arXiv subjects

D. C. Johnston

Publications and source records attributed to D. C. Johnston.

At least 73 records · Page 4Linked to original sources

arXiv2015

Coexistence of antiferromagnetic and ferromagnetic spin correlations in SrCo2As2 revealed by 59Co and 75As NMR

In nonsuperconducting, metallic paramagnetic SrCo2As2, inelastic neutron scattering measurements have revealed strong stripe-type $χ$(q) = ($π$,0) antiferromagnetic (AFM) spin correlations. Here, using nuclear magnetic resonance (NMR) measurements on 59Co and 75As nuclei, we demonstrate that stronger ferromagnetic (FM) spin correlations coexist in SrCo2As2. Our NMR data are consistent with density functional theory (DFT) calculations which show enhancements at both q = ($π$,0) and the in-plane FM q = 0 wavevectors in static magnetic susceptibility $χ$(q). We suggest that the strong FM fluctuations prevent superconductivity in SrCo2As2, despite the presence of stripe-type AFM fluctuations. Furthermore, since DFT calculations have consistently revealed similar enhancements of the $χ$(q) at both q = ($π$,0) and q = 0 in the iron-based superconductors and parent compounds, our observation of FM correlations in SrCo2As2 calls for detailed studies of FM correlations in the iron-based superconductors.

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arXiv2015

Antiferromagnetism in EuCu2As2 and EuCu1.82Sb2 Single Crystals

Single crystals of EuCu2As2 and EuCu2Sb2 were grown from CuAs and CuSb self-flux, respectively. The crystallographic, magnetic, thermal and electronic transport properties of the single crystals were investigated by room-temperature x-ray diffraction (XRD), magnetic susceptibility χversus temperature T, isothermal magnetization M versus magnetic field H, specific heat Cp(T) and electrical resistivity ρ(T) measurements. EuCu2As2 crystallizes in the body-centered tetragonal ThCr2Si2-type structure (space group I4/mmm), whereas EuCu2Sb2 crystallizes in the related primitive tetragonal CaBe2Ge2-type structure (space group P4/nmm). The energy-dispersive x-ray spectroscopy and XRD data for the EuCu2Sb2 crystals showed the presence of vacancies on the Cu sites, yielding the actual composition EuCu1.82Sb2. The ρ(T) and Cp(T) data reveal metallic character for both EuCu2As2 and EuCu1.82Sb2. Antiferromagnetic (AFM) ordering is indicated from the χ(T), Cp(T), and ρ(T) data for both EuCu2As2 (T_N = 17.5 K) and EuCu1.82Sb2 (T_N = 5.1 K). In EuCu1.82Sb2, the ordered-state χ(T) and M(H) data suggest either a collinear A-type AFM ordering of Eu+2 spins S=7/2 or a planar noncollinear AFM structure, with the ordered moments oriented in the tetragonal ab plane in either case. This ordered-moment orientation for the A-type AFM is consistent with calculations with magnetic dipole interactions. The anisotropic χ(T) and isothermal M(H) data for EuCu2As2, also containing Eu+2 spins S=7/2, strongly deviate from the predictions of molecular field theory for collinear AFM ordering and the AFM structure appears to be both noncollinear and noncoplanar.

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arXiv2015

Itinerant ferromagnetism in the As 4$p$ conduction band of Ba$_{0.6}$K$_{0.4}$Mn$_{2}$As$_{2}$ identified by x-ray magnetic circular dichroism

X-ray magnetic circular dichroism (XMCD) measurements on single-crystal and powder samples of Ba$_{0.6}$K$_{0.4}$Mn$_{2}$As$_{2}$ show that the ferromagnetism below $T_{\textrm{C}}\approx$ 100 K arises in the As $4p$ conduction band. No XMCD signal is observed at the Mn x-ray absorption edges. Below $T_{\textrm{C}}$, however, a clear XMCD signal is found at the As $K$ edge which increases with decreasing temperature. The XMCD signal is absent in data taken with the beam directed parallel to the crystallographic $\textrm{c}$ axis indicating that the orbital magnetic moment lies in the basal plane of the tetragonal lattice. These results show that the previously reported itinerant ferromagnetism is associated with the As $4p$ conduction band and that distinct local-moment antiferromagnetism and itinerant ferromagnetism with perpendicular easy axes coexist in this compound at low temperature.

