Skip to main content
SpringerLink
Log in

Sm valence determination of Sm-based Intermetallics using 149Sm Mössbauer and Sm LIII-edge X-ray absorption spectroscopies

  • Published:
Hyperfine Interactions Aims and scope Submit manuscript

Abstract

149Sm synchrotron-radiation-based Mössbauer spectroscopy was performed in Sm-based intermetallics having a cubic crystal structure, Sm3Tr4Ge13, SmB6, SmBe13, and SmTr2Al20 (Tr = transition metals). In spite of the difference of the local structure around the Sm sites, the observed Mössbauer spectra consist of a single line at 300 K. On the other hand, Sm LIII-edge X-ray absorption spectra consist of two components, suggesting Sm2+ and Sm3+ states. Difference of the number of the spectral components between the Mössbauer spectroscopy and X-ray absorption spectroscopy is caused by the difference of the time window in the scattering process of these measurements. Correlation between the isomer shifts in the Mössbauer spectroscopy and average Sm valence states estimated from the X-ray absorption spectroscopy exhibits a linear correlation.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Similar content being viewed by others

References

  1. Sanada, S., Aoki, Y., Aoki, H., Tsuchiya, A., Kikuchi, D., Sugawara, H., Sato, H.: Exotic heavy-fermion state in filled Skutterudite SmOs4Sb12. J. Phys. Soc. Jpn. 74, 246 (2005)

    Article  ADS  Google Scholar 

  2. Higashinaka, R., Maruyama, T., Nakama, A., Miyazaki, R., Aoki, Y., Sato, H.: Unusual field-insensitive phase transition and Kondo behavior in SmTi2Al20. J. Phys. Soc. Jpn. 80, 093703 (2011)

    Article  ADS  Google Scholar 

  3. Sakai, A., Nakatsuji, S.: Strong valence fluctuation effects in SmTr2Al20 (Tr = Ti, V, Cr). Phys. Rev. B. 84, 201106 (2011)

    Article  ADS  Google Scholar 

  4. Fushiya, K., Matsuda, T.D., Higashinaka, R., Akiyama, K., Aoki, Y.: Possible existence of partially disordered SmIons in magnetically ordered state of Ising magnet SmPt2Si2: a single crystal study. J. Phys. Soc. Jpn. 83, 113708 (2014)

    Article  ADS  Google Scholar 

  5. Higashinaka, R., Matsuda, T.D., Aoki, Y.: Relationship between specific heat, valence and effective magnetic moment of Sm ions in strongly correlated Sm compounds. AIP Adv. 8, 125017 (2018)

    Article  ADS  Google Scholar 

  6. Kemly, E., Croft, M., Murgai, V., Gupta, L.C., Godart, C., Parks, R.D., Segre, C.U.: Mössbauer effects and LIII absorption measurements on EuPd2Si2. J. Magn. Magn. Mater. 47-48, 403 (1985)

    Article  ADS  Google Scholar 

  7. Wortmann, G., Frank, K.H., Sampathkumaran, E.V., Perscheid, B., Schmiester, G., Kaindl, G.: Combined Mössbauer and LIII-edge X-ray absorption study of mixed-valent EuPd2Si2 and EuNi2P2. J. Magn. Magn. Mater. 49, 325 (1985)

    Article  ADS  Google Scholar 

  8. Wortmann, G., Nowik, I., Perscheid, B., Kaindl, G., Felner, I.: Critical evaluation of Eu valences from LIII-edge x-ray-absorption and Mössbauer spectroscopy of EuNi2Si2-xGex. Phys. Rev. B. 43, 5261 (1991)

    Article  ADS  Google Scholar 

  9. Mitsuda, A., Wada, H., Shiga, M., Tanaka, T.: The Eu valence state and valence transition in Eu(Pd1-xPtx)2Si2. J. Phys. Condens. Matter. 12, 5287 (2000)

    Article  ADS  Google Scholar 

  10. Bonville, P., Godart, C., Alleno, E., Takahashi, F., Matsuoka, E., Ishikawa, M.: Heterogeneous mixed valence in YbPd3S4: evidence from 170Yb Mössbauer and x-ray LIII-edge absorption measurements. J. Phys. Condens. Matter. 17, L263 (2003)

