arXiv subjects

G. Christou

Publications and source records attributed to G. Christou.

At least 19 recordsLinked to original sources

arXiv2014

Partial spin reversal in magnetic deflagration

The reversal of spins in a magnetic material as they relax toward equilibrium is accompanied by the release of Zeeman energy which can lead to accelerated spin relaxation and the formation of a well-defined self-sustained propagating spin-reversal front known as magnetic deflagration. To date, studies of Mn$_{12}$-acetate single crystals have focused mainly on deflagration in large longitudinal magnetic fields and found a fully spin-reversed final state. We report a systematic study of the effect of transverse magnetic field on magnetic deflagration and demonstrate that in small longitudinal fields the final state consists of only partially reversed spins. Further, we measured the front speed as a function of applied magnetic field. The theory of magnetic deflagration, together with a modification that takes into account the partial spin reversal, fits the transverse field dependence of the front speed but not its dependence on longitudinal field. The most significant result of this study is the finding of a partially spin-reversed final state, which is evidence that the spins at the deflagration front are also only partially reversed.

cond-mat.mes-hall↗

arXiv2013

Geometric-phase interference in a Mn_{12} single-molecule magnet with four-fold rotational symmetry

We study the magnetic relaxation rate Gamma of the single-molecule magnet Mn_{12}-tBuAc as a function of magnetic field component H_T transverse to the molecule's easy axis. When the spin is near a magnetic quantum tunneling resonance, we find that Gamma increases abruptly at certain values of H_T. These increases are observed just beyond values of H_T at which a geometric-phase interference effect suppresses tunneling between two excited energy levels. The effect is washed out by rotating H_T away from the spin's hard axis, thereby suppressing the interference effect. Detailed numerical calculations of Gamma using the known spin Hamiltonian accurately reproduce the observed behavior. These results are the first experimental evidence for geometric-phase interference in a single-molecule magnet with true four-fold symmetry.

cond-mat.mes-hall↗

arXiv2013

Onset of a Propagating Self-Sustained Spin Reversal Front in a Magnetic System

The energy released in a magnetic material by reversing spins as they relax toward equilibrium can lead to a dynamical instability that ignites self-sustained rapid relaxation along a deflagration front that propagates at a constant subsonic speed. Using a trigger heat pulse and transverse and longitudinal magnetic fields, we investigate and control the crossover between thermally driven magnetic relaxation and magnetic deflagration in single crystals of Mn$_{12}$-acetate.

cond-mat.mes-hall↗

arXiv2012

Discrete antiferromagnetic spin-wave excitations in the giant ferric wheel Fe18

The low-temperature elementary spin excitations in the AFM molecular wheel Fe18 were studied experimentally by inelastic neutron scattering and theoretically by modern numerical methods, such as dynamical density matrix renormalization group or quantum Monte Carlo techniques, and analytical spin-wave theory calculations. Fe18 involves eighteen spin-5/2 Fe(III) ions with a Hilbert space dimension of 10^14, constituting a physical system that is situated in a region between microscopic and macroscopic. The combined experimental and theoretical approach allowed us to characterize and discuss the magnetic properties of Fe18 in great detail. It is demonstrated that physical concepts such as the rotational-band or L&E-band concepts developed for smaller rings are still applicable. In particular, the higher-lying low-temperature elementary spin excitations in Fe18 or AFM wheels in general are of discrete antiferromagnetic spin-wave character.

cond-mat.str-el↗

arXiv2012

Transverse Field Ising Ferromagnetism in Mn$_{12}$-acetate-MeOH

We report measurements of the magnetic susceptibility of single crystals of Mn$_{12}$-acetate-MeOH, a new high-symmetry variant of the original single molecule magnet Mn$_{12}$-acetate. A comparison of these data to theory and to data for the Mn$_{12}$ acetate material shows that Mn$_{12}$-acetate-MeOH is a realization of a transverse-field Ising ferromagnet in contrast to the original Mn$_{12}$ acetate material, in which solvent disorder leads to effects attributed to random field Ising ferromagnetism.

cond-mat.mtrl-sci↗

arXiv2010

On-chip SQUID measurements in the presence of high magnetic fields

We report a low temperature measurement technique and magnetization data of a quantum molecular spin, by implementing an on-chip SQUID technique. This technique enables the SQUID magnetometery in high magnetic fields, up to 7 Tesla. The main challenges and the calibration process are detailed. The measurement protocol is used to observe quantum tunneling jumps of the S=10 molecular magnet, Mn12-tBuAc. The effect of transverse field on the tunneling splitting for this molecular system is addressed as well.

