The crystalline electric field as a probe for long range antiferromagnetic order and superconductivity in CeFeAsO$_{1-x}$F$_x$
Songxue Chi, D. T. Adroja, T. Guidi, R. Bewley, Shiliang Li, Jun Zhao, J. W. Lynn, C. M. Brown, Y. Qiu, G. F. Chen, J. L. Lou, N. L. Wang, Pengcheng Dai
We use inelastic neutron scattering to study the crystalline electric field (CEF) excitations of Ce$^{3+}$ in CeFeAsO$_{1-x}$F$_{x}$($x=0,0.16$). For nonsuperconducting CeFeAsO, the Ce CEF levels have three magnetic doublets in the paramagnetic state, but these doublets split into six singlets when Fe ions order antiferromagnetically. For superconducting CeFeAsO$_{0.84}$F$_{0.16}$ ($T_c=41$ K), where the static AF order is suppressed, the Ce CEF levels have three magnetic doublets at $\hbarω=0,18.7,58.4$ meV at all temperatures. Careful measurements of the intrinsic linewidth $Γ$ and the peak position of the 18.7 meV mode reveal clear anomaly at $T_c$, consistent with a strong enhancement of local magnetic susceptibility $χ^{\prime\prime}(\hbarω)$ below $T_c$. These results suggest that CEF excitations in the rare-earth oxypnictides can be used as a probe of spin dynamics in the nearby FeAs planes.
Single-crystal synchrotron x-ray diffraction studies of CeFeAsO reveal strong anisotropy in the charge correlation lengths along or perpendicular to the in-plane antiferromagnetic (AFM) wave-vector at low temperatures, indicating an anisotropic two-dimensional magnetoelastic coupling. The high-resolution setup allows to distinctly monitor each of the twin domains by virtue of a finite misfit angle between them that follows the order parameter. In addition, we find that the in-plane correlations, above the orthorhombic (O)-to-tetragonal (T) transition, are shorter than those in each of the doma…
We use neutron scattering to study the structural and magnetic phase transitions in the iron pnictides CeFeAsO1-xFx as the system is tuned from a semimetal to a high-transition-temperature (high-Tc) superconductor through Fluorine (F) doping x. In the undoped state, CeFeAsO develops a structural lattice distortion followed by a stripe like commensurate antiferromagnetic order with decreasing temperature. With increasing Fluorine doping, the structural phase transition decreases gradually while the antiferromagnetic order is suppressed before the appearance of superconductivity, resulting an el…
In the iron-pnictide material CeFeAsO not only the Fe moments, but also the local 4f moments of the Ce order antiferromagnetically at low temperatures. We elucidate on the peculiar role of the Ce on the emergence of superconductivity. While application of pressure suppresses the iron SDW ordering temperature monotonously up to 4 GPa, the Ce-4f magnetism is stabilized, until both types of magnetic orders disappear abruptly and a narrow SC dome develops. With further increasing pressure characteristics of a Kondo-lattice system become more and more apparent in the electrical resistivity. This su…
The electrical resistance of CeFeAsO$_{1-x}$F$_x$ (x = 0.06 and 0.08) has been measured in a magnetic field up to 40T. At zero field, the sample with x = 0.06 shows a structural phase transition around T$_S$~100K, followed by a spin-density-wave (SDW) transition around T$_{SDW}$~30K. For x = 0.08, the structural phase transition is suppressed down to T$_S$~60K without a clear anomaly associated with the Fe-SDW transition, and superconductivity shows up at T$_C$~25K. At lower temperatures, both samples show a clear resistive peak around T$_N$~4K, which is associated with the antiferromagnetic (…
We report on superconductivity in CeFeAs1-xPxO and the possible coexistence with Ce- ferromagnetism (FM) in a small homogeneity range around x = 30% with ordering temperatures of T_SC = T_C = 4K. The antiferromagnetic (AFM) ordering temperature of Fe at this critical concentration is suppressed to T^N_Fe ~ 40K and does not shift to lower temperatures with further increase of the P concentration. Therefore, a quantum-critical-point scenario with T^N_Fe -> 0K which is widely discussed for the iron based superconductors can be excluded for this alloy series. Surprisingly, thermal expansion and X-…
Neutron and synchrotron resonant X-ray magnetic scattering (RXMS) complemented by heat capacity and resistivity measurements reveal the evolution of the magnetic structures of Fe and Ce sublattices in single crystal CeFeAsO. The RXMS of magnetic reflections at the Ce $L_{\rm II}$-edge shows a magnetic transition that is specific to the Ce antiferromagnetic long-range ordering at $T_\texttt{Ce}\approx$ 4 K with short-range Ce ordering above $T_\texttt{Ce}$, whereas neutron diffraction measurements of a few magnetic reflections indicate a transition at $T^{*}\approx$ 12 K with unusual order para…
