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L. J. de Jongh

Publications and source records attributed to L. J. de Jongh.

13 recordsLinked to original sources
arXiv2013

Observation of zero-point quantum fluctuations of a single-molecule magnet through the relaxation of its nuclear spin bath

A single-molecule magnet placed in a magnetic field perpendicular to its anisotropy axis can be truncated to an effective two-level system, with easily tunable energy splitting. The quantum coherence of the molecular spin is largely determined by the dynamics of the surrounding nuclear spin bath. Here we report the measurement of the nuclear spin--lattice relaxation in a single crystal of the single-molecule magnet Mn$_{12}$-ac, at $T \approx 30$ mK in perpendicular fields $B_{\perp}$ up to 9 T. Although the molecular spin is in its ground state, we observe an increase of the nuclear relaxation rates by several orders of magnitude up to the highest $B_{\perp}$. This unique finding is a consequence of the zero-point quantum fluctuations of the Mn$_{12}$-ac spin, which allow it to efficiently transfer energy from the excited nuclear spin bath to the lattice. Our experiment highlights the importance of quantum fluctuations in the interaction between an `effective two-level system' and its surrounding spin bath.

cond-mat.mes-hall↗
arXiv2012

Realization of the anisotropic XY model in a Tb(III)-W(V) chain compound

We present evidence of 1D S=1/2 anisotropic XY ferromagnetism in the paramagnetic phase of the cyanido-bridged chain complex [Tb(pzam)3(H2O)M(CN)8]H2O, with M=W(V), based upon the measurement of the specific heat, the uniform susceptibility and the magnetization curve on a powder sample. Both the specific heat and the susceptibility exhibit a transition peak to long-range ferromagnetism, mediated by the residual interchain couplings, at a critical temperature Tc=1.15 K. Yet in the temperature range T > Tc the specific heat exhibits a broad Schottky anomaly which can be very well fitted by the exact result for the 1D S=1/2 XY model with strong anisotropy in the XY plane (Jx = 1.89 K, Jy=2Jx). For the analysis of the susceptibility and magnetization, not directly accessible theoretically via the exact solution of the XY model, we resort to numerically exact quantum Monte Carlo simulations. Very good agreement is found between the powder-sample data and the Monte Carlo data using an effective average g-factor.

cond-mat.str-el↗
arXiv2007

Dynamics and thermalization of the nuclear spin bath in the single-molecule magnet Mn12-ac: test for the theory of spin tunneling

The description of the tunneling of a macroscopic variable in the presence of a bath of localized spins is a subject of great fundamental and practical interest, and is relevant for many solid-state qubit designs. Instead of focusing on the the "central spin" (as is most often done), here we present a detailed study of the dynamics of the nuclear spin bath in the Mn12-ac single-molecule magnet, probed by NMR experiments down to very low temperatures (T = 20 mK). We find that the longitudinal relaxation rate of the 55Mn nuclei in Mn12-ac becomes roughly T-independent below T = 0.8 K, and can be strongly suppressed with a longitudinal magnetic field. This is consistent with the nuclear relaxation being caused by quantum tunneling of the molecular spin, and we attribute the tunneling fluctuations to the minority of fast-relaxing molecules present in the sample. The transverse nuclear relaxation is also T-independent for T < 0.8 K, and can be explained qualitatively and quantitatively by the dipolar coupling between like nuclei in neighboring molecules. We also show that the isotopic substitution of 1H by 2H leads to a slower nuclear longitudinal relaxation, consistent with the decreased tunneling probability of the molecular spin. Finally, we demonstrate that, even at the lowest temperatures, the nuclear spins remain in thermal equilibrium with the lattice phonons, and we investigate the timescale for their thermal equilibration. After a review of the theory of macroscopic spin tunneling in the presence of a spin bath, we argue that most of our experimental results are consistent with that theory, but the thermalization of the nuclear spins is not.

cond-mat.mes-hall↗
arXiv2006

Magnetic dipolar ordering and relaxation in the high-spin molecular cluster compound Mn6

Few examples of magnetic systems displaying a transition to pure dipolar magnetic order are known to date, and single-molecule magnets can provide an interesting example. The molecular cluster spins and thus their dipolar interaction energy can be quite high, leading to reasonably accessible ordering temperatures, provided the crystal field anisotropy is sufficiently small. This condition can be met for molecular clusters of sufficiently high symmetry, as for the Mn6 compound studied here. Magnetic specific heat and susceptibility experiments show a transition to ferromagnetic dipolar order at T_{c} = 0.16 K. Classical Monte-Carlo calculations indeed predict ferromagnetic ordering and account for the correct value of T_{c}. In high magnetic fields we detected the contribution of the ^{55}Mn nuclei to the specific heat, and the characteristic timescale of nuclear relaxation. This was compared with results obtained directly from pulse-NMR experiments. The data are in good mutual agreement and can be well described by the theory for magnetic relaxation in highly polarized paramagnetic crystals and for dynamic nuclear polarization, which we extensively review. The experiments provide an interesting comparison with the recently investigated nuclear spin dynamics in the anisotropic single molecule magnet Mn12-ac.

cond-mat.mes-hall↗
arXiv2005

Giant isotope effect in the incoherent tunneling specific heat of the molecular nanomagnet Fe8

Time-dependent specific heat experiments on the molecular nanomagnet Fe8 and the isotopic enriched analogue 57Fe8 are presented. The inclusion of the 57Fe nuclear spins leads to a huge enhancement of the specific heat below 1 K, ascribed to a strong increase in the spin-lattice relaxation rate Gamma arising from incoherent, nuclear-spin-mediated magnetic quantum tunneling in the ground-doublet. Since Gamma is found comparable to the expected tunneling rate, the latter process has to be inelastic. A model for the coupling of the tunneling levels to the lattice is presented. Under transverse field, a crossover from nuclear-spin-mediated to phonon-induced tunneling is observed.

cond-mat.mes-hall↗
arXiv2004

An automated and versatile ultra-low temperature SQUID magnetometer

We present the design and construction of a SQUID-based magnetometer for operation down to temperatures T = 10 mK, while retaining the compatibility with the sample holders typically used in commercial SQUID magnetometers. The system is based on a dc-SQUID coupled to a second-order gradiometer. The sample is placed inside the plastic mixing chamber of a dilution refrigerator and is thermalized directly by the 3He flow. The movement though the pickup coils is obtained by lifting the whole dilution refrigerator insert. A home-developed software provides full automation and an easy user interface.

physics.ins-det↗
arXiv2004

Magnetic long-range order induced by quantum relaxation in single-molecule magnets

Can magnetic interactions between single-molecule magnets (SMMs) in a crystal establish long-range magnetic order at low temperatures deep in the quantum regime, where the only electron spin-fluctuations are due to incoherent magnetic quantum tunneling (MQT)? Put inversely: can MQT provide the temperature dependent fluctuations needed to destroy the ordered state above some finite Tc, although it should basically itself be a T-independent process? Our experiments on two novel Mn4 SMMs provide a positive answer to the above, showing at the same time that MQT in the SMMs has to involve spin-lattice coupling at a relaxation rate equaling that predicted and observed recently for nuclear spin-mediated quantum relaxation.

cond-mat.mes-hall↗
arXiv2003

Superparamagnetic behaviour of antiferromagnetic DyPO4 nanoparticles

We report on the low-temperature magnetic ac-susceptibility of antiferromagnetic DyPO4 nanoparticles with a very high surface to volume ratio. The results are interpreted in terms of superparamagnetic relaxation of the Neel vector arising from a relatively large number approx 0.2 Na of uncompensated spins probably existing on the surface of the nanoparticles. The activation energy of the relaxation process is found to be Ea / kB = (2.6+-0.1) K within a model taking into account the magnetic interaction between nanoparticles.

