The missing hole packets near the Brillouin zone center render unique electronic structures to the heavily electron doped FeSe-based superconductors with Tc above 40 K. It challenges the existing scenario accounting for the nature of superconductivity in the iron-based family. Yet, one hurdle that has to be overcome is the materials complexity in the rather limited number of compounds. Here we report the growth of heavily electron doped Li-NH3 intercalated FeSe single crystals that are free of such complexities and allow access to the intrinsic superconducting properties. Our results show extremely large electronic anisotropy in both normal and superconducting states. Moreover, the anomalous transport properties appear in normal state, which are believed related to the anisotropy of relaxation time and/or temperature dependent electron carrier concentration. In view of the great chemical flexibility of intercalants, our findings provide novel platform to understanding of superconductivity origin of FeSe-related superconductors.
We have systematically studied the structural and physical properties of the superconducting hydrated Lix(H2O)yTaS2. The powder X-ray diffraction patterns suggest that all the samples are single-phase compounds, and the crystal structure is similar to that of 2H-TaS2. The transition temperature to superconductivity shows a dome-shape dependence on the lithium content x with a maximum Tc of 4.6 K for x=0.42, which is larger than in corresponding optimally doped 2H-TaS2 superconductors without water or organic intercalants (Tc ~ 4.2 K). There are no signs for a charge-density-wave formation in h…
We report the crystal structure, superconductivity and normal state properties of two iron-based materials, Li0.15(C3H10N2)0.32FeSe(P-4) and Lix(C3H10N2)0.32FeSe(P4/nmm, 0.25<x<0.4) with superconducting transition temperature from 40~46K. The determined crystal structures revealed a coupling between Li concentration and the oritation of 1,2-Diaminopropane molecules within the hyper expanded FeSe layers. Further fitting on resistivity in terms of the Lawence-Doniach model suggests the two superconductors belong to the quasi-two dimonsional system. With increasing temperature, a differences in c…
Superconductivity mostly appears in high carrier density systems and sometimes exhibits common phase diagrams in which the critical temperature Tc continuously develops with carrier density. Superconductivity enhanced in lightly doped regime has seldom been reported, although it is an ideal direction towards the crossover between Bardeen-Cooper-Schrieffer (BCS) and Bose-Einstein condensate (BEC) limits, where the behavior of Cooper pairs changes dramatically. Here we report transport properties and superconducting gaps in single-crystalline lithium-intercalated layered nitrides (LixHfNCl and L…
Recent experiments reported an unusual nematic behavior of heavily hole-doped pnictides $A$Fe$_{2}$As$_{2}$, with alkali $A$ = Rb, Cs. In contrast to the $B_{2g}$ nematic order of the parent $Ae$Fe$_{2}$As$_{2}$ compounds (with alkaline earth $Ae$ = Sr, Ba), characterized by unequal nearest-neighbor Fe-Fe bonds, in the hole-doped systems nematic order is observed in the $B_{1g}$ channel, characterized by unequal next-nearest-neighbor Fe-Fe (diagonal Fe-As-Fe) bonds. In this work, using density functional theory, we attribute this behavior to the evolution of the magnetic ground state along the…