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arXiv2014

Crystallography and Physical Properties of BaCo2As2, Ba{0.94}K{0.06}Co2As2 and Ba{0.78}K{0.22}Co2As2

The crystallographic and physical properties of polycrystalline and single crystal samples of BaCo2As2 and K-doped Ba{1-x}K{x}Co2As2 (x = 0.06, 0.22) are investigated by x-ray and neutron powder diffraction, magnetic susceptibility chi, magnetization, heat capacity Cp, {75}As NMR and electrical resistivity rho measurements versus temperature T. The crystals were grown using both Sn flux and CoAs self-flux, where the Sn-grown crystals contain 1.6-2.0 mol% Sn. All samples crystallize in the tetragonal ThCr2Si2-type structure (space group I4/mmm). For BaCo2As2, powder neutron diffraction data show that the c-axis lattice parameter exhibits anomalous negative thermal expansion from 10 to 300 K, whereas the a-axis lattice parameter and the unit cell volume show normal positive thermal expansion over this T range. No transitions in BaCo2As2 were found in this T range from any of the measurements. Below 40-50 K, we find rho ~ T^2 indicating a Fermi liquid ground state. A large density of states at the Fermi energy D(EF) ~ 18 states/(eV f.u.) for both spin directions is found from low-T Cp(T) measurements, whereas the band structure calculations give D(EF) = 8.23 states/(eV f.u.). The {75}As NMR shift data versus T have the same T dependence as the chi(T) data, demonstrating that the derived chi(T) data are intrinsic. The observed {75}As nuclear spin dynamics are consistent with the presence of ferromagnetic and/or stripe-type antiferromagnetic spin fluctuations. The crystals of Ba{0.78}K{0.22}Co2As2 were grown in Sn flux and show properties very similar to those of undoped BaCo2As2. On the other hand, the crystals from two batches of Ba{0.94}K{0.06}Co2As2 grown in CoAs self-flux show evidence of weak ferromagnetism at T < 10 K with small ordered moments at 1.8 K of 0.007 and 0.03 muB per formula unit, respectively.

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arXiv2014

Magnetic transitions in the spin S=5/2 frustrated magnet BiMn2PO6 and strong lattice softening in BiMn2PO6 and BiZn2PO6 below 200 K

The crystallographic, magnetic and thermal properties of BiMn2PO6 and BiZn2PO6 were investigated by x-ray diffraction, magnetic susceptibility χ, heat capacity Cp, and 31P NMR measurements as well as by density-functional band-theory calculations. Both compounds show a strong monotonic lattice softening on cooling, where the Debye temperature decreases by a factor of two from Θ_D=650K at T=300K to Θ_D=300K at T=2K. The χ(T) data for BiMn2PO6 above 150K follow a Curie-Weiss law with a Curie constant consistent with a S=5/2 with g=2 and an antiferromagnetic (AFM) Weiss temperature θ_CW= -78K. The χdata indicate long-range AFM ordering below TN=30K, confirmed by a sharp lambda-type peak in Cp(T) at 28.8K. The band-theory calculations indicate that BiMn2PO6 is an AFM compound with dominant interactions J1/kB= 6.7K and J3/kB= 5.6K along the legs and rungs of a two-leg spin-ladder, respectively. In addition to the long-range AFM ordering at TN=30K, a second transition at 10 K is observed from the χand NMR measurements but is not evident in the Cp data. The Cp data at low T suggest a significant contribution from AFM spin waves moving in three dimensions and the absence of a spin-wave gap. A detailed analysis of the NMR spectra indicates commensurate magnetic order between 10K and 30K and a possible incommensurate modulation and/or spin canting below 10K. The commensurate order is consistent with microscopic simulations that yield a collinear Neel-type AFM spin arrangement both within and between the ladders, despite the presence of multiple weak interactions frustrating this magnetic structure. Frustration for AFM ordering and 1D spatial anisotropy of the 3D spin interactions are manifested in the frustration ratio f=|θCW|/TN=2.6, indicating a suppression of TN from 68K in the absence of these effects to 30K in BiMn2PO6.

