Synchrotron-based Nickel Mössbauer Spectroscopy

Leland B. Gee, Chun Yi Lin, Francis E. Jenney, Michael W.W. Adams, Yoshitaka Yoda, Ryo Masuda, Makina Saito, Yasuhiro Kobayashi, Kenji Tamasaku, Michael Lerche, Makoto Seto, Charles G. Riordan, Ann Ploskonka, Philip P. Power, Stephen P. Cramer, Lars Lauterbach

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

We used a novel experimental setup to conduct the first synchrotron-based 61Ni Mössbauer spectroscopy measurements in the energy domain on Ni coordination complexes and metalloproteins. A representative set of samples was chosen to demonstrate the potential of this approach. 61NiCr2O4 was examined as a case with strong Zeeman splittings. Simulations of the spectra yielded an internal magnetic field of 44.6 T, consistent with previous work by the traditional 61Ni Mössbauer approach with a radioactive source. A linear Ni amido complex, 61Ni{N(SiMe3)Dipp}2, where Dipp = C6H3-2,6-iPr2, was chosen as a sample with an "extreme" geometry and large quadrupole splitting. Finally, to demonstrate the feasibility of metalloprotein studies using synchrotron-based 61Ni Mössbauer spectroscopy, we examined the spectra of 61Ni-substituted rubredoxin in reduced and oxidized forms, along with [Et4N]2[61Ni(SPh)4] as a model compound. For each of the above samples, a reasonable spectrum could be obtained in ∼1 d. Given that there is still room for considerable improvement in experimental sensitivity, synchrotron-based 61Ni Mössbauer spectroscopy appears to be a promising alternative to measurements with radioactive sources.

Original languageEnglish
Pages (from-to)6866-6872
Number of pages7
JournalInorganic Chemistry
Volume55
Issue number14
DOIs
Publication statusPublished - 2016 Jul 18

Fingerprint

Nickel
Synchrotrons
Metalloproteins
synchrotrons
nickel
Spectroscopy
Rubredoxins
spectroscopy
Coordination Complexes
rooms
quadrupoles
Magnetic fields
Geometry
geometry
magnetic fields
simulation
energy

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry
  • Inorganic Chemistry

Cite this

Gee, L. B., Lin, C. Y., Jenney, F. E., Adams, M. W. W., Yoda, Y., Masuda, R., ... Lauterbach, L. (2016). Synchrotron-based Nickel Mössbauer Spectroscopy. Inorganic Chemistry, 55(14), 6866-6872. https://doi.org/10.1021/acs.inorgchem.5b03004
Gee, Leland B. ; Lin, Chun Yi ; Jenney, Francis E. ; Adams, Michael W.W. ; Yoda, Yoshitaka ; Masuda, Ryo ; Saito, Makina ; Kobayashi, Yasuhiro ; Tamasaku, Kenji ; Lerche, Michael ; Seto, Makoto ; Riordan, Charles G. ; Ploskonka, Ann ; Power, Philip P. ; Cramer, Stephen P. ; Lauterbach, Lars. / Synchrotron-based Nickel Mössbauer Spectroscopy. In: Inorganic Chemistry. 2016 ; Vol. 55, No. 14. pp. 6866-6872.
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abstract = "We used a novel experimental setup to conduct the first synchrotron-based 61Ni M{\"o}ssbauer spectroscopy measurements in the energy domain on Ni coordination complexes and metalloproteins. A representative set of samples was chosen to demonstrate the potential of this approach. 61NiCr2O4 was examined as a case with strong Zeeman splittings. Simulations of the spectra yielded an internal magnetic field of 44.6 T, consistent with previous work by the traditional 61Ni M{\"o}ssbauer approach with a radioactive source. A linear Ni amido complex, 61Ni{N(SiMe3)Dipp}2, where Dipp = C6H3-2,6-iPr2, was chosen as a sample with an {"}extreme{"} geometry and large quadrupole splitting. Finally, to demonstrate the feasibility of metalloprotein studies using synchrotron-based 61Ni M{\"o}ssbauer spectroscopy, we examined the spectra of 61Ni-substituted rubredoxin in reduced and oxidized forms, along with [Et4N]2[61Ni(SPh)4] as a model compound. For each of the above samples, a reasonable spectrum could be obtained in ∼1 d. Given that there is still room for considerable improvement in experimental sensitivity, synchrotron-based 61Ni M{\"o}ssbauer spectroscopy appears to be a promising alternative to measurements with radioactive sources.",
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Gee, LB, Lin, CY, Jenney, FE, Adams, MWW, Yoda, Y, Masuda, R, Saito, M, Kobayashi, Y, Tamasaku, K, Lerche, M, Seto, M, Riordan, CG, Ploskonka, A, Power, PP, Cramer, SP & Lauterbach, L 2016, 'Synchrotron-based Nickel Mössbauer Spectroscopy', Inorganic Chemistry, vol. 55, no. 14, pp. 6866-6872. https://doi.org/10.1021/acs.inorgchem.5b03004