cond-mat.mtrl-sci↗
arXiv2003

Magnetic and thermal properties of 4f-3d ladder-type molecular compounds

We report on the low-temperature magnetic susceptibilities and specific heats of the isostructural spin-ladder molecular complexes L$_{2}$[M(opba)]$_{3\cdot x$DMSO$\cdot y$H$_{2}$O, hereafter abbreviated with L$_{2}$M$_{3}$ (where L = La, Gd, Tb, Dy, Ho and M = Cu, Zn). The results show that the Cu containing complexes (with the exception of La$_{2}$Cu$_{3}$) undergo long range magnetic order at temperatures below 2 K, and that for Gd$_{2}$Cu$_{3}$ this ordering is ferromagnetic, whereas for Tb$_{2}$Cu$_{3}$ and Dy$_{2}$Cu$_{3}$ it is probably antiferromagnetic. The susceptibilities and specific heats of Tb$_{2}$Cu$_{3}$ and Dy$_{2}$Cu$_{3}$ above $T_{C}$ have been explained by means of a model taking into account nearest as well as next-nearest neighbor magnetic interactions. We show that the intraladder L--Cu interaction is the predominant one and that it is ferromagnetic for L = Gd, Tb and Dy. For the cases of Tb, Dy and Ho containing complexes, strong crystal field effects on the magnetic and thermal properties have to be taken into account. The magnetic coupling between the (ferromagnetic) ladders is found to be very weak and is probably of dipolar origin.

cond-mat↗
arXiv2002

Long-range ferromagnetic dipolar ordering of high-spin molecular clusters

We report the first example of a transition to long-range magnetic order in a purely dipolarly interacting molecular magnet. For the magnetic cluster compound Mn6O4Br4(Et2dbm)6, the anisotropy experienced by the total spin S=12 of each cluster is so small that spin-lattice relaxation remains fast down to the lowest temperatures, thus enabling dipolar order to occur within experimental times at Tc = 0.16 K. In high magnetic fields, the relaxation rate becomes drastically reduced and the interplay between nuclear- and electron-spin lattice relaxation is revealed.

cond-mat.mes-hall↗
arXiv2002

Quantum tunnelling of magnetization in Mn12-ac studied by 55Mn NMR

We present an ultra-low temperature study (down to T = 20 mK) of the nuclear spin-lattice relaxation (SLR) in the 55Mn nuclei of the molecular magnet Mn12-ac. The nuclear spins act as local probes for the electronic spin fluctuations, due to thermal excitations and to tunnelling events. In the quantum regime (below T = 0.75 K), the nuclear SLR becomes temperature-independent and is driven by fluctuations of the cluster's electronic spin due to the quantum tunnelling of magnetization in the ground doublet. The quantitative analysis of the nuclear SLR shows that the presence of fast-tunnelling molecules, combined with nuclear intercluster spin diffusion, plays an important role in the relaxation process.

cond-mat.mes-hall↗
arXiv2002

Magnetic properties of alpha-iron(II) phthalocyanine

We report on the magnetic properties of the supra-molecular compound iron(II) phthalocyanine in its alpha-form. dc- and ac-susceptometry measurements and Mossbauer experiments show that the iron atoms are strongly magnetically coupled into ferromagnetic Ising chains with very weak antiferromagnetic interchain coupling. The transition to 3D magnetic ordering below 10 K is hindered by the presence of impurities or other defects, by which the domain-wall arrangements along individual chains become gradually blocked/frozen, leading to a disordered 3D distribution of ferromagnetic chain segments. Below 5 K, field-cooled and zero-field-cooled magnetization measurements show strong irreversible behavior, attributed to pinning of the domain-walls by the randomly distributed defects in combination with the interchain coupling. High-field magnetization experiments reveal a canted arrangement of the moments in adjacent ferromagnetic chains.

cond-mat↗