Temperature and pressure dependence of lattice parameters of the XCu2Si2 compounds (X=Ce,Eu, Yb,La, Gd,Lu, Ca,Th)

The RECU₂Si₂(RE=Rare Earth) series shows pronounced anomalies of the lattice parameters. In those stable valent compounds with 4f orbital angular momentumL0 thec/a ratio shows an anomalous temperature dependence due to crystal field effects. The compounds with unstable valence (RE=Ce, Eu, Yb) show less or no such effects but on the other hand show anomalies of the volume which are temperature dependent. Using these volume anomalies of the unstable valent systems and the measured bulk moduli of the reference compounds we have extracted the valence as function of temperature.Between 4K and 300K the valences of CeCu₂Si₂ and YbCu₂Si₂ change by only a few percent towards 3, while it changes for EuCu₂Si₂ by ca. 20% towards 2. A critical discussion of these valences will be given.     

Magnetic order in RCr\mathsf{_{2}}Si\mathsf{_{2}} intermetallics

The magnetic structure and ordering temperatures of three intermetallic compounds which crystallize in the tetragonal ThCr₂Si₂ structure, TbCr₂Si₂, HoCr₂Si₂ and ErCr₂Si₂, have been determined by neutron diffraction, differential scanning calorimetry and magnetization measurements. The Cr-sublattice orders anti-ferromagnetically with Néel temperatures of 758 K for TbCr₂Si₂, 718 K for HoCr₂Si₂ and 692 K for ErCr₂Si₂. Chromium atoms located at 4d crystallographic sites are aligned anti-parallel along the c-axis, with G_ZCr magnetic modes. In contrast with metallic bcc Cr, the refined room temperature value of the ordered Cr moment is anomalously large for all three compounds. No long range magnetic order of the R sublattice in TbCr₂Si₂ and HoCr₂Si₂ is observed, whilst the Er sublattice in ErCr₂Si₂ orders independently of the Cr sublattice below 2.4 K with moments ferromagnetically aligned in the basal plane.Received: 4 November 2003, Published online: 30 January 2004PACS: 75.25. + z Spin arrangements in magnetically ordered materials (including neutron and spin-polarized electron studies, synchrotron-source X-ray scattering, etc.) - 75.30.Cr Saturation moments and magnetic susceptibilities - 75.50.Ee Antiferromagnetics     

The studies of high-temperature and short-time annealing,phase transition process,and magnetic property for LaFe11.7Si1.3 compound

The high-temperature phase transition is analyzed according to the DSC of as-cast LaFe_11.7 Si_1.3 compound and the X-ray patterns of LaFe_11.7Si_1.3 compounds prepared by high-temperature and short-time annealing. Large amount of 1:13 phase begins to appear in LaFe_11.7Si_1.3 compound annealed near the melting point of LaFeSi phase (about 1422?K). When the annealing temperature is close to the temperature of peritectic reaction (about 1497?K), the speed of 1:13 phase formation is the fastest. The phase relation and microstructure of the LaFe_11.7Si_1.3 compounds annealed at 1523?K (5?h), 1373?K (2?h)?+?1523?K (5?h), and 1523?K (7?h) +1373?K (2?h) show that longer time annealing near peritectic reaction is helpful to decrease the impurity phases. For studying the influence of different high-temperature and short-time annealing on magnetic property, the Curie temperature, thermal, and magnetic hystereses, and the magnetocaloric effect of LaFe_11.7Si_1.3 compound annealed at three different temperatures are also investigated. Three compounds all keep the first order of magnetic transition behavior. The maximal magnetic entropy change ΔS_M (T, H) of the samples is 12.9, 16.04, and 23.8?J?kg^?1?K^?1 under a magnetic field of 0–2?T, respectively.     