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arXiv2014

Physical Properties of Metallic Antiferromagnetic CaCo{1.86}As2 Single Crystals

We report studies of CaCo{1.86}As2 single crystals. The electronic structure is probed by angle-resolved photoemission spectroscopy (ARPES) measurements of CaCo{1.86}As2 and by full-potential linearized augmented-plane-wave calculations for the supercell Ca8Co15As16 (CaCo{1.88}As2). Our XRD crystal structure refinement is consistent with the previous combined refinement of x-ray and neutron powder diffraction data showing a collapsed-tetragonal ThCr2Si2-type structure with 7(1)% vacancies on the Co sites corresponding to the composition CaCo{1.86}As2 [D. G. Quirinale et al., Phys. Rev. B 88, 174420 (2013)]. The anisotropic magnetic susceptibility chi(T) data are consistent with the magnetic neutron diffraction data of Quirianale et al. that demonstrate the presence of A-type collinear antiferromagnetic order below the Neel temperature TN = 52(1) K with the easy axis being the tetragonal c axis. However, no clear evidence from the resistivity rho(T) and heat capacity Cp(T) data for a magnetic transition at TN is observed. A metallic ground state is demonstrated from band calculations and the rho(T), Cp(T) and ARPES data, and spin-polarized calculations indicate a competition between the A-type AFM and FM ground states. The Cp(T) data exhibit a large Sommerfield electronic coefficient reflecting a large density of states at the Fermi energy D(EF), consistent with the band structure calculations which also indicate a large D(EF) arising from Co 3d bands. At 1.8 K the M(H) data for H|| c exhibit a well-defined first-order spin-flop transition at an applied field of 3.5 T. The small ordered moment of 0.3 muB/Co obtained from the M(H) data at low T, the large exchange enhancement of chi and the lack of a self-consistent interpretation of the chi(T) and M(H,T) data in terms of a local moment Heisenberg model together indicate that the magnetism of CaCo{1.86}As2 is itinerant.

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arXiv2014

Physical properties of EuPd2As2 single crystals

The physical properties of self-flux grown EuPd2As2 single crystals have been investigated by magnetization M, magnetic susceptibility chi, specific heat Cp, and electrical resistivity rho measurements versus temperature T and magnetic field H. The crystal structure was determined by powder x-ray diffraction measurements, which confirmed the ThCr2Si2-type body-centered tetragonal structure (space group I4/mmm) reported previously. The rho(T) data indicate that state of EuPd2As2 is metallic. Long-range antiferromagnetic (AFM) ordering is apparent from the chi(T), Cp(T), and rho(T) measurements. For H \parallel c the chi(T) indicates two transitions at TN1 = 11.0 K and TN2 = 5.5 K, whereas for H \perp c only one transition is observed at TN1 = 11.0 K. Between TN1 and TN2 the anisotropic chi(T) data suggest a planar noncollinear AFM structure, whereas at T < TN2 the chi(T) and M(H,T) data suggest a spin reorientation transition in which equal numbers of spins cant in opposite directions out of the ab plane. We estimate the critical field at 2 K at which all Eu moments become aligned with the field to be about 22 T. The magnetic entropy at 25 K estimated from the Cp(T) measurements is about $11\%$ smaller than expected, possibly due to an inaccuracy in the lattice heat capacity contribution. An upturn in rho at T < TN1 suggests superzone energy gap formation below TN1. This behavior of rho(T < TN1) is not sensitive to applied magnetic fields up to H = 12 T.

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arXiv2014

Helical Antiferromagnetic Ordering in Lu{1-x}Sc{x}MnSi (x = 0, 0.25, 0.50)

Polycrystalline samples of Lu{1-x}Sc{x}MnSi (x= 0, 0.25, 0.50) are studied using powder x-ray diffraction (XRD), heat capacity Cp, magnetization M, magnetic susceptibility chi, and electrical resistivity rho measurements versus temperature T and magnetic field H. This system crystallizes in the primitive orthorhombic TiNiSi-type structure (space group Pnma) as previously reported. The rho(T) data indicate metallic behavior. The Cp(T), chi(T), and rho(T) measurements consistently indicate long-range antiferromagnetic (AF) transitions with AF ordering temperatures TN = 246, 215 and 188 K for x = 0, 0.025 and 0.50, respectively. A second transition is observed at somewhat lower T for each sample from the chi(T) and rho(T) measurements, which we speculate are due to spin reorientation transitions; these second transitions are completely suppressed in H = 5.5 T. The Cp data below 10 K for each composition indicate an enhanced Sommerfeld electronic heat capacity coefficient for the series in the range gamma = 24 to 29 mJ/mol K^2. The chi(T) measurements up to 1000 K were fitted by local-moment Curie-Weiss behaviors which indicate a low Mn spin S ~ 1. The chi data below TN are analyzed using the Weiss molecular field theory for a planar noncollinear helical AF structure with a composition-dependent pitch, following the previous neutron diffraction work of Venturini et al. [J. Alloys Compd. 256, 65 (1997)]. Within this model, the fits indicate a turn angle between Mn moments along the helix axis of ~100 degrees or ~145 degrees, either of which indicate dominant AF interactions between the Mn spins in the Lu{1-x}Sc{x}MnSi series of compounds.

