Search

We study the effect of uniaxial pressure on the magnetic hysteresis loops of the single-molecule magnet Mn_{12}-Ac. We find that the application of pressure along the easy axis increases the fields at which quantum tunneling of magnetization occurs. The observations are attributed to an increase in the molecule's magnetic anisotropy constant D of 0.142(1)%/kbar. The increase in D produces a small, but measurable increase in the effective energy barrier for magnetization reversal. Density-functional theory calculations also predict an increase in the barrier with applied pressure., Comment: version accepted by EPL; 6 pages, including 7 figures. Small changes and added references

We report the observation of strong coupling of a macroscopic ensemble of ~10^{16} Fe_8 molecular nanomagnets to the resonant mode of a microwave cavity. We use millimeter-wave spectroscopy to measure the splitting of the system's resonant frequency induced by the coupling between the spins and the cavity mode. The magnitude of this splitting is found to scale with Sqrt[N], where N is the number of collectively coupled spins. We control N by changing the system's temperature and, thereby, the populations of the relevant spin energy levels. Strong coupling is observed for two distinct transitions between spin energy states. Our results indicate that at low temperatures nearly all of the spins in the sample couple with the cavity's resonant mode even though there is substantial inhomogeneous broadening of the Fe8 spin resonances., Comment: Main text: 12 pages, including 3 figures. Supplement: 5 pages, including 2 figures. 17 pages total

Decoherence in Nature has become one of the most pressing problems in physics. Many applications, including quantum information processing, depend on understanding it; and fundamental theories going beyond quantum mechanics have been suggested [1-3], where the breakdown of quantum theory appears as an 'intrinsic decoherence', mimicking environmental decoherence [4]. Such theories cannot be tested until we have a handle on ordinary environmental decoherence processes. Here we show that the theory for insulating electronic spin systems can make accurate predictions for environmental decoherence in molecular-based quantum magnets [5]. Experimental understanding of decoherence in molecular magnets has been limited by short decoherence times, which make coherent spin manipulation extremely difficult [6-9]. Here we reduce the decoherence by applying a strong magnetic field. The theory predicts the contributions to the decoherence from phonons, nuclear spins, and intermolecular dipolar interactions, for a single crystal of the Fe8 molecular magnet. In experiments we find that the decoherence time varies strongly as a function of temperature and magnetic field. The theoretical predictions are fully verified experimentally - there are no other visible decoherence sources. Our investigation suggests that the decoherence time is ultimately limited by nuclear spins, and can be extended up to about 500 microseconds, by optimizing the temperature, magnetic field, and nuclear isotopic concentrations., Comment: Submitted version including 11 pages, 3 figures and online supporting materials. Appeared on Nature Advance Online Publication (AOP) on July 20th, 2011. (http://www.nature.com/nature/journal/vaop/ncurrent/full/nature10314.html)

A Mn4 single-molecule magnet displays asymmetric Berry-phase interference patterns in the transverse-field (HT) dependence of the magnetization tunneling probability when a longitudinal field (HL) is present, contrary to symmetric patterns observed for HL=0. Reversal of HL results in a reflection of the transverse-field asymmetry about HT=0, as expected on the basis of the time-reversal invariance of the spin-orbit Hamiltonian which is responsible for the tunneling oscillations. A fascinating motion of Berry-phase minima within the transverse-field magnitude-direction phase space results from a competition between noncollinear magnetoanisotropy tensors at the two distinct Mn sites., Comment: 4 double-column pages

We present a detailed study of the influence of various interactions on the spin quantum tunneling in a Mn12 wheel molecule. The effects of single-ion and exchange (spin-orbit) anisotropy are first considered, followed by an analysis of the roles played by secondary influences, e.g. disorder, dipolar and hyperfine fields, and magnetoacoustic interactions. Special attention is paid to the role of the antisymmetric Dzyaloshinski-Moriya (DM) interaction. This is done within the framework of a 12-spin microscopic model, and also using simplified dimer and tetramer approximations in which the electronic spins are grouped in 2 or 4 blocks, respectively. If the molecule is inversion symmetric, the DM interaction between the dimer halves must be zero. In an inversion symmetric tetramer, two independent DM vectors are allowed, but no new tunneling transitions are generated by the DM interaction. Experiments on the Mn12 wheel can only be explained if the molecular inversion symmetry is broken, and we explore this in detail using both models, focussing on the asymmetric disposition and rounding of Berry phase minima associated with quantum interference between states of opposite parity. A remarkable behavior exists for the `Berry phase zeroes' as a function of the directions of the internal DM vectors and the external transverse field. A rather drastic breaking of the molecular inversion-symmetry is required to explain the experiments; in the tetramer model this requires a reorientation of the DM vectors on one half of the molecule by nearly 180 degrees. This cannot be attributed to sample disorder. These results are of general interest for the quantum dynamics of tunneling spins, and lead to some interesting experimental predictions., Comment: Submitted to PRB. 23 double-column pages, 16 figures

