Structural and magnetic properties of CaCo2-xAs2 (x = 0–0.3) in ThCr2Si2-type structure

Defects is of special importance in tuning the structure and physical properties of layered materials. Here the influence of transition metal Co vacancies on the structure and magnetism in collapsed tetragonal CaCo 2- x As 2 (0 ≤  x  ≤ 0.3) solid solutions are systematically investigated. The electrical properties show metallicity in all compounds. The crystal structure refinement exhibits that the lattice constant of the c axis and c / a ratio decreases as Co vacancies increase, revealing the formation of a more collapsed tetragonal structure in CaCo 2- x As 2 . Moreover, these introduced Co vacancies suppress the antiferromagnetic Néel temperature from 80 K down to 18 K until it disappears above 10 K in CaCo 1 · 7 As 2 . X-ray photoelectron spectroscopy reveals increased Co 3+ /Co 2+ value in CaCo 2- x As 2 with higher Co vacancies, which may result in the charge balance and the gradually suppressed T N . This study offers insights into tuning and understanding the magneto-structural characteristics in ThCr 2 Si 2 -type layered materials through transition metal vacancies.