G.Le Bras*, P.Bonville*,

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Low temperature magnetism in YbPtBi by 70Yb MSssbauer spectroscopy G.Le Bras*, P.Bonville*, P.C.Canfieldt, J.A.Hodges*, P.mbert* * C.E.Saclay, DSMSPEC, 99 GF-SUR-YVETTE France T Ames Laboratory, owa State Univ., owa 500-3020 USA We report on 7'Yb Mossbauer spectroscopy data in the cubic fcc alloy YbPtBi, in the temperature range 0.06-30 K. The zero field spectra show a two component structure above.5 K, which can be analysed as due to 85% of Yb3+ ions at a site with cubic symmetry and 5% at a site with non-cubic symmetry. Below 0.3 K, the spectra are resolved and can also be interpreted in terms of two sites, but with a dominant non-cubic site (- 60%) with Yb ions bearing small magnetic moments. The spectra with a large applied magnetic field give information on the Yb3+ C.E.F. level scheme and on the exchange interaction. The relation of the Mossbauer data with the results of psr measurements is discussed. Keywords: Yb intermetallics, magnetic ordering, imossbauer spectroscopy. Present at ion preference: poster Address or correspondance: Pierre B 0 NVLLE CEA, C.E. Saclay, D RECAM /SPEC 99 GF- SUR-YVETTE France tel: 33 69087437 FAX: 33 69088786 e-mail: bonville@amoco. saclay cea.fr

DSCLAMER Portions of this document may be illegible in electronic image products. mages are produced from the best available original document.

DSCLAMER This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, make any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof.

.,The intermetallic compound YbPtBi, crystallising into a cubic f c c structure (MgAgAs type), has recently attracted much interest due to its intriguing low temperature properties. The specific heat shows a small peak at 0.45 K, attributed to a magnetic transition, and the ratio C / T reaches very high values (8 JK-2mol- at the lowest ternperature) []. Subsequent work tried to unravel the problem of the Yb3+ ground state [2-4. Zero field psr experiments [3] give evidence for the coexistence of spin- glass like and paramagnetic domains in the sample below 0.5 K, in roughly equal proportions; the inferred magnitude of the Yb3+ magnetic moment in the spin-glass domains is 0. pg. n the present work, we report on a Mossbauer spectroscopy study, on the isotope lt0yb(eo=84 kev, g = 0, e=2), of a polycrystalline YbPtBi sample, grown by a Bi flux method, in the temperature range 0.06-30 K, in magnetic fields from 0 to 7 T. The spectrum at 4.2 K in zero field, represented in figure la, shows the presence of two components: a rather broad single line and a split symmetrical spectrum. The single line corresponds to a Yb3+ ion at a cubic site, whereas we interpret the split spectrum as a three line hyperfine quadrupolar spectrum due to a Yb3+ ion at a low symmetry site, with a relative weight of 5(2)%. The quadrupolar moment tensor of the Yb3+ ion at this latter site is such that: Qzz = -Qxx, Q y y = 0, with the rather large value: Qzz N 4. t is striking to observe that the unique Yb site in the isostructural compound YbPdBi has very similar characteristics (figure lb). -2-0 v (cm/s) 2 Figure : Zero field Yb Mossbauer absorption spectra at 4.2 < in YbPtBi (a) and YbPdBi (b). n YbPtBi this low symmetry quadrupolar component is resolved between.5 and 30 <. with a slowly decreasing weight (7% at 30 K). t is rather surprising to find such a low symmetry site in cubic compounds. The regular Yb site in YbPtBi and YbPdBi 2

is the cubic tetrahedral (/4 /4 /4) site; the occurence of a non-axial quadrupolar spectrum means that the Yb ion lies at a strongly distorted site. t is worth noticing that the weight of the low symmetry site above.5 K (- 5%) is the same as that of the fast component observed in the psr spectra of YbPtBi above K [3]. The spectrum at 0.06 K in zero field is shown in figure 2a. A possible interpretation is to assign this spectrum to a magnetic hyperfine interaction, with a hyperfine field of 25 T, corresponding to a spontaneous Yb3+ moment of.25 p ~ An. alternative interpretation, more coherent with that of the 4.2 K spectrum, assigns this spectrum to a superposition of a very broad single line, corresponding to paramagnetic Yb3+ ions at a cubic site, and of a low symmetry quadrupolar spectrum, similar to that at 4.2 K, but with a higher relative weight of -60(5)% and a much broader right-side line. The broadening of this line is compatible with the presence of a distribution of small hyperfine fields of a few 0 T, corresponding to Yb3+ magnetic moments of a few 0. p ~ At. 0.4 K, the weight of this low symmetry component has decreased to -20%. Figure 2: 7 Yb Mossbauer absorption spectra in YbPtBi at 0.06 K in zero field (a) and in a field of 7 T (b). This interpretation strengthens the identification of the sample domains giving rise to the fast psr component with the regions where the Yb ion lies at a non-cubic site: the thermal variation of the size of these domains is very similar in both types of measurements, except around 0.5 < where the psr derived weight is ~ 5 0 % us 20% with Mossbauer spectroscopy. As to t,he cubic spectral component. its large width indicates the presence of Yb3+ paramagnetic fluctuations down to the lowest temperature. The measured Yb3+ fluctuation frequency l/tl is constant and equal to 2 GHz below <. n terms of single ion Kondo fluctuations, this gives the small Kondo temperature: 3

