arXiv subjects

D. N. Hendrickson

Publications and source records attributed to D. N. Hendrickson.

At least 37 records · Page 2Linked to original sources

arXiv2004

Experimental Upper Bound on Superradiance Emission from Mn12 Acetate

We used a Josephson junction as a radiation detector to look for evidence of the emission of electromagnetic radiation during magnetization avalanches in a crystal assembly of Mn_12-Acetate. The crystal assembly exhibits avalanches at several magnetic fields in the temperature range from 1.8 to 2.6 K with durations of the order of 1 ms. Although a recent study shows evidence of electromagnetic radiation bursts during these avalanches [J. Tejada, et al., Appl. Phys. Lett. {\bf 84}, 2373 (2004)], we were unable to detect any significant radiation at well-defined frequencies. A control experiment with external radiation pulses allows us to determine that the energy released as radiation during an avalanche is less than 1 part in 10^4 of the total energy released. In addition, our avalanche data indicates that the magnetization reversal process does not occur uniformly throughout the sample.

cond-mat.mes-hall↗

arXiv2004

Quantum Coherence between High Spin Superposition States of Single Molecule Magnet Ni$_4$

Magnetic quantum tunneling in a single molecule magnet (SMM) has been studied in experiments that combine microwave spectroscopy with high sensitivity magnetic measurements. By monitoring spin-state populations in the presence of microwave magnetic fields, the energy splittings between low lying high spin superposition states of SMM Ni$_4$ ($S$ = 4) have been measured. Absorption linewidths give an upper bound on the rate of decoherence. Pulsed microwave experiments provide a direct measure of the spin-lattice relaxation time, which is found to be remarkably long ($\sim$sec) and to increase with the energy splitting.

cond-mat.mes-hall↗

arXiv2004

Photon-Induced Magnetization Reversal in Single-Molecule Magnets

We use millimeter wave radiation to manipulate the populations of the energy levels of a single crystal molecular magnet Fe8. When a continuous wave radiation is in resonance with the transitions from the ground state to the first excited state, the equilibrium magnetization exhibits a dip. The position of this dip varies linearly with the radiation frequency. Our results provide a lower bound of 0.17 ns for transverse relaxation time and suggest the possibility that single-molecule magnets might be utilized for quantum computation.

cond-mat.mes-hall↗

arXiv2003

Observation of a Distribution of Internal Transverse Magnetic Fields in a Mn12-Based Single Molecule Magnet

A distribution of internal transverse magnetic fields has been observed in single molecule magnet (SMM) Mn12-BrAc in the pure magnetic quantum tunneling (MQT) regime. Magnetic relaxation experiments at 0.4 K are used to produce a hole in the distribution of transverse fields whose angle and depth depend on the orientation and amplitude of an applied transverse ``digging field.'' The presence of such transverse magnetic fields can explain the main features of resonant MQT in this material, including the tunneling rates, the form of the relaxation and the absence of tunneling selection rules. We propose a model in which the transverse fields originate from a distribution of tilts of the molecular magnetic easy axes.

cond-mat.mes-hall↗

arXiv2003

Symmetry of Magnetic Quantum Tunneling in Single Molecule Magnet Mn12-acetate

The symmetry of magnetic quantum tunneling has been studied in the prototype single molecule magnet Mn$_{12}$-acetate using a micro-Hall effect magnetometer and superconducting high field vector magnet system. An average crystal fourfold symmetry is shown to be due to local molecular environments of twofold symmetry that are rotated by 90$^o$ with respect to one another, confirming that disorder which lowers the molecule symmetry is at important to magnetic quantum tunneling. We have studied a subset of these lower (twofold) site symmetry molecules and present evidence for a Berry phase effect consistent with a local twofold symmetry.

cond-mat.mes-hall↗

arXiv2003

Quantum tunneling in a three dimensional network of exchange coupled single-molecule magnets

A Mn4 single-molecule magnet (SMM) is used to show that quantum tunneling of magnetization (QTM) is not suppressed by moderate three dimensional exchange coupling between molecules. Instead, it leads to an exchange bias of the quantum resonances which allows precise measurements of the effective exchange coupling that is mainly due to weak intermolecular hydrogen bounds. The magnetization versus applied field was recorded on single crystals of [Mn4]2 using an array of micro-SQUIDs. The step fine structure was studied via minor hysteresis loops.