We present low temperature magnetometry measurements on a new Mn3 single-molecule magnet (SMM) in which the quantum tunneling of magnetization (QTM) displays clear evidence for quantum mechanical selection rules. A QTM resonance appearing only at elevated temperatures demonstrates tunneling between excited states with spin projections differing by a multiple of three: this is dictated by the C3 symmetry of the molecule, which forbids pure tunneling from the lowest metastable state. Resonances forbidden by the molecular symmetry are explained by correctly orienting the Jahn-Teller axes of the individual manganese ions, and by including transverse dipolar fields. These factors are likely to be important for QTM in all SMMs., Comment: Physical Review Letters (in press) Preprint form: 16 pages, 4 figures

In a recent Letter [1], Wernsdorfer et al. report an experimental study of a Mn12 molecular wheel which shows essentially identical behavior to the Mn12 wheel studied by Ramsey et al. [2]. In their Letter, Wernsdorfer et al. use the same model of a dimer of two exchange-coupled spins used in [2] as a basis to extend the study of the influence of the Dzyaloshinskii-Moriya (DM) interaction on the quantum tunneling of the magnetization of this system; in particular, they show that a tilt of the DM vector away from the uniaxial anisotropy axis can account for the asymmetric nature of the quantum interference minima associated with resonances between states of opposite parity, e.g., k = 1(A). We want to stress that the inclusion of DM interactions in a system with inversion symmetry cannot mix states of opposite parity; i.e., the parity operator commutes with the Hamiltonian. Consequently, the use by Wernsdorfer et al. of a single DM vector in a centrosymmetric dimer is strictly forbidden since it implicitly violates parity conservation. The authors correctly point out that the lack of an inversion center between each pair of manganese ions on the wheel justifies the possibility of local DM interactions, even though the complete molecule has an inversion center. However, these local DM interactions must also satisfy the molecular inversion symmetry; i.e., they cannot mix states of opposite parity.We agree that such DM interactions are not always completely innocuous; e.g., they can mix spin states having the same parity. Indeed, in kagome systems [3] (cited in [1]), this can lead to weak ferromagnetism. Nevertheless, the inversion symmetry of the lattice is preserved and parity is still conserved., Comment: Version published in PRL. Preprint: 4 pages, 1 figure

Spin relaxation between the two lowest-lying spin-states has been studied in the S=4 single molecule magnet Ni$_4$ under steady state conditions of low amplitude and continuous microwave irradiation. The relaxation rate was determined as a function of temperature at two frequencies, 10 and 27.8 GHz, by simultaneously measuring the magnetization and the absorbed microwave power. A strong temperature dependence is observed below 1.5 K, which is not consistent with a direct single-spin-phonon relaxation process. The data instead suggest that the spin relaxation is dominated by a phonon bottleneck at low temperatures and occurs by an Orbach mechanism involving excited spin-levels at higher temperatures. Experimental results are compared with detailed calculations of the relaxation rate using the universal density matrix equation., Comment: 6 pages, 4 figures, submitted to Europhys. Lett

Dilute frozen solutions of the single molecule magnet Ni$_4$ (S=4) have been studied using high frequency D-band (130 GHz) EPR. Despite the random orientation of the molecules, well defined EPR absorption peaks are observed, due to the strong variation of the splittings between the different spin-states on magnetic field. Temperature dependent studies above 4 K and comparison with simulations enable identification of the spin transitions and determination of the Hamiltonian parameters. The latter are found to be close to those of Ni$_4$ single crystals. No echo was detected from Ni$_4$ in pulsed experiments, which sets an upper bound of about 50 ns on the spin coherence time., Comment: 4 pages, 3 figures, accepted for publication in Journal of Applied Physics (52nd MMM conference proceedings)