    Article  Google Scholar 

  11. Bauminger, E.R., Froindlich, D., Nowik, I., Ofer, S., Felner, I., Mayer, I.: Charge fluctuations in europium in metallic EuCu2Si2. Phys. Rev. Lett. 30, 1053 (1973)

    Article  ADS  Google Scholar 

  12. Abd-Elmeguid, M.M., Sauer, C., Zinn, W.: On the problem of the valence determination of Eu in mixed-valence compounds EuCu2Si2 and EuPd2Si2. J. Phys. C: Solid State Physics. 18, 345 (1985)

    Article  ADS  Google Scholar 

  13. Scherzberg, A., Sauer, C., Abd-Elmeguid, M.M., Zinn, W.: Anomaly of the quadrupole interaction in mixed EuPd2Si2. Phys. Rev. B. 31, 106 (1985)

    Article  ADS  Google Scholar 

  14. Hastings, J.B., Siddons, D.P., van Bürck, U., Hollatz, R., Bergmann, U.: Mössbauer spectroscopy using synchrotron radiation. Phys. Rev. Lett. 66, 770 (1991)

    Article  ADS  Google Scholar 

  15. Seto, M., Masuda, R., Higashitaniguchi, S., Kitao, S., Kobayashi, Y., Inaba, C., Mitsui, T., Yoda, Y.: Synchrotron-radiation-based Mössbauer spectroscopy. Phys. Rev. Lett. 102, 217602 (2009)

    Article  ADS  Google Scholar 

  16. Tsutsui, S., Hanate, H., Yoda, Y., Matsuhira, K., Application of Dynchrotron-radiation-based Mössbauer spectroscopy to 193Ir 73 keV transition. Hyperfine Interact. in this issue in press

  17. Tsutsui, S., Masuda, R., Kobayashi, Y., Yoda, Y., Mizuuchi, K., Shimizu, Y., Hidaka, H., Yanagisawa, T., Amitsuka, H., Iga, F., Seto, M.: Synchrotron radiation Mössbauer spectroscopy using 149Sm nuclei. J. Phys. Soc. Jpn. 85, 083704 (2016)

    Article  ADS  Google Scholar 

  18. Tsutsui, S., Kobayashi, Y., Nakamura, J., Kubo, M.K., Amagasa, S., Yamada, Y., Yoda, Y., Shimizu, Y., Hidaka, H., Yanagisawa, T., Amitsuka, H., Yamada, A., Higashinaka, R., Matsuda, T.D., Aoki, Y.: Sm valence states and magnetic properties in SmBe13 and SmTi2Al20 investigated by Sm synchrotron-radiation-based Mössbauer spectroscopy. Hyperfine Interact. 238, 100 (2017)

    Article  ADS  Google Scholar 

  19. Tsutsui, S., Masuda, R., Yoda, Y., Seto, M.: Precise determination of hyperfine interactions and second-order Doppler shift in 149Sm Mössbauer transition. Hyperfine Interact. 239, 50 (2018)

    Article  ADS  Google Scholar 

  20. Tsutsui, S., Mizumaki, M., Kobayashi, Y.: Electronic and atomic dynamics in Sm and Eu cage-structured intermetallics. Hyperfine Interact. 240, 84 (2019)

    Article  ADS  Google Scholar 

  21. Cohen, R.L., Eibschütz, M., West, K.W.: Electronic and magnetic structure of SmB6. Phys. Rev. Lett. 24, 283 (1970)

    Article  ADS  Google Scholar 

  22. Cohen, R.L., Eibschütz, M., West, K.W., Buehler, E.: Electronic configuration of SmB6. J. Appl. Phys. 41, 898 (1970)

    Article  ADS  Google Scholar 

  23. Eibschütz, M., Cohen, R.L., Buehler, E., Wernick, J.H.: Mössbauer isomer shifts in Sm149 compounds. Phys. Rev. B. 6, 18 (1972)

    Article  ADS  Google Scholar 

  24. Nair, H.S.: Ramesh Kumar K., Douglas Britzm Sarit K. Ghosh, Chriestian Reinke, André M. Strydom, field-insensitive heavy fermion features and phase transition in the caged-structure quasi-skutterudite Sm3Ru4Ge13. J. Alloys Compd. 669(254), (2016)

