Elucidating the microscopic origin of nematic order in iron-based superconducting materials is important because the interactions that drive nematic order may also mediate the Cooper pairing 1 .Nematic order breaks fourfold rotational symmetry in the iron plane, which is believed to be driven by either orbital or spin degrees of freedom [1][2][3][4][5] . However, as the nematic phase often develops at a temperature just above or coincides with a stripe magnetic phase transition, experimentally determining the dominant driving force of nematic order is difficult 1,6 . Here, we use neutron scat- tering to study structurally the simplest iron-based superconductor FeSe (ref. 7), which displays a nematic (orthorhombic) phase transition at T s = 90 K, but does not order antiferromagnetically.Our data reveal substantial stripe spin fluctuations, which are coupled with orthorhombicity and are enhanced abruptly on cooling to below T s . Moreover, a sharp spin resonance develops in the superconducting state, whose energy (∼ 4 meV) is consistent with an electron boson coupling mode revealed by scanning tunneling spectroscopy 8 , thereby suggesting a spin fluctuation-mediated signchanging pairing symmetry. By normalizing the dynamic susceptibility into absolute units, we show that the magnetic spectral weight in FeSe is comparable to that of the iron arsenides 9,10 . Our findings support recent theoretical proposals that both nematicity and superconductivity are driven by spin fluctuations 1,2,11-14 .Most parent compounds of iron-based superconductors exhibit a stripe-type long-range antiferromagnetic (AFM) order which is pre-empted by a nematic order: a correlation of electronic states which breaks rotational, but not translational, symmetry. Superconductivity emerges when the magnetic and nematic order are partially or completely suppressed by chemical doping or by the application of pressure 1,6 . The stripe AFM order consists of columns of parallel spins along the orthorhombic b direction, together with antiparallel spins along the a direction. Similar to the stripe AFM order, the nematic order also breaks the fourfold rotational symmetry, which is signaled by the tetragonal to orthorhombic structure phase transition and pronounced in-plane anisotropy of electronic and magnetic properties 1,6,[15][16][17][18] . It has been proposed that nematicity could be driven either by orbital or spin fluctuations, and that orbital fluctuations tend to lead to a sign-preserving s ++ -wave pairing, while spin fluctuations favor a sign-changing s ± -wave or d-wave pairing [1][2][3][4][5][6]14,19,20 . However, as orbital and spin degrees of freedom are coupled and could be easily affected by the nearby stripe magnetic order, it remains elusive which of them is the primary driving force of nematicity [1][2][3][4][5]14,19 .FeSe (T c ≈ 8 K) has attracted great attention not only because of the simple crystal structure (Fig. 1a), 3 but also because it displays a variety of exotic properties unprecedented for other iron based superconduc...

Elucidating the nature of the magnetism of a high-temperature superconductor is crucial for establishing its pairing mechanism. The parent compounds of the cuprate and iron-pnictide superconductors exhibit Néel and stripe magnetic order, respectively. However, FeSe, the structurally simplest iron-based superconductor, shows nematic order (Ts=90 K), but not magnetic order in the parent phase, and its magnetic ground state is intensely debated. Here we report inelastic neutron-scattering experiments that reveal both stripe and Néel spin fluctuations over a wide energy range at 110 K. On entering the nematic phase, a substantial amount of spectral weight is transferred from the Néel to the stripe spin fluctuations. Moreover, the total fluctuating magnetic moment of FeSe is ∼60% larger than that in the iron pnictide BaFe2As2. Our results suggest that FeSe is a novel S=1 nematic quantum-disordered paramagnet interpolating between the Néel and stripe magnetic instabilities.

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FeSe layer-based superconductors exhibit exotic and distinctive properties. The undoped FeSe shows nematicity and superconductivity, while the heavily electron-doped KxFe2−ySe2 and single-layer FeSe/SrTiO3 possess high superconducting transition temperatures that pose theoretical challenges. However, a comprehensive study on the doping dependence of an FeSe layer-based superconductor is still lacking due to the lack of a clean means of doping control. Through angle-resolved photoemission spectroscopy studies on K-dosed thick FeSe films and FeSe0.93S0.07 bulk crystals, here we reveal the internal connections between these two types of FeSe-based superconductors, and obtain superconductivity below ∼46 K in an FeSe layer under electron doping without interfacial effects. Moreover, we discover an exotic phase diagram of FeSe with electron doping, including a nematic phase, a superconducting dome, a correlation-driven insulating phase and a metallic phase. Such an anomalous phase diagram unveils the remarkable complexity, and highlights the importance of correlations in FeSe layer-based superconductors.