The evolution of the antiferromagnetic order parameter in CeFeAsO_{1-x}F_{x} as a function of the fluorine content x was investigated primarily via zero-field muon-spin spectroscopy. The long-range magnetic order observed in the undoped compound gradually turns into a short-range order at x=0.04, seemingly accompanied/induced by a drastic reduction of the magnetic moment of the iron ions. Superconductivity appears upon a further increase in doping (x>0.04) when, unlike in the cuprates, the Fe magnetic moments become even weaker. The resulting phase diagram evidences the presence of a crossover…
We present results of transport and magnetic properties and heat capacity measurements on polycrystalline CeFeAsO, PrFeAsO, and NdFeAsO. These materials undergo structural phase transitions, spin density wave-like magnetic ordering of small moments on iron, and antiferromagnetic ordering of rare earth moments. The temperature dependence of the electrical resistivity, Seebeck coefficient, thermal conductivity, Hall coefficient, and magnetoresistance are reported. The magnetic behavior of the materials have been investigated using Mossbauer spectroscopy and magnetization measurements. Transport …
Single crystals of CeFeAsO, large enough to study the anisotropy of the magnetic properties, were grown by an optimized Sn-flux technique. The high quality of our single crystals is apparent from the highest residual resistivity ratio, RRR = 12, reported among undoped RFeAsO compounds (R=rare earth) as well as sharp anomalies in resistivity, specific heat, C(T), and thermal expansion at the different phase transitions. The magnetic susceptibility chi(T) presents a large easy-plane anisotropy consistent with the lowest crystal electric field doublet having a dominant Gamma_6 character. Curie-We…
We present a detailed study of RNi1-xBi2+-y (R = La-Nd, Sm, Gd-Dy) single crystals by measurements of stoichiometry and temperature dependent magnetic susceptibility, magnetization, and electrical resistivity. This series forms with partial Ni occupancy as well as a variable Bi occupancy. For R = Ce-Nd, Sm, Gd-Dy, the RNi1-xBi2+-y compounds show local-moment like behavior and order antiferromagnetically at low temperatures. Determination of anisotropies as well as antiferromagnetic ordering temperatures for RNi1-xBi2+-y (R = Ce-Nd, Sm, Gd-Dy) have been made. Although crystalline samples from t…
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 …
We present an inelastic neutron scattering study on single-crystalline LiFeAs devoted to the characterization of the incommensurate antiferromagnetic fluctuations at $\mathbf{Q}=(0.5\pmδ, 0.5\mpδ, q_l)$. Time-of-flight measurements show the presence of these magnetic fluctuations up to an energy transfer of 60 meV, while polarized neutrons in combination with longitudinal polarization analysis on a triple-axis spectrometer prove the pure magnetic origin of this signal. The normalization of the magnetic scattering to an absolute scale yields that magnetic fluctuations in LiFeAs are by a factor …
The structural and magnetic phase transitions have been studied on NdFeAsO single crystals by neutron and x-ray diffraction complemented by resistivity and specific heat measurements. Two low-temperature phase transitions have been observed in addition to the tetragonal-to-orthorhombic transition at T_S = 142 K and the onset of antiferromagnetic (AFM) Fe order below T_N = 137 K. The Fe moments order AFM in the well-known stripe-like structure in the (ab) plane, but change from AFM to ferromagnetic (FM) arrangement along the c direction below T* = 15 K accompanied by the onset of Nd AFM order b…
The low-energy charge excitations of a doped antiferromagnetic ladder are modeled by a system of interacting spinless fermions that live on the same ladder. A relatively large spin gap is assumed to ``freeze out'' all spin fluctuations. We find that the formation of rung hole pairs coincides with the opening of a single-particle gap for charge excitations along chains and with the absence of coherent tunneling in between chains. We also find that such hole pairs condense into either a crystalline or superconducting state as a function of the binding energy.