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arXiv2014

Superconductivity and Physical Properties of CaPd2Ge2 Single Crystals

We present the superconducting and normal state properties of CaPd2Ge2 single crystal investigated by magnetic susceptibility χ, isothermal magnetization M, heat capacity C_p, in-plane electrical resistivity ρand London penetration depth λversus temperature T and magnetic field H measurements. Bulk superconductivity is inferred from the ρ(T) and C_p(T) data. The ρ(T) data exhibit metallic behavior and undergoes a superconducting transition with T_c onset = 1.98 K and zero resistivity state at T_c 0 = 1.67 K. The χ(T) reveal the onset of superconductivity at 2.0 K. For T>2.0 K, the χ(T) and M(H) are weakly anisotropic paramagnetic with χ_ab > χ_c. The C_p(T) confirm the bulk superconductivity below T_c = 1.69(3) K. The superconducting state electronic heat capacity is analyzed within the framework of a single-band α-model of BCS superconductivity and various normal and superconducting state parameters are estimated. Within the α-model, the C_p(T) data and the ab plane λ(T) data consistently indicate a moderately anisotropic s-wave gap with Δ(0)/k_B T_c ~ 1.6, somewhat smaller than the BCS value of 1.764. The relationship of the heat capacity jump at T_c and the penetration depth measurement to the anisotropy in the s-wave gap is discussed.

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arXiv2014

Magnetic susceptibility of frustrated spin-s J1-J2 quantum Heisenberg magnets: High-temperature expansion and exact diagonalization data

Motivated by recent experiments on low-dimensional frustrated quantum magnets with competing nearest-neighbor exchange coupling J1 and next nearest-neighbor exchange coupling J2 we investigate the magnetic susceptibility of two-dimensional J1-J2 Heisenberg models with arbitrary spin quantum number s. We use exact diagonalization and high-temperature expansion up to order 10 to analyze the influence of the frustration strength J2/J1 and the spin quantum number s on the position and the height of the maximum of the susceptibility. The derived theoretical data can be used to get information on the ratio J2/J1 by comparing with susceptibility measurements on corresponding magnetic compounds.

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arXiv2013

Metal-insulator transition in antiferromagnetic $Ba_{1-x}K_xMn_2As_2$ $(0\le x\le0.4)$ single crystals studied by $^{55}$Mn and $^{75}$As NMR

The magnetic structure and metal-insulator transition in antiferromagnetic (AFM) BaMn2As2 and Ba1-xKxMn2As2 single crystals have been investigated by 55Mn and 75As nuclear magnetic resonance (NMR) measurements. In the parent AFM insulator BaMn2As2 with a Neel temperature TN = 625 K, we observed a 55Mn zero-field NMR (ZFNMR) spectrum and confirmed the G-type AFM structure from the field dependence of the 55Mn spectra and 75As-NMR spectra below TN. In hole-doped crystals with x > 0.01, similar 55Mn ZFNMR spectra were observed and the AFM state was revealed to be robust up to x = 0.4 with the ordered moment nearly independent of x. The nuclear spin-lattice relaxation rates (1/T1) for both nuclei in the doped samples follow the Korringa relation T1T = const., indicating a metallic state. This confirms the coexistence of AFM ordered localized Mn spins and conduction carriers from a microscopic point of view. From the x-dependence of (T1T)^(-1/2) for both nuclei, we conclude that this transition is caused by vanishing of the hole concentration as the transition is approached from the metallic side.

