arXiv subjects

S. Hill

Publications and source records attributed to S. Hill.

At least 37 records · Page 2Linked to original sources

arXiv2004

Dendritic flux jumps in an organic superconducting crystal

Angle dependent torque measurements have been carried out on the organic superconductor, kappa-(ET)2Cu(NCS)2 at extremely low temperatures (25 - 300 mK). Magneto-thermal instabilities are observed in the form of abrupt magnetization (flux) jumps for magnetic field sweeps of 0 - 20 tesla. A fractal analysis of the flux jumps indicates that the instabilities do show a self similar structure with a fractal dimension varying between 1.15 - 1.6. The fractal structure of the flux jumps in our sample shows a stricking similarity to that of MgB2 thin film samples, in which magneto-optical experiments have recently shown that the small flux jumps are due to the formation of dendritic flux structures. These smaller instabilities act to suppress the critical current density of these thin films. The similarity of the flux jump structure of our samples suggests that we are also observing the dendritic instability, but in a bulk sample rather than a thin film. This is the first observation of the dendritic instability in a bulk superconducing sample, and is likely due to the layered nature of kappa-(ET)2Cu(NCS)2, which results in a quasi-two dimensional flux structure over the majority of it's mixed state phase diagram.

cond-mat.supr-con↗

arXiv2004

Evidence for the S=9 excited state in Mn12-bromoacetate measured by electron paramagnetic resonance

We present high-frequency high-field electron paramagnetic resonance (EPR) measurements on the dodecanuclear manganese complex Mn12-bromoacetate (Mn12-BrAc). The crystal-field parameters are found to be identical to those of the original compound Mn12-acetate (Mn12-Ac). A detailed analysis of the frequency and temperature dependence of anomalous peaks observed in the EPR spectra of Mn12-BrAc enables us to locate the S=9 manifold at about 40 K above the Ms= +/-10 ground state of this nominally S=10 system. This is very close to the Ms = +/-6 state of the S = 10 manifold, thus suggesting pathways for the thermally assisted magnetization dynamics and related properties. Finally, the EPR fine structures recently attributed to disorder associated with the acetic acid of crystallization in Mn12-Ac are absent in the present measurements, thus suggesting that the Mn12-BrAc complex represents a more suitable candidate for measurements of quantum effects in high symmetry S=10 SMMs.

cond-mat.mes-hall↗

arXiv2003

Quantum Coherence in an Exchange-Coupled Dimer of Single-Molecule Magnets

A multi-high-frequency electron paramagnetic resonance method is used to probe the magnetic excitations of a dimer of single-molecule magnets. The measured spectra display well resolved quantum transitions involving coherent superposition states of both molecules. The behavior may be understood in terms of an isotropic superexchange coupling between pairs of single-molecule magnets, in analogy with several recently proposed quantum devices based on artificially fabricated quantum dots or clusters. These findings highlight the potential utility of supramolecular chemistry in the design of future quantum devices based on molecular nanomagnets.

cond-mat.mes-hall↗

arXiv2003

Characterization of the S = 9 excited state in Fe8Br8 by Electron Paramagnetic Resonance

High Frequency electron paramagnetic resonance has been used to observe the magnetic dipole, $Δ$ M$_s$ = $\pm$ 1, transitions in the $S = 9$ excited state of the single molecule magnet Fe$_8$Br$_8$. A Boltzmann analysis of the measured intensities locates it at 24 $\pm$ 2 K above the $S = 10$ ground state, while the line positions yield its magnetic parameters D = -0.27 K, E = $\pm$0.05 K, and B$_4^0$ = -1.3$\times$ 10$^{-6}$ K. D is thus smaller by 8% and E larger by 7% than for $S = 10$. The anisotropy barrier for $S = 9$ is estimated as 22 K,which is 25% smaller than that for $S = 10$ (29 K). These data also help assign the spin exchange constants(J's) and thus provide a basis for improved electronic structure calculations of Fe$_8$Br$_8$.

cond-mat.str-el↗

arXiv2003

Mapping the Fermi velocity in the quasi-2D organic conductor k-(BEDT-TTF)2I3

We demonstrate a new method for determining the Fermi velocity in quasi-two-dimensional (Q2D) organic conductors. Application of a magnetic field parallel to the conducting layers results in periodic open orbit quasiparticle trajectories along the Q2D Fermi surface. Averaging of this motion over the Fermi surface leads to a resonance in the interlayer microwave conductivity. The resonance frequency is simply related to the extremal value of the Fermi velocity perpendicular to the applied field. Thus, angle dependent microwave studies enable a complete mapping of the Fermi velocity. We illustrate the applicability of this method for the highly-2D organic conductor k-(BEDT-TTF)2I3.

cond-mat.str-el↗

arXiv2003

Definitive spectroscopic determination of the transverse interactions responsible for the magnetic quantum tunneling in Mn12-acetate