We report 75As-NMR/NQR results on new iron-arsenide compounds (La0.5-xNa0.5+x)Fe2As2. The parent compound x=0 exhibits a stripe-type antiferromagnetic (AFM) order below T_N=130 K. The measurement of nuclear spin relaxation rate at hole-doped x=+0.3 and heavily electron-doped x=-0.5 revealed that the normal-state properties are dominated by AFM spin fluctuations (AFMSFs), which are more significant at x=+0.3 than at x=-0.5. Their superconducting (SC) phases are characterized by unconventional multi-gap SC state, where the smaller SC gaps are particularly weaken in common. The experimental resul…
Electronic and magnetic properties of the heavily H-doped LaFeAsO$_{1-x}$H$_x$ $(x\sim0.5 )$ were studied in the framework of the density functional theory combined with the dynamical mean field theory (DFT+DMFT). We found a stripe-like-ordered structure of hydrogen and oxygen atoms, as a ground state, with the same configuration as the antiferromagnetic (AF) order. The new configuration could explain the existing experimental results related to the heavily H-doped LaFeAsO$_{1-x}$H$_x$, such as an in-plane electronic anisotropy and a non-uniform magnetic behavior. A significant anisotropy was …
The van-der-Waals gap of iron chalcogenide superconductors can be intercalated with a variety of inorganic and organic compounds that modify the electron doping level of the iron layers. In Lix(C3N2H10)0.37FeSe, a dome in the superconducting transition temperature Tc has been reported to occur in the doping range of x=0.06 to x=0.68. We use a combination of density functional theory and spin fluctuation theory to capture the evolution of superconducting transition temperatures theoretically. We clearly demonstrate how the changing electronic structure supports an increasing superconducting Tc.…
We investigate the electronic structure of a recently discovered, heavily electron-doped iron based superconductor LaFe$_2$As$_2$. Although first principles calculation shows apparent absence of hole Fermi surfaces around the $Γ$ point, we reveal, by hypothetically removing the La $d$ orbital contribution, that a hole Fermi surface around the $Γ$ point is essentially present. In the collapsed phase of LaFe$_2$As$_2$, which is non-superconducting, the hole Fermi surface is found to be absent, and the difference from the uncollapsed superconducting phase can be naturally understood within the sp…
Bulk Fermi surface and momentum density in heavily doped La$_{2-x}$Sr$_x$CuO$_4$ using high resolution Compton scattering and positron annihilation spectroscopies
本文用康普顿散射法观察了La $_{2-x}$ Sr $_x$ CuO $_4$的过掺杂($x$ =0.3)单晶体费米面(FS)。根据测量的康普顿剖面进行的二维(2D)动量密度重建在沿[100]的第三布里渊区产生了清晰的FS特征。密度泛函理论(DFT)计算与动量密度实验之间的定量一致表明,费米液体物理恢复在过掺杂制度。特别是预测的FS拓扑被发现是在良好的符合相应的实验数据。我们发现测量的正电子湮没辐射(2D-ACAR)谱的二维角相关和基于DFT的计算之间类似的定量协议。然而,无论是在理论上还是在实验上,2D-ACAR都没有给出扩展动量空间中FS的清晰特征。
Quantitative Determination of Eliashberg Function and Evidence of Strong Electron Coupling with Multiple Phonon Modes in Heavily Over doped (Bi,Pb)2Sr2CuO6
To elucidate the origin of re-enhanced high-$T_c$ phase in the heavily electron-doped Fe-pnictides, systematic $^{75}$As NMR studies are performed on heavily electron-doped LaFe$Pn$O$_{0.75}$H$_{0.25}$ by controlling the pnictogen height ($h_{Pn}$) from the Fe plane through the substitution at $Pn$(=As) site with Sb or P. The measurements of nuclear spin relaxation rate (1/$T_1$) and Knight shift ($K$) reveal that the moderate spin fluctuations at high temperatures are suppressed toward low temperatures. Such characteristic spin fluctuations with gap like feature at low energies are more enlar…