kbto - K. The spectra at 0.06 and 4.2 K in high magnetic field ( H 2.5 T) are characteristic h/ti 2 0. of a Yb3f ion having a low lying 's quartet, with line broadenings showing the presence of sizeable axial distortions of the Yb cubic site. They consist of two lines (figure 2b), expected when the magnetic moment, hence the hyperfine field, is parallel to the applied field. n these high field spectra, there is no hint of the presence of Yb ions at a non-cubic site whereas at low fields (0.5 and T) at 4.2 K the low symmetry spectral component is present. At 0.06 K the spectra for 0.4 and T show five lines, which is characteristic of a cubic Yb3+ ion in the presence of an antiferromagnetic (AF) exchange interaction, when the applied field is too small to align the magnetic moments along its direction. As alignment occurs for Ha =.5 T,the exchange field magnitude is Hex Ha/2 = 0.75 - T. The magnetisation curve at 0.35 <, taken from ref.2, together with the Mossbauer derived magnetic moment values at 0.06 and 4.2 K, are represented in figure 3. 3.0 2.5 c 2.0 5.5 E.0 0.5 e // 0 -----calc. 4 2 H (T T=4.2K 6 Figure3: Magnetisation (from ref.2) and Mossbauer derived moment values as a function of magnetic field in YbPtBi. When the magnetic moments are not aligned along the external field direction, the Mossbauer technique yields the magnitude of the moment, whereas the magnetisation data yields its projection onto the field direction. The Mossbauer derived moment values at 0.06 < interpolate smoothly with the magnetisation data at 0.35 K for a field of.5 T, confirming that the alignment of the A F structure along the field direction occurs for this field value. The moment value extrapolated to zero field at 0.06 < is mo N.4,UB which is the expected value for the spontaneous moment of a r6 C.E.F. ground state. Then the exchange energy scale is: E e x = mohex 0.7 K, which is close to - 4

TN = 0.45 <, and the (assumed isotropic) molecular field constant: X N -0.4 T / ~ B. Using the above information, we tried to derive the cubic C.E.F. level scheme of the Yb3+ ion from the magnetisation curves. The solid and dashed lines in fig.3, as well as B the following the theoretical spectrum in fig.zb, are calculated using X = -0.3 T / ~ and level scheme: r s ground state, r8 at 6 K and '7 at 75 K. The agreement is satisfatory and the derived C.E.F. scheme agrees qualitatively with the inelastic neutron scattering data 5. To summarise, the ioyb Mossbauer spectroscopy data in YbPtBi show the presence of two kinds of Yb sites: a cubic site and a low symmetry site, probably distributed in domains. The occurence of the low symmetry Yb environment could be due to a Jahn-Teller distortion, linked to the presence of a low lying 'g state; in the isostructural compound YbPdBi, the "OYb Mossbauer data have shown that all the Yb sites are of the low symmetry type. n YbPtBi. the importance of the distorted site domains is strongly diminished by increasing temperature or magnetic field, suggesting that this compound is at the verge of a Jahn-Teller instability. Below 0.3 K, the Mossbauer data can be interpreted in a way that confirms and extends the psr results: 60% of the Yb ions are at the low symmetry site and bear small magnetic moments (<0.5 p g ), whereas the Yb ions at the cubic sites remain paramagnetic down to 0.06 K and fluctuate with a frequency 2 GHz. The Mossbauer data with a magnetic field could give an estimation for the exchange energy scale (0.7 K) and for the A F molecular field constant (-0.3 TCLB). Ames Laboratory is operated for the U.S. DOE by owa State University under Contract No. W-7405-Eng-82. This work was supported by the-director for Energy Research, Officeof Basic Energy Science. REFERENCES. Z.Fisk e t al, Phys.Rev. 67 (99) 330 2. J.D.Thompson e t al, Physica B86-88 (993) 355 3. A.Amato e t al, Phys.Rev. B46 (992) 35 4. P.C.Canfield e t al, Physica B97 (994) 0 5. R.A.Robinson et al, Physica B86-88 (993) 550 DSCLAMER This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any leg& liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or p m s disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof.