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The antiferromagnetism in transition metal compounds is mostly mediated by the bridging anions through a so-called superexchange mechanism. However, in materials like normal spinels $AB_2X_4$ with local moments only at the $A$ site, such an anion-mediated superexchange needs to be modified. Here we report a new spinel compound Co$_{1+x}$Ir$_{2-x}$S$_4$ ($x$ = 0.3). The physical property measurements strongly suggest an antiferromagnetic-like transition at 292 K in the Co($A$) diamond sublattice. The first-principle calculations reveal that the nearest-neighbor Co($A$) spins align antiferromagnetically with an ordered magnetic moment of 1.67 $\mu_\mathrm{B}$, smaller than the expected $S = 3/2$ for Co$^{2+}$. In the antiferromagnetic state, there exists an inter-cation charge-transfer gap between the non-bonding Ir-$t_\mathrm{2g}$ orbitals at the valence band maximum and the Co-S antibonding molecular orbitals at the conduction band minimum. The small charge transfer energy significantly enhances the virtual hopping between these two states, facilitating a robust long-range superexchange interaction between two neighboring CoS$_4$ complexes, which accounts for the high N\'{e}el temperature in Co$_{1+x}$Ir$_{2-x}$S$_4$. This inter-cation charge transfer mediated magnetic interaction expands the traditional superexchange theory, which could be applicable in complex magnetic materials with multiple cations., Comment: 10 pages, 7 figures

We report the physical properties of ThRu$_3$Si$_2$ featured with distorted Ru kagome lattice. The combined experiments of resistivity, magnetization and specific heat reveal bulk superconductivity with $T_{\rm{c}}$ = 3.8 K. The specific heat jump and calculated electron-phonon coupling indicate a moderate coupled BCS superconductor. In comparison with LaRu$_3$Si$_2$, the calculated electronic structure in ThRu$_3$Si$_2$ shows an electron-doping effect with electron filling lifted from 100 meV below flat bands to 300 meV above it. This explains the lower superconducting transition temperature and weaker electron correlations observed in ThRu$_3$Si$_2$. Our work suggests the $T_{\rm{c}}$ and electronic correlations in kagome superconductor could have intimate connection with the flat bands., Comment: 7 pages, 5 figures

We report the synthesis, crystal structure, and physical properties of a novel ternary compound, Th$_2$Cu$_4$As$_5$. The material crystallizes in a tetragonal structure with lattice parameters $a=4.0716(1)$ {\AA} and $c=24.8131(4)$ {\AA}. Its structure can be described as an alternating stacking of fluorite-type Th$_2$As$_2$ layers with antifluorite-type double-layered Cu$_4$As$_3$ slabs. The measurement of electrical resistivity, magnetic susceptibility and specific heat reveals that Th$_2$Cu$_4$As$_5$ undergoes bulk superconducting transition at 4.2 K. Moreover, all these physical quantities exhibit anomalies at 48 K, where the Hall coefficient change the sign. These findings suggest a charge-density-wave-like (CDW) transition, making Th$_2$Cu$_4$As$_5$ a rare example for studying the interplay between CDW and superconductivity., Comment: 11 pages, 6 figures, and 1 table

Unconventional superconductivity (USC) in a highly correlated kagome system has been theoretically proposed for years, yet the experimental realization is hard to achieve. The recently discovered vanadium-based kagome materials, which exhibit both superconductivity and charge density wave (CDW) orders, are nonmagnetic and weakly correlated, thus unlikely host USC as theories proposed. Here we report the discovery of a chromium-based kagome metal, CsCr$_3$Sb$_5$, which is contrastingly characterised by strong electron correlations, frustrated magnetism, and characteristic flat bands close to the Fermi level. Under ambient pressure, it undergoes a concurrent structural and magnetic phase transition at 55 K, accompanying with a stripe-like $4a_0$ structural modulation. At high pressure, the phase transition evolves into two transitions, probably associated with CDW and antiferromagnetic spin-density-wave orderings, respectively. These density-wave (DW)-like orders are gradually suppressed with pressure and, remarkably, a superconducting dome emerges at 3.65-8.0 GPa. The maximum of the superconducting transition temperature, $T_\mathrm{c}^{\mathrm{max}}=$ 6.4 K, appears when the DW-like orders are completely suppressed at 4.2 GPa, and the normal state exhibits a non-Fermi-liquid behaviour, reminiscent of USC and quantum criticality in iron-based superconductors. Our work offers an unprecedented platform for investigating possible USC in a correlated kagome system., Comment: 32 pages, 14 figures