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arXiv2013

Stripe Antiferromagnetic Spin Fluctuations in SrCo$_{2}$As$_{2}$

Inelastic neutron scattering measurements of paramagnetic SrCo$_{2}$As$_{2}$ at T=5 K reveal antiferromagnetic (AFM) spin fluctuations that are peaked at a wavevector of $\textbf{Q}_{\mathrm{AFM}}=(1/2,1/2,1)$ and possess a large energy scale. These stripe spin fluctuations are similar to those found in $A$Fe$_{2}$As$_{2}$ compounds, where spin-density wave AFM is driven by Fermi surface nesting between electron and hole pockets separated by $\textbf{Q}_{\mathrm{AFM}}$. SrCo$_{2}$As$_{2}$ has a more complex Fermi surface and band structure calculations indicate a potential instability towards either a ferromagnetic or stripe AFM ground state. The results suggest that stripe AFM magnetism is a general feature of both iron and cobalt-based arsenides and the search for spin fluctuation-induced unconventional superconductivity should be expanded to include cobalt-based compounds.

cond-mat.supr-con↗

arXiv2013

Crystal and Magnetic Structure of CaCo{1.86}As2 Studied by X-ray and Neutron Diffraction

Neutron and x-ray diffraction measurements are presented for powders and single crystals of CaCo{1.86}As2. The crystal structure is a collapsed-tetragonal ThCr2Si2-type structure as previously reported, but with 7(1)% vacancies on the Co sites corresponding to the composition CaCo{1.86(2)}As2. The thermal expansion coefficients for both the a- and c-axes are positive from 10 to 300 K. Neutron diffraction measurements on single crystals demonstrate the onset of A-type collinear antiferromagnetic order below the Neel temperature TN = 52(1) K with the ordered moments directed along the tetragonal c-axis, aligned ferromagnetically in the ab-plane and antiferromagnetically stacked along the c-axis.

cond-mat.supr-con↗

arXiv2013

Experimental evidence of a collinear antiferromagnetic ordering in the frustrated CoAl2O4 spinel

Nuclear magnetic resonance (NMR), neutron diffaction (ND), x-ray diffraction, magnetic susceptibility and specific heat measurements on the frustrated A-site spinel CoAl2O4 compound reveal a collinear antiferromagnetic ordering below Tn = 9.8(2) K. A high quality powder sample characterized by x-ray diffraction that indicates a relatively low Co-Al inversion parameter x = 0.057(20) in (Co1-xAlx)[Al2-xCox]O4, shows a broad maximum around 15 K in magnetic susceptibility and a sharp peak at Tn in heat capacity. The average ordered magnetic moment of Co^2+ (S = 3/2) ions at the A-site is estimated to be 2.4(1) Bohr magneton from NMR and 1.9(5) Bohr magneton from ND which are smaller than the expected value of 3 Bohr magneton for S = 3/2 and g = 2. Antiferromagnetic spin uctuations and correlations in the paramagnetic state are revealed from the magnetic susceptibility, NMR and ND measurements, which are due to spin frustration and site inversion effects in the system. The ND data also show short-range dynamic magnetic ordering that persists to a temperature that is almost twice Tn.

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arXiv2013

Crystallographic, Electronic, Thermal and Magnetic Properties of Single-Crystal SrCo2As2

In tetragonal SrCo2As2 single crystals, inelastic neutron scattering measurements demonstrated that strong stripe-type antiferromagnetic (AFM) correlations occur at a temperature T = 5 K [W. Jayasekara et al., arXiv:1306.5174] that are the same as in the isostructural AFe2As2 (A = Ca, Sr, Ba) parent compounds of high-Tc superconductors. This surprising discovery suggests that SrCo2As2 may also be a good parent compound for high-Tc superconductivity. Here, structural and thermal expansion, electrical resistivity rho, angle-resolved photoemission spectroscopy (ARPES), heat capacity Cp, magnetic susceptibility chi, 75As NMR and neutron diffraction measurements of SrCo2As2 crystals are reported together with LDA band structure calculations that shed further light on this fascinating material. The c-axis thermal expansion coefficient alpha_c is negative from 7 to 300 K, whereas alpha_a is positive over this T range. The rho(T) shows metallic character. The ARPES measurements and band theory confirm the metallic character and in addition show the presence of a flat band near the Fermi energy E_F. The band calculations exhibit an extremely sharp peak in the density of states D(E_F) arising from a flat d_{x^2 - y^2} band. A comparison of the Sommerfeld coefficient of the electronic specific heat with chi(T = 0) suggests the presence of strong ferromagnetic itinerant spin correlations which on the basis of the Stoner criterion predicts that SrCo2As2 should be an itinerant ferromagnet, in conflict with the magnetization data. The chi(T) does have a large magnitude, but also exhibits a broad maximum at 115 K suggestive of dynamic short-range AFM spin correlations, in agreement with the neutron scattering data. The measurements show no evidence for any type of phase transition between 1.3 and 300 K and we propose that metallic SrCo2As2 has a gapless quantum spin-liquid ground state.

