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The coexistence of superconductivity and ferromagnetism is an intrinsically interesting research focus in condensed matter physics, but the study is limited by low superconducting (Tc) and magnetic (Tm) transition temperatures in related materials. Here, we used a scanning superconducting quantum interference device to image the in situ diamagnetic and ferromagnetic responses of RbEuFe4As4 with high Tc and Tm. We observed significant suppression of the superfluid density in the vicinity of the magnetic phase transition, signifying fluctuation-enhanced magnetic scatterings between Eu spins and Fe 3d conduction electrons. Intriguingly, we observed multiple ferromagnetic domains that should be absent in an ideal magnetic helical phase. The formation of these domains demonstrates a weak c-axis ferromagnetic component probably arising from the Eu spin-canting effect, indicative of possible superconductivity-driven domain Meissner and domain vortex-antivortex phases, as revealed in EuFe2(As0.79P0.21)2. Our observations highlight that RbEuFe4As4 is a unique system that includes multiple interplay channels between superconductivity and ferromagnetism.
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We report the synthesis, crystal structure, and physical properties of a novel ternary compound, Th2Cu4As5. The material crystallizes in a tetragonal structure with lattice parameters a = 4.0639(3) Å and c = 24.8221(17) Å. Its structure can be described as an alternating stacking of fluorite-type Th2As2 layers with antifluorite-type double-layered Cu4As3 slabs. The measurement of electrical resistivity, magnetic susceptibility, and specific heat reveals that Th2Cu4As5 undergoes bulk superconducting transition at 4.2 K. Additionally, all these physical quantities exhibit anomalies at 48 K, accompanied by a sign change in the Hall coefficient, suggesting a charge-density-wave-like (CDW) phase transition. Drawing from both experimental data and band calculations, we propose that the superconducting and CDW-like phase transitions are, respectively, associated with the Cu4As3 slabs and the As plane in the Th2As2 layers.
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Owing to its inherent non-trivial geometry, the unique structural motif of the recently discovered kagome topological superconductor AV3 Sb5 (A = K, Rb, Cs) is an ideal host of diverse topologically non-trivial phenomena, including giant anomalous Hall conductivity, topological charge order, charge density wave (CDW), and unconventional superconductivity. Despite possessing a normal-state CDW order in the form of topological chiral charge order and diverse superconducting gaps structures, it remains unclear how fundamental atomic-level properties and many-body effects including Fermi surface nesting, electron-phonon coupling, and orbital hybridization contribute to these symmetry-breaking phenomena. Here, the direct participation of the V3d-Sb5p orbital hybridization in mediating the CDW phase transition in CsV3 Sb5 is reported. The combination of temperature-dependent X-ray absorption and first-principles studies clearly indicates the inverse Star-of-David structure as the preferred reconstruction in the low-temperature CDW phase. The results highlight the critical role that Sb orbitals play and establish orbital hybridization as the direct mediator of the CDW states and structural transition dynamics in kagome unconventional superconductors. This is a significant step toward the fundamental understanding and control of the emerging correlated phases from the kagome lattice through the orbital interactions and provides promising approaches to novel regimes in unconventional orders and topology.
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EuAl4 possesses the BaAl4 crystal structure type with tetragonal symmetry I4/mmm. It undergoes a charge density wave (CDW) transition at T CDW = 145â K and features four consecutive antiferromagnetic phase transitions below 16â K. Here we use single-crystal X-ray diffraction to determine the incommensurately modulated crystal structure of EuAl4 in its CDW state. The CDW is shown to be incommensurate with modulation wave vector q = (0,0,0.1781â (3)) at 70â K. The symmetry of the incommensurately modulated crystal structure is orthorhombic with superspace group Fmmm(00σ)s00, where Fmmm is a subgroup of I4/mmm of index 2. Both the lattice and the atomic coordinates of the basic structure remain tetragonal. Symmetry breaking is entirely due to the modulation wave, where atoms Eu and Al1 have displacements exclusively along a, while the fourfold rotation would require equal displacement amplitudes along a and b. The calculated band structure of the basic structure and interatomic distances in the modulated crystal structure both indicate the Al atoms as the location of the CDW. The tem-per-ature dependence of the specific heat reveals an anomaly at T CDW = 145â K of a magnitude similar to canonical CDW systems. The present discovery of orthorhombic symmetry for the CDW state of EuAl4 leads to the suggestion of monoclinic instead of orthorhombic symmetry for the third AFM state.
