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A. Caneschi

Publications and source records attributed to A. Caneschi.

16 recordsLinked to original sources
arXiv2011

Finite-size effects on the dynamic susceptibility of CoPhOMe single-chain molecular magnets in presence of a static magnetic field

The static and dynamic properties of the single-chain molecular magnet [Co(hfac)$_2$NITPhOMe] are investigated in the framework of the Ising model with Glauber dynamics, in order to take into account both the effect of an applied magnetic field and a finite size of the chains. For static fields of moderate intensity and short chain lengths, the approximation of a mono-exponential decay of the magnetization fluctuations is found to be valid at low temperatures; for strong fields and long chains, a multi-exponential decay should rather be assumed. The effect of an oscillating magnetic field, with intensity much smaller than that of the static one, is included in the theory in order to obtain the dynamic susceptibility $χ(ω)$. We find that, for an open chain with $N$ spins, $χ(ω)$ can be written as a weighted sum of $N$ frequency contributions, with a sum rule relating the frequency weights to the static susceptibility of the chain. Very good agreement is found between the theoretical dynamic susceptibility and the ac susceptibility measured in moderate static fields ($H_{\rm dc}\le 2$ kOe), where the approximation of a single dominating frequency turns out to be valid. For static fields in this range, new data for the relaxation time, $τ$ versus $H_{\rm dc}$, of the magnetization of CoPhOMe at low temperature are also well reproduced by theory, provided that finite-size effects are included.

cond-mat.mtrl-sci↗
arXiv2009

Spin canting in a Dy-based Single-Chain Magnet with dominant next-nearest neighbor antiferromagnetic interactions

We investigate theoretically and experimentally the static magnetic properties of single crystals of the molecular-based Single-Chain Magnet (SCM) of formula [Dy(hfac)$_{3}$NIT(C$_{6}$H$_{4}$OPh)]$_{\infty}$ comprising alternating Dy$^{3+}$ and organic radicals. A peculiar inversion between maxima and minima in the angular dependence of the magnetic molar susceptibility $χ_{M}$ occurs on increasing temperature. Using information regarding the monomeric building block as well as an {\it ab initio} estimation of the magnetic anisotropy of the Dy$^{3+}$ ion, this anisotropy-inversion phenomenon can be assigned to weak one-dimensional ferromagnetism along the chain axis. This indicates that antiferromagnetic next-nearest-neighbor interactions between Dy$^{3+}$ ions dominate, despite the large Dy-Dy separation, over the nearest-neighbor interactions between the radicals and the Dy$^{3+}$ ions. Measurements of the field dependence of the magnetization, both along and perpendicularly to the chain, and of the angular dependence of $χ_{M}$ in a strong magnetic field confirm such an interpretation. Transfer matrix simulations of the experimental measurements are performed using a classical one-dimensional spin model with antiferromagnetic Heisenberg exchange interaction and non-collinear uniaxial single-ion anisotropies favoring a canted antiferromagnetic spin arrangement, with a net magnetic moment along the chain axis. The fine agreement obtained with experimental data provides estimates of the Hamiltonian parameters, essential for further study of the dynamics of rare-earths based molecular chains.

cond-mat.mtrl-sci↗
arXiv2005

Fast Switching of Bistable Magnetic Nanowires Through Collective Spin Reversal

The use of magnetic nanowires as memory units is made possible by the exponential divergence of the characteristic time for magnetization reversal at low temperature, but the slow relaxation makes the manipulation of the frozen magnetic states difficult. We suggest that finite-size segments can show a fast switching if collective reversal of the spins is taken into account. This mechanism gives rise at low temperatures to a scaling law for the dynamic susceptibility that has been experimentally observed for the dilute molecular chain Co(hfac)2NitPhOMe. These results suggest a possible way of engineering nanowires for fast switching of the magnetization.

cond-mat.mtrl-sci↗
arXiv2004

Finite-Size effects in "Single Chain Magnets": an experimental and theoretical study

The problem of finite size effects in s=1/2 Ising systems showing slow dynamics of the magnetization is investigated introducing diamagnetic impurities in a Co$^{2+}$-radical chain. The static magnetic properties have been measured and analyzed considering the peculiarities induced by the ferrimagnetic character of the compound. The dynamic susceptibility shows that an Arrhenius law is observed with the same energy barrier for the pure and the doped compounds while the prefactor decreases, as theoretically predicted. Multiple spins reversal has also been investigated.

cond-mat.mes-hall↗
arXiv2003

Specific heat and muon spin resonance measurements in Gd(hfac)3NITiPr molecular magnetic chains: indications for a chiral phase without long range helical order

Low temperature specific heat $C(T)$ and zero-field muon spin resonance ($μ^+$SR) measurements were performed in Gd(hfac)$_3$NITiPr, a quasi one-dimensional molecular magnet with competing nearest neighbor and next-nearest neighbor intrachain exchange interactions. The specific heat data exhibit a $λ$-peak at $T_0$=2.08$\pm$0.01K that disappears upon the application of a 5 Tesla magnetic field. Conversely, the $μ^+$SR data do not present any anomaly at $T\approx 2$ K, proving the lack of divergence of the two-spin correlation function as required for usual three-dimensional (3D) long range helical order. Moreover, no muon spin precession can be evinced from the $μ^+$SR asimmetry curves, thus excluding the presence of a long range ordered magnetic lattice. These results provide indications for a low $T$ phase where chiral order is established in absence of long range helical order.

cond-mat.mtrl-sci↗
arXiv2002

Investigation of a ring single molecular magnet Mn$_6$R$_6$ in megagauss fields

The dependence of the magnetic susceptibility on the magnetic field is investigated for the single molecular magnet [Mn(hfac)$_2$NITPh]$_6$. The spikes of the susceptibility detected in a magnetic field ranging from 90 T to 285 T are interpreted as a manifestation of magnetic quantum jumps under spins reorientation from ferrimagnetic to ferromagnetic structure. The characteristic feature of the single molecular magnet Mn$_6$ R$_6$ is a deficiency of pair Heisenberg exchange interactions for the description of its magnetic properties in high magnetic fields. The comparison of the experimental data with the results of theoretical calculations allows us to prove the existence of strong three-spin interaction in this molecular cluster and to determine the values of exchange constants. For the calculation of the ground state spin structure the modified Lanczos method is used.

cond-mat.str-el↗
arXiv2001

Glauber slow dynamics of the magnetization in a molecular Ising chain

The slow dynamics (10^-6 s - 10^4 s) of the magnetization in the paramagnetic phase, predicted by Glauber for 1d Ising ferromagnets, has been observed with ac susceptibility and SQUID magnetometry measurements in a molecular chain comprising alternating Co{2+} spins and organic radical spins strongly antiferromagnetically coupled. An Arrhenius behavior with activation energy Delta=152 K has been observed for ten decades of relaxation time and found to be consistent with the Glauber model. We have extended this model to take into account the ferrimagnetic nature of the chain as well as its helicoidal structure.

cond-mat.stat-mech↗
arXiv2001

Tuning of the magnetic properties of the high spin molecular cluster Fe8

The synthesis, crystal structure and magnetic characterization of a high spin cluster comprising eight iron ions, are presented in this contribution. The cluster has formula [(tacn)6Fe8O2(OH)12Br4.3(ClO4)3.7]6H2O, (Fe8PCL) where tacn is the organic ligand 1,4,7-triazacyclononane. It can be considered a derivative of Fe8Br8, a cluster whose low temperature dynamics of the magnetization has been deeply investigated, where four of the bromide ions have been replaced by perchlorate anions. The structure of the central core of the two molecules, [Fe8O(OH)12(tacn)6]8+, is essentially the same, but Fe8PCL has a higher symmetry (Fe8Br8 crystallizes in the acentric P1 space group, while Fe8PCL crystallizes in the P21/c space group, monoclinic). The magnetic properties of Fe8PCL suggest it is very similar to Fe8Br having a S=10 ground state as well. The zero field splitting parameters were accurately determined by HF-EPR measurements. The two clusters have similar axial anisotropy but Fe8PCL has a larger transverse anisotropy. Ac susceptibility measurements revealed the cluster behaves like a superparamagnetic particle. However, due to the occurrence of large terms in the transverse anisotropy, the temperature dependence of the relaxation time can not be reproduced by a simple Arrhenius law. As observed in Fe8Br8, below 350 mK the relaxation time becomes temperature independent, indicating that a pure tunneling regime is attained. The comparison of the tunneling rate in the two clusters shows that in the perchlorate derivative the relaxation process is 35 times faster. The observed ratio of the tunneling rates is in reasonable agreement with that calculated from the tunneling splitting, i.e. the energy difference between the two almost degenerate lowest levels Ms = +/-10, in the two clusters.

cond-mat.mes-hall↗
arXiv2000

Phonon-assisted tunneling in the quantum regime of Mn12-ac

Longitudinal or transverse magnetic fields applied on a crystal of Mn12-ac allows to observe independent tunnel transitions between m=-S+p and m=S-n-p (n=6-10, p=0-2 in longitudinal field and n=p=0 in transverse field). We observe a smooth transition (in longitudinal) from coherent ground-state to thermally activated tunneling. Furthermore two ground-state relaxation regimes showing a crossover between quantum spin relaxation far from equilibrium and near equilibrium, when the environment destroys multimolecule correlations. Finally, we stress that the complete Hamiltonian of Mn12 should contain odd spin operators of low order.

cond-mat.mes-hall↗
arXiv2000

Mesoscopic Spin Tunneling in Molecular Crystals

The phenomenon of Quantum Tunneling of Mesoscopic Spins is reviewed in the light of the behavior of the archetype of these systems: the molecular complex Mn12-ac. Most observations can be understood in the framework of the reduced Hilbert space dimension 2S+1=21. Due to the large spin S=10, the energy barrier preventing spin rotation is large, and as a consequence, quantum relaxation is very slow. The application of a magnetic field of a few Tesla below 1 K allows to observe tunneling (i) between the states m=-10 and m=10-n with n=8 to 11 if the field is longitudinal, or (ii) between the two ground-states m~-10 and m~10 if the field is transverse. The crossover temperature between ground-state and thermally assisted tunneling in a longitudinal field extrapolates in zero field at ~1.7 K. The observation of square root relaxation at short-times/low-temperatures and of exponential relaxation at long-times/high-temperatures, as observed previously above 1.5 K, confirms the important role of the spin bath dynamics which is out of equilibrium in the first regime and at equilibrium in the second one. In a second part of this paper a new molecule, so-called V15, with resultant spin S=1/2 is investigated. Contrary to high spin molecules, the energy barrier of low spin molecules is small or null, and the splitting between the symmetrical and anti-symmetrical states is sufficiently large to allow spin-phonon transitions during spin rotation. In low spin molecules the coupling to the environment is quite different from the one found in large spin molecules in low fields.

cond-mat.mes-hall↗
arXiv2000

Nonadiabatic Landau Zener tunneling in Fe_8 molecular nanomagnets

The Landau Zener method allows to measure very small tunnel splittings Δin molecular clusters Fe_8. The observed oscillations of Δas a function of the magnetic field applied along the hard anisotropy axis are explained in terms of topological quantum interference of two tunnel paths of opposite windings. Studies of the temperature dependence of the Landau Zener transition rate P gives access to the topological quantum interference between exited spin levels. The influence of nuclear spins is demonstrated by comparing P of the standard Fe_8 sample with two isotopically substituted samples. The need of a generalized Landau Zener transition rate theory is shown.

cond-mat.mes-hall↗
arXiv2000

The effects of nuclear spins on the quantum relaxation of the magnetization for the molecular nanomagnet Fe_8

The strong influence of nuclear spins on resonant quantum tunneling in the molecular cluster Fe_8 is demonstrated for the first time by comparing the relaxation rate of the standard Fe_8 sample with two isotopic modified samples: (i) 56_Fe is replaced by 57_Fe, and (ii) a fraction of 1_H is replaced by 2_H. By using a recently developed "hole digging" method, we measured an intrinsic broadening which is driven by the hyperfine fields. Our measurements are in good agreement with numerical hyperfine calculations. For T > 1.5 K, the influence of nuclear spins on the relaxation rate is less important, suggesting that spin-phonon coupling dominates the relaxation rate at higher temperature.

cond-mat.mes-hall↗
arXiv1999

Landau Zener method to study quantum phase interference of Fe8 molecular nanomagnets

We present details about an experimental method based on the Landau Zener model which allows to measure very small tunnel splittings $Δ$ in molecular clusters Fe8. The measurements are performed with an array of micro-SQUIDs. The observed oscillations of Delta as a function of the magnetic field applied along the hard anisotropy axis are explained in terms of topological quantum interference of two tunnel paths of opposite windings. Transitions between M = -S and (S - n), with n even or odd, revealed a parity (symmetry) effect which is analogous to the suppression of tunneling predicted for half integer spins. This observation is the first direct evidence of the topological part of the quantum spin phase (Berry phase) in a magnetic system. The influence of intermolecular dipole interactions on the measured tunnel splittings $Δ$ are shown.

cond-mat.mes-hall↗
arXiv1999

Proton NMR for Measuring Quantum-Level Crossing in the Magnetic Molecular Ring Fe10

The proton nuclear spin-lattice relaxation rate 1/T1 has been measured as a function of temperature and magnetic field (up to 15 T) in the molecular magnetic ring Fe10. Striking enhancement of 1/T1 is observed around magnetic field values corresponding to a crossing between the ground state and the excited states of the molecule. We propose that this is due to a cross-relaxation effect between the nuclear Zeeman reservoir and the reservoir of the Zeeman levels of the molecule. This effect provides a powerful tool to investigate quantum dynamical phenomena at level crossing.

cond-mat.mes-hall↗
arXiv1999

Low energy magnetic excitations of the Mn_{12}-acetate spin cluster observed by neutron scattering

We performed high resolution diffraction and inelastic neutron scattering measurements of Mn_{12}-acetate. Using a very high energy resolution, we could separate the energy levels corresponding to the splitting of the lowest S multiplet. Data were analyzed within a single spin model (S=10 ground state), using a spin Hamiltonian with parameters up to 4^{th} order. The non regular spacing of the transition energies unambiguously shows the presence of high order terms in the anisotropy (D= -0.457(2) cm^{-1}, B_4^0 = -2.33(4) 10^{-5}cm^{-1}). The relative intensity of the lowest energy peaks is very sensitive to the small transverse term, supposed to be mainly responsible for quantum tunneling. This allows an accurate determination of this term in zero magnetic field (B_4^4 = \pm 3.0(5) 10^{-5} cm^{-1}). The neutron results are discussed in view of recent experiments and theories.

cond-mat.mes-hall↗