  25. Goh, S.K., Tompsett, D.A., Saines, P.J., Chang, H.C., Matsumoto, T., Imai, M., Yoshimura, K., Grosche, F.M.: Ambient pressure structural quantum critical point in the phase diagram of (CaxSr1-x)3Rh4Sn13. Phys. Rev. Lett. 114, 097002 (2015)

    Article  ADS  Google Scholar 

  26. Yu, W.C., Cheung, Y.W., Saines, P.J., Imai, M., Matsumoto, T., Michioka, C., Yoshimura, K., Goh, S.K.: Strong coupling superconductivity in the vicinity of the structural quantum critical point in (CaxSr1-x)3Rh4Sn13. Phys. Rev. Lett. 115, 207003 (2015)

    Article  ADS  Google Scholar 

  27. Cheung, Y. W., Hu, Y. J., Goh, S. K., Kaneko, K., Tsutsui, S., Logg, P. W., Grousch, F. M., Kanagawa, H., Tanioku, Y., Imai, M., Matsumoto, T., and Yoshimura, K., Second-order Structural Transition in(Ca0.5Sr0.5)3Rh4Sn13, J. Phys. Conf. Ser. 807, 032002 (2017)

  28. Cheung, Y.W., Hu, Y.J., Imai, M., Tanioku, Y., Kanagawa, H., Murakawa, J., Moriyama, K., Zhang, W., Lai, K.T., Yoshimura, K., Grosche, F.M., Kaneko, K., Tsutsui, S., Goh, S.K.: Evidence of a structural quantum critical point in (CaxSr1-x)3Rh4Sn13. Phys. Rev. B. 98, 161103 (2018)

    Article  ADS  Google Scholar 

  29. Kaneko, K., Cheung, Y.W., Hu, Y., Imai, M., Tanioku, Y., Kanagawa, H., Murakawa, J., Moriyama, K., Zhang, W., Lai, K.T., Matsuda, M., Yoshimura, K., Tsutsui, S., Goh, S.K.: Nature of structural instabilities in superconducting Sr3Ir4Sn13. JPS Conf. Proc. 30, 011032 (2020)

    Google Scholar 

  30. Higashinaka, R., Private Communication

  31. Yoda, Y., Yabashi, M., Izumi, K., Zhang, X. W., Kishimoto, S., Kitao, S., Seto, M., Mitsui, T., Harami, T., Imai, Y., and Kikuta, S., Nuclear resonant scattering beamline at SPring-8, Nucl. Instrum. Methods Phys. Res., Sect. A 467–468, 715 (2001)

  32. Tsutsui, S., Shimomura, S., Yoda, Y., Kobayashi, H., Onodera, H.: Sm atomic dynamics in a charge density wave compound SmNiC2. Hyperfine Interact. 226, 637 (2014)

    Article  ADS  Google Scholar 

  33. Sergueev, I., Wille, H.-C., Hermann, R.P., Bessas, D., Shvyd’ko, Y.V., Zajac, M., Rüffer, R.: Milli-electronvolt monochromatization of hard x-rays with sapphire backscattering monochromator. J. Synchrotron Rad. 18, 802 (2011)

    Article  Google Scholar 

  34. Inoyatov, A. K., Filosofov, D. V., Gorozhankin, V. M., Kovalik, A., Adam, I., Perevoshchikov, L. L., Rysavy, M., Improved characteristics of the 22.5 keV (M1+E2) nuclear transition in 149Sm, Eur. Phys. J. A 47, 64 (2011)

  35. Greenwood, N.N., Gibb, T.C.: Mössbauer Spectroscopy. Chapman and Hall, London (1971)

    Book  Google Scholar 

  36. Kitao, S., Mitsui, T., Seto, M.: Nuclear resonant scattering of synchrotron radiation by 121Sb nd 149Sm. J. Phys. Soc. Jpn. 69, 683 (2000)

    Article  ADS  Google Scholar 

  37. Uruga, T., Tanida, H., Yoneda, Y., Takeshita, K., Emura, S., Takahashi, M., Harada, M., Nishihata, Y., Kubozono, Y., Tanaka, T., Yamamoto, T., Maeda, H., Kamishima, O., Takabayashi, Y., Nakata, Y., Kimura, H., Goto, S., Ishikawa, T.: The XAFS beamline BL01B1 at SPring-8. J. Synchrotron Radiat. 6, 143 (1999)