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Intercalation and stacking-order modulation are two active ways in manipulating the interlayer interaction of transition metal dichalcogenides (TMDCs), which lead to a variety of emergent phases and allow for engineering material properties. Herein, the growth of Pb-intercalated TMDCs-Pb(Ta1+x Se2 )2 , the first 124-phase, is reported. Pb(Ta1+x Se2 )2 exhibits a unique two-step first-order structural phase transition at around 230 K. The transitions are solely associated with the stacking degree of freedom, evolving from a high-temperature (high-T) phase with ABC stacking and R3m symmetry to an intermediate phase with AB stacking and P3m1, and finally to a low-temperature (low-T) phase again with R3msymmetry, but with ACB stacking. Each step involves a rigid slide of building blocks by a vector [1/3, 2/3, 0]. Intriguingly, gigantic lattice contractions occur at the transitions on warming. At low-T, bulk superconductivity with Tc ≈ 1.8 K is observed. The underlying physics of the structural phase transitions are discussed from first-principle calculations. The symmetry analysis reveals topological nodal lines in the band structure. The results demonstrate the possibility of realizing higher-order metal-intercalated phases of TMDCs and advance the knowledge of polymorphic transitions, and may inspire stacking-order engineering in TMDCs and beyond.
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We report a new polymorph of LuRuGe, obtained in indium flux. This phase exhibits the noncentrosymmetric ZrNiAl-type structure with the space group P6Ì 2m as determined by single-crystal X-ray diffraction. This polymorph can convert into another centrosymmetric polymorph (TiNiSi-type structure, space group Pnma) at high temperatures. We performed electrical transport, magnetization, and specific heat measurements on this new phase. It shows metallic behavior with a Hall sign change from negative at 2 K to positive at 125 K. LuRuGe exhibits Pauli paramagnetism as the ground state with no local magnetic moments from either the Ru or Lu site. The Debye temperature Θ = 348 K and electronic coefficient γe = 3.6 mJ K-2 mol-1 are extracted from the low-temperature specific heat data in LuRuGe. We also carried out first-principles density functional theory calculations to map out the electronic band structure and density of states. There are several electronic bands crossing the Fermi level, supporting a multiband scenario consistent with the Hall sign change. The density of states around the Fermi level is mainly from Ru 4d and Ge 4p electrons, indicating a strong hybridization between those atomic orbitals.
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Spintronics holds great potential for next-generation high-speed and low-power consumption information technology. Recently, lead halide perovskites (LHPs), which have gained great success in optoelectronics, also show interesting magnetic properties. However, the spin-related properties in LHPs originate from the spin-orbit coupling of Pb, limiting further development of these materials in spintronics. Here, we demonstrate a new generation of halide perovskites, by alloying magnetic elements into optoelectronic double perovskites, which provide rich chemical and structural diversities to host different magnetic elements. In our iron-alloyed double perovskite, Cs2Ag(Bi:Fe)Br6, Fe3+ replaces Bi3+ and forms FeBr6 clusters that homogenously distribute throughout the double perovskite crystals. We observe a strong temperature-dependent magnetic response at temperatures below 30 K, which is tentatively attributed to a weak ferromagnetic or antiferromagnetic response from localized regions. We anticipate that this work will stimulate future efforts in exploring this simple yet efficient approach to develop new spintronic materials based on lead-free double perovskites.
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Halide perovskites are anticipated to impact next generation high performance solar cells because of their extraordinary charge transport and optoelectronic properties. However, their thermal transport behavior has received limited attention. In this work, we studied the thermal transport and thermoelectric properties of the CsSnBr3-xIx perovskites. We find a strong correlation between lattice dynamics and an ultralow thermal conductivity for series CsSnBr3-xIx reaching 0.32 Wm-1K-1 at 550 K. The CsSnBr3-xIx also possess a decent Seebeck coefficient and controllable electrical transport properties. The crystallography data and theoretical calculations suggest the Cs atom deviates from its ideal cuboctahedral geometry imposed by the perovskite cage and behaves as a heavy atom rattling oscillator. This off-center tendency of Cs, together with the distortion of SnX6 (X = Br or I) octahedra, produces a highly dynamic and disordered structure in CsSnBr3-xIx, which gives rise to a very low Debye temperature and phonon velocity. Moreover, the low temperature heat capacity data suggests strong coupling between the low frequency optical phonons and heat carrying acoustical phonons. This induces strong phonon resonance scattering that induces the ultralow lattice thermal conductivity of CsSnBr3-xIx.