cond-mat.mes-hall↗

arXiv2003

Quantum Tunneling of Magnetization in a Large Molecular Nanomagnet -- Approaching the Mesoscale

A Mn30 molecular cluster is established to be the largest single-molecule magnet (SMM) discovered to date. Magnetization versus field measurements show coercive fields of about 0.5 T at low temperatures. Magnetization decay experiments reveal an Arrhenius behavior and temperature-independent relaxation below 0.2 K diagnostic of quantum tunneling of magnetization through the anisotropy barrier.The quantum hole digging method is used to establish resonant quantum tunneling. These results demonstrate that large molecular nanomagnets,having a volume of 15 nm^3, with dimensions approaching the mesoscale can still exhibit the quantum physics of the microscale.

cond-mat.mes-hall↗

arXiv2003

Two-body tunnel transitions in a Mn4 Single-Molecule Magnet

The one-body tunnel picture of single-molecule magnets (SMMs) is not always sufficient to explain the measured tunnel transitions. An improvement to the picture is proposed by including also two-body tunnel transitions such as spin-spin cross-relaxation (SSCR) which are mediated by dipolar and weak superexchange interactions between molecules. A Mn4 SMM is used as a model system. At certain external fields, SSCRs lead to additional quantum resonances which show up in hysteresis loop measurements as well defined steps.

cond-mat.mes-hall↗

arXiv2003

Quantum dynamics of exchange biased Single Molecule Magnets

We present a new family of exchange biased Single Molecule Magnets in which antiferromagnetic coupling between the two components results in quantum behaviour different from that of the individual SMMs. Our experimental observations and theoretical analysis suggest a means of tuning the quantum tunnelling of magnetization in SMMs. See also: W. Wernsdorfer, N. Aliaga-Alcalde, D. Hendrickson, G. Christou, Nature 416 (2002) 406.

cond-mat.mes-hall↗

arXiv2003

Defects, Tunneling, and EPR Spectra of Single-Molecule Magnets

We examine theoretically electron paramagnetic resonance (EPR) lineshapes as functions of resonance frequency, energy level, and temperature for single crystals of three different kinds of single-molecule nanomagnets (SMMs): Mn$_{12}$ acetate, Fe$_8$Br, and the $S=9/2$ Mn$_4$ compound. We use a density-matrix equation and consider distributions in the uniaxial (second-order) anisotropy parameter $D$ and the $g$ factor, caused by possible defects in the samples. Additionally, weak intermolecular exchange and electronic dipole interactions are included in a mean-field approximation. Our calculated linewidths are in good agreement with experiments. We find that the distribution in $D$ is common to the three examined single-molecule magnets. This could provide a basis for a proposed tunneling mechanism due to lattice defects or imperfections. We also find that weak intermolecular exchange and dipolar interactions are mainly responsible for the temperature dependence of the lineshapes for all three SMMs, and that the intermolecular exchange interaction is more significant for Mn$_4$ than for the other two SMMs. This finding is consistent with earlier experiments and suggests the role of spin-spin relaxation processes in the mechanism of magnetization tunneling.

cond-mat.mtrl-sci↗

arXiv2002

Tunneling Splittings in Mn12-Acetate Single Crystals

A Landau-Zener multi-crossing method has been used to investigate the tunnel splittings in high quality Mn$_{12}$-acetate single crystals in the pure quantum relaxation regime and for fields applied parallel to the magnetic easy axis. With this method several individual tunneling resonances have been studied over a broad range of time scales. The relaxation is found to be non-exponential and a distribution of tunnel splittings is inferred from the data. The distributions suggest that the inhomogeneity in the tunneling rates is due to disorder that produces a non-zero mean value of the average transverse anisotropy, such as in a solvent disorder model. Further, the effect of intermolecular dipolar interaction on the magnetic relaxation has been studied.

cond-mat.mes-hall↗

arXiv2002

More Evidence for a Distribution of Tunnel Splittings in Mn$_{12}$-acetate

In magnetic fields applied parallel to the anisotropy axis, the magnetization of Mn$_{12}$ has been measured in response to a field that is swept back and forth across the resonances corresponding to steps $N=4,5,...9$. The fraction of molecules remaining in the metastable well after each sweep through the resonance is inconsistent with expectations for an ensemble of identical molecules. The data are consistent instead with the presence of a broad distribution of tunnel splittings. A very good fit is obtained for a Gaussian distribution of the second-order anisotropy tunneling parameter $X_E=-\ln(\mid E\mid/2D)$. We show that dipolar shuffling is a negligible effect which cannot explain our data.

