No Arabic abstract
The origin of the electronic nematicity in FeSe, which occurs below a tetragonal-to-orthorhombic structural transition temperature $T_s$ ~ 90 K, well above the superconducting transition temperature $T_c = 9$ K, is one of the most important unresolved puzzles in the study of iron-based superconductors. In both spin- and orbital-nematic models, the intrinsic magnetic excitations at $mathbf{Q}_1=(1, 0)$ and $mathbf{Q}_2=(0, 1)$ of twin-free FeSe are expected to behave differently below $T_s$. Although anisotropic spin fluctuations below 10 meV between $mathbf{Q}_1$ and $mathbf{Q}_2$ have been unambiguously observed by inelastic neutron scattering around $T_c (<<T_s)$, it remains unclear whether such an anisotropy also persists at higher energies and associates with the nematic transition $T_s$. Here we use resonant inelastic x-ray scattering (RIXS) to probe the high-energy magnetic excitations of uniaxial-strain detwinned FeSe. A prominent anisotropy between the magnetic excitations along the $H$ and $K$ directions is found to persist to $sim200$ meV, which is even more pronounced than the anisotropy of spin waves in BaFe$_2$As$_2$. This anisotropy decreases gradually with increasing temperature and finally vanishes at a temperature around the nematic transition temperature $T_s$. Our results reveal an unprecedented strong spin-excitation anisotropy with a large energy scale well above the $d_{xz}/d_{yz}$ orbital splitting, suggesting that the nematic phase transition is primarily spin-driven. Moreover, the measured high-energy spin excitations are dispersive and underdamped, which can be understood from a local-moment perspective. Our findings provide the much-needed understanding of the mechanism for the nematicity of FeSe and point to a unified description of the correlation physics across seemingly distinct classes of Fe-based superconductors.
FeSe is arguably the simplest, yet the most enigmatic, iron-based superconductor. Its nematic but non-magnetic ground state is unprecedented in this class of materials and stands out as a current puzzle. Here, our NMR measurements in the nematic state of mechanically detwinned FeSe reveal that both the Knight shift and the spin-lattice relaxation rate 1/T_1 possess an in-plane anisotropy opposite to that of the iron pnictides LaFeAsO and BaFe2As2. Using a microscopic electron model that includes spin-orbit coupling, our calculations show that an opposite quasiparticle weight ratio between the d_xz and d_yz orbitals leads to an opposite anisotropy of the orbital magnetic susceptibility, which explains our Knight shift results. We attribute this property to a different nature of nematic order in the two compounds, predominantly bond-type in FeSe and onsite ferro-orbital in pnictides. The T_1 anisotropy is found to be inconsistent with existing neutron scattering data in FeSe, showing that the spin fluctuation spectrum reveals surprises at low energy, possibly from fluctuations that do not break C_4 symmetry. Therefore, our results reveal that important information is hidden in these anisotropies and they place stringent constraints on the low-energy spin correlations as well as on the nature of nematicity in FeSe.
The importance of the spin-orbit coupling (SOC) effect in Fe-based superconductors (FeSCs) has recently been under hot debate. Considering the Hunds coupling-induced electronic correlation, the understanding of the role of SOC in FeSCs is not trivial and is still elusive. Here, through a comprehensive study of 77Se and 57Fe nuclear magnetic resonance, a nontrivial SOC effect is revealed in the nematic state of FeSe. First, the orbital-dependent spin susceptibility, determined by the anisotropy of the 57Fe Knight shift, indicates a predominant role from the 3dxy orbital, which suggests the coexistence of local and itinerant spin degrees of freedom (d.o.f.) in the FeSe. Then, we reconfirm that the orbital reconstruction below the nematic transition temperature (Tnem ~ 90 K) happens not only on the 3dxz and 3dyz orbitals but also on the 3dxy orbital, which is beyond a trivial ferro-orbital order picture. Moreover, our results also indicate the development of a coherent coupling between the local and itinerant spin d.o.f. below Tnem, which is ascribed to a Hunds coupling-induced electronic crossover on the 3dxy orbital. Finally, due to a nontrivial SOC effect, sizable in-plane anisotropy of the spin susceptibility emerges in the nematic state, suggesting a spin-orbital-intertwined nematicity rather than simply spin- or orbital-driven nematicity}. The present work not only reveals a nontrivial SOC effect in the nematic state but also sheds light on the mechanism of nematic transition in FeSe.
We report high resolution ARPES measurements of detwinned FeSe single crystals. The application of a mechanical strain is used to promote the volume fraction of one of the orthorhombic domains in the sample, which we estimate to be 80$%$ detwinned. While the full structure of the electron pockets consisting of two crossed ellipses may be observed in the tetragonal phase at temperatures above 90~K, we find that remarkably, only one peanut-shaped electron pocket oriented along the longer $a$ axis contributes to the ARPES measurement at low temperatures in the nematic phase, with the expected pocket along $b$ being not observed. Thus the low temperature Fermi surface of FeSe as experimentally determined by ARPES consists of one elliptical hole pocket and one orthogonally-oriented peanut-shaped electron pocket. Our measurements clarify the long-standing controversies over the interpretation of ARPES measurements of FeSe.
Nematic state, where the system is translationally invariant but breaks the rotational symmetry, has drawn great attentions recently due to experimental observations of such a state in both cuprates and iron-based superconductors. The mechanism of nematicity that is likely tied to the pairing mechanism of high-Tc, however, still remains controversial. Here, we studied the electronic structure of multilayer FeSe film by angle-resolved photoemission spectroscopy (ARPES). We found that the FeSe film enters the nematic state around 125 K, while the electronic signature of long range magnetic order has not been observed down to 20K indicating the non-magnetic origin of the nematicity. The band reconstruction in the nematic state is characterized by the splitting of the dxz and dyz bands. More intriguingly, such energy splitting is strong momentum dependent with the largest band splitting of ~80meV at the zone corner. The simple on-site ferro-orbital ordering is insufficient to reproduce the nontrivial momentum dependence of the band reconstruction. Instead, our results suggest that the nearest-neighbor hopping of dxz and dyz is highly anisotropic in the nematic state, the origin of which holds the key in understanding the nematicity in iron-based superconductors.
We study superconducting FeSe (Tc = 9 K) exhibiting the tetragonal-orthorhombic structural transition (Ts = 90 K) without any antiferromagnetic ordering, by utilizing angle-resolved photoemission spectroscopy. In the detwinned orthorhombic state, the energy position of the dyz orbital band at the Brillouin zone corner is 50 meV higher than that of dxz, indicating the orbital order similar to NaFeAs and BaFe2As2 families. Evidence of orbital order also appears in the hole bands at the Brillouin zone center. Precisely measured temperature dependence using strain-free samples shows that the onset of the orbital ordering (To) occurs very close to Ts, thus suggesting that the electronic nematicity above Ts is considerably weaker in FeSe compared to BaFe2As2 family.