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Semiconductors possessing both magnetic and optoelectronic properties are rare and promise applications in opto-spintronics. Here we report the mixed-anion semiconductor BaFMn0.5Te with a band gap of 1.76 eV and a work function of 5.08 eV, harboring both antiferromagnetism (AFM) and strong red photoluminescence (PL). The synthesis of BaFMn0.5Te in quantitative yield was accomplished using the "panoramic synthesis" technique and synchrotron radiation to obtain the full reaction map, from which we determined that the compound forms upon heating at 850 °C via an intermediate unknown phase. The structure refinement required the use of a (3+1)-dimensional superspace group Cmme(α01/2)0ss. The material crystallizes into a ZrCuSiAs-like structure with alternating [BaF]+ and [Mn0.5Te]- layers and has a commensurately modulated structure with the q-vector of 1/6a* + 1/6b* + 1/2c* at room temperature arising from the unique ordering pattern of Mn2+ cations. Long-range AFM order emerges below 90 K, with two-dimensional short-range AFM correlations above the transition temperature. First-principles calculations indicate that BaFMn0.5Te is an indirect band gap semiconductor with the gap opening between Te 5p and Mn 3d orbitals, and the magnetic interactions between nearest-neighbor Mn2+ atoms are antiferromagnetic. Steady-state PL spectra show a broad strong emission centered at â¼700 nm, which we believe originates from the energy manifolds of the modulated Mn2+ sublattice and its defects. Time-resolved PL measurements reveal an increase in excited-state lifetimes with longer probe wavelengths, from 93 ns (at 650 nm) to 345 ns (at 800 nm), and a delayed growth (6.5 ± 0.3 ns) in the kinetics at 800 nm with a concomitant decay (4.1 ± 0.1 ns) at 675 nm. Together, these observations suggest that there are multiple emissive states, with higher energy states populating lower energy states by energy transfer.
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Quasi-one-dimensional (Q1D) structures comprising a compact array of indefinitely long 1D nanowires (NWs) are scarce, especially in a bulk device-scale showing metallic and semiconducting behaviors along different axes. Unlike plentiful observations of nature of defects in three-/two-dimensional materials, there is a notable paucity of such reports in Q1D. Herein we present unconventional motific defects and their properties in a bulk Q1D KMn6Bi5 crystal, in which an individual NW motif acts as one body. We discovered motific inter- and intra-NW defects, such that a linear set of 1D motifs are displaced. Stress generates two domains with altered inter-NW spacings and a Bi-Mn solid solution grain, leading to a local bulk plasmon shift due to NW array reconfiguration as well as atomic rearrangement. The observation of such exotic defects and associated phenomena in this Q1D may provide guidance on overall defect mechanism in other Q1D systems and their collective anisotropic properties.
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The two major classes of unconventional superconductors, cuprates and Fe-based superconductors, have magnetic parent compounds, are layered, and generally feature square-lattice symmetry. We report the discovery of pressure-induced superconductivity in a nonmagnetic and wide band gap 1.95 eV semiconductor, Cu2I2Se6, with a unique anisotropic structure composed of two types of distinct molecules: Se6 rings and Cu2I2 dimers, which are linked in a three-dimensional framework. Cu2I2Se6 exhibits a concurrent pressure-induced metallization and superconductivity at â¼21.0 GPa with critical temperature (Tc) of â¼2.8 K. The Tc monotonically increases within the range of our study reaching â¼9.0 K around 41.0 GPa. These observations coincide with unprecedented chair-to-planar conformational changes of Se6 rings, an abrupt decrease along the c-axis, and negative compression within the ab plane during the phase transition. DFT calculations demonstrate that the flattened Se6 rings within the CuSe layer create a high density of states at the Fermi level. The unique structural features of Cu2I2Se6 imply that superconductivity may emerge in anisotropic Cu-containing materials without square-lattice geometry and magnetic order in the parent compound.
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We report a 2D material, KCu7P3, with a noncentrosymmetric structure (trigonal space group P31m, a = 6.9637(2) Å, c = 24.1338 (10) Å), which forms both from a molten potassium polyphosphide flux and from the elements. This phase consists of infinite [Cu7P3]- layers with hexagonal P sheets separated by K+ ions. The structure of the layers is unique but related to both Cu3P and the CaCu4P2 structure-types. Single-crystal refinement reveals extensive disorder within the Cu3P-like slabs. KCu7P3 is paramagnetic and exhibits a room temperature resistivity of â¼335 µΩ cm with a metal-like temperature dependence. The metallic character is supported by density functional theory electronic structure calculations. Hall and Seebeck effect measurements yield p-type behavior with a hole mobility of â¼15 cm2 V-1 s-1 at 300 K and a carrier concentration on the order of 1021 cm-3. KCu7P3 is chemically stable in ambient conditions, as well as in aqueous neutral and acidic solutions.