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The comprehensive low-temperature specific heat C(T) data identify both an isotropic s-wave and an extended s-wave order parameters coexisting in a superconducting single crystal FeSe with T c =8.11 K. The isotropic gap Δ 0 =1.33 meV on the hole Fermi sheets and the extended s-wave gap = e (1+cos2) with Δ e =1.13 meV and =0.78 on the electron Fermi sheets. The extended s-wave is rather anisotropic but the low energy quasiparticle excitations demonstrate no sign of the accidental nodes. The coefficient (H) manifesting the quasiparticle contribution to C is a non-linear function of the applied magnetic field H in the mixed state in accord with the anisotropic multi-order parameters.

The recent discovery of high-temperature superconductivity in single-layer iron selenide has generated significant experimental interest for optimizing the superconducting properties of iron-based superconductors through the lattice modification. For simulating the similar effect by changing the chemical composition due to S doping, we investigate the superconducting properties of high-quality single crystals of FeSe$_{1-x}$S$_{x}$ ($x$=0, 0.04, 0.09, and 0.11) using magnetization, resistivity, the London penetration depth, and low temperature specific heat measurements. We show that the introduction of S to FeSe enhances the superconducting transition temperature $T_{c}$, anisotropy, upper critical field $H_{c2}$, and critical current density $J_{c}$. The upper critical field $H_{c2}(T)$ and its anisotropy are strongly temperature dependent, indicating a multiband superconductivity in this system. Through the measurements and analysis of the London penetration depth $\lambda _{ab}(T)$ and specific heat, we show clear evidence for strong coupling two-gap $s$-wave superconductivity. The temperature-dependence of $\lambda _{ab}(T)$ calculated from the lower critical field and electronic specific heat can be well described by using a two-band model with $s$-wave-like gaps. We find that a $d$-wave and single-gap BCS theory under the weak-coupling approach can not describe our experiments. The change of specific heat induced by the magnetic field can be understood only in terms of multiband superconductivity.Comment: 13 pages, 7 figure

FeSe exhibits a novel ground state in which superconductivity coexists with a nematic order in the absence of any long-range magnetic order. Here we report an angle-resolved photoemission study on the superconducting gap structure in the nematic state of FeSe 0.93 S 0.07 , without the complication caused by Fermi surface reconstruction induced by magnetic order. We found that the superconducting gap shows a pronounced 2-fold anisotropy around the elliptical hole pocket near the Z point of the Brillouin zone, with gap minima at the endpoints of its major axis, while no detectable gap was observed around the zone center and zone corner. The large anisotropy and nodal gap distribution demonstrate the substantial effects of the nematicity on the superconductivity, and thus put strong constraints on the current theories. PACS numbers: 74.70.Xa, 74.25.Jb, 74.20.Mn The pairing mechanism underlying unconventional superconductivity is often related to the quantum fluctuations of nearby orders. In most Fe-based superconductors, both magnetic and nematic orders appear simultaneously near the superconducting state. Accordingly, both spin-fluctuationmediated and orbital-fluctuation-mediated superconducting pairing mechanisms have been proposed [1][2][3][4][5]. Although intense experimental studies have been conducted [6][7][8][9][10][11][12][13], the exact pairing mechanism of Fe-based superconductors is still under heated debate.FeSe is a unique material with a novel superconducting state. Orbital order develops in the nematic state of FeSe without breaking the translational symmetry as shown by angle resolved photoemission spectroscopy (ARPES) studies [14,15]. The superconductivity coexists with the nematic order without any long range magnetic order [16], thus disentangling the magnetic and orbital orders. Moreover, recent results suggest that FeSe is a quantum paramagnet [4] with coexisting Néel and stripe antiferromagnetic interactions [17,18]. The novel ground state in FeSe provides a fresh perspective for studying the effect of nematic order on the superconducting gap structure in the absence of the Fermi surface reconstruction induced by magnetic order, which helps to reveal the roles of spin and orbital degrees of freedom in unconventional superconductivity. A nodeless superconducting gap structure in FeSe was suggested by previous reports on specific heat [19], Andreev reflection spectroscopy [20], and thermal conductivity measurements [21]. In contrast, scanning tunnelling spectroscopy (STS) studies on FeSe films [22] and transport measurements on bulk FeSe/FeSe 1−x S x crystals with improved quality [23,24] all demonstrate a nodal gap structure. However, due to the low T c and small gap size of FeSe/FeSe 1−x S x single crystals, the gap distribution in momentum-space is still unknown.In this work, we studied the superconducting gap structure of high-quality FeSe 0.93 S 0.07 single crystals (T c = 10 K) with high resolution ARPES [25]. At 6.3 K, both the nematic electronic structure and the superconducting gap ...