Suppression of Magnetic Quantum Tunneling in a Chiral Single Molecule Magnet by Ferromagnetic Interactions

Lippert K-A, Mukherjee C, Broschinski J-P, Lippert Y, Walleck S, Stammler A, Boege H, Schnack J, Glaser T (2017)
INORGANIC CHEMISTRY 56(24): 15119-15129.

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Abstract / Notes
Single-molecule magnets (SMMs) retain a magnetization without applied magnetic field for a decent time due to an energy barrier U for spin-reversal. Despite the success to increase U, the difficult to control magnetic quantum tunneling often leads to a decreased effective barrier U-eff and a fast relaxation. Here, we demonstrate the influence of the exchange coupling on the tunneling probability in two heptanuclear SMMs hosting the same spin-system with the same high spin ground state S-t = 21/2. A chirality-induced symmetry reduction leads to a switch of the Mn-III-Mn-III exchange from antiferromagnetic in the achiral SMM [(Mn6CrIII)-Cr-III](3+) to ferromagnetic in the new chiral SMM (RR)[(Mn6CrIII)-Cr-III](3+). Multispin Hamiltonian analysis by full-matrix i diagonalization demonstrates that the ferromagnetic interactions in (RR)[(Mn6CrIII)-Cr-III](3+) enforce a well-defined S, = 21/2 ground state with substantially less mixing of Ms substates in contrast to [(Mn6CrIII)-Cr-III](3+)and no tunneling pathways below the top of the energy barrier. This is experimentally verified as U-eff is smaller than the calculated energy barrier U in [114.n1116Cr1193 due to tunneling pathways, whereas U-eff equals U in (RR)[(Mn6CrIII)-Cr-III](3+) demonstrating the absence of quantum tunneling.
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Lippert K-A, Mukherjee C, Broschinski J-P, et al. Suppression of Magnetic Quantum Tunneling in a Chiral Single Molecule Magnet by Ferromagnetic Interactions. INORGANIC CHEMISTRY. 2017;56(24):15119-15129.
Lippert, K. - A., Mukherjee, C., Broschinski, J. - P., Lippert, Y., Walleck, S., Stammler, A., Boege, H., et al. (2017). Suppression of Magnetic Quantum Tunneling in a Chiral Single Molecule Magnet by Ferromagnetic Interactions. INORGANIC CHEMISTRY, 56(24), 15119-15129. doi:10.1021/acs.inorgchem.7b02453
Lippert, K. - A., Mukherjee, C., Broschinski, J. - P., Lippert, Y., Walleck, S., Stammler, A., Boege, H., Schnack, J., and Glaser, T. (2017). Suppression of Magnetic Quantum Tunneling in a Chiral Single Molecule Magnet by Ferromagnetic Interactions. INORGANIC CHEMISTRY 56, 15119-15129.
Lippert, K.-A., et al., 2017. Suppression of Magnetic Quantum Tunneling in a Chiral Single Molecule Magnet by Ferromagnetic Interactions. INORGANIC CHEMISTRY, 56(24), p 15119-15129.
K.-A. Lippert, et al., “Suppression of Magnetic Quantum Tunneling in a Chiral Single Molecule Magnet by Ferromagnetic Interactions”, INORGANIC CHEMISTRY, vol. 56, 2017, pp. 15119-15129.
Lippert, K.-A., Mukherjee, C., Broschinski, J.-P., Lippert, Y., Walleck, S., Stammler, A., Boege, H., Schnack, J., Glaser, T.: Suppression of Magnetic Quantum Tunneling in a Chiral Single Molecule Magnet by Ferromagnetic Interactions. INORGANIC CHEMISTRY. 56, 15119-15129 (2017).
Lippert, Kai-Alexander, Mukherjee, Chandan, Broschinski, Jan-Philipp, Lippert, Yvonne, Walleck, Stephan, Stammler, Anja, Boege, Hartmut, Schnack, Jürgen, and Glaser, Thorsten. “Suppression of Magnetic Quantum Tunneling in a Chiral Single Molecule Magnet by Ferromagnetic Interactions”. INORGANIC CHEMISTRY 56.24 (2017): 15119-15129.
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