and distinct $^{75}$As NMR lines were observed in SrMn$_2$As$_2$ and the NMR spectra were shifted to lower fields for both magnetic fields $H$ $||$ $c$ axis and $H$ $||$ $ab$ plane, suggesting that the internal fields $B_{\rm int}$ at the As site produced by the Mn ordered moments are nearly perpendicular to the external magnetic field direction. No obvious distribution of $B_{\rm int}$ was observed in SrMn$_2$As$_2$, which clearly indicates a commensurate AFM state. In sharp contrast to SrMn$_2$As$_2$, broad and complex NMR spectra were observed in CaMn$_2$As$_2$ in the AFM state, which clearly shows a distribution of $B_{\rm int}$ at the As site, indicating an incommensurate state. From the analysis of the characteristic shape of the observed spectra, the AFM state of CaMn$_2$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 CaMn$_2$As$_2$ and SrMn$_2$As$_2$ show very large anisotropy in the nuclear spin-lattice relaxation rate 1/$T_1$ in the paramagnetic state. 1/$T_1$ for $H$ $||$ $ab$ is much larger than that for $H$ $|| $c$, indicating strong anisotropic AFM spin fluctuations in both compounds.

cond-mat.str-el↗

arXiv2021

First-order transitions at the Neel temperatures of trigonal SrMn2P2 and CaMn2P2 single crystals containing corrugated-honeycomb Mn sublattices

Single crystals of SrMn2P2 and CaMn2P2 were grown using Sn flux and characterized by single-crystal x-ray diffraction, electrical resistivity rho, heat capacity Cp, and magnetic susceptibility chi = M/H measurements versus temperature T and magnetization M versus applied magnetic field H isotherm measurements. The x-ray diffraction results show that both compounds adopt the trigonal CaAl2Si2-type structure. The rho(T) measurements demonstrate insulating ground states for both compounds. The chi(T) and Cp(T) data reveal a weak first-order antiferromagnetic (AFM) transition at the Neel temperature TN = 53(1) K for SrMn2P2 and a strong first-order AFM transition at TN = 69.8(3) K for CaMn2P2. Both compounds show an isotropic and nearly T-independent chi(T < TN). {31}P NMR measurements confirm the strong first-order transition in CaMn2P2 but show critical slowing down near TN for SrMn2P2 thus evidencing second-order character. The NMR measurements also 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 trigonal (Ca, Sr, Ba)Mn2(P, As, Sb, Bi)2 compounds which otherwise exhibit second-order AFM transitions. This result presents a challenge to understand the systematics of magnetic ordering in this class of materials in which magnetically-frustrated antiferromagnetism is quasi-two-dimensional.

cond-mat.str-el↗

arXiv2020

Magnetic detwinning and biquadratic magnetic interaction in EuFe2As2 revealed by 153Eu NMR

In the nematic state of iron-based superconductors, twin formation often obscures the intrinsic, anisotropic, in-plane physical properties.Relatively high in-plane external magnetic fields $H_{\rm ext}$ greater than the typical lab-scale magnetic fields 10--15 T are usually required to completely detwin a sample. However, recently a very small in-plane $H_{\rm ext} \sim$ 0.1 T was found to be sufficient for detwinning the nematic domains in EuFe$_2$As$_2$. To explain this behavior, a microscopic theory based on biquadratic magnetic interactions between the Eu and Fe spins has been proposed. Here, using $^{153}$Eu nuclear magnetic resonance (NMR) measurements below the Eu$^{2+}$ ordering temperature, we show experimental evidence of the detwinning under small in-plane $H_{\rm ext}$. Our NMR study also reveals the evolution of the angles between the Eu and Fe spins during the detwinning process, which provides the first experimental evidence for the existence of biquadratic coupling in the system.