We derived explicit expressions of symmetry operators on Wannier basis, and implemented these operators in WannSymm software. Based on this implementation, WannSymm can i) symmetrize the real-space Hamiltonian output from Wannier90 code, ii) generate symmetry operators of the little group at a specific k-point, and iii) perform symmetry analysis for Wannier band structure. In general, symmetrized Hamiltonians yield improved results compared with the original ones when they are employed for nodal structure searching, surface Green's function calculations, and other model calculations., Comment: 22 pages, 7 figures, WannSymm code can be downloaded from https://github.com/ccao/WannSymm ; typos corrected, references added

We report the design, synthesis, structure, and properties of two complex layered phosphide nitrides, $Ak$Th$_2$Mn$_4$P$_4$N$_2$ ($Ak$ = Rb, Cs), which contain anti-fluorite-type [Mn$_2$P$_2$] bilayers separated by fluorite-type [Th2N2] layers as a result of the intergrowth between AkMn$_2$P$_2$ and ThMnPN. The new compounds are featured with an intrinsic hole doping associated with the interlayer charge transfer and a built-in chemical pressure from the [Th$_2$N$_2$] layers, both of which are reflected by the changes in the lattice and the atomic position of phosphorus. The measurements of magnetic susceptibility, electrical resistivity, and specific heat indicate existence of local moments as well as itinerant electrons in relation with d-p hybridizations. The expected dominant antiferromagnetic interactions with enhanced d-p hybridizations were demonstrated by the first-principles calculations only when additional Coulomb repulsions are included. The density of states at the Fermi level derived from the specific-heat analysis are 3.5 and 7.5 times of the calculated ones for Ak = Rb and Cs, respectively, suggesting strong electron correlations in the title compounds., Comment: 12 pages, 5 figures, 3 tables; Supporting information available on request

We report the Ni-doping effect on magnetism and superconductivity (SC) in an Eu-containing 112-type system Eu(Fe$_{1-x}$Ni$_{x})$As$_{2}$ ($0\leq x\leq 0.15$) by the measurements of resistivity, magnetization, and specific heat. The undoped EuFeAs$_2$ undergoes a spin-density-wave (SDW) transition at $T_\mathrm{SDW}\sim$ 105 K in the Fe sublattice and a magnetic ordering at $T_\mathrm{m}\sim$ 40 K in the Eu sublattice. Complex Eu-spin magnetism is manifested by a spin-glass reentrance at $T_\mathrm{SG}\sim$ 15 K and an additional spin reorientation at $T_\mathrm{SR}\sim$ 7 K. With Ni doping, the SDW order is rapidly suppressed, and SC emerges in the Ni-doping range of 0.01 $\leq x\leq$ 0.1 where a maximum of the superconducting transition temperature $T_\mathrm{c}^{\mathrm{max}}=$ 17.6 K shows up at $x$ = 0.04. On the other hand, $T_\mathrm{m}$ decreases very slowly, yet $T_\mathrm{SG}$ and $T_\mathrm{SR}$ hardly change with the Ni doping. The phase diagram has been established, which suggests a very weak coupling between SC and Eu spins. The complex Eu-spin magnetism is discussed in terms of the Ruderman-Kittel-Kasuya-Yosida interactions mediated by the conduction electrons from both layers of FeAs and As surrounding Eu$^{2+}$ ions., Comment: 10 pages, 7 figures; supplemental materials available on request

We report the first-principles study on the H-intercalated Cr-based superconductor KCr$_3$As$_3$H$_x$. Our results show a paramagnetic ground state for KCr$_3$As$_3$H. The electronic structure consists of two quasi-one-dimensional (Q1D) Fermi-surfaces and one 3D Fermi-surface which are mainly contributed by Cr-d$_{z^2}$, d$_{x^2-y^2}$ and d$_{xy}$ orbitals. The bare electron susceptibility shows a $\Gamma$-centered imaginary peak, indicating possible ferromagnetic spin fluctuations. Upon moderate hole doping, the system undergoes a Lifshitz transition, which may enhance the Q1D feature of the system. The Bader charge analysis and electron localization functions reveal a strong bonding nature of hydrogen in KCr$_3$As$_3$H, which results in a nontrivial electron doping in KCr$_3$As$_3$H.