μ+SR study of LaNi2As2, URh2Si2 and CeRh2Si2

Muon spin relaxation experiments have been carried out in the paramagnetic and magnetically ordered states of URh₂Si₂ and CeRh₂Si₂. As the magnetic structure of these compounds is well known, these measurements can help to characterise their magnetic properties probed by μSR and to understand the μSR results of the heavy fermion compounds of the same crystallographic family. Our measurements show that the muons occupy two different crystallographic sites. The spectra of URh₂Si₂ and CeRh₂Si₂ in the magnetically ordered states are very different, probably reflecting their different magnetic structures. The spectra obtained on CeRh₂Si₂ are similar to the published spectra of the heavy fermion compound CeCu_2.1 Si₂. Muon spin rotation measurements on LaNi₂As₂ indicate that the muon is diffusing at 150 K.     

A non-magnetic Fe probe of multiple magnetic phase transitions in RMn2Si2−x Ge x,R=rare earth

Summary Dilute⁵⁷Fe M?ssbauer-spectroscopy studies of RMn₂X₂ (X=Si and/or Ge, R=La, Ce, Pr, Nd, Sm, Eu and Gd) at 4.2 to 650 K yield the following results: Fe in RMn₂X₂ does not carry a magnetic moment. It reveals the magnetic order in the Mn and R sublattices through transferred hyperfine fields (∼100 kOe). The compounds LaMn₂Si₂, LaMn₂Ge₂, CeMn₂Ge₂, PrMn₂Ge₂, NdMn₂Ge₂ and SmMn₂Ge₂, known to be ferromagnets withT _c=300–350 K, are antiferromagnetically ordered above their correspondingT _c. TherT _N values extend from 385 K (SmMn₂Ge₂) to 470 K (LaMn₂Si₂). At the ferromagnetic-antiferromagnetic phase transition, a sharp reorientation of the Mn magnetic moments relative to the crystalline axes occurs. In RMn₂Si_2−x Ge _x with intermediatex values, the Ge is much more dominant in determining the magnetic properties of the Mn sublattice. While PrMn₂Si₂ is an antiferromagnet (T _N=365 K) and PrMn₂Ge₂ is a ferromagnetantiferromagnet (T _c=328 K,T _N=415 K), we find that in PrMn₂SiGe, the magnetic behaviour is similar to that in pure PrMn₂Ge₂,T _c=305 K andT _N=395 K. Paper presented at ICAME-95, Rimini, 10–16 September 1995.     

Magnetic properties of RAu2Si2 rare earth compounds

The magnetic properties of the R Au₂Si₂ compounds with R = Ce-Er have been investigated. It was found that the compounds for which R = Ce, Sm, Gd, Tb and Dy are antiferromagnetically ordered at temperatures ranging from 5.7 to 15.9°K. PrAu₂Si₂ and NdAu₂Si₂ exhibit paramagnetic behavior for temperatures as low as 4.2°K. The magnetic structure is ferrimagnetic for the compounds in which R = Eu, Ho, and Er. The Eu compound is in the divalent state. The Néel and Curie points for this system do not follow the De-Gemnes function. Curie-Weiss Behavior is exhibited by all the compounds with effective moments in good agreement with that of a free tripositive lanthanide ion. The difference in magnetic properties between R Au₂Si₂ and the isomorphous R Fe₂Si₂ series is discussed.     

Itinerant and local magnetism,superconductivity and mixed valency phenomena in RM2Si2, (R = rare earth,M = Rh,Ru)°

X-Ray, magnetization and Mossbauer (¹⁵¹Eu, ¹⁵⁵Gd, ¹⁶¹Dy and dilute ⁵⁷Fe) studies of RM₂Si₂ reveal that when R is a magnetic ion the compounds order antiferromagnetically. For M = Rh a second antiferromagnetic phase transition is observed, corresponding to Rh itinerant electron magnetic ordering. In EuRh₂Si₂ the Eu ion is predominantly divalent with a mixed valent component. In EuRu₂Si₂ the Eu is predominantly trivalent. LaRu₂Si₂ and LuRu₂Si₂ display enhanced electron paramagnetism and become superconducting at 3.5 K and 2.4 K respectively. LaRh₂Si₂, YRh₂Si₂ and LuRh₂Si₂ display an itinerant electron magnetic phase transition, T_M (LaRh₂Si₂) = 7 K, and at lower temperatures a superconducting phase transition, T_c(LaRh₂Si₂) = 3.8 K. There is evidence that in the superconducting phase the itinerant magnetic order survives.     

