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.Comment: 5 pages, 4 figure

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

Under the terms of the Creative Commons Attribution License 3.0 (CC-BY).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 rate 1/T1n in a single crystal of the single-molecule magnet Mn12-ac, at T≈30 mK in perpendicular fields B⊥ up to 9 T. The relaxation channel at B≈0 is dominated by incoherent quantum tunneling of the Mn12-ac spin S, aided by the nuclear bath itself. However for B⊥>5 T we observe an increase of 1/T1n by several orders of magnitude up to the highest field, despite the fact that the molecular spin is in its quantum mechanical ground state. This striking observation is a consequence of the zero-point quantum fluctuations of S, which allow it to mediate the transfer of energy from the excited nuclear spin bath to the crystal lattice at much higher rates. Our experiment highlights the importance of quantum fluctuations in the interaction between an >effective two-level system> and its surrounding spin bath. © 2014 American Physical Society.This work has been part of the research program of the “Stichting FOM.”Peer Reviewe

Muon Spin Relaxation Studies of Superconductivity in a Crystalline Array of Weakly Coupled Metal Nanoparticles

We report Muon Spin Relaxation studies in weak transverse fields of the superconductivity in the metal cluster compound, Ga$\_{84}$[N(SiMe$\_{3}$)$\_{2}$]$\_{20}$-Li$\_{6}$Br$\_{2}$(thf)$\_{20}\cdot$2toluene. The temperature and field dependence of the muon spin relaxation rate and Knight shift clearly evidence type II bulk superconductivity below $T\_{\text{c}}\approx7.8$ K, with $B\_{\text{c1}}\approx 0.06$ T, $B\_{\text{c2}}\approx 0.26$ T, $\kappa\sim 2$ and weak flux pinning. The data are well described by the s-wave BCS model with weak electron-phonon coupling in the clean limit. A qualitative explanation for the conduction mechanism in this novel type of narrow band superconductor is presented.Comment: 4 figures, 5 page

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.Comment: 19 pages, 11 eps figures. Contains extensive discussions on dipolar ordering, specific heat and nuclear relaxation in molecular magnet

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.Comment: 4 pages, 3 figure

Superconductivity in a Molecular Metal Cluster Compound

Compelling evidence for band-type conductivity and even bulk superconductivity below $T\_{\text{c}}\approx 8$ K has been found in $^{69,71}$Ga-NMR experiments in crystalline ordered, giant Ga$\_{84}$ cluster-compounds. This material appears to represent the first realization of a theoretical model proposed by Friedel in 1992 for superconductivity in ordered arrays of weakly coupled, identical metal nanoparticles.Comment: 5 pages, 4 figure

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.Comment: Replaced with version accepted for publication in Physical Review Letter

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.Comment: RevTex, 10 pages, 10 eps figures. High-resolution figures available upon reques

Two dimensional frustrated magnetic state in superconducting RuSr2Eu1.5Ce0.5Cu2O10 (Ru-1222)

In this paper we investigate the magnetic state and the role of the crystalline structure in RuSr2Eu1.5Ce0.5Cu2O10 (Ru-1222). Measurements were made in the isomorphic series (Nb1-xRux)Sr2Eu1.5Ce0.5Cu2O10 [(Nb,Ru)-1222], with x between 0 and 1. 3D XY fluctuations above the magnetic transition were not observed in Ru-1222, suggesting a weak inter-plane coupling between the RuO2 layers. The compositional dependence of the magnetic susceptibility shows a rapid broadening with increasing Nb content, explained in terms of a cluster-glass state. The variation of several superconducting parameters as a function of Ru content is linear in the whole concentration range, with no jumps at the critical concentration for which percolation of long range order is expected. 3D Arrhenius and Vogel-Fulcher-type dependencies fail to describe the dynamic properties. Fitting of a generalized Vogel-Fulcher-type dependence, with ln(tau/tau0) = A(T-T0)^-B, yield B = 2.0, in excellent agreement with Monte Carlo simulations for 2D systems. The value deduced for T0 agrees well with the re-opening of hysteresis in the M(H) curves. The observed superconducting and magnetic features are explained in terms of a scenario of 2D magnetic islands at the RuO2 layers, with no long range magnetic order.Comment: submitted to Phys. Rev.

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

We report the magnetic behavior of the one-dimensional (1D) cyanido-bridged chain complex [Tb(pzam) 3(H 2O)M(CN) 8] •H 2O, where M = W(V). The system shows qualitatively similar magnetic behavior with its already reported M = Mo(V): a broad anomaly in the specific heat ascribed to the magnetic interactions, a transition to three-dimensional magnetic order at T C = 1.15 K, and comparable magnetization and susceptibility. However, substituting the Mo(V) ion by the larger W(V) causes a drastic change in the symmetry of the Tb(III) g tensor, whereby the magnetic interaction between the Tb(III) and M(V) changes from Ising type into an anisotropic XY exchange. We analyze the data in terms of theoretical predictions for the 1D XYZ Hamiltonian and we find an excellent agreement between the theory and experimental data (J x = 1.89 K, J y = 2J x, J z = 0). © 2012 American Physical Society.This research was supported by a Veni grant from the Netherlands Organization for Scientific Research (NWO) to S.T.. We acknowledge Spanish MINECO for Grants MAT2009-13977-C03 and CSD2007-00010.Peer Reviewe