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The charge and spin of the electrons in solids have been extensively exploited in electronic devices and in the development of spintronics. Another attribute of electrons-their orbital nature-is attracting growing interest for understanding exotic phenomena and in creating the next-generation of quantum devices such as orbital qubits. Here, we report on orbital-flop induced magnetoresistance anisotropy in CeSb. In the low temperature high magnetic-field driven ferromagnetic state, a series of additional minima appear in the angle-dependent magnetoresistance. These minima arise from the anisotropic magnetization originating from orbital-flops and from the enhanced electron scattering from magnetic multidomains formed around the first-order orbital-flop transition. The measured magnetization anisotropy can be accounted for with a phenomenological model involving orbital-flops and a spin-valve-like structure is used to demonstrate the viable utilization of orbital-flop phenomenon. Our results showcase a contribution of orbital behavior in the emergence of intriguing phenomena.
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We report the two-dimensional (2D) natural heterostructure [Pb3.1Sb0.9S4][Au xTe2- x] ( x = 0.52-0.36) which shows anomalous, transverse nonsaturating negative magnetoresistance (MR). For x = 0.52, the material has a commensurately modulated structure with alternating [Pb3.1Sb0.9S4] rocksalt layers and atomically thin [Au xTe2- x] sheets, as determined by single-crystal X-ray diffraction using a (3 + 1)-dimensional space group; for other x compositions, the modulated structure is absent and the Au and Te atoms are disordered. The transport properties in this system at low temperature (<100 K) are dominated by an unusual 2D hopping mechanism, while at room temperature a high carrier mobility of â¼1352 cm2 V-1 s-1 is obtained ( x = 0.36). The confined electrons within the [Au xTe2- x] layers are also exposed to interlayer coupling with the insulating [Pb3.1Sb0.9S4] layers, and as a result, the properties of the heterostructures emerge not only from the constituent layers but also the interactions between them. Furthermore, the various Au and Te coordination patterns found in the [Au xTe2- x] sheets as a function of x further contribute to a unique electronic structure that leads to the anomalous nonsaturating negative MR with different field dependent behaviors. First-principles calculations indicate that the [Au xTe2- x] sheets are responsible for the unusual electrical transport properties in this 2D system.
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The new compound NaCu4Se4 forms by the reaction of CuO and Cu in a molten sodium polyselenide flux, with the existence of CuO being unexpectedly critical to its synthesis. It adopts a layered hexagonal structure (space group P63/ mmc with cell parameters a = 3.9931(6) Å and c = 25.167(5) Å), consisting of infinite two-dimensional [Cu4Se4]- slabs separated by Na+ cations. X-ray photoelectron spectroscopy suggests that NaCu4Se4 is mixed-valent with the formula (Na+)(Cu+)4(Se2-)(Se-)(Se2)2-. NaCu4Se4 is a p-type metal with a carrier density of â¼1021 cm-3 and a high hole mobility of â¼808 cm2 V-1 s-1 at 2 K based on electronic transport measurements. First-principles calculations suggest the density of states around the Fermi level are composed of Cu-d and Se-p orbitals. At 2 K, a very large transverse magnetoresistance of â¼1400% was observed, with a nonsaturating, linear dependence on field up to 9 T. Our results indicate that the use of metal oxide chemical precursors can open reaction paths to new low-dimensional compounds.
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We report a new quasi-one-dimensional compound KMn6Bi5 composed of parallel nanowires crystallizing in a monoclinic space group C2/ m with a = 22.994(2) Å, b = 4.6128(3) Å, c = 13.3830(13) Å and ß = 124.578(6)°. The nanowires are infinite [Mn6Bi5]- columns each of which is composed of a nanotube of Bi atoms acting as the cladding with a nanorod of Mn atoms located in the central axis of the nanotubes. The nanorods of Mn atoms inside the Bi cladding are stabilized by Mn-Mn bonding and are defined by distorted Mn-centered cluster icosahedra of Mn13 sharing their vertices along the b axis. The [Mn6Bi5]- nanowires are linked with weak internanowire Bi-Bi bonds and charge balanced with K+ ions. The [Mn6Bi5]- nanowires were directly imaged by high-resolution transmission electron microscopy and scanning transmission electron microscopy. Magnetic susceptibility studies show one-dimensional characteristics with an antiferromagnetic transition at â¼75 K and a small average effective magnetic moment (1.56 µB/Mn for H ⥠b and 1.37 µB/Mn for H ⥠b) of Mn from Curie-Weiss fits above 150 K. Specific heat measurements reveal an electronic specific heat coefficient γ of 6.5(2) mJ K-2(mol-Mn)-1 and a small magnetic entropy change Δ Smag ≈ 1.6 J K-1 (mol-Mn)-1 across the antiferromagnetic transition. In contrast to a metallic resistivity along the column, the resistivity perpendicular to the column shows a change from a semiconducting behavior at high temperatures to a metallic one at low temperatures, indicating an incoherent-to-coherent crossover of the intercolumn tunneling of electrons.