Magnetic ordering in NdRh2Si2 and ErRH2Si2

Neutron diffraction and magnetization study of polycrystalline NdRh₂Si₂ and ErRh₂Si₂ was performed in the temperature range from 4.2 to 293 K. Both compounds are of ThCr₂Si₂ type crystal structure and exhibit antiferromagnetic ordering below T_N = 53 K and T_N = 12.8 K respectively. The magnetic structure wave vector is τ = [0, 0, 1].     

Magnetic ordering in HoRu2Si2, HoRh2Si2, TbRh2Si2 and TbIr2Si2 by neutron diffraction

Neutron diffraction study of polycrystalline HoRu₂Si₂, HoRh₂Si₂, TbRh₂Si₂, and TbIr₂Si₂ was performed in the temperature range between 4.2 and 300 K. For HoRu₂Si₂ the magnetic spin alignment of a linear transverse wave mode below the Néel temperature 19 K is observed. This static moment wave is propagating along the b-axis with k=(0, 0.2, 0) and is polarized in the c-axis. The root-mean-square and maximum saturation moments per Ho atom are 9.26 and 13.09μ_B, respectively. HoRh₂Si₂, TbRh₂Si₂ an TbIr₂Si₂ are simple collinear antiferromagnets of +-+- type with Néel temperatures of (27±1), (98±2) and (72±3) K, respectively. For TbRh₂Si₂ and TbIr₂Si₂ magnetic moments are localized on RE ions only and are aligned along the tetragonal axis, while for HoRh₂Si₂ they form an angle ø = (28±3)°.     

Investigation of the magnetic behavior and structural chemistry within the pseudobinary silicide system CeOs x Ru2−x Si2

The crystal chemistry and the magnetism in the pseudobinary system CeOs _x Ru_2–x Si₂ has been investigated in the temperature range of 1.5 K to 1,100 K and for various concentrations. From Guinier X-ray powder diffractometry all alloys were found to be isostructural and to crystallize with the ThCr₂Si₂-type of structure. No significant deviations from the ThCr₂Si₂-atomic order and symmetry were observed in the as-cast alloys with respect to those heat treated at 1,000°C and at 500°C, quenched. From magnetic susceptibilities it is shown that the 4f-electrons demagnetize at low temperatures. The data were interpreted in terms of interconfiguration fluctuations, based on a model derived by Sales and Wohlleben. A maximum valence change is observed in CeOs_1.4Ru_0.6Si₂, ranging from 3.27 at 700 K to 3.70 at 5 K.     

Magnetic properties of a new Kondo lattice compound: CePt2Si2

Measurements of magnetic susceptibility, electrical resistivity and specific heat on CePt₂Si₂ and LaPt₂Si₂ compounds are reported. Several anomalous properties are observed in CePt₂Si₂, characteristic of Kondo lattice and Fermi liquid systems with indication of coherence effects below 2 K.     

Magnetic properties of the compounds ThCO2Ge2 and ThCo2Si2

Rather old preparation of the compounds ThCo₂Ge₂ and ThCo₂Si₂ and their magnetic study in the temperature range 100–570 K, published by Omejec and Ban [Z. Anorg. Allg. Chem. 380 (1971) 111], indicated that both compounds ordered ferrromagnetically below 100 K. In order to verify the old data, polycrystalline samples of ThCo₂Ge₂ and ThCo₂Si₂ have been prepared by arc melting and subsequent annealing, and studied by X-ray diffraction at room temperature (RT), by superconducting quantum interference device (SQUID)-magnetization and AC-susceptibility measurements at 2–320 K, and by dc-magnetization measurements in variable magnetic fields up to 120 kOe at 5, 80, and 283 K. The magnetic measurements confirm the ferromagnetic ordering in both compounds, but with totally different Curie temperatures: ≈120(20) K for ThCo₂Ge₂ and above 320 K for ThCo₂Si₂. The paramagnetic values of ThCo₂Ge₂ and the ordering of both compounds are discussed and compared with the old results of Omejec and Ban.     

Interrelation between electronic structure and interatomic distances for compounds

The heat capacity was studied for LaMn₂Si₂, La_0.75Y_0.25Mn₂Si₂, La_0.7Y_0.3Mn₂Si₂, YMn₂Si₂ and LaFe₂Si₂ isostructural intermetallic compounds in the temperature range 1.8–360 K. The electronic, magnetic and lattice contributions to the heat capacity of the compounds were determined and analyzed. The interrelation was found between values of the electronic contribution to the heat capacity (density of states at the Fermi level) and crystal lattice parameters of R(Mn,Fe,Ni)₂Si₂ compounds. The electronic contribution and the density of states at Fermi level increase with increasing lattice parameters of the compounds. The change of interlayer Mn–Mn exchange interactions with change of Y concentration in La_1-xY_xMn₂Si₂ compounds is not accompanied by considerable changes in the electronic contribution to the heat capacity and density of states at the Fermi level. The performed analysis of the magnetic contribution shows that no essential differences exist between the behavior of the heat capacity of the compounds with d_Mn–Mnd_c and with d_Mn–Mn<d_c upon various types of the magnetic phase transitions.     

Mixed valence on dilute Eu in YCu2Si2

We report measurements of electrical resistivity, thermopower, thermal conductivity, magnetic susceptibility, Mößbauer andL _III x-ray absorption of intermediate valent Eu in Y_1–x Eu _x Cu₂Si₂ alloys withx=0.03,x=0.07 andx=0.10. A qualitative comparison of the physical properties of dilute Eu in YCu₂Si₂ with concentrated Eu in EuCu₂Si₂ shows only slight differences; the dominant feature is a very strong variation of the Eu valence with temperature, from about 2.8 at 4 K to about 2.45 at 800 K, in the concentrated compound as well as in the dilute alloys.     

Interpretation of neutron magnetic scattering in the Kondo lattices YbPd2Si2 and YbAgCu4

We present an interpretation of published neutron inelastic scattering spectra in the Kondo lattices YbPd₂Si₂ and YbAgCu₄ obtained in terms of the Anderson impurity model, describing the hybridisation of the 4f Yb electrons with the band electrons, and also including the crystal electric field interaction. In YbPd₂Si₂, the tetragonal crystal field parameters were determined. In YbAgCu₄ the crystal field interaction was taken to exist by analogy with the isoelectronic compound YbAuCu₄ where it has been identified. Both compounds can be described by a Kondo temperature,T ₀=60 K and a Yb valency very close to 3.     

Magnetocaloric effects in Mn1.35Fe0.65P1-xSix compounds

The structural and magnetocaloric properties of Mn_1.35Fe_0.65P_1-xSi_x compounds are investigated. The Si-substituted compounds, Mn_1.35Fe_0.65P_1-xSi_x with x = 0.52, 0.54, 0.55, 0.56, and 0.57, are prepared by high-energy ball milling and the solid-state reaction. The X-ray diffraction shows that the compounds crystallize into the Fe₂P-type hexagonal structure with space group P62m. The magnetic measurements show that the Curie temperature of the compound increases from 253 K for x = 0.52 to 296 K for x = 0.56. The isothermal magnetic-entropy change of the Mn_1.35Fe_0.65P_1-xSi_x compound decreases with the Si content increasing. The maximal value of the magnetic-entropy change is about 7.0 J/kg稫 in the Mn_1.35Fe_0.65P_0.48Si_0.52 compound with a field change of 1.5 T. The compound quenched in water possesses a larger magnetic entropy change and a smaller thermal hysteresis than the non-quenched samples. The thermal hysteresis of the compound is less than 3.5 K. The maximum adiabatic temperature change is about 1.4 K in the Mn_1.35Fe_0.65P_0.45Si_0.55 compound with a field change of 1.48 T.     

Magnetic properties of RCr2Si2 compounds (R=Tb,Er)

We report on magnetic properties of RCr₂Si₂ compounds with R=Tb, Er. The polycrystalline samples were characterized by powder X-ray diffraction and found to be isostructurally crystallizing in the ThCr₂Si₂-type tetragonal structure. The samples were further investigated by specific heat, AC-susceptibility and magnetization methods in the temperature range 2–900 K and in magnetic fields up to 9 T. The magnetic measurements revealed the magnetic ordering of the rare-earth moments below about 2 K, whilst no high-temperature ordering of the Cr moments was observed. The evidence of for Cr magnetism is corroborated by results of first-principles calculations based on the density functional theory (DFT).     

TmCu2Si2, a two-singlet magnetic system?

New¹⁶⁹Tm Mössbauer and specific heat data recorded for TmCu₂Si₂ and Tm_1/2Lu_1/2Cu₂Si₂ in the temperature range 1.4K to 20K verify that TmCu₂Si₂ orders magnetically at T_N=3K and support earlier conjecture that TmCu₂Si₂ behaves as a 2-singlet system at low temperatures. However attempts to describe the available data in terms of a single set of parameters suggest that the single-ion and molecular field approximations are an oversimplification of the true situation.     

First order magnetic phase transition in tetragonal NpCu2Si2

Magnetization and Np²³⁷ Mössbauer studies of the tetragonal compounds NpM₂Si₂ (M = Cr, Mn, Fe, Co, Ni, Cu) were performed. NpMn₂Si₂ is ferromagnetic. All other compounds order antiferromagnetically. Only in NpCu₂Si₂ the Mössbauer studies reveal a first order magnetic phase transition at T_N = 34 K. It is interpreted in terms of Blume's model, originally developed for cubic UO₂.     

Magnetic properties and structural data of ternary silicides: (RE,Th,U) Os2Si2 (RE= rare earth)

New ternary silicides (RE,Th,U) Os₂Si₂ have been synthesized from the elements. All the compounds (RE= Y,La,Ce,Pr,Nd,Sm,Gd,Tb,Dy,Ho,Er,Tm,Yb, Lu) were found to be isotypic and to crystallize with the ordered BaAl₄-type of structure (ThCr₂Si₂-type). Magnetic properties of these alloys — studied in the temperature range 1.5<T<1100 K — reveal a typical Van Vleck paramagnetism of free RE³⁺ ions at temperatures higher than 300 K. The observed effective paramagnetic moment of CeOs₂Si₂, μ(eff)=0.98 BM, is compatible with a rather low concentration (15%) of Ce³⁺. The effective moment of SmOs₂Si₂, μ(eff)=0.47 BM, is in reasonable agreement with a Hund's rule $\text{J=}\text{5}\text{2}$ ground level for free Sm³⁺. For temperatures above 25 K, the magnetic susceptibility as a function of temperature corresponds to the Van Vleck behavior for free Sm³⁺ (closely spaced multiplet, $\text{J=}\text{5}\text{2}$,$\text{J=}\text{7}\text{2}$. Magnetic ordering temperatures of REOs₂Si₂ silicides are generally below 42 K. (Pr,Nd,Ho,Er,Tm) Os₂Si₂ exhibit ferromagnetic ordering whereas (Sm,Gd, Tb,Dy) Os₂Si₂ show antiferromagnetic behavior. Above 1.8 K none of the samples was found to be superconducting.