Abstract
We revisit the intriguing magnetic behavior of the paradigmatic itinerant frustrated magnet SrCo2As2, which shows strong and competing magnetic fluctuations yet does not develop long-range magnetic order. By calculating the static spin susceptibility χ(q) within a realistic 16-orbital Hubbard-Hund model, we determine the leading instability to be ferromagnetic (FM). We then explore the effect of doping and calculate the critical Hubbard interaction strength Uc that is required for the development of magnetic order. We find that Uc decreases under electron doping and with increasing Hund's coupling J, but increases rapidly under hole doping. This suggests that magnetic order could possibly emerge under electron doping but not under hole doping, which agrees with experimental findings. We map out the leading magnetic instability as a function of doping and Hund's coupling and find several antiferromagnetic phases in addition to FM. We also quantify the degree of itinerant frustration in the model and resolve the contributions of different orbitals to the magnetic susceptibility. Finally, we discuss the dynamic spin susceptibility χ(q,ω) at finite frequencies, where we recover the anisotropy of the peaks at Qπ=(π,0) and (0,π) observed by inelastic neutron scattering that is associated with the phenomenon of itinerant magnetic frustration. By comparing results between theory and experiment, we conclude that the essential experimental features of doped SrCo2As2 are well captured by an itinerant Hubbard-Hund multiorbital model if one considers a small shift of the chemical potential towards hole doping.
| Original language | English |
|---|---|
| Article number | 245149 |
| Journal | Physical Review B |
| Volume | 108 |
| Issue number | 24 |
| DOIs | |
| State | Published - Dec 15 2023 |
| Externally published | Yes |
Funding
The notion of itinerant frustration is supported by the observation that remains paramagnetic down to the lowest temperatures. The absence of magnetic order in was confirmed in NMR measurements down to 50 mK . While magnetic order is absent under hole doping to , minute amounts of electron doping induce long-range FM order in the Co layers. This suggests a complex and delicate balance between FM and AF fluctuations. For example, exhibits long-range magnetic order for with a complex helical magnetic structure, where FM Co layers (with moments in the layer) stack to form an incommensurate helix . We note that a symmetry-equivalent incommensurate spin-density wave structure is also consistent with the diffraction results. Electron doping via La substitution in and 2.5% Nd substitution in leads to the formation of 3D FM order .
| Funders | Funder number |
|---|---|
| National Science Foundation | MRI2018594, MRI1726447 |
| U.S. Department of Energy | |
| Office of Science | |
| Basic Energy Sciences | |
| Iowa State University | DE-AC02-07CH11358 |
| Division of Materials Sciences and Engineering | DE-SC0020045 |