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Condens. Matter 2019, 4, 86 13 of 15 AuthorContributions: Conceptualizationandmethodology,T.K.,J.K.(JaroslavKohout)andJ.K.(JanKuriplach); measurements and data evaluations, T.K., J.K. (Jaroslav Kohout), M.D., and M.V.; computations and formal analysis, J.Ku.; writing—review and editing, T.K., J.K. (Jaroslav Kohout) and J.K. (Jan Kuriplach). Funding: The support by projects SVV-2017-260442 and NanoCent—Nanomaterials Centre for Advanced Applications, project No. CZ.02.1.01/0.0/0.0/15_003/0000485, financed by ERDF, is gratefully acknowledged. Magnetic experiments were performed in MGML—Materials Growth & Measurement Laboratory (http://www. mgml.eu), which is supported within the program of Czech Research Infrastructures (project No. LM2018096). Jan Kuriplach was partially supported by the Czech Republic’s Ministry of Education, Youth and Sports from the Large Infrastructures for Research, Experimental Development and Innovations project “IT4Innovations National Supercomputing Center—LM2015070”. Acknowledgments: Fruitful discussions with B. Barbiellini are appreciated. The authors gratefully acknowledge K. Záveˇta for his advices and help concerning the interpretation of magnetic measurements. Figures related to the visualization of the LiFePO4 crystal structure were generated using CrystalMaker⃝R . CrystalMaker Software Ltd., Oxford, England (http://www.crystalmaker.com). Conflicts of Interest: The authors declare no conflict of interest. References and Notes 1. Padhi, A.K.; Nanjundaswamy, K.S.; Goodenough, J.B. Phospho-olivines as Positive-Electrode Materials for Rechargeable Lithium Batteries. J. Electrochem. Soc. 1997, 144, 1188–1194. [CrossRef] 2. Mauger, A.; Julien, C.M. Olivine Positive Electrodes for Li-Ion Batteries: Status and Perspectives. Batteries 2018, 4, 39. [CrossRef] 3. Streltsov, V.A.; Belokoneva, E.L.; Tsirelson, V.G.; Hansen, N.K. Multipole analysis of the electron density in triphylite, LiFePO4, using X-ray diffraction data. Acta Cryst. B 1993, 49, 147–153. [CrossRef] 4. Liu, C.; Neale, Z.G.; Cao, G. Understanding electrochemical potentials of cathode materials in rechargeable batteries. Mater. Today 2016, 19, 109–123. [CrossRef] 5. Liu, X.; Wang, Y.J.; Barbiellini, B.; Hafiz, H.; Basak, S.; Liu, J.; Richardson, T.; Shu, G.; Chou, F.; Weng, T.C.; et al. Why LiFePO4 is a safe battery electrode: Coulomb repulsion induced electron-state reshuffling upon lithiation. Phys. Chem. Chem. Phys. 2015, 17, 26369–26377. [CrossRef] [PubMed] 6. Kuriplach, J.; Pulkkinen, A.; Barbiellini, B. First principles study of the impact of grain boundary formation in the cathode material LiFePO4. Condens. Matter 2019, 4, 80. [CrossRef] 7. Lachal, M.; Bouchet, R.; Boulineau, A.; Surblé, S.; Rossignol, C.; Alloin, F.; Obbade, S. Remarkable impact of grains boundaries on the chemical delithiation kinetics of LiFePO4. Solid State Ion. 2017, 300, 187–194. [CrossRef] 8. Jena, A.; Nanda, B.R.K. Unconventional magnetism and band gap formation in LiFePO4: Consequence of polyanion induced non-planarity. Sci. Rep. 2016, 6, 19573. [CrossRef] 9. Santoro, R.P.; Newnham, R.E. Antiferromagnetism in LiFePO4. Acta Cryst. 1967, 22, 344–347. [CrossRef] 10. Rousse, G.; Rodriguez-Carvajal, J.; Patoux, S.; Masquelier, C. Magnetic structures of the triphylite LiFePO4 and of its delithiated form FePO4. Chem. Mater. 2003, 15, 4082–4090. [CrossRef] 11. Li, J.; Garlea, V.O.; Zarestky, J.L.; Vaknin, D. Spin-waves in antiferromagnetic single-crystal LiFePO4. Phys. Rev. B 2006, 73, 024410. [CrossRef] 12. Liang, G.; Park, K.; Li, J.; Benson, R.E.; Vaknin, D.; Markert, J.T.; Croft, M.C. Anisotropy in magnetic properties and electronic structure of single-crystal LiFePO4. Phys. Rev. B 2008, 77, 064414. [CrossRef] 13. Toft-Petersen, R.; Reehuis, M.; Jensen, T.B.S.; Andersen, N.H.; Li, J.; Le, M.D.; Laver, M.; Niedermayer, C.; Klemke, B.; Lefmann, K.; et al. Anomalous magnetic structure and spin dynamics in magnetoelectric LiFePO4. Phys. Rev. B 2015, 92, 024404. [CrossRef] 14. Werner, J.; Sauerland, S.; Koo, C.; Neef, C.; Pollithy, A.; Skourski, Y.; Klingeler, R. High magnetic field phase diagram and failure of the magnetic Grüneisen scaling in LiFePO4. Phys. Rev. B 2019, 99, 214432. [CrossRef] 15. Gütlich, P.; Bill, E.; Trautwein, A.X. Mössbauer Spectroscopy and Transition Metal Chemistry. Fundamentals and Applications; Springer: Berlin/Heidelberg, Germany, 2011. [CrossRef] 16. Van Alboom, A.; De Grave, E.; Wohlfahrt-Mehrens, M. Temperature dependence of the Fe2+ Mössbauer parameters in triphylite (LiFePO4). Am. Mineral. 2011, 96, 408–416. [CrossRef]PDF Image | Mossbauer Spectroscopy of Triphylite (LiFePO4) at Low Temperatures
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