Magnetic Properties Controlled by Interstitial or Interlayer Cations in Iron Chalcogenides

By applying density functional theory calculations to iron chalcogenides, we find that magnetic order in Fe${}_{1+y}$Te and magnetic instability at $(\pi ,\pi )$ in K${}_y$Fe${}_2$Se${}_2$ are controlled by interstitial and interlayer cations, respectively. While in Fe${}_{1+y}$Te, magnetic phase transitions occur among collinear, exotic bicollinear and plaquette-ordered antiferronmagnetic states when the height of interstitial irons measured from iron plane or the concentration of interstitial irons is varied, the magnetic instability at $(\pi ,\pi )$ which is believed to be responsible for the Cooper pairing in iron pnictides is significantly enhanced when $y$ is much smaller than $1$ in K${}_y$Fe${}_2$Se${}_2$. Our results indicate that, similar to iron pnictides, itinerant electrons play important roles in iron chalcogenides, even though the fluctuating local moments become larger.