cond-mat.supr-con↗

arXiv2013

Coexistence of Half-Metallic Itinerant Ferromagnetism with Local-Moment Antiferromagnetism in Ba{0.60}K{0.40}Mn2As2

Magnetization, nuclear magnetic resonance, high-resolution x-ray diffraction and magnetic field-dependent neutron diffraction measurements reveal a novel magnetic ground state of Ba{0.60}K{0.40}Mn2As2 in which itinerant ferromagnetism (FM) below a Curie temperature TC = 100 K arising from the doped conduction holes coexists with collinear antiferromagnetism (AFM) of the Mn local moments that order below a Neel temperature TN = 480 K. The FM ordered moments are aligned in the tetragonal ab-plane and are orthogonal to the AFM-ordered Mn moments that are aligned along the c-axis. The magnitude and nature of the low-T FM ordered moment correspond to complete polarization of the doped-hole spins (half-metallic itinerant FM) as deduced from magnetization and ab-plane electrical resistivity measurements.

cond-mat.supr-con↗

arXiv2013

Superconducting and Normal State Properties of APd2As2 (A = Ca, Sr, Ba) Single Crystals

The synthesis and crystallography, magnetic susceptibility chi, magnetization M, specific heat Cp, in-plane electrical resistivity rho and in-plane magnetic penetration depth measurements are reported for single crystals of APd2As2 (A = Ca, Sr, Ba) versus temperature T and magnetic field H. The crystals were grown using PdAs self-flux. CaPd2As2 and SrPd2As2 crystallize in a collapsed body-centered tetragonal ThCr2Si2-type structure (I4/mmm), whereas BaPd2As2 crystallizes in the primitive tetragonal CeMg2Si2-type structure (P4/mmm), in agreement with literature data. The rho(T) data exhibit metallic behavior for all three compounds. Bulk superconductivity is reported for CaPd2As2 and SrPd2As2 below Tc = 1.27 and 0.92 K, respectively, whereas only a trace of superconductivity is found in BaPd2As2. No other phase transitions were observed. The chi(T) and M(H) data reveal anisotropic diamagnetism in the normal state, with chi_c > chi_ab for CaPd2As2 and BaPd2As2, and chi_c < chi_ab for SrPd2As2. The normal and superconducting state data indicate that CaPd2As2 and SrPd2As2 are conventional type-II nodeless s-wave electron-phonon superconductors. The electronic superconducting-state heat capacity data for CaPd2As2, which has an extremely sharp heat capacity jump at Tc, are analyzed using our recent elaboration of the alpha-model of the BCS theory of superconductivity, which indicates that the s-wave gap in this compound is anisotropic in momentum space.

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arXiv2013

Angle-Resolved Photoemission Spectroscopy Study of BaCo2As2

We use angle-resolved photoemission spectroscopy and full-potential linearized augmented-plane-wave (FP-LAPW) calculations to study the electronic structure of BaCo2As2. The Fermi surface (FS) maps and the corresponding band dispersion data (at 90 K and 200 K) reveal a small electron pocket at the center and a large electron pocket at the corner of the Brillouin zone. Therefore the nesting between electron and hole FS pockets is absent in this compound, in contrast to the parent compounds of FeAs-based high-T_c superconductors. The electronic structure at about 500 meV binding energy is very similar to features at the chemical potential in BaFe2As2. This indicates that complete substitution of Co for Fe causes a nearly rigid shift in the Fermi energy by adding two electrons per formula unit without significant changes in the band dispersions. The experimental FS topology as well as band dispersion data are in reasonable agreement with the FP-LAPW calculations.

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