We measure magnetization changes in a single crystal of the single-molecule magnet Fe8 when exposed to intense, short (<20 $\mu$s) pulses of microwave radiation resonant with the m = 10 to 9 transition. We find that radiation induces a phonon bottleneck in the system with a time scale of ~5 $\mu$s. The phonon bottleneck, in turn, drives the spin dynamics, allowing observation of thermally assisted resonant tunneling between spin states at the 100-ns time scale. Detailed numerical simulations quantitatively reproduce the data and yield a spin-phonon relaxation time of T1 ~ 40 ns., Comment: 6 RevTeX pages, including 4 EPS figures, version accepted for publication

Integrated magnetic sensors that allow simultaneous EPR and magnetization measurements have been developed to study single molecule magnets. A high frequency microstrip resonator has been integrated with a micro-Hall effect magnetometer. EPR spectroscopy is used to determine the energy splitting between the low lying spin-states of a Ni$_4$ single crystal, with an S=4 ground state, as a function of applied fields, both longitudinal and transverse to the easy axis at 0.4 K. Concurrent magnetization measurements show changes in spin-population associated with microwave absorption. Such studies enable determination of the energy relaxation time of the spin system., Comment: 4 pages, 4 figures, accepted for publication (Proceedings of the 10th Joint MMM/Intermag Conference, which will be published as special issues of the Journal of Applied Physics)

EPR studies of a Ni4 single-molecule magnet yield the zero-field-splitting (zfs) parameters, D, B40 and B44, based on a giant spin approximation (GSA) with S = 4. Experiments on an isostructural Ni-doped Zn4 crystal establish the Ni(II) ion zfs parameters. The 4th-order zfs parameters in the GSA arise from the interplay between the Heisenberg interaction, Js1.s2, and the 2nd-order single-ion anisotropy, giving rise to mixing of higher lying states into the S = 4 state. Consequently, J directly influences the zfs in the ground state, enabling its direct determination by EPR., Comment: 5 pages, including figures

We describe an experiment aimed at measuring the spin dynamics of the Fe8 single-molecule magnet in the presence of pulsed microwave radiation. In earlier work, heating was observed after a 0.2-ms pulse of intense radiation, indicating that the spin system and the lattice were out of thermal equilibrium at millisecond time scale [Bal et al., Europhys. Lett. 71, 110 (2005)]. In the current work, an inductive pick-up loop is used to probe the photon-induced magnetization dynamics between only two levels of the spin system at much shorter time scales (from ns to us). The relaxation time for the magnetization, induced by a pulse of radiation, is found to be on the order of 10 us., Comment: 3 RevTeX pages, including 3 eps figures. The paper will appear in the Journal of Applied Physics as MMM'05 conference proceedings

Microwave radiation applied to single-molecule magnets can induce large magnetization changes when the radiation is resonant with transitions between spin levels. These changes are interpreted as due to resonant heating of the sample by the microwaves. Pulsed-radiation studies show that the magnetization continues to decrease after the radiation has been turned off with a rate that is consistent with the spin's characteristic relaxation rate. The measured rate increases with pulse duration and microwave power, indicating that greater absorbed radiation energy results in a higher sample temperature. We also performed numerical simulations that qualitatively reproduce many of the experimental results. Our results indicate that experiments aimed at measuring the magnetization dynamics between two levels resonant with the radiation must be done much faster than the >20-microsecond time scales probed in these experiments., Comment: 6 RevTeX pages, including 8 eps figures. Revision: Simulations added to paper. Version accepted by J. Appl. Phys. (MMM'05 conference proceedings)

We present high-frequency angle-dependent EPR data for crystals of [NixZn1-x(hmp)(t-BuEtOH)Cl]4 (x = 1 and 0.02). The x = 1 complex behaves as a single-molecule magnet at low temperatures, displaying hysteresis and exceptionally fast magnetization tunneling. We show that this behavior is related to a 4th-order transverse crystal-field interaction, which produces a significant tunnel-splitting (~10 MHz) of the ground state of this S = 4 system. The magnitude of the 4th-order anisotropy, and the dominant axial term (D), can be related to the single-ion interactions (Di and Ei) at the individual NiII sites, as determined for the x = 0.02 crystals., Comment: 11 pages including 2 figures