cond-mat.str-el↗

arXiv2020

Magnetic phase transitions in Eu(Co,Ni)2As2 single crystals

The effects of Ni doping in Eu(Co{1-x}Ni{x})2As2 single crystals with x =0 to 1 grown out of self flux are investigated via crystallographic, electronic transport, magnetic, and thermal measurements. All compositions adopt the body-centered-tetragonal ThCr2Si2 structure with space group I4/mmm. We also find 3-4% of randomly-distributed vacancies on the Co/Ni site. Anisotropic magnetic susceptibility chi(T) data versus temperature T show clear signatures of an antiferromagnetic (AFM) c-axis helix structure associated with the Eu{+2} spins-7/2 for x = 0 and x = 1 as previously reported. The chi(T) data for x = 0.03 and 0.10 suggest an anomalous 2q magnetic structure containing two helix axes along the c axis and in the ab plane, respectively, whereas for x = 0.75 and 0.82, a c-axis helix is inferred as previously found for x = 0 and 1. At intermediate compositions x = 0.2, 0.32, 0.42, 0.54, and 0.65 a magnetic structure with a large ferromagnetic (FM) c-axis component is found from magnetization versus field isotherms, suggested to be an incommensurate FM cone structure associated with the Eu spins, which consists of both AFM and FM components. In addition, the chi(T) and heat capacity data for x = 0.2--0.65 indicate the occurrence of itinerant FM order associated with the Co/Ni atoms with Curie temperatures from 60 K to 25 K, respectively. Electrical resistivity measurements indicate metallic character for all compositions with abrupt increases in slope on cooling below the Eu AFM transition temperatures. In addition to this panoply of magnetic transitions, {151}Eu Mossbauer measurements indicate that ordering of the Eu moments proceeds via an incommensurate sine amplitude-modulated structure with additional transition temperatures associated with this effect.

cond-mat.str-el↗

arXiv2020

Emergence of ferromagnetism due to Ir substitutions in single-crystalline Ba[Co(1 x)Ir(x)]2As2

The ternary-arsenide compound BaCo2As2 was previously proposed to be in proximity to a quantum-critical point where long-range ferromagnetic (FM) order is suppressed by quantum fluctuations. Here we report the effect of Ir substitution for Co on the magnetic and thermal properties of Ba[Co(1-x)Ir(x)]2As2 (0 <= x <= 0.25) single crystals. These compositions all crystallize in an uncollapsed body-centered-tetragonal ThCr2Si2 structure with space group I4/mmm. Magnetic susceptibility measurements reveal clear signatures of FM ordering for x >= 0.11 with a nearly composition-independent Curie temperature TC = 13 K. The small variation of TC with x, the occurrence of hysteresis in magnetization versus field isotherms at low field and temperature, very small spontaneous and remanent magnetizations < 0.01 muB/f.u., and thermomagnetic irreversibility in the low-temperature region together indicate that the FM response arises from short-range FM ordering of spin clusters as previously inferred to occur in Ca[Co{1-x}Ir{x}]{2-y}As2. Heat-capacity Cp(T) data do not exhibit any clear feature around TC, further indicating that the FM ordering is short-range and/or associated with itinerant moments. The Cp(T) in the paramagnetic temperature regime 25-300 K is well described by the sum of a Sommerfeld electronic contribution and Debye and Einstein lattice contributions where the latter suggests the occurrence of low-frequency optic modes associated with the heavy Ba atoms in the crystals.

cond-mat.str-el↗

arXiv2020

Ferromagnetic cluster-glass phase in Ca(Co,Ir)2As2 crystals

Single crystals of Ca[Co_(2-x)Ir_(x)]_(2-y)As2 with 0 <= x <= 0.35 and 0.10 <= y <= 0.14 have been grown using the self-flux technique and characterized by single-crystal x-ray diffraction (XRD), energy-dispersive x-ray spectroscopy, magnetization M and magnetic susceptibility chi measurements versus temperature T, magnetic field H, and time t, and heat capacity Cp(H,T) measurements. The XRD refinements reveal that all the Ir-substituted crystals crystallize in a collapsed-tetragonal structure as does the parent CaCo_(2-y)As2 compound. A small 3.3% Ir substitution for Co in CaCo_(1.86)As2 drastically lowers the A-type antiferromagnetic (AFM) transition temperature TN from 52 to 23 K with a significant enhancement of the Sommerfeld electronic heat-capacity coefficient. The positive Weiss temperatures obtained from Curie-Weiss fits to the chi(T>TN) data indicate that the dominant magnetic interactions are ferromagnetic (FM) for all x. A magnetic phase boundary is inferred to be present between x = 0.14 and x = 0.17 from a discontinuity in the x dependences of the effective moment and Weiss temperature in the Curie-Weiss fits. FM fluctuations that strongly increase with increasing x are also revealed from the chi(T) data. The magnetic ground state for x >= 0.17 is a spin glass as indicated by hysteresis in chi(T) between field-cooling and zero-field-cooling measurements and from the relaxation of M in a small field that exhibits a stretched-exponential time dependence. The spin glass has a small FM component to the ordering and is hence inferred to be comprised of small FM clusters. A logarithmic T dependence of Cp at low T for x = 0.14 is consistent with the presence of significant FM quantum fluctuations. This composition is near the T = 0 boundary at x = 0.16 between the A-type AFM phase containing ferromagnetically-aligned layers of spins and the FM cluster-glass phase.