We report systematic 31P-NMR study on iron (Fe)-based superconductors SrFe2(As_{1-x}P_{x})2 (Sr122AsP), in which a superconducting (SC) transition temperature Tc at x=0.35 increases from Tc=26 K up to 33 K by annealing an as-grown mono-crystalline sample. The present NMR study has unraveled that Tc reaches a highest value of 33 K at x=0.35 around a quantum critical point at which antiferromagnetic (AFM) order disappears. When noting that the SC transition disappears at x=0.6 where the AFM spin fluctuations (SFs) are no longer present, we remark that the onset and increase of Tc are apparently …
The magnetic structure of BaFe2As2 was completely determined from polycrystalline neutron diffraction measurements soon after the ThCr2Si2-type FeAs-based superconductors were discovered. Both the moment direction and the in-plane antiferromagnetic wavevector are along the longer a-axis of the orthorhombic unit cell. There is only one combined magnetostructural transition at about 140 K. However, a later single-crystal neutron diffraction work reported contradicting results. Here we show neutron diffraction results from a clean single crystal sample, grown by a self-flux method, that support t…
An overview on recent efforts in point-contact (PC) spectroscopy of title superconductors is given. Distinct phonon features and crystalline-electric-field effects are observed in PC spectra of HoNi2B2C. Results of study of superconducting (SC) gap and excess current versus temperature and magnetic field reflecting specific multi-band electronic structure in MgB2 are presented. The nature of the extremely nonlinear I(V) curves in the antiferromagnetic (AF) and SC state are elucidated for UPd2Al3 break-junctions and MgCNi3 point contacts.
We report an optical investigation on the in-plane charge dynamics for Na$_{1-δ}$FeAs single crystal. A clear optical evidence for the spin-density wave (SDW) gap is observed. As the structural/magnetic transitions are separated in the Na$_{1-δ}$FeAs case, we find the SDW gap opens in accordance with the magnetic transition. Comparing with the optical response of other FeAs-based parent compounds, both the gap value 2$Δ$ and the energy scale for the gap-induced spectral weight redistribution are smaller in Na$_{1-δ}$FeAs. Our findings support the itinerant origin of the antiferromagnetic trans…
A new ternary platinum phosphide CePt$_{3}$P was synthesized and characterized by means of magnetic, thermodynamic and transport measurements. The compound crystallizes in an antiperovskite tetragonal structure similar to that in the canonical family of platinum-based superconductors $A$Pt$_{3}$P ($A$ = Sr, Ca, La) and closely related to the noncentrosymmetric heavy fermion superconductor CePt$_{3}$Si. In contrast to all the superconducting counterparts, however, no superconductivity is observed in CePt$_{3}$P down to 0.5 K. Instead, CePt$_{3}$P displays a coexistence of antiferromagnetic orde…
We present the results of our comprehensive investigation on the antiferromagnetic heavy-fermion superconductor Ce$_3$PtIn$_{11}$ carried out by means of electrical transport, heat capacity and ac magnetic susceptibility measurements, performed on single-crystalline specimens down to 50 mK in external magnetic fields up to 9~T. Our experimental results elucidate a complex magnetic field -- temperature phase diagram which contains both first- and second-order field-induced magnetic transitions and highlights the emergence of field stabilized phases. Remarkably, a prominent metamagnetic transiti…
57Fe-Mössbauer studies of superconducting Rb0.8Fe1.6Se2.0 with TC = 32.4 K were performed on single-crystalline and polycrystalline samples in the temperature range 4.2 K to 295 K. They reveal the presence of 88% magnetic and 12% non-magnetic Fe2+ species with the same polarization dependence of their hyperfine spectra. The magnetic species are attributed to the 16i sites of the \surd5 x \surd5 x 1 superstructure, and non-magnetic species to a nano-sized phase postulated from recent studies of superconducting KxFe2-ySe2 systems. The 57Fe-spectrum of a single-crystalline sample in an external f…
We have investigated the evolution of the low temperature specific heat anomaly (TN=5.4K in zero field) in polycrystalline SmFeAsO samples with magnetic fields up to 35T. The anomaly remains very sharp up to 16T and becomes rounded with little shift in temperature at higher fields. Doped (superconducting) SmFeAsO0.85F0.15 sample shows a similar behavior up to 16T. The initial slope of the critical field dBc/dT is 160T/K for undoped SmFeAsO and 70T/K for doped SmFeAsO0.85F0.15, with Bc(T) defined at the peak of the specific heat anomaly. The insensitivity to the application of an external magne…
