13.07.2015 Views

Mise en page 1 - Laboratoire National des Champs Magnétiques ...

Mise en page 1 - Laboratoire National des Champs Magnétiques ...

Mise en page 1 - Laboratoire National des Champs Magnétiques ...

SHOW MORE
SHOW LESS

Create successful ePaper yourself

Turn your PDF publications into a flip-book with our unique Google optimized e-Paper software.

2009 MAGNETIC SYSTEMSHigh field torque magnetometry on a molecular Dysprosium triangleLanthanide based molecular nanomagnets have be<strong>en</strong> attractingconsiderable att<strong>en</strong>tion due to their interesting magneticproperties. Mononuclear complexes of 4f ions haveshown slow relaxation of the magnetization at very hightemperatures compared to those observed in transition metals.Despite their out of phase ac signal observed above 40K, hysteresis curves were observed only at very low temperatures[Ishikawa et al., Angew. Chem. 117, 2991 (2005)].On cooling, deviations from the Arrh<strong>en</strong>ius law predictedfor single molecule magnet behavior become more important,which indicates that tunnelling plays a crucial role inthe relaxation of the magnetization. It is therefore of crucialimportance to obtain information on the low lying sublevelsof the 4f electronic systems, in order to understand the magnetism,and especially the relaxation mechanisms of thesecompounds.We have performed high field torque magnetometry measurem<strong>en</strong>tson the rec<strong>en</strong>tly investigated molecular Dy triangle[Luzon et al., Phys. Rev. Lett. 100 247205(2008)]. This compound shows an unpreced<strong>en</strong>ted magneticbehaviour having a non-magnetic ground doublet whichoriginates from the noncollinearity of the single-ion easyaxes of the Dy 3+ ions that lie in the plane of the triangleat 120 ◦ one from each other. This gives rise to a peculiarchiral nature of the ground nonmagnetic doublet and toslow relaxation of the magnetization which exhibits abruptaccelerations at the crossings of the discrete <strong>en</strong>ergy levels.The ground (|J = 15/2,m J = ±15/2〉) and the first excited(|J = 15/2,m J = ±13/2〉) doublets, were considered to <strong>des</strong>cribethe <strong>en</strong>ergy levels of the single ion assuming that theother excited states are very high in <strong>en</strong>ergy and do not contributeto the magnetic properties at low temperatures. Thesystem therefore mimics the behaviour of an S=3/2 spin.We have used the spin Hamiltonian approach to <strong>des</strong>cribethe low lying <strong>en</strong>ergy levels. The expression of the Hamiltonianused is,anisotropy in the system. The performed high field torquemeasurem<strong>en</strong>ts at 50 mK <strong>en</strong>abled us to quantify the crystalfield splitting betwe<strong>en</strong> the 15/2 and the 13/2 doubletsin Dy 3+ . Figure 109 (a) shows the measured torque signalat 50 mK up to 32 Tesla for the magnetic field applied atdiffer<strong>en</strong>t angles to the plane of the triangle. A peak in thetorque is evid<strong>en</strong>t at around 28 Tesla. Figure 109 (b) showsthe calculated torque signals for δ = 250 cm −1 , j = 0.064cm −1 , and g = 1.35 at 50 mK, which reproduce fairly wellthe experim<strong>en</strong>tally observed curves. The observed peak inthe torque signal at around 28 Tesla for transverse magneticfields points towards the high anisotropy in the system. Thecrystal field splitting of δ = 250 ± 10 cm −1 is close to thatexpected from previously performed ab initio calculations[Chibotaru et al., Angew. Chem. Int. Ed. 47, 4126 (2008)].In a more g<strong>en</strong>eral picture, this study has contributed to abetter understanding of lanthanide based systems. In particular,we have prov<strong>en</strong> that high field torque magnetometrycan be a good substitute to spectroscopy in systems whichare spectroscopically inactive.Ĥ = − j(Ŝ 1 · Ŝ 2 + Ŝ 2 · Ŝ 3 + Ŝ 3 · Ŝ 1 )− gµ B ∑ B · Ŝ i + δ oi=1,314 ∑ (( 15i=1,32 )2 − Ŝ 2 z i)(16)The first term is the isotropic exchange betwe<strong>en</strong> the Dy 3+ions, the second is the Zeeman term, and the last term<strong>des</strong>cribes the single-ion anisotropy where δ o is the zerofield splitting betwe<strong>en</strong> |J = 15/2,m J = ±15/2〉 and |J =15/2,m J = ±13/2〉 states of each Dy 3+ ion. We have particularychos<strong>en</strong> torque magnetometry as it is a strong tool toinvestigate the anisotropy in high-spin clusters, especiallyin systems which are not accessible by spectroscopy. Apeak in the torque signal occurs at a characteristic fieldwhich dep<strong>en</strong>ds on the temperature as well as the magneticFigure 109: (a) Torque signals for the magnetic field applied atdiffer<strong>en</strong>t angles close to 90 ◦ from the plane of the triangle at 50mK. (b) Similar calculated torque curves with the best fit parameters(δ = 250 cm −1 , j = 0.064 cm −1 , and g = 1.35). The temperatureand anisotropy dep<strong>en</strong>d<strong>en</strong>t peak in the torque signal is evid<strong>en</strong>tat around 28 Tesla. The inset shows the molecular structure of theDy 3 cluster.A. B. Antunes, I. SheikinF. El Hallak, J. van Slager<strong>en</strong>, M. Dressel (University of Stuttgart, Germany), M. Eti<strong>en</strong>ne, J. Luzon, R. Sessoli (Universityof Flor<strong>en</strong>ce, Italy), C. Anson, A. Powell (University of Karlsruhe, Germany)81

Hooray! Your file is uploaded and ready to be published.

Saved successfully!

Ooh no, something went wrong!