cond-mat.str-el↗

arXiv2019

Helical magnetic ordering in Sr(Co1-xNix)2As2

SrCo2As2 is a peculiar itinerant magnetic system that does not order magnetically, but inelastic neutron scattering experiments observe the same stripe-type antiferromagnetic (AF) fluctuations found in many of the Fe-based superconductors along with evidence of magnetic frustration. Here we present results from neutron diffraction measurements on single crystals of Sr(Co1-xNix)2As2 that show the development of long-range AF order with Ni-doping. However, the AF order is not stripe-type. Rather, the magnetic structure consists of ferromagnetically-aligned (FM) layers (with moments laying in the layer) that are AF arranged along c with an incommensurate propagation vector of (0 0 tau), i.e. a helix. Using high-energy x-ray diffraction, we find no evidence for a temperature-induced structural phase transition that would indicate a collinear AF order. This finding supports a picture of competing FM and AF interactions within the square transition-metal layers due to flat-band magnetic instabilities. However, the composition dependence of the propagation vector suggests that far more subtle Fermi surface and orbital effects control the interlayer magnetic correlations.

cond-mat.str-el↗

arXiv2019

Competing magnetic phases and itinerant magnetic frustration in SrCo$_{2}$As$_{2}$

Whereas magnetic frustration is typically associated with local-moment magnets in special geometric arrangements, here we show that SrCo$_{2}$As$_{2}$ is a candidate for frustrated itinerant magnetism. Using inelastic neutron scattering (INS), we find that antiferromagnetic (AF) spin fluctuations develop in the square Co layers of SrCo$_{2}$As$_{2}$ below $T\approx100$ K centered at the stripe-type AF propagation vector of $(\frac{1}{2},~\frac{1}{2})$, and that their development is concomitant with a suppression of the uniform magnetic susceptibility determined via magnetization measurements. We interpret this switch in spectral weight as signaling a temperature-induced crossover from an instability towards FM ordering to an instability towards stripe-type AF ordering on cooling, and show results from Monte-Carlo simulations for a $J_{1}$-$J_{2}$ Heisenberg model that illustrate how the crossover develops as a function of the frustration ratio $-J_1/(2J_2)$. By putting our INS data on an absolute scale, we quantitatively compare them and our magnetization data to exact-diagonalization calculations for the $J_{1}$-$J_{2}$ model [N. Shannon et al., Eur. Phys. J. B 38, 599 (2004)], and show that the calculations predict a lower level of magnetic frustration than indicated by experiment. We trace this discrepancy to the large energy scale of the fluctuations ($J_{\text{avg}}\gtrsim75$ meV), which, in addition to the steep dispersion, is more characteristic of itinerant magnetism.

cond-mat.str-el↗

arXiv2019

Non-Fermi-liquid behaviors associated with a magnetic quantum-critical point in Sr(Co{1-x}Ni{x})2As2 single crystals

