Light-induced spin transition in the spin-crossover complex FePt2 detected by optical pump -coherent resonant nuclear elastic scattering

Abstract

We report the results of optical pump-nuclear resonance probe experiments on the SCO complex [FeII(L-PtII(t-but-tpy))2](BF4)2 with L being 2,6-di(pyrazol-1-yl)-4-(trimethylsilylethynyl)pyridine) and t-but-tpy being 4,4′,4″-Tri-tert-Butyl-2,2′:6′,2″-terpyridine using a novel experimental set-up at the beamline P01, Petra III, DESY Hamburg. We investigate the changes in the spin state of the complex when it is excited by laser pulses of 766 nm wavelength and pulse width < 100 ps. Our simulations of the nuclear forward scattering data indicate a dominant low spin state along with some high spin fraction in the absence of laser pulses. We observe clear changes in the time-spectrum following the instant at which the laser pulse hits the sample. Furthermore, these alterations are recorded as the relative timing of the laser pulses with respect to the synchrotron pulses is varied.

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References

  1. 1.

    Senthil Kumar, K., Ruben, M.: Emerging trends in spin crossover (SCO) based functional materials and devices. Coord. Chem. Rev. 346, 176–205 (2017). https://doi.org/10.1016/j.ccr.2017.03.024

    Article  Google Scholar 

  2. 2.

    Molnár, G., Rat, S., Salmon, L., Nicolazzi, W., Bousseksou, A.: Spin crossover Nanomaterials: from fundamental concepts to devices. Adv. Mater. 30, 1–23 (2018). https://doi.org/10.1002/adma.201703862

    Article  Google Scholar 

  3. 3.

    Wolf, M.M.N., Gross, R., Schumann, C., Wolny, J.A., Schuenemann, V., Dossing, A., Paulsen, H., McGarvey, J.J., Diller, R.: Sub-picosecond time resolved infrared spectroscopy of high-spin state formation in Fe(II) spin crossover complexesw. Phys. Chem. Chem. Phys. 10, 4264–4273 (2008). https://doi.org/10.1039/b802607f

    Article  Google Scholar 

  4. 4.

    Bertoni, R., Lorenc, M., Cailleau, H., Tissot, A., Laisney, J., Boillot, M.-L., Stoleriu, L., Stancu, A., Enachescu, C., Collet, E.: Elastically driven cooperative response of a molecular material impacted by a laser pulse. Nat. Mater. 15, 606–610 (2016). https://doi.org/10.1038/nmat4606

    ADS  Article  Google Scholar 

  5. 5.

    Enachescu, C., Hauser, A., Girerd, J.-J., Boillot, M.-L.: Photoexcitation and relaxation dynamics of Catecholato–Iron(III) spin-crossover complexes. ChemPhysChem. 7, 1127–1135 (2006). https://doi.org/10.1002/cphc.200500671

    Article  Google Scholar 

  6. 6.

    Wolny, J.A., Diller, R., Schünemann, V.: Vibrational spectroscopy of mono- and polynuclear spin-crossover systems. Eur. J. Inorg. Chem. 2635–2648 (2012). https://doi.org/10.1002/ejic.201200059

  7. 7.

    Anastassakis, E.: Selection rules of Raman scattering by optical phonons in strained cubic crystals. J. Appl. Phys. 82, 1582–1591 (1997). https://doi.org/10.1063/1.365958

    ADS  Article  Google Scholar 

  8. 8.

    Röhlsberger, R.: Nuclear condensed matter physics with synchrotron radiation: basic principles, methodology and applications. in: nuclear condensed matter physics with synchrotron radiation: basic principles, methodology and applications. pp. 1–6. Springer-Verlag Berlin, Heidelberger Platz 3, D-14197 Berlin, Germany (2004)

  9. 9.

    Schäfer, B., Bauer, T., Faus, I., Wolny, J.A., Dahms, F., Fuhr, O., Lebedkin, S., Wille, H.C., Schlage, K., Chevalier, K., Rupp, F., Diller, R., Schünemann, V., Kappes, M.M., Ruben, M.: A luminescent Pt 2 Fe spin crossover complex. Dalton Trans. 46, 2289–2302 (2017). https://doi.org/10.1039/c6dt04360g

    Article  Google Scholar 

  10. 10.

    Bauer, T., Omlor, A., Auerbach, H., Jenni, K., Schäfer, B., Diller, R., Ruben, M., Schünemann, V.: Characterization of the light induced excited spin state of a heterometallic FePt2 complex by high-field Mössbauer spectroscopy. Hyperfine Interact. 238, 98–96 (2017). https://doi.org/10.1007/s10751-017-1464-0

    ADS  Article  Google Scholar 

  11. 11.

    Sakshath, S., Jenni, K., Scherthan, L., Würtz, P., Herlitschke, M., Sergeev, I., Strohm, C., Wille, H.C., Röhlsberger, R., Wolny, J.A., Schünemann, V.: Optical pump - nuclear resonance probe experiments on spin crossover complexes. Hyperfine Interact. 238, 1–7 (2017). https://doi.org/10.1007/s10751-017-1461-3

    Article  Google Scholar 

  12. 12.

    Sturhahn, W.: CONUSS and PHOENIX: evaluation of nuclear resonant scattering data. Hyperfine Interact. 125, 149–172 (2000). https://doi.org/10.1023/A:1012681503686

    Article  Google Scholar 

  13. 13.

    Hauser, A.: Excited-state lifetimes of [ Fe ( bipy ) 3 ] 2 + and [ Fe ( phen ). Chem. Phys. Lett. 173, 507–512 (1990)

Download references

Acknowledgements

This work has been supported by the German Ministry of Research (BMBF) under 05K16UKA and by the German Science foundation (DFG) via SFB/TRR 88 3MET and SFB/TRR 173 Spin+X.

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Correspondence to Sakshath Sadashivaiah.

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This article is part of the Topical Collection on Proceedings of the International Conference on the Applications of the Mössbauer Effect (ICAME2019), 1-6 September 2019, Dalian, China

Edited by Tao Zhang, Junhu Wang and Xiaodong Wang

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Sadashivaiah, S., Jenni, K., Scherthan, L. et al. Light-induced spin transition in the spin-crossover complex FePt2 detected by optical pump -coherent resonant nuclear elastic scattering. Hyperfine Interact 241, 3 (2020). https://doi.org/10.1007/s10751-019-1673-9

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Keywords

  • Nuclear forward scattering
  • NRS pump-probe experiments
  • Spin crossover