La$_{0.4}$Na$_{0.6}$Fe$_2$As$_2$ single crystals have been grown out of an NaAs flux in an alumina crucible and characterized by measuring magnetic susceptibility, electrical resistivity, specific heat, as well as single crystal x-ray and neutron dif
fraction. La$_{0.4}$Na$_{0.6}$Fe$_2$As$_2$ single crystals show a structural phase transition from a high temperature tetragonal phase to a low-temperature orthorhombic phase at T$_s$,=,125,K. This structural transition is accompanied by an anomaly in the temperature dependence of electrical resistivity, anisotropic magnetic susceptibility, and specific heat. Concomitant with the structural phase transition, the Fe moments order along the emph{a} direction with an ordered moment of 0.7(1),$mu_{textup{B}}$ at emph{T},=,5 K. The low temperature stripe antiferromagnetic structure is the same as that in other emph{A}Fe$_{2}$As$_{2}$ (emph{A},=,Ca, Sr, Ba) compounds. La$_{0.5-x}$Na$_{0.5+x}$Fe$_2$As$_2$ provides a new material platform for the study of iron-based superconductors where the electron-hole asymmetry could be studied by simply varying La/Na ratio.
The phonon dispersion was measured at room temperature along (0,0,L) in the tetragonal phase of LaFeAsO using inelastic x-ray scattering. Spin-polarized first-principles calculations imposing various types of antiferromagnetic order are in better agr
eement with the experimental results than nonmagnetic calculations, although the measurements were made well above the magnetic ordering temperature, T_N. Splitting observed between two A_{1g} phonon modes at 22 and 26 meV is only observed in spin-polarized calculations. Magneto-structural effects similar to those observed in the AFe_2As_2 materials are confirmed present in LaFeAsO. The presence of Fe-spin is necessary to find reasonable agreement of the calculations with the measured spectrum well above T_N. On-site Fe and As force constants show significant softening compared to nonmagnetic calculations, however an investigation of the real-space force constants associates the magnetoelastic coupling with a complex renormalization instead of softening of a specific pairwise force.
Microscopic, structural, transport and thermodynamic measurements of single crystalline Ba(Fe1-xTMx)2As2 (TM = Ni and Cu) series, as well as two mixed TM = Cu / Co series, are reported. All the transport and thermodynamic measurements indicate that t
he structural and magnetic phase transitions at 134 K in pure BaFe2As2 are monotonically suppressed and increasingly separated in a similar manner by these dopants. In the Ba(Fe1-xNix)2As2 (x =< 0.072), superconductivity, with Tc up to 19 K, is stabilized for 0.024 =< x =< 0.072. In the Ba(Fe1-xCux)2As2 (x =< 0.356) series, although the structural and magnetic transitions are suppressed, there is only a very limited region of superconductivity: a sharp drop of the resistivity to zero near 2.1 K is found only for the x = 0.044 samples. In the Ba(Fe1-x-yCoxCuy)2As2 series, superconductivity, with Tc values up to 12 K (x ~ 0.022 series) and 20 K (x ~ 0.047 series), is stabilized. Quantitative analysis of the detailed temperature-dopant concentration (T-x) and temperature-extra electrons (T-e) phase diagrams of these series shows that there exists a limited range of the number of extra electrons added, inside which the superconductivity can be stabilized if the structural and magnetic phase transitions are suppressed enough. Moreover, comparison with pressure-temperature phase diagram data, for samples spanning the whole doping range, further reenforces the conclusion that suppression of the structural / magnetic phase transition temperature enhances Tc on the underdoped side, but for the overdoped side Tcmax is determined by e. Therefore, by choosing the combination of dopants that are used, we can adjust the relative positions of the upper phase lines (structural and magnetic phase transitions) and the superconducting dome to control the occurrence and disappearance of the superconductivity in transition metal, electron-doped BaFe2As2.
Millimeter-sized single crystals of LaFeAsO, LaFeAsO1-xFx, and LaFe1-xCoxAsO were grown in NaAs flux at ambient pressure. The detailed growth procedure and crystal characterizations are reported. The as-grown crystals have typical dimensions of 3 * 4
* 0.05-0.3 mm3 with the crystallographic c-axis perpendicular to the plane of the plate-like single crystals. Some crystals manifest linear dimensions as large as 4-5 mm. X-ray and neutron single crystal scattering confirmed that LaFeAsO crystals exhibit a structural phase transition at Ts ~ 154 K and a magnetic phase transition at TSDW ~ 140 K. The transition temperatures agree with those determined by anisotropic magnetization, in-plane electrical resistivity and specific heat measurements and are consistent with previous reports on polycrystalline samples. Co and F were successfully introduced into the lattice leading to superconducting LaFe1-xCoxAsO and LaFeAsO1-xFx single crystals, respectively. This growth protocol has been successfully employed to grow single crystals of NdFeAsO. Thus it is expected to be broadly applicable to grow other RMAsO (R = rare earth, M = transition metal) compounds. These large crystals will facilitate the efforts of unraveling the underlying physics of iron pniticide superconductors.
Single crystalline samples of Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$ with $x < 0.12$ have been grown and characterized via microscopic, thermodynamic and transport measurements. With increasing Co substitution, the thermodynamic and transport signatures of t
he structural (high temperature tetragonal to low temperature orthorhombic) and magnetic (high temperature non magnetic to low temperature antiferromagnetic) transitions are suppressed at a rate of roughly 15 K per percent Co. In addition, for $x ge 0.038$ superconductivity is stabilized, rising to a maximum $T_c$ of approximately 23 K for $x approx 0.07$ and decreasing for higher $x$ values. The $T - x$ phase diagram for Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$ indicates that either superconductivity can exist in both low temperature crystallographic phases or that there is a structural phase separation. Anisotropic, superconducting, upper critical field data ($H_{c2}(T)$) show a significant and clear change in anisotropy between samples that have higher temperature structural phase transitions and those that do not. These data show that the superconductivity is sensitive to the suppression of the higher temperature phase transition.
Plate-like single crystals of SrFe2As2 as large as 3x3x0.5 mm3 have been grown out of Sn flux. The SrFe2As2 single crystals show a structural phase transition from a high temperature tetragonal phase to a low temperature orthorhombic phase at To = 19
8 K, and do not show any sign of superconductivity down to 1.8 K. The structural transition is accompanied by an anomaly in the electrical resistivity, Hall resistivity, specific heat, and the anisotropic magnetic susceptibility. In an intermediate temperature range from 198 K to 160 K, single crystal X-ray diffraction suggests a coexistence of the high-temperature tetragonal and the low-temperature orthorhombic phases.