We present detailed angle-dependent single crystal electron paramagnetic resonance (EPR) data for field rotations in the hard plane of the S=10 single molecule magnet Mn12-acetate. A clear four-fold variation in the resonance positions may be attributed to an intrinsic fourth order transverse anisotropy (O44). Meanwhile, a four-fold variation of the EPR lineshapes confirms a recently proposed model wherein disorder associated with the acetic acid of crystallization induces a locally varying quadratic (rhombic) transverse anisotropy (O22). These findings explain most aspects of the magnetic quantum tunneling observed in Mn12-acetate.

cond-mat.mtrl-sci↗

arXiv2003

Electron Paramagnetic Resonance Linewidths and Lineshapes for the Molecular Magnets Fe8 and Mn12

We study theoretically Electron Paramagentic Resonance (EPR) linewidths for single crystals of the molecular magnets Fe$_8$ and Mn$_{12}$ as functions of energy eigenstates $M_s$, frequency, and temperature when a magnetic field along the easy axis is swept at fixed excitation frequency. This work was motivated by recent EPR experiments. To calculate the linewidths, we use density-matrix equations, including dipolar interactions and distributions of the uniaxial anisotropy parameter $D$ and the Landé $g$ factor. Our calculated linewidths agree well with the experimental data. We also examine the lineshapes of the EPR spectra due to local rotations of the magnetic anisotropy axes caused by defects in samples. Our preliminary results predict that this effect leads to asymmetry in the EPR spectra.

cond-mat↗

arXiv2003

Effects of D-strain, g-strain, and dipolar interactions on EPR linewidths of the molecular magnets Fe8 and Mn12

Electron paramagnetic resonance (EPR) measurements on single crystals of the molecular magnets Fe$_8$ and Mn$_{12}$ reveal complex nonlinearities in the linewidths as functions of energy eigenstate, frequency, and temperature. Using a density-matrix equation with distributions of the uniaxial anisotropy parameter $D$, the Landé $g$ factor, and dipolar interactions, we obtain linewidths in good agreement with experiments. Our study shows that the distribution in $D$ is common to the examined molecular magnets Fe$_8$ and Mn$_{12}$ regardless of the qualities of the samples. This could provide the basis for a proposed tunneling mechanism due to lattice defects. The distribution in $g$ is also quite significant for Mn$_{12}$.

cond-mat↗

arXiv2003

Role of dipolar and exchange interactions in the positions and widths of EPR transitions for the single-molecule magnets Fe8 and Mn12

We examine quantitatively the temperature dependence of the linewidths and line shifts in electron paramagnetic resonance experiments on single crystals of the single-molecule magnets Fe$_8$ and Mn$_{12}$, at fixed frequency, with an applied magnetic field along the easy axis. We include inter-molecular spin-spin interactions (dipolar and exchange) and distributions in both the uniaxial anisotropy parameter $D$ and the Landé $g$-factor. The temperature dependence of the linewidths and the line shifts are mainly caused by the spin-spin interactions. For Fe$_8$ and Mn$_{12}$, the temperature dependence of the calculated line shifts and linewidths agrees well with the trends of the experimental data. The linewidths for Fe$_8$ reveal a stronger temperature dependence than those for Mn$_{12}$, because for Mn$_{12}$ a much wider distribution in $D$ overshadows the temperature dependence of the spin-spin interactions. For Fe$_8$, the line-shift analysis suggests two competing interactions: a weak ferromagnetic exchange coupling between neighboring molecules and a longer-ranged dipolar interaction. This result could have implications for ordering in Fe$_8$ at low temperatures.

cond-mat↗

arXiv2003

Effect of an in-plane magnetic field on the interlayer phase coherence in the extreme-2D organic superconductor k-(BEDT-TTF)2Cu(NCS)2

Using a high-sensitivity cavity perturbation technique (40 to 180 GHz), we have probed the angle dependent interlayer magneto-electrodynamic response within the vortex state of the extreme two-dimensional organic superconductor k-(BEDT-TTF)2Cu(NCS)2. A previously reported Josephson plasma resonance [M. Mola et al., Phys. Rev. B 62, 5965 (2000)] exhibits a dramatic re-entrant behavior for fields very close (<1 degree) to alignment with the layers. In this same narrow angle range, a new resonant mode develops which appears to be associated with the non-equilibrium critical state. Fits to the angle dependence of the Josephson plasma resonance provide microscopic information concerning the superconducting phase correlation function within the vortex state. We also show that the effect of an in-plane magnetic field on the temperature dependence of the interlayer phase coherence is quite different from what we have previously observed for perpendicular magnetic fields.

cond-mat.supr-con↗

arXiv2003

Evidence for a very low-lying S = 9 excited state of the S = 10 single molecule magnet Mn12-acetate