cond-mat.mes-hall↗

arXiv2010

Experimental determination of the Weiss temperature of Mn$_{12}$-ac and Mn$_{12}$-ac-MeOH

We report measurements of the susceptibility in the temperature range from $3.5$ K to $6.0$ K of a series of Mn$_{12}$-ac and Mn$_{12}$-ac-MeOH samples in the shape of rectangular prisms of length $l_c$ and square cross-section of side $l_a$. The susceptibility obeys a Curie-Weiss Law, $χ=C/(T-θ)$, where $θ$ varies systematically with sample aspect ratio. Using published demagnetization factors, we obtain $θ$ for an infinitely long sample corresponding to intrinsic ordering temperatures $T_c \approx 0.85$ K and $\approx 0.74$ K for Mn$_{12}$-ac and Mn$_{12}$-ac-MeOH, respectively. The difference in $T_c$ for two materials that have nearly identical unit cell volumes and lattice constant ratios suggests that, in addition to dipolar interactions, there is a non-dipolar (exchange) contribution to the Weiss temperature that differs in the two materials because of the difference in ligand molecules.

cond-mat.mtrl-sci↗

arXiv2009

Realization of random-field dipolar Ising ferromagnetism in a molecular magnet

The longitudinal magnetic susceptibility of single crystals of the molecular magnet Mn$_{12}$-acetate obeys a Curie-Weiss law, indicating a transition to a ferromagnetic phase due to dipolar interactions. With increasing magnetic field applied transverse to the easy axis, the transition temperature decreases considerably more rapidly than predicted by mean field theory to a T=0 quantum critical point. Our results are consistent with an effective Hamiltonian for a random-field Ising ferromagnet in a transverse field, where the randomness is induced by an external field applied to Mn$_{12}$-acetate crystals that are known to have an intrinsic distribution of locally tilted magnetic easy axes.

cond-mat.mes-hall↗

arXiv2009

Crystal lattice desolvation effects on the magnetic quantum tunneling of single-molecule magnets

High-frequency electron paramagnetic resonance (HFEPR) and AC susceptibility measurements are reported for a new high-symmetry Mn12 complex, [Mn12O12(O2CCH3)16(CH3OH)4].CH3OH. The results are compared with those of other high-symmetry spin S = 10 Mn12 single-molecule magnets (SMMs), including the original acetate, [Mn12(O2CCH3)16(H2O)4].2CH3CO2H.4H2O, and the [Mn12O12(O2CCH2Br)16(H2O)4].4CH2Cl2 & [Mn12O12(O2CCH2But)16(CH3OH)4].CH3OH complexes. These comparisons reveal important insights into the factors that influence the values of the effective barrier to magnetization reversal, Ueff, deduced on the basis of AC susceptibility measurements. In particular, we find that variations in Ueff can be correlated with the degree of disorder in a crystal which can be controlled by desolvating (drying) samples. This highlights the importance of careful sample handling when making measurements on SMM crystals containing volatile lattice solvents. The HFEPR data additionally provide important spectroscopic evidence suggesting that the relatively weak disorder induced by desolvation strongly influences the quantum tunneling interactions, and that it is under-barrier tunneling that is responsible for a consistent reduction in Ueff that is found upon drying samples. Meanwhile, the axial anisotropy deduced from HFEPR is found to be virtually identical for all four Mn12 complexes, with essentially no measurable reduction upon desolvation.

cond-mat.mes-hall↗

arXiv2009

Reply to the comment on "Influence of the Dzyaloshinskii-Moriya Exchange Interaction on Quantum Phase Interference of Spins"

First version: del Barco et al. submitted recently a comment [arXiv:0812.4070] on our latest Phys. Rev. Lett. [Phys. Rev. Lett. 101, 237204 (2008)], claiming three basic mistakes. We show here that their claims are unjustified and based on erroneous calculations and hasty conclusions. Second version: reply to the modified version of del Barco et al. submitted to Phys. Rev. Lett.

cond-mat.mes-hall↗

arXiv2009

Magnetic avalanches of minor fast-relaxing species of Mn12-acetate

Using micron-sized thermometers and Hall bars, we report time-resolved studies of the local temperature and local magnetization for two types of magnetic avalanches (abrupt spin reversals) in the molecular magneti Mn12-acetate, corresponding to avalanches of the main slow-relaxing crystalline form and avalanches of the fast-relaxing minor species that exists in all as-grown crystals of this material. An experimental protocol is used that allows the study of each type of avalanche without triggering avalanches in the other, and of both types of avalanches simultaneously. In samples prepared magnetically to enable both types of avalanches, minor species avalanches are found to act as a catalyst for the major species avalanches. magnetically to enable both types of avalanches, minor species avalanches are found to act as a catalyst for the major species avalanches.

