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D. N. Hendrickson

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

At least 19 recordsLinked to original sources

The effect of uniaxial pressure on the magnetic anisotropy of the Mn_{12}-Ac single-molecule magnet

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.

cond-mat.mes-hall

Collective coupling of a macroscopic number of single-molecule magnets with a microwave cavity mode

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.

cond-mat.mes-hall

Decoherence in Crystals of Quantum Molecular Magnets

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.

cond-mat.mes-hall

Asymmetric Berry-Phase Interference Patterns in a Single-Molecule Magnet

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.

cond-mat.mes-hall

Tunneling and inversion symmetry in single-molecule magnets: the case of the Mn12 wheel molecule

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.

cond-mat.mtrl-sci

Comment on "Influence of Dzyaloshinskii-Moriya Exchange Interaction on Quantum Phase Interference of Spins"

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.

cond-mat.mes-hall

Manifestation of Spin Selection Rules on the Quantum Tunneling of Magnetization in a Single Molecule Magnet

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.

cond-mat.mes-hall

Magnetization relaxation in the single molecule magnet Ni$_4$ under continuous microwave irradiation

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.

cond-mat.mes-hall

Radiation- and Phonon-Bottleneck-Induced Tunneling in the Fe8 Single-Molecule Magnet

We measure magnetization changes in a single crystal of the single-molecule magnet Fe8 when exposed to intense, short (<20 $μ$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 $μ$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.

cond-mat.mes-hall

High frequency EPR on dilute solutions of the single molecule magnet Ni$_4$

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.

cond-mat.other

Magnetization and EPR studies of the single molecule magnet Ni$_4$ with integrated sensors

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.

cond-mat.mtrl-sci

Limitations of the Giant Spin Hamiltonian in Explaining Magnetization Tunneling in a Single-Molecule Magnet

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.

cond-mat.mes-hall

Photon-Induced Magnetization Changes in Single-Molecule Magnets

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.

cond-mat.mes-hall

Measurement of Magnetization Dynamics in Single-Molecule Magnets Induced by Pulsed Millimeter-Wave Radiation

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.

cond-mat.mes-hall

Local Measurements of Magnetization in Mn12 Crystals

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.

cond-mat.mes-hall

Origin of the fast magnetization tunneling in the single-molecule magnet [Ni(hmp)(tBuEtOH)Cl]4

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.

cond-mat.mes-hall

Non-equilibrium Magnetization Dynamics in the Fe_8 Single-Molecule Magnet Induced by High-Intensity Microwave Radiation

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.

cond-mat.mes-hall

Symmetry of Magnetic Quantum Tunneling in the Single-Molecule Magnet Mn12-Acetate

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.

cond-mat.mes-hall