The spatial profile of the magnetization of Mn12 crystals in a swept magnetic field applied along the easy axis is determined from measurements of the local magnetic induction along the sample surface using an array of Hall sensors. We find that the magnetization is not uniform inside the sample, but rather shows some spatial oscillations which become more prominent around the resonance field values. Moreover, it appears that different regions of the sample are at resonance at different values of the applied field and that the sweep rate of the internal magnetic induction is spatially non-uniform. We present a model which describes the evolution of the non-uniformities as a function of the applied field. Finally we show that the degree of non-uniformity can be manipulated by sweeping the magnetic field back and forth through part of the resonance., Comment: 6 pages, 5 figures; A typo was corrected in Eq. (8)

Resonant microwave radiation applied to a single crystal of the molecular magnet Fe_8 induces dramatic changes in the sample's magnetization. Transitions between excited states are found even though at the nominal system temperature these levels have negligible population. We find evidence that the sample heats significantly when the resonance condition is met. In addition, heating is observed after a short pulse of intense radiation has been turned off, indicating that the spin system is out of equilibrium with the lattice., Comment: Version to appear in Europhysics Letters. Minor changes and updated references

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., Comment: 4 RevTeX pages, 3 eps figures

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., Comment: 4 two-coulumn pages, 4 figures

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., Comment: 16 pages, 3 figures

The symmetry of magnetic quantum tunneling (MQT) in the single molecule magnet Mn12-acetate has been determined by sensitive low-temperature magnetic measurements in the pure quantum tunneling regime and high frequency EPR spectroscopy in the presence of large transverse magnetic fields. The combined data set definitely establishes the transverse anisotropy terms responsible for the low temperature quantum dynamics. MQT is due to a disorder induced locally varying quadratic transverse anisotropy associated with rhombic distortions in the molecular environment (2nd order in the spin-operators). This is superimposed on a 4th order transverse magnetic anisotropy consistent with the global (average) S4 molecule site symmetry. The hard axes associated with these forms of the transverse anisotropy are not collinear, leading to a complex interplay between local and global symmetries, the consequences of which are analyzed in detail., Comment: 26 two-column pages, 34 figures - content changed Accepted in Journal of Low Temperature Physics

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., Comment: 4 pages

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., Comment: 4 pages, 4 figures

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., Comment: 4 pages, 4 figures

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., Comment: 6 pages, 9 figures, ICM 2003 in Rome

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., Comment: 2 pages, 2 figures, ICM 2003 in Rome

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., Comment: 4 pages and 3 figures

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., Comment: To appear in the proceedings of 2002 MRS fall meeting

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., Comment: Europhysics Letters (in press). 7 pages, including 3 figures

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., Comment: minor corrections (PACS nos, signs in Fig. 2)

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., Comment: 5 pages, 5 figures

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., Comment: 4 pages, 6 figures

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., Comment: 3 pages, 4 figures, MMM'01 conference (12-16 Nov.)

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., Comment: 5 pages including 4 figures. Minor revisions to clarify explanations

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)., Comment: 4 pages, 5 figures. New title; text more clearly written

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., Comment: 4 pages, including 7 figures

The term in spin Hamiltonian, which determines the quantum tunneling rate in Mn12, is measured with neutron scattering. It is much smaller than previously reported values. This may imply that other mechanisms such as hyperfine fields may be more important in driving the tunneling., Comment: 1 page, 1 figure, comment to Phys Rev Letter

We report point by point measurements below the blocking temperature of the magnetic relaxation of Mn$_{12}$-acetate as a function of magnetic field applied along the easy axis of magnetization. Unexpectedly complex structure is observed which we attribute to the effect of higher-order terms of the spin Hamiltonianon on the tunneling process., Comment: 4 pages. Revised version includes new references and acknowledgments

We report zero-field inelastic neutron scattering experiments on a deuterated powder sample of Mn12-Acetate consisting of a large number of nominally identical spin-10 magnetic clusters. Our resolution enables us to see a series of peaks corresponding to transitions between the anisotropy levels within the spin-10 manifold. A fit to the spin Hamiltonian yields an anisotropy constant D=0.54 K and a fourth-order diagonal anisotropy coefficient A = 1.2x10^-3 K. Performed in the absence of a magnetic field, our experiments do not involve the g-values as fitting parameters, thereby yielding particularly reliable values of D and A., Comment: Submission to Conference on Magnetism and Magnetic Materials. Will appear in proceedings of the conference published in JAP in April 1999