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.Comment: 18 pages, 15 figures, 4 tables, 61 references; v2: extended the fits
of experimental data by additional electronic structure calculations;
published versio