Electron-doped Sr(Co{1-x}Ni{x})2As2 single crystals with compositions x = 0 to 0.9 were grown out of self-flux and SrNi2As2 single crystals out of Bi flux. The crystals were characterized using single-crystal x-ray diffraction (XRD), magnetic susceptibility chi(H,T), isothermal magnetization M(H,T), heat capacity Cp(H,T), and electrical resistivity ho(H,T) measurements versus applied magnetic field H and temperature T. The chi(T) data show that the crystals exhibit an antiferromagnetic (AFM) ground state almost immediately upon Ni doping on the Co site. Ab-initio electronic-structure calculations for x = 0 and x = 0.15 indicate that a flat band with a peak in the density of states just above the Fermi energy is responsible for this initial magnetic-ordering behavior on Ni doping. The Curie-Weiss-like T dependence of χin the paramagnetic (PM) state indicates dominant ferromagnetic (FM) interactions. The small ordered moments ~0.1 muB per transition metal atom and the values of the Rhodes-Wohlfarth ratio indicate that the magnetism is itinerant. The Cp(T) at low T exhibits Fermi-liquid behavior for 0 < x < 0.15 whereas an evolution to a logarithmic non-Fermi-liquid (NFL) behavior is found for x = 0.2 to 0.3. The logarithmic dependence is suppressed in an applied magnetic field. The low- T rho(H = 0,T) data show a T^2 dependence for 0 < x < 0.20 and a power-law dependence with n < 2 for x = 0.20 and 0.30. These low-T NFL behaviors observed in the Cp and rho measurements are most evident near the quantum-critical concentration x ~ 0.3 at which a T = 0 composition-induced transition from the AFM phase to the PM phase occurs.

cond-mat.str-el↗

arXiv2019

Antiferromagnetic Stacking of Ferromagnetic Layers and Doping Controlled Phase Competition in Ca$_{1-x}$Sr$_{x}$Co$_{2-y}$As$_{2}$

In search of a quantum phase transition between the two-dimensional ($2$D) ferromagnetism of CaCo$_{2-y}$As$_{2}$ and stripe-type antiferromagnetism in SrCo$_{2}$As$_{2}$, we rather find evidence for $1$D magnetic frustration between magnetic square Co layers. We present neutron diffraction data for Ca$_{1-x}$Sr$_{x}$Co$_{2-y}$As$_{2}$ that reveal a sequence of $x$-dependent magnetic transitions which involve different stacking of $2$D ferromagnetically-aligned layers with different magnetic anisotropy. We explain the $x$-dependent changes to the magnetic order by utilizing classical analytical calculations of a $1$D Heisenberg model where single-ion magnetic anisotropy and frustration of antiferromagnetic nearest- and next-nearest-layer exchange are all composition dependent.

cond-mat.str-el↗

arXiv2019

Helical Antiferromagnetic Ordering in EuNi{1.95}As2

The Eu{+2} spins-7/2 in EuNi2As2 with the body-centered tetragonal ThCr2Si2 structure order antiferromagnetically below the Neel temperature TN =15 K into a helical antiferromagnetic (AFM) structure with the helix axis aligned along the tetragonal c axis and the Eu ordered moments aligned ferromagnetically within the ab plane as previously reported from neutron diffraction measurements [T. Jin, et al., Phys. Rev. B 99, 014425 (2019)]. Here we study the crystallographic, magnetic, thermal, and electronic transport properties of Bi-flux-grown single crystals using single-crystal x-ray diffraction, anisotropic magnetic susceptibility chi, isothermal magnetization M, heat capacity Cp, and electrical resistivity rho measurements versus applied magnetic field H and temperature T. Vacancies are found on the Ni sites corresponding to the composition EuNi{1.95}As2. The chi{ab}(T) data below TN are fitted well by molecular field theory (MFT), and the helix turn angle kd and the Eu-Eu Heisenberg exchange constants are extracted from the fit parameters. The kd value is in good agreement with the neutron-diffraction result. The magnetic contribution to the zero-field heat capacity below TN is also fitted by MFT. The isothermal in-plane magnetization Mab exhibits two metamagnetic transitions versus H, whereas Mc(T = 2 K) is nearly linear up to H =14 T, both behaviors being consistent with MFT. The Mc(H,T), rho(Hc,T), and Cp(Hc,T) data yielded a Hc-T phase diagram separating the AFM and paramagnetic phases in good agreement with MFT. Anisotropic chi(T) literature data for the ThCr2Si2-type helical antiferromagnet EuRh2As2 are also fitted well by MFT. A comparison is made between the crystallographic and magnetic properties of ThCr2Si2- type EuM2Pn2 compounds with M = Fe, Co, Ni, Cu, or Rh, and Pn = P or As, where only ferromagnetic and c-axis helical AFM structures are found.

