No Arabic abstract
The electronic nematic phase is an unconventional state of matter that spontaneously breaks the rotational symmetry of electrons. In iron-pnictides/chalcogenides and cuprates, the nematic ordering and fluctuations have been suggested to have as-yet-unconfirmed roles in superconductivity. However, most studies have been conducted in thermal equilibrium, where the dynamical property and excitation can be masked by the coupling with the lattice. Here we use femtosecond optical pulse to perturb the electronic nematic order in FeSe. Through time-, energy-, momentum- and orbital-resolved photo-emission spectroscopy, we detect the ultrafast dynamics of electronic nematicity. In the strong-excitation regime, through the observation of Fermi surface anisotropy, we find a quick disappearance of the nematicity followed by a heavily-damped oscillation. This short-life nematicity oscillation is seemingly related to the imbalance of Fe 3dxz and dyz orbitals. These phenomena show critical behavior as a function of pump fluence. Our real-time observations reveal the nature of the electronic nematic excitation instantly decoupled from the underlying lattice.
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.
In the mixed-valence manganites, a near-infrared laser typically melts the orbital and spin order simultaneously, corresponding to the photoinduced $d^{1}d^{0}$ $xrightarrow{}$ $d^{0}d^{1}$ excitations in the Mott-Hubbard bands of manganese. Here, we use ultrafast methods -- both femtosecond resonant x-ray diffraction and optical reflectivity -- to demonstrate that the orbital response in the layered manganite Nd$_{1-x}$Sr$_{1+x}$MnO$_{4}$ ($it{x}$ = 2/3) does not follow this scheme. At the photoexcitation saturation fluence, the orbital order is only diminished by a few percent in the transient state. Instead of the typical $d^{1}d^{0}$ $xrightarrow{}$ $d^{0}d^{1}$ transition, a near-infrared pump in this compound promotes a fundamentally distinct mechanism of charge transfer, the $d^{0}$ $ xrightarrow{}$ $d^{1}L$, where $it{L}$ denotes a hole in the oxygen band. This novel finding may pave a new avenue for selectively manipulating specific types of order in complex materials of this class.
FeSe$_{x}$Te$_{1-x}$ compounds present a complex phase diagram, ranging from the nematicity of FeSe to the $(pi, pi)$ magnetism of FeTe. We focus on FeSe$_{0.4}$Te$_{0.6}$, where the nematic ordering is absent at equilibrium. We use a time-resolved approach based on femtosecond light pulses to study the dynamics following photoexcitation in this system. The use of polarization-dependent time- and angle-resolved photoelectron spectroscopy allows us to reveal a photoinduced nematic metastable state, whose stabilization cannot be interpreted in terms of an effective photodoping. We argue that the 1.55 eV photon-energy-pump-pulse perturbs the $C_4$ symmetry of the system triggering the realization of the nematic state. The possibility to induce nematicity using an ultra-short pulse sheds a new light on the driving force behind the nematic symmetry breaking in iron-based superconductors. Our results weaken the idea that a low-energy coupling with fluctuations is a necessary condition to stabilize the nematic order and ascribe the origin of the nematic order in iron-based superconductors to a clear tendency of those systems towards orbital differentiation due to strong electronic correlations induced by the Hunds coupling.
Raman experiments on bulk FeSe revealed that the low-frequency part of $B_{1g}$ Raman response $R_{B_{1g}}$, which probes nematic fluctuations, rapidly decreases below the nematic transition at $T_n sim 85$K. Such behavior is usually associated with the gap opening and at a first glance is inconsistent with the fact that FeSe remains a metal below $T_n$, with sizable hole and electron pockets. We argue that the drop of $R_{B_{1g}}$ in a nematic metal comes about because the nematic order drastically changes the orbital content of the pockets and makes them nearly mono-orbital. In this situation $B_{1g}$ Raman response gets reduced by the same vertex corrections that enforce charge conservation. The reduction holds at low frequencies and gives rise to gap-like behavior of $R_{B_{1g}}$, in full agreement with the experimental data.
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.