We theoretically study ferromagnetic (FM) fluctuations that are experimentally observed in the heavily overdoped region of cuprate superconductors. To explore the origin of FM fluctuations, we evaluate the spin susceptibilities of a single-band Hubbard model within the fluctuation exchange approximation. Model parameters are derived using the Wannierization technique and the constrained random phase approximation method based on the maximally localized Wannier functions. The constrained random phase approximation calculations reveal that the on-site Coulomb interaction decreases with an increa…
High-critical-temperature (Tc) superconductivity at 48 K is reported for hydrogen-doped SmFeAsO epitaxial films on MgO single-crystal substrates. The key processes are pulsed laser deposition to grow undoped SmFeAsO epitaxial films and subsequent topotactic chemical reaction using CaH2 powders under evacuated silica-glass ampule atmosphere. Based on this post-deposition thermal annealing treatment that we have developed, a maximum hydrogen concentration x = ~0.35 was realized in SmFeAs(O1-xHx). Disordered hydrogen-substitution at O sites is experimentally confirmed directly by atomic-scale mic…
Nematicity in the heavily hole-doped iron pnictide superconductors remains controversial. Sizeable nematic fluctuations and even nematic orders far from a magnetic instability were declared in RbFe$_2$As$_2$ and its sister compounds. Here we report a systematic elastoresistance study of series of isovalent- and electron-doped KFe$_2$As$_2$ crystals. We found divergent elastoresistance upon cooling for all the crystals along their [110] direction. The amplitude of elastoresistivity diverges if K is substituted with larger ions or if the system is driven towards a Lifshitz transition. However, w…
An iron-based superconductor LaFeAsO$_{1-x}$H$_x$ (0 $\leq x \leq$ 0.6) undergoes two antiferromagnetic (AF) phases upon H doping. We investigated the second AF phase ($x$=0.6) using NMR techniques under pressure. At pressures up to 2 GPa, the ground state is a spin-density-wave state with a large gap; however, the gap closes at 4.0 GPa, suggesting a pressure-induced quantum critical point. Interestingly, the gapped excitation coexists with gapless magnetic fluctuations at pressures between 2 and 4 GPa. This coexistence is attributable to the lift up of the $d_{xy}$ orbital to the Fermi level,…
Two-gap superconductivity in heavily n-doped graphene: ab initio Migdal-Eliashberg theory
石墨烯是从零维到三维材料的碳家族中唯一尚未观察到超导性的成员。目前尚不清楚对超导石墨烯的探索是否受到技术挑战的阻碍,或者是二维序参量的波动。在这一领域,从头计算是有用的,以指导实验工作,缩小搜索空间。本着这种精神,我们从第一原理研究了使用由Wannier-Fourier插值提供动力的完全各向异性Migdal-Eliashberg理论在掺杂石墨烯中诱导超导性的可能性。为了解决最好的情况下,我们考虑在高载流子密度的电子和空穴掺杂,以便对准费米能级的范霍夫奇点。在这些条件下,我们发现超导间隙的$s$波对称性,与轻微的各向异性引起的三角形翘曲,并在$n$掺杂的石墨烯的情况下,一个意想不到的两个间隙结构联想到MgB $_2$。我们的Migdal-Eliashberg计算表明,对于载流子密度超过$10^{15}$ cm $^{-2}$的$n$掺杂的石墨烯,在低温下观察到超导性应该是可能的。
Electronic structure of heavily electron-doped BaFe$_{1.7}$Co$_{0.3}$As$_2$ studied by angle-resolved photoemission
我们对重电子掺杂非超导BaFe $_{1.7}$ Co $_{0.3}$ As $_2$进行了高分辨角分辨光电子能谱研究。我们发现在空穴掺杂的超导体Ba $_{0.6}$ K $_{0.4}$ Fe $_2$ As $_2$中观察到的两个空穴费米面口袋在该化合物中不存在或非常小,而在M点处的两个电子口袋由于Co替代的电子掺杂而显著膨胀。非SC和SC样品的费米面的比较表明,通过反铁磁波矢连接的空穴和电子口袋的共存是实现铁基超导体的超导性机制的必要条件。
We report high-resolution neutron scattering measurements of the low energy spin fluctuations of KFe$_{2}$As$_{2}$, the end member of the hole-doped Ba$_{1-x}$K$_x$Fe$_2$As$_2$ family with only hole pockets, above and below its superconducting transition temperature $T_c$ ($\sim$ 3.5 K). Our data reveals clear spin fluctuations at the incommensurate wave vector ($0.5\pmδ$, 0, $L$), ($δ$ = 0.2)(1-Fe unit cell), which exhibit $L$-modulation peaking at $L=0.5$. Upon cooling to the superconducting state, the incommensurate spin fluctuations gradually open a spin-gap and form a sharp spin resonance…