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Rb2Cr3As3 is a structurally one-dimensional superconductor containing Cr3As3 chains with a superconducting transition temperature of [Formula: see text] K. Here we report the electrical resistance measurements for Rb2Cr3As3 single crystals, under magnetic fields up to 29.5 T and at temperatures down to 0.36 K, from which the upper critical fields, [Formula: see text], can be obtained in a broad temperature range. For field parallel to the Cr3As3 chains, [Formula: see text] is paramagnetically limited with an initial slope of [Formula: see text]d[Formula: see text]/d[Formula: see text] T [Formula: see text] and a zero-temperature upper critical field of [Formula: see text] T. For field perpendicular to the Cr3As3 chains, however, [Formula: see text] is only limited by orbital pair-breaking effect with [Formula: see text]d[Formula: see text]/d[Formula: see text] T [Formula: see text]. As a consequence, the anisotropy [Formula: see text] decreases sharply near T c and reverses below 2 K. Remarkably, the low-temperature [Formula: see text] down to 0.075 [Formula: see text] remains to increase linearly up to over three times the Pauli paramagnetic limit, which strongly suggests dominant spin-triplet superconductivity in Rb2Cr3As3.
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Non-centrosymmetric superconductors, whose crystal structure is absent of inversion symmetry, have recently received special attentions due to the expectation of unconventional pairings and exotic physics associated with such pairings. The newly discovered superconductors A2Cr3As3 (A = K, Rb), featured by the quasi-one dimensional structure with conducting CrAs chains, belongs to such kind of superconductor. In this study, we are the first to report the finding that superconductivity of A2Cr3As3 (A = K, Rb) has a positive correlation with the extent of non-centrosymmetry. Our in-situ high pressure ac susceptibility and synchrotron x-ray diffraction measurements reveal that the larger bond angle of As-Cr-As (defined as α) in the CrAs chains can be taken as a key factor controlling superconductivity. While the smaller bond angle (defined as ß) and the distance between the CrAs chains also affect the superconductivity due to their structural connections with the α angle. We find that the larger value of α-ß, which is associated with the extent of the non-centrosymmetry of the lattice structure, is in favor of superconductivity. These results are expected to shed a new light on the underlying mechanism of the superconductivity in these Q1D superconductors and also to provide new perspective in understanding other non-centrosymmetric superconductors.
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EuBiS2F is a self-doped superconductor due to the mixed valence of Eu. Here we report that, with the Ce substitution for Eu by 50 at.%, the material exhibits ferromagnetic ordering at 8 K for the Ce-4 f moment, superconductivity at 2.2 K in the BiS2 layers and possibly antiferromagnetic ordering at 2.1 K for the Eu-4 f spins. The Eu valence is essentially divalent with the Ce incorporation. We tentatively interpret the coexistence of ferromagnetism and superconductivity by considering different Bi-6p orbitals that are responsible for the superconductivity itself and for mediating the ferromagnetic interaction, respectively. We argue that the antiferromagnetic ordering of the Eu-4 f spins is most likely due to a magnetic dipole-dipole interaction.
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We carried out measurements of the magnetoresistance, magnetic susceptibility and specific heat on crystals of the low-dimensional transition metal telluride Ta4Pd3Te16. Our results indicate that Ta4Pd3Te16 is an anisotropic type-II superconductor in the clean limit with the extracted Ginzburg-Landau parameter KGL = 84. The upper critical field Hc2(T) shows an anomalous temperature dependence at low temperatures and the anisotropy of Hc2(T) is strongly T-dependent, both of which indicate a multiband scenario. The electronic specific heat Cel(T) can be consistently described by a two-gap (s + d waves) model from the base temperature T/Tc ~ 0.12 up to Tc. Our results suggest nodal and multiband superconductivity in Ta4Pd3Te16.