We present a detailed investigation of the temperature and frequency dependence of the anomalous EPR transitions first observed in Mn12-acetate by Hill et al. [Phys. Rev. Lett. 80, 2453 (1998)]. The most dominant of these transitions manifest themselves as an extra series of EPR absorption peaks for spectra obtained with the DC field applied within the hard magnetic plane of a single crystal sample. Recent studies by Amigo et al. [Phys. Rev. B 65, 172403 (2002)] have attributed these extra peaks to a strain induced transverse quadratic anisotropy which gives rise to distinct Mn12-acetate species, each having a distinct EPR spectrum; on the basis of these measurements, it has been suggested that this transverse anisotropy is responsible for the tunneling in Mn12-acetate. Our temperature and frequency dependent measurements demonstrate unambiguously that these anomalous EPR absorptions vanish as the temperature tends to zero, thereby indicating that they correspond to transitions from an excited state of the molecule. We argue that this low lying excited state corresponds to an S = 9 multiplet having very similar zero-field crystal parameters to the S = 10 state, and lying only about 10-15 k_B above the S = 10 (M_S = +/-9) ground state. These findings also compare favorably with available neutron scattering data.

cond-mat.mtrl-sci↗

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

Interlayer electrodynamics in the organic superconductor k-(BEDT-TTF)_2Cu(NCS)_2: evidence for a transformation within the vortex state

A microwave cavity perturbation technique is used to probe the interlayer electrodynamics within the vortex state of the organic superconductor kappa-(BEDT-TTF)2Cu(NCS)2. A Josephson plasma mode is observed which is extremely sensitive to correlations in the locations of vortices in adjacent layers and may, therefore, be used to gauge collective effects between vortices and crystal pinning sites in the title compound. Our previous investigations [M. M. Mola et al., Phys. Rev. B 62 (2000) 5965] revealed a transformation from a correlated quasi-two-dimensional pinned vortex phase, to either a depinned or liquid state. In this study, we carry out a detailed analysis of the magnetic field dependence of the Josephson plasma frequency within the two phases. Our findings agree favorably with recent theoretical models: within the liquid state, the squared plasma frequency decays with the inverse of the magnetic field strength, B; whereas, in the pinned phase, a much slower decay is observed, which is indicative of weak pinning.

cond-mat.supr-con↗

arXiv2002

Determination of the Fermi Velocity by Angle-dependent Periodic Orbit Resonance Measurements in the Organic Conductor alpha-(BEDT-TTF)2KHg(SCN)4

We report detailed angle-dependent studies of the microwave (f=50 to 90 GHz) interlayer magneto-electrodynamics of a single crystal sample of the organic charge-density-wave (CDW) conductor alpha-(BEDT-TTF)2KHg(SCN)4. Recently developed instrumentation enables both magnetic field (B) sweeps for a fixed sample orientation and, for the first time, angle sweeps at fixed f/B. We observe series' of resonant absorptions which we attribute to periodic orbit resonances (POR) - a phenomenon closely related to cyclotron resonance. The angle dependence of the POR indicate that they are associated with the low temperature quasi-one-dimensional (Q1D) Fermi surface (FS) of the title compound; indeed, all of the resonance peaks collapse beautifully onto a single set of f/B versus angle curves, generated using a semiclassical magneto-transport theory for a single Q1D FS. We show that Q1D POR measurements provide one of the most direct methods for determining the Fermi velocity, without any detailed assumptions concerning the bandstructure; our analysis yields an average value of v_F=6.5x10^4 m/s. Quantitative analysis of the POR harmonic content indicates that the Q1D FS is strongly corrugated. This is consistent with the assumption that the low-temperature FS derives from a reconstruction of the high temperature quasi-two-dimensional FS, caused by the CDW instability. Detailed analysis of the angle dependence of the POR yields parameters associated with the CDW superstructure which are consistent with published results. Finally, we address the issue as to whether or not the interlayer electrodynamics are coherent in the title compound.

cond-mat.str-el↗

arXiv2002

Detailed single crystal EPR lineshape measurements for the single molecule magnets Fe8Br and Mn12-ac

It is shown that our multi-high-frequency (40-200 GHz) resonant cavity technique yields distortion-free high field EPR spectra for single crystal samples of the uniaxial and biaxial spin S = 10 single molecule magnets (SMMs) [Mn12O12(CH3COO)16(H2O)4].2CH3COOH.4H2O and [Fe8O2(OH)12(tacn)6]Br8.9H2O. The observed lineshapes exhibit a pronounced dependence on temperature, magnetic field, and the spin quantum numbers (Ms values) associated with the levels involved in the transitions. Measurements at many frequencies allow us to separate various contributions to the EPR linewidths, including significant D-strain, g-strain and broadening due to the random dipolar fields of neighboring molecules. We also identify asymmetry in some of the EPR lineshapes for Fe8, and a previously unobserved fine structure to some of the EPR lines for both the Fe8 and Mn12 systems. These findings prove relevant to the mechanism of quantum tunneling of magnetization in these SMMs.

cond-mat.mes-hall↗

arXiv2001

Quantum melting of the quasi-two-dimensional vortex lattice in kappa-(ET)2Cu(NCS)2

We report torque magnetization measurements in regions of the mixed state phase diagram (${\bf B}\simμ_o{\bf H}_{c2}$ and T$_c$/$10^3$) of the organic superconductor $κ-$(ET)$_2$Cu(NCS)$_2$ where quantum fluctuations are expected to dominate thermal effects. Over most of the field range below the irreversibility