Synchrotron-based Nickel Mössbauer Spectroscopy. / Gee, Leland B.; Lin, Chun Yi; Jenney, Francis E.; Adams, Michael W.W.; Yoda, Yoshitaka; Masuda, Ryo; Saito, Makina; Kobayashi, Yasuhiro; Tamasaku, Kenji; Lerche, Michael; Seto, Makoto; Riordan, Charles G.; Ploskonka, Ann; Power, Philip P.; Cramer, Stephen P.; Lauterbach, Lars.

In: Inorganic Chemistry, Vol. 55, No. 14, 18.07.2016, p. 6866-6872.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Synchrotron-based Nickel Mössbauer Spectroscopy

AU - Gee, Leland B.

AU - Lin, Chun Yi

AU - Jenney, Francis E.

AU - Adams, Michael W.W.

AU - Yoda, Yoshitaka

AU - Masuda, Ryo

AU - Saito, Makina

AU - Kobayashi, Yasuhiro

AU - Tamasaku, Kenji

AU - Lerche, Michael

AU - Seto, Makoto

AU - Riordan, Charles G.

AU - Ploskonka, Ann

AU - Power, Philip P.

AU - Cramer, Stephen P.

AU - Lauterbach, Lars

PY - 2016/7/18

Y1 - 2016/7/18

N2 - We used a novel experimental setup to conduct the first synchrotron-based 61Ni Mössbauer spectroscopy measurements in the energy domain on Ni coordination complexes and metalloproteins. A representative set of samples was chosen to demonstrate the potential of this approach. 61NiCr2O4 was examined as a case with strong Zeeman splittings. Simulations of the spectra yielded an internal magnetic field of 44.6 T, consistent with previous work by the traditional 61Ni Mössbauer approach with a radioactive source. A linear Ni amido complex, 61Ni{N(SiMe3)Dipp}2, where Dipp = C6H3-2,6-iPr2, was chosen as a sample with an "extreme" geometry and large quadrupole splitting. Finally, to demonstrate the feasibility of metalloprotein studies using synchrotron-based 61Ni Mössbauer spectroscopy, we examined the spectra of 61Ni-substituted rubredoxin in reduced and oxidized forms, along with [Et4N]2[61Ni(SPh)4] as a model compound. For each of the above samples, a reasonable spectrum could be obtained in ∼1 d. Given that there is still room for considerable improvement in experimental sensitivity, synchrotron-based 61Ni Mössbauer spectroscopy appears to be a promising alternative to measurements with radioactive sources.

AB - We used a novel experimental setup to conduct the first synchrotron-based 61Ni Mössbauer spectroscopy measurements in the energy domain on Ni coordination complexes and metalloproteins. A representative set of samples was chosen to demonstrate the potential of this approach. 61NiCr2O4 was examined as a case with strong Zeeman splittings. Simulations of the spectra yielded an internal magnetic field of 44.6 T, consistent with previous work by the traditional 61Ni Mössbauer approach with a radioactive source. A linear Ni amido complex, 61Ni{N(SiMe3)Dipp}2, where Dipp = C6H3-2,6-iPr2, was chosen as a sample with an "extreme" geometry and large quadrupole splitting. Finally, to demonstrate the feasibility of metalloprotein studies using synchrotron-based 61Ni Mössbauer spectroscopy, we examined the spectra of 61Ni-substituted rubredoxin in reduced and oxidized forms, along with [Et4N]2[61Ni(SPh)4] as a model compound. For each of the above samples, a reasonable spectrum could be obtained in ∼1 d. Given that there is still room for considerable improvement in experimental sensitivity, synchrotron-based 61Ni Mössbauer spectroscopy appears to be a promising alternative to measurements with radioactive sources.

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Gee LB, Lin CY, Jenney FE, Adams MWW, Yoda Y, Masuda R et al. Synchrotron-based Nickel Mössbauer Spectroscopy. Inorganic Chemistry. 2016 Jul 18;55(14):6866-6872. https://doi.org/10.1021/acs.inorgchem.5b03004