    Article  Google Scholar 

  38. Mizumaki, M., Tsutsui, S., Tanida, H., Uruga, T., Kikuchi, D., Sugawara, H., Sato, H.: The mixed valence states in the unconventional heavy fermion compound SmOs4Sb12. J. Phys. Soc. Jpn. 76, 053706 (2007)

    Article  ADS  Google Scholar 

  39. Mizumaki, M., Tsutsui, S., Iga, F.: Temperature dependence of Sm valence in SmB6 studied by X-ray absorption spectroscopy. J. Phys. Conf. Ser. 176, 012034 (2009)

    Article  Google Scholar 

  40. Blume, M., Tjon, J.A.: Mössbauer spectra in a fluctuating environment. Phys. Rev. 165, 446 (1968)

    Article  ADS  Google Scholar 

  41. Keski-Rahkonen, O., Krause, M.O.: Total and partial atomic-level width. At. Data Nucl. Data Tables. 14, 139 (1974)

    Article  ADS  Google Scholar 

  42. Shiina, R., Kuniyoshi, S.: Effect of magnetic field on quantum phase transition and heavy fermion state in two-orbital impurity Anderson model. J. Phys. Soc. Jpn. 90, 074708 (2021)

    Article  ADS  Google Scholar 

Download references

Acknowledgements

Synchrotron radiation experiments of 149Sm SR-based Mössbauer spectroscopy and Sm LIII-edge XAS were performed under the approval of JASRI (Proposal Nos. 2007B1351, 2012B1538, 2014B1139, 2015B1947, 2016A1413, 2017A1060, 2017B1275, 2018A1534, 2018B2038, 2019A1226, 2020A1346, 2020A2025, 2020A2131, and 2021A2052). This work is financially supported by JSPS KAKENHI (Grant Nos. JP20102005 (HeavyElectron), JP21H00157 (High-Entropy Alloy), JP15K14170, JP15H03697, 15K05178, 15H05884, 16K05454, 24740239, JP19H01839 and JP19H04408).

Author information

Authors and Affiliations

  1. Japan Synchrotron Radiation Research Institute (JASRI), SPring-8, Sayo, Hyogo, 679-5198, Japan

    Satoshi Tsutsui, Kosuke Fujiwara, Yoshitaka Yoda, Kazuo Kato, Kiyofumi Nitta, Naomi Kawamura & Masaichiro Mizumaki

  2. Institute of Quantum Beam Science, Graduate School of Science and Engineering, Ibaraki University, Hitachi, Ibaraki, 316-8511, Japan

    Satoshi Tsutsui

  3. Department of Physics, Tokyo Metropolitan University, Hachioji, Tokyo, 192-0397, Japan

    Ryuji Higashinaka, Tatsuma D. Matsuda & Yuji Aoki

  4. The University of Electro-Communications, Chofu, Tokyo, 182-8585, Japan

    Raito Nakamura, Jin Nakamura & Yoshio Kobayashi

  5. Nishina Center for Accelerator Based Science, RIKEN, Wako, Saitama, 351-0198, Japan

    Yoshio Kobayashi

  6. Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki, 319-1195, Japan

    Takashi U. Ito

Authors
  1. Satoshi Tsutsui
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Ryuji Higashinaka
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Raito Nakamura
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Kosuke Fujiwara
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Jin Nakamura
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Yoshio Kobayashi
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Takashi U. Ito
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Yoshitaka Yoda
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Kazuo Kato
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Kiyofumi Nitta
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Naomi Kawamura
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. Masaichiro Mizumaki
    View author publications

    You can also search for this author in PubMed Google Scholar

  13. Tatsuma D. Matsuda
    View author publications

    You can also search for this author in PubMed Google Scholar

  14. Yuji Aoki
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Satoshi Tsutsui.

Additional information

Publisher’s note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

This article is part of the Topical Collection on Proceedings of the International Conference on the Applications of the Mössbauer Effect (ICAME 2021), 5-10 September 2021, Brasov, Romania

Edited by Victor Kuncser

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Tsutsui, S., Higashinaka, R., Nakamura, R. et al. Sm valence determination of Sm-based Intermetallics using 149Sm Mössbauer and Sm LIII-edge X-ray absorption spectroscopies. Hyperfine Interact 242, 32 (2021). https://doi.org/10.1007/s10751-021-01759-x

Download citation

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s10751-021-01759-x

Keywords

Search

Navigation