A comparison between high-symmetry Mn12 single-molecule magnets in different ligand/solvent environments

作者: S. Hill , N. Anderson , A. Wilson , S. Takahashi , K. Petukhov

DOI: 10.1016/J.POLY.2005.03.079

关键词: ChemistryCrystallographyMoleculeNanomagnetElectron paramagnetic resonanceComputational chemistryDeuteriumSpin (physics)Resolution (electron density)LigandSpectral line

摘要: Abstract We present angle-resolved high-frequency electron paramagnetic resonance (HFEPR) data collected for single-crystal samples of deuterated and undeuterated Mn12-acetate. The spectra reveal fine structures associated with the various Mn12 species corresponding to different local solvent environments proposed by Cornia et al. [A. Cornia, R. Sessoli, L. Sorace, D. Gatteschi, A.L. Barra, C. Daiguebonne, Phys. Rev. Lett. 89 (2002) 257201], recently confirmed Hill [S. Hill, R.S. Edwards, S.I. Jones, J.M. North, N.S. Dalal, 90 (2003) 217204] del Barco [E. Barco, A.D. Kent, E.M. Rumberger, D.N. Hendrickson, G. Christou, 91 047203]. Each exhibits a distinct dependence on applied field orientation, thereby highlighting discrete nature disorder. then compare these obtained two discovered high-symmetry (S4) analogs Mn12-Ac, differing only in their ligand structures. None highly reproducible fine-structures seen Mn12-Ac are found new complexes, thus confirming idea that structure significantly influences QMT dynamics Mn12-Ac. Indeed, HFEPR Mn12-BrAc Mn12-tBuAc provide spectacular resolution, allowing unique spectroscopic insights into giant spin SMMs.

参考文章(27)
S. Hill, S. Maccagnano, Kyungwha Park, R. M. Achey, J. M. North, N. S. Dalal, Detailed single-crystal EPR line shape measurements for the single-molecule magnetsFe8BrandMn12−acetate Physical Review B. ,vol. 65, pp. 224410- ,(2002) , 10.1103/PHYSREVB.65.224410
S. Takahashi, R. S. Edwards, J. M. North, S. Hill, N. S. Dalal, Discrete easy-axis tilting in Mn12-acetate, as determined by EPR: implications for the magnetic quantum tunneling mechanism Physical Review B. ,vol. 70, pp. 094429- ,(2004) , 10.1103/PHYSREVB.70.094429
Jonathan R. Friedman, M. P. Sarachik, J. Tejada, R. Ziolo, MACROSCOPIC MEASUREMENT OF RESONANT MAGNETIZATION TUNNELING IN HIGH-SPIN MOLECULES Physical Review Letters. ,vol. 76, pp. 3830- 3833 ,(1996) , 10.1103/PHYSREVLETT.76.3830
Mònica Soler, Wolfgang Wernsdorfer, Ziming Sun, John C. Huffman, David N. Hendrickson, George Christou, Single-molecule magnets: control by a single solvent molecule of Jahn–Teller isomerism in [Mn12O12(O2CCH2But)16(H2O)4] Chemical Communications. pp. 2672- 2673 ,(2003) , 10.1039/B306246E
S. Hill, J. A. A. J. Perenboom, N. S. Dalal, T. Hathaway, T. Stalcup, J. S. Brooks, High-sensitivity electron paramagnetic resonance of Mn-12-acetate Physical Review Letters. ,vol. 80, pp. 2453- 2456 ,(1998) , 10.1103/PHYSREVLETT.80.2453
Claus JH Jacobsen, Erik Pedersen, Joergen Villadsen, Hoegni Weihe, None, ESR characterization of trans-diacidatotetrakis(pyridine)vanadium and -manganese trans-VII(py)4X2 and trans-MnII(py)4X2 (X = NCS, Cl, Br, I; py = pyridine) Inorganic Chemistry. ,vol. 32, pp. 1216- 1221 ,(1993) , 10.1021/IC00059A031
Hui-Lien Tsai, Da-Min Chen, Chen-I Yang, Tyn-Yih Jwo, Ching-Shuei Wur, Gene-Hsiang Lee, Yu Wang, A single-molecular magnet: [Mn12O12(O2CCH2Br)16(H2O)4] Inorganic Chemistry Communications. ,vol. 4, pp. 511- 514 ,(2001) , 10.1016/S1387-7003(01)00265-9
Joel S. Miller, Arthur J. Epstein, Molecule-Based Magnets—An Overview Mrs Bulletin. ,vol. 25, pp. 21- 30 ,(2000) , 10.1557/MRS2000.221
E. del Barco, A. D. Kent, E. M. Rumberger, D. N. Hendrickson, G. Christou, Symmetry of magnetic quantum tunneling in single molecule magnet Mn12-acetate. Physical Review Letters. ,vol. 91, pp. 047203- ,(2003) , 10.1103/PHYSREVLETT.91.047203
W. Wernsdorfer, N. E. Chakov, G. Christou, Determination of the magnetic anisotropy axes of single-molecule magnets Physical Review B. ,vol. 70, pp. 132413- ,(2004) , 10.1103/PHYSREVB.70.132413