We report the anomalous Hall effect (AHE) in antiperovskite Mn$_{3}$NiN with substantial doping of Cu on the Ni site (i.e. Mn$_{3}$Ni$_{1-x}$Cu$_{x}$N), which stabilizes a noncollinear antiferromagnetic (AFM) order compatible with the AHE. Observed on both sintered polycrystalline pieces and single crystalline films, the AHE does not scale with the net magnetization, contrary to the conventional ferromagnetic case. The existence of the AHE is explained through symmetry analysis based on the $Γ_{\rm 4g}$ AFM order in Cu doped Mn$_{3}$NiN. DFT calculations of the intrinsic contribution to the AH…
The discovery of superconductivity in the two-leg ladder compound BaFe$_2$S$_3$ has established the 123-type iron chalcogenides as a novel and interesting subgroup of the iron-based superconductors family. However, in this 123 series, BaFe$_2$Se$_3$ is an exceptional member, with a magnetic order and crystalline structure different from all others. Recently, an exciting experiment reported the emergence of superconductivity in BaFe$_2$Se$_3$ at high pressure [J.-J. Ying, et al., Phys. Rev. B 95, 241109 (R) (2017)]. In this publication, we report a first principles study of BaFe$_2$Se$_3$. Our …
Single crystals of Fe(1+x)Te(1-y)Se(y) have been grown with a controlled Fe excess and Se doping, and the crystal structure has been refined for various compositions. The systematic investigation of magnetic and superconducting properties as a function of the structural parameters shows how the material can be driven into various ground states, depending on doping and the structural modifications. Our results prove that the occupation of the additional Fe site, Fe2, enhances the spin localization. By reducing the excess Fe, the antiferromagnetic ordering is weakened, and the superconducting gr…
We report 31P-NMR and specific heat measurements on an iron (Fe)-based superconductor SrFe2(As0.65P0.35)2 with Tc=26 K, which have revealed the development of antiferromagnetic correlations in the normal state and the unconventional superconductivity(SC) with nodal gap dominated by the gapless low-lying quasiparticle excitations. The results are consistently argued with an unconventional multiband SC state with the gap-size ratio of different bands being significantly large; the large full gaps in s\pm-wave state keep Tc high, whereas a small gap with a nodal-structure causes gapless feature u…
Doped BaCoSO was recently predicted to be a high-temperature superconductor in a new class based on Co and Ni. Using a Co-S self flux method, we synthesized single crystals of the antiferromagnetic insulator BaCoSO. Our magnetic and specific heat measurements and neutron diffraction provide details of its magnetic anisotropy and order. Its band gap was determined to be about 1.3 eV by our measurements of its photoemission spectrum and infrared optical conductivity. Our results can pave the way to exploring the predicted superconductivity in this Co-based material.
Systematic studies of magnetic properties of LaSr2Mn2O7 as a function of crystalline grain size provide information on how the crystalline grain size affects the magnetic and charge ordering in this compound. The half-doped bi-layered manganite LaSr2Mn2O7 (x=0.5) in its bulk form has CE-type antiferromagnetic (CE-AFM) charge ordering phase transition. In this work, we have prepared LaSr2Mn2O7 ceramic samples using Pechini sol-gel method to produce different grain sizes and the effect of crystalline grain sizes between 150 200 to 1000 nm on magnetic properties results obtained by the SQUID magn…
The point-contact (PC) spectroscopy study of the electron-phonon(boson) interaction (EP(B)I) spectral function in HoNi2B2C reveals phonon maxima at 16 and 22meV and 34meV. For the first time the pronounced high energy maxima at about 50meV and 100meV were resolved. Additionally, an admixture of a crystalline-electric-field (CEF) excitation with a maximum near 10meV and a `magnetic` peak near 3meV are observed. The contribution of the CEF peak in EP(B)I constant λ_{PC} is evaluated as 20-30%, while contribution of the high frequency modes at 50 and 100meV amounts about 10% for each maxima. PC A…
We report the effects of cobalt doping on the magnetic properties of two-dimensional van der Waals ferromagnet Fe3GeTe2. Single crystals of (Fe{1-x}Cox)3GeTe2 with x=0-0.78 were successfully synthesized and characterized with x-ray diffraction, energy dispersive x-ray spectroscopy and magnetization measurements. Both the Curie-Weiss temperature and ferromagnetic (FM) ordered moment of Fe3GeTe2 are gradually suppressed upon Co doping. A kink in zero-field-cooling low field M(T) curve which is previously explained as an antiferromagnetic transition is observed for samples with x=0-0.58. Our deta…