cond-mat.mtrl-sci↗

arXiv2009

Tuning Magnetic Avalanches in Mn12-ac

Using micron-sized Hall sensor arrays to obtain time-resolved measurements of the local magnetization, we report a systematic study in the molecular magnet Mn$_{12}$-acetate of magnetic avalanches controllably triggered in different fixed external magnetic fields and for different values of the initial magnetization. The speeds of propagation of the spin-reversal fronts are in good overall agreement with the theory of magnetic deflagration of Garanin and Chudnovsky \cite{Garanin}.

cond-mat.mtrl-sci↗

arXiv2009

Quantum Phase Interference and Neel-Vector Tunneling in Antiferromagnetic Molecular Wheels

The antiferromagnetic molecular wheel Fe18 of eighteen exchange-coupled Fe(III) ions has been studied by measurements of the magnetic torque, the magnetization, and the inelastic neutron scattering spectra. The combined data show that the low-temperature magnetism of Fe18 is very accurately described by the Neel-vector tunneling (NVT) scenario, as unfolded by semiclassical theory. In addition, the magnetic torque as a function of applied field exhibits oscillations that reflect the oscillations in the NVT tunnel splitting with field due to quantum phase interference.

cond-mat.str-el↗

arXiv2008

Experimental determination of the dipolar field in Mn12-acetate

Crystals of the molecular magnet Mn12-acetate are known to contain a small fraction of low- symmetry (minor) species with a small anisotropy barrier against spin reversal. The lower barrier leads to faster magnetic relaxation and lower coercive field. We exploit the low coercive fields of the minor species to make a direct determination of the dipole field in Mn12-ac. We find that the dipolar field of a fully magnetized crystal is 51.5 \pm 8.5 mT, consistent with theoretical expectations.

cond-mat.other↗

arXiv2008

Influence of the Dzyaloshinskii-Moriya exchange interaction on quantum phase interference of spins

Magnetization measurements of a Mn12mda wheel single-molecule magnet with a spin ground state of S = 7 show resonant tunneling and quantum phase interference, which are established by studying the tunnel rates as a function of a transverse field applied along the hard magnetization axis. Dzyaloshinskii-Moriya (DM) exchange interaction allows the tunneling between different spin multiplets. It is shown that the quantum phase interference of these transitions is strongly dependent on the direction of the DM vector.

cond-mat.mes-hall↗

arXiv2007

Ignition and Propagation of Magnetic Avalanches in Mn$_{12}$-Acetate: the effect of quantum tunneling

Using a wire heater to ignite magnetic avalanches in fixed magnetic field applied along the easy axis of single crystals of the molecular magnet Mn$_{12}$-acetate, we report fast local measurements of the temperature and time-resolved measurements of the local magnetization as a function of magnetic field. In addition to confirming maxima in the velocity of propagation, we find that avalanches trigger at a threshold temperature which exhibits pronounced minima at resonant magnetic fields, demonstrating that thermally assisted quantum tunneling plays an important role in the ignition as well as the propagation of magnetic avalanches in molecular magnets.

cond-mat.mes-hall↗

arXiv2007

Spatial Determination of Magnetic Avalanche Ignition Points

Using time-resolved measurements of local magnetization in the molecular magnet Mn12-ac, we report studies of the propagation of magnetic avalanches (fast magnetization reversals) that originate from points inside the crystals rather than at the edges. The curved nature of the fronts produced by avalanches is reflected in the time-of-arrival at micro-Hall sensors placed at the surface of the sample. Assuming that the avalanche interface is a spherical bubble that grows with a radius proportional to time, we are able to locate the approximate ignition point of each avalanche in a two-dimensional cross-section of the crystal. For the samples used in these studies, avalanches in a given crystal are found to originate in a small region with a radius of roughly 150 microns.

cond-mat.mtrl-sci↗

arXiv2007

Fabrication of Nano-Gapped Single-Electron Transistors for Transport Studies of Individual Single-Molecule Magnets

Three terminal single-electron transistor devices utilizing Al/Al2O3 gate electrodes were developed for the study of electron transport through individual single-molecule magnets. The devices were patterned via multiple layers of optical and electron beam lithography. Electromigration induced breaking of the nanowires reliably produces 1-3 nm gaps between which the SMM can be situated. Conductance through a single Mn12(3-thiophenecarboxylate) displays the coulomb blockade effect with several excitations within +/- 40 meV.

cond-mat.mes-hall↗