cond-mat.mes-hall↗

arXiv2002

Spin-spin cross-relaxation in single-molecule magnets

It is shown that dipolar and weak superexchange interactions between the spin systems of single-molecule magnets (SMM) play an important role in the relaxation of magnetization. These interactions can reduce or increase resonant tunneling. The one-body tunnel picture of SMMs is not always sufficient to explain the measured tunnel transitions. We propose to improve the picture by including also two-body tunnel transitions such as spin-spin cross-relaxation (SSCR). A Mn4 SMM is used as a model system to study the SSCR which plays also an important role for other SMMs like Mn12 or Fe8. At certain external fields, SSCRs can lead to quantum resonances which can show up in hysteresis loop measurements as well defined steps. A simple model allows us to explain quantitatively all observed transitions. Including three-body transitions or dealing with the many-body problem is beyond the slope of this paper.

cond-mat.mes-hall↗

arXiv2001

Quantum phase interference (Berry phase) in single-molecule magnets of Mn12

Magnetization measurements of a molecular clusters Mn12 with a spin ground state of S = 10 show resonance tunneling at avoided energy level crossings. The observed oscillations of the tunnel probability as a function of the magnetic field applied along the hard anisotropy axis are due to topological quantum phase interference of two tunnel paths of opposite windings. Mn12 is therefore the second molecular clusters presenting quantum phase interference.

cond-mat.mes-hall↗

arXiv2001

Spin-parity dependent tunneling of magnetization in single-molecule magnets

Single-molecule magnets facilitate the study of quantum tunneling of magnetization at the mesoscopic level. The spin-parity effect is among the fundamental predictions that have yet to be clearly observed. It is predicted that quantum tunneling is suppressed at zero transverse field if the total spin of the magnetic system is half-integer (Kramers degeneracy) but is allowed in integer spin systems. The Landau-Zener method is used to measure the tunnel splitting as a function of transverse field. Spin-parity dependent tunneling is established by comparing the transverse field dependence of the tunnel splitting of integer and half-integer spin systems.

cond-mat.mes-hall↗

arXiv2001

On Ground State Tunneling in Mn$_{12}$-Acetate

We report Hall sensor measurements of the magnetic relaxation of Mn$_{12}$-acetate as a function of magnetic field applied along the easy axis of magnetization for a series of closely-spaced temperatures between 0.24 K and 1.9 K. We map out a region in the $H-T$ plane where ground state tunneling is observed, a region where tunneling proceeds via thermally-assisted tunneling, and a crossover region where both participate in the relaxation. We observe the occasional absence of ground-state tunneling under conditions where one would expect it to be present, and suggest a resolution to the enigma.

cond-mat↗

arXiv2001

A Distribution of Tunnel Splittings in Mn$_{12}$-Acetate

In magnetic fields applied parallel to the anisotropy axis, the relaxation of the magnetization of Mn$_{12}$ measured for different sweep rates is shown to collapse onto a single scaled curve. The form of the scaling implies that the dominant symmetry-breaking process that gives rise to tunneling is a locally varying second-order anisotropy, forbidden by tetragonal symmetry in the perfect crystal, which gives rise to a broad distribution of tunnel splittings in a real crystal of Mn$_{12}$-acetate. Different forms applied to even and odd-numbered steps provide a distinction between even step resonances (associated with crystal anisotropy) and odd resonances (which require a transverse component of magnetic field).

cond-mat↗

arXiv2000

Abrupt Transition between Thermally-Activated Relaxation and Quantum Tunneling in a Molecular Magnet

We report Hall sensor measurements of the magnetic relaxation of Mn$_{12}$ acetate as a function of magnetic field applied along the easy axis of magnetization. Data taken at a series of closely-spaced temperatures between 0.24 K and 1.4 K provide strong new evidence for an abrupt ``first-order'' transition between thermally-assisted relaxation and magnetic decay via quantum tunneling.

cond-mat.mes-hall↗