cond-mat.str-el↗

arXiv2018

EPR measurements of Eu{+2} spins in metallic EuCo{2-y}As2 single crystals

The Eu{+2} spins S = 7/2 in the metallic compound EuCo{2-y}As2 order into an antiferromagnetic helical structure below a Neel temperature TN = 40 to 45 K. The effective magnetic moment mu_eff of the Eu spins in the paramagnetic state from 100 to 300 K is found from static magnetic susceptibility measurements to be enhanced by about 7% compared to the value expected for spectroscopic splitting factor g = 2, and the saturation moment at high applied fields H and low temperatures T is also sometimes enhanced. Here electron-paramagnetic-resonance (CW EPR) measurements versus applied magnetic field H at fixed X-band rf (microwave) angular frequency omega were carried out using a linearly-polarized rf magnetic field oriented perpendicular to H to study the microscopic magnetic properties of the Eu spins. In order to analyze the data, the complex magnetic susceptibility chi(omega) at fixed H was used that was derived for linearly-polarized rf fields from the modified Bloch equations [M. A. Garstens and J. I. Kaplan, Phys. Rev. 99, 459 (1955)] (GK). It is shown that their formulation when applied to calculate the Dysonian absorptive susceptibility chi_D''(H) of local magnetic moments in metals yields a prediction that can be very different from the traditionally-used form of chi_D''(H). By fitting the derivative of the field-swept CW EPR data for EuCo{2-y}As2 by chi_D''(H) at fixed omega derived from the GK chi_D''(omega) at fixed H, the Eu spin spectroscopic splitting factor (g-factor) is found to be approximately 2.00 from 300 to ~125 K, and then to continuously increase to approximately 2.16 on further cooling to 50 K. We speculate that the enhancement of the Eu g-factor on cooling from 125 to 50 K arises from continuously-increasing local short-range ferromagnetic correlations between the Co 3d-band electrons and the Eu spins.

cond-mat.str-el↗

arXiv2018

Enhanced moments of Eu in single crystals of the metallic helical antiferromagnet EuCo{2-y}As2

The compound EuCo{2-y}As2 with the tetragonal ThCr2Si2 structure is known to contain Eu{+2} ions with spin S = 7/2 that order below a temperature TN = 47 K into an antiferromagnetic (AFM) proper helical structure with the ordered moments aligned in the tetragonal ab plane, perpendicular to the helix axis along the c axis, with no contribution from the Co atoms. Here we carry out a detailed investigation of the properties of single crystals. Enhanced ordered and effective moments of the Eu spins are found in most of our crystals. Electronic structure calculations indicate that the enhanced moments arise from polarization of the d bands, as occurs in ferromagnetic Gd metal. Electrical resistivity measurements indicate metallic behavior. The low-field in-plane magnetic susceptibilities chi{ab}(T < TN) for several crystals are reported that are fitted well by unified molecular field theory (MFT), and the Eu-Eu exchange interactions Jij are extracted from the fits. High-field magnetization M data for magnetic fields H||ab reveal what appears to be a first-order spin-flop transition followed at higher field by a second-order metamagnetic transition of unknown origin, and then by another second-order transition to the paramagnetic (PM) state. For H||c, the magnetization shows only a second-order transition from the canted AFM to the PM state, as expected. The critical fields for the AFM to PM transition are in approximate agreement with the predictions of MFT. Heat capacity Cp measurements in zero and high H are reported. Phase diagrams for H||c and H||ab versus T are constructed from the high-field M(H,T) and Cp(H,T) measurements. The magnetic part Cmag(T, H = 0) of Cp(T, H = 0) is extracted and is fitted rather well below TN by MFT, although dynamic short-range AFM order is apparent in Cmag(T) up to about 70 K, where the molar entropy attains its high-T limit of R ln8.

cond-mat.str-el↗