Diamond, a wide band-gap semiconductor, can be engineered to exhibit superconductivity when doped heavily with boron. The phenomena has been demonstrated in samples grown by chemical vapour deposition where the boron concentration exceeds the critical concentration for the metal-to-insulator transition of $n_{MIT} \gtrsim 4\times10^{20}/\text{cm}^3$. While the threshold carrier concentration for superconductivity is generally well established in the literature, it is unclear how well correlated higher critical temperatures are with increased boron concentration. Previous studies have generally…
Iron-based superconductors have grown to be a new continent of high Tc superconductors comparable to cuprates. The optimal critical temperature (Tc) of 56 K in electron-doped 1111-type iron oxypnictides attracts considerable attention of physicists and chemists. Carrier doping is not only essential to induce superconductivity but also is a critical parameter that governs the electronic, magnetic, and crystallographic properties of ground states in high-Tc superconductors. Hydride ion (H-) which is an anionic state of hydrogen acts as an efficient electron donor in the 1111-type, leading to sev…
We studied the relationship between the charge doping and the correlation, and its effects on the spectral function of the BaFe$_2$As$_2$ compound in the framework of the density functional theory combined with the dynamical mean field theory (DFT+DMFT). The calculated mass enhancements showed that the electronic correlation varies systematically from weak to strong when moving from the heavily electron-doped regime to the heavily hole-doped one. Since the compound has a multi-orbital nature, the correlation is orbital-dependent and it increases as hole-doping increases. The Fe-3d$_{xy}$ (xy) …
Evolution of band structure from optimally doped to heavily overdoped Co-substituted NaFeAs
用角分辨光电子能谱研究了NaFe $_{1-x}$ Co $_x$ As从最佳掺杂超导化合物($x=0.028$)到重过掺杂非超导化合物($x=0.109$)的电子结构。与“122”型铁磷属元素化合物的情况类似,我们的数据表明,在NaFe $_{1-x}$ Co $_x$ As中的Co掺杂提供了额外的载流子,并相应地移动了费米能级。在$x=0.109$化合物中,围绕带中心$Γ$的空穴状带移动到更深的结合能,而出现电子口袋。在整个掺杂范围内,我们研究的整体能带重整化基本上保持不变,这表明局部磁/电子相关性不受载流子掺杂的影响。我们推测,流动载流子的巡游特性和局域相互作用之间的平衡可能对超导性起着重要的作用。
Hidden itinerant-spin phase in heavily-overdoped La2-xSrxCuO4 revealed by dilute Fe doping: A combined neutron scattering and angle-resolved photoemission study
Angle-resolved photoemission spectroscopy of Na-doped Ca2CuO2Cl2 single crystals: Fingerprints of a magnetic insulator in a heavily underdoped superconductor
Superconducting gap with sign reversal between hole pockets in heavily hole-doped Ba1-xKxFe2As2
为了深入了解铁磷族元素化物的非常规超导性,没有电子口袋,我们测量了重空穴掺杂制度的Ba $_{1-x}$ K $_x$ Fe $_2$ As $_2$的热导率$κ$和穿透深度$λ$。剩余热导率$(κ/T)_{T \rightarrow 0\,{\rm K}}$和$λ$的$T$依赖性一致地表明在$x=0.76$处的完全带隙超导性和在较高空穴浓度处的(线)节超导性。在低温下的$\fracκ{T}\cdot T_c|_{T \rightarrow 0\,{\rm K}}$和$\frac{dλ}{d(T/T_c)}$的大小,这两者都是由低能量激发的性质决定的,表现出非常不寻常的非单调x依赖性。这些结果表明,在一个狭窄的掺杂范围内的节点特性的显着变化,表明掺杂交叉的s波状态之间的间隙函数与$Γ$中心的空穴袋之间的符号反转和没有。
Orbital and Pauli limiting effects in heavily doped Ba$_{1-x}$K$_x$Fe$_2$As$_2$
研究了Fe基轻无序超导体Ba $_{0.05}$ K $_{0.95}$ Fe $_2$ As $_2$在沿FeAs层(H//ab面)外加磁场H中的热力学性质.该掺杂水平的超导(SC)转变温度为T $_c$ = 6.6 K。对T < T $_c$的比热C(T,H)的分析表明,在不同的费米口袋中,超导序参量的符号发生了变化。为三组分超导序参量提供了实验依据。我们发现,所有这三个组件的值与以前报道的化学计量化合物KFe $_2$作为$_2$。我们的C(T,H)和电阻率ρ(T,H)的数据可以解释为有利于占主导地位的轨道贡献的对破缺机制在低场,而泡利限制效应占主导地位,在高场,产生一个无带隙超导态,只有领先的非零间隙。