Recently, An electron-doped 12442-type iron-based superconductor BaTh$_2$Fe$_4$As$_4$(N$_{0.7}$O$_{0.3}$)$_2$ has been successfully synthesized with high-temperature solid-state reactions on basis of a structural design. The inter-block-layer charge transfer between the constituent units of "BaFe$_2$As$_2$" and "ThFeAsN$_{0.7}$O$_{0.3}$" was found to be essential to stabilize the target compound. Dominant electron-type conduction and bulk superconducting transition at ~22 K were demonstrated., Comment: 16 pages in total. 5 figures, 1 table (main article); 6 figures, 3 tables (Supporting Information)

CsCa$_2$Fe$_4$As$_4$F$_2$ is a newly discovered iron-based superconductor with $T_\mathrm{c}\sim$ 30 K containing double Fe$_2$As$_2$ layers that are separated by insulating Ca$_2$F$_2$ spacer layers. Here we report the transport and magnetization measurements on CsCa$_2$Fe$_4$As$_4$F$_2$ single crystals grown for the first time using the self flux of CsAs. We observed a huge resistivity anisotropy $\rho_c(T)/\rho_{ab}(T)$, which increases with decreasing temperature, from 750 at 300 K to 3150 at 32 K. The $\rho_c(T)$ data exhibit a non-metallic behavior above $\sim$140 K, suggesting an incoherent electronic state at high temperatures due to the dimension crossover. The superconducting onset transition temperature in $\rho_{ab}$ is 0.7 K higher than that in $\rho_c$, suggesting two-dimensional (2D) superconducting fluctuations. The lower and upper critical fields also show an exceptional anisotropy among iron-based superconductors. The $H_{c1}^\bot(T)$ data are well fitted using the model with two $s$-wave-like superconducting gaps, $\Delta_1(0)=6.75$ meV and $\Delta_2(0)=2.32$ meV. The inter-plane coherence length $\xi_c(0)$ is $3.6$ \AA, remarkably smaller than the distance between conducting layers (8.6 \AA), consolidating the 2D nature in the title material., Comment: 8 pages, 5 figures, 1 Table

We report the synthesis, crystal structure, physical properties, and first-principles calculations of a vanadium-based oxytelluride Rb$_{1-\delta}$V$_2$Te$_2$O ($\delta\approx0.2$). The crystal structure bears two-dimensional V$_2$O square nets sandwiched with tellurium layers, mimicking the structural motifs of cuprate and iron-based superconductors. The material exhibits metallic conductivity with dominant hole-type charge carriers. A weak metal-to-metal transition takes place at $\sim$100 K, which is conformably characterized by a slight kink/hump in the electrical resistivity, jumps in the Hall and Seebeck coefficients, a minute drop in the magnetic susceptibility, and a small peak in the heat capacity. Neither Bragg-peak splitting nor superlattice reflections can be detected within the resolution of conventional x-ray diffractions. The band-structure calculations show that V-3$d$ orbitals dominate the electronic states at around Fermi energy where a $d_{yz}/d_{xz}$ orbital polarization shows up. There are three Fermi-surface sheets that seem unfavorable for nesting. Our results suggest an orbital or spin-density-wave order for the low-temperature state and, upon suppression of the competing order, emergence of superconductivity could be expected., Comment: 11 pages, 2 tables, and 9 figures

We have synthesized 10 new iron oxyarsenides, K$Ln_2$Fe$_4$As$_4$O$_2$ ($Ln$ = Gd, Tb, Dy, and Ho) and Cs$Ln_2$Fe$_4$As$_4$O$_2$ ($Ln$ = Nd, Sm, Gd, Tb, Dy, and Ho), with the aid of lattice-match [between $A$Fe$_2$As$_2$ ($A$ = K and Cs) and $Ln$FeAsO] approach. The resultant compounds possess hole-doped conducting double FeAs layers, [$A$Fe$_4$As$_4$]$^{2-}$, that are separated by the insulating [$Ln_2$O$_2$]$^{2+}$ slabs. Measurements of electrical resistivity and dc magnetic susceptibility demonstrate bulk superconductivity at $T_\mathrm{c}$ = 33 - 37 K. We find that $T_\mathrm{c}$ correlates with the axis ratio $c/a$ for all 12442-type superconductors discovered. Also, $T_\mathrm{c}$ tends to increase with the lattice mismatch, implying a role of lattice instability for the enhancement of superconductivity., Comment: 8 pages, 6 figures, 2 tables

We have synthesized four iron-based oxyarsenide superconductors Rb$Ln_2$Fe$_4$As$_4$O$_2$ ($Ln$ = Sm, Tb, Dy and Ho) resulting from the intergrowth of RbFe$_2$As$_2$ and $Ln$FeAsO. It is found that the lattice match between RbFe$_2$As$_2$ and $Ln$FeAsO is crucial for the phase formation. The structural intergrowth leads to double asymmetric Fe$_2$As$_2$ layers that are separated by insulating $Ln_2$O$_2$ slabs. Consequently, the materials are intrinsically doped at a level of 0.25 holes/Fe-atom and, bulk superconductivity emerges at $T_\mathrm{c}$ = 35.8, 34.7, 34.3 and 33.8 K, respectively, for $Ln$ = Sm, Tb, Dy and Ho. Investigation on the correlation between crystal structure and $T_\mathrm{c}$ suggests that interlayer couplings may play an additional role for optimization of superconductivity., Comment: 20 pages, 9 figures, 1 table

We have synthesized two iron fluo-arsenides $A$Ca$_2$Fe$_4$As$_4$F$_2$ with $A$ = Rb and Cs, analogous to the newly discovered superconductor KCa$_2$Fe$_4$As$_4$F$_2$. The quinary inorganic compounds crystallize in a body-centered tetragonal lattice with space group I4/mmm, which contain double Fe$_2$As$_2$ layers that are separated by insulating Ca$_2$F$_2$ layers. Our electrical and magnetic measurements on the polycrystalline samples demonstrate that the new materials undergo superconducting transitions at Tc = 30.5 K and 28.2 K, respectively, without extrinsic doping. The correlations between Tc and structural parameters are discussed., Comment: 9 pages,4 figures, 1 table

We report synthesis, crystal structure and physical properties of a quinary iron-arsenide fluoride KCa$_2$Fe$_4$As$_4$F$_2$. The new compound crystallizes in a body-centered tetragonal lattice (with space group $I4/mmm$, $a$ = 3.8684(2) {\AA}, c = 31.007(1) {\AA}, and $Z$ = 2), which contains double Fe$_2$As$_2$ conducting layers separated by insulating Ca$_2$F$_2$ layers. Our measurements of electrical resistivity, dc magnetic susceptibility and heat capacity demonstrate bulk superconductivity at 33 K in KCa$_2$Fe$_4$As$_4$F$_2$., Comment: 11 pages, 7 figures, 2 tables

We report synthesis, crystal structure and physical properties of a novel quinary compound RbGd$_2$Fe$_4$As$_4$O$_2$. The new iron oxyarsenide is isostructural to the fluo-arsenide KCa$_2$Fe$_4$As$_4$F$_2$, both of which contain separate double Fe$_2$As$_2$ layers that are self hole-doped in the stoichiometric composition. Bulk superconductivity at $T_\mathrm{c}$ = 35 K is demonstrated by the measurements of electrical resistivity, dc magnetic susceptibility and heat capacity. An exceptionally high value of the initial slope of the upper critical field ($\mu_0$d$H_{\mathrm{c2}}$/d$T|_{T_\mathrm{c}}$ = 16.5 T/K) is measured for the polycrystalline sample., Comment: 10 pages, 6 figures, 1 table, the crystal structure is amended

We have synthesized a novel europium bismuth sulfofluoride, Eu3Bi2S4F4, by solid-state reactions in sealed evacuated quartz ampoules. The compound crystallizes in a tetragonal lattice (space group I4/mmm, a = 4.0771(1) A, c = 32.4330(6) A, and Z = 2), in which CaF2-type Eu3F4 layers and NaCl-like BiS2 bilayers stack alternately along the crystallographic c axis. There are two crystallographically distinct Eu sites, Eu(1) and Eu(2) at the Wyckoff positions 4e and 2a, respectively. Our bond-valence-sum calculation, based on the refined structural data, indicates that Eu(1) is essentially divalent, whilst Eu(2) has an average valence of +2.64(5). This anomalous Eu valence state is further confirmed and supported, respectively, by Mossbauer and magnetization measurements. The Eu3+ components donate electrons into the conduction bands that are mainly composed of Bi- 6px and 6py states. Consequently, the material itself shows metallic conduction, and superconducts at 1.5 K without extrinsic chemical doping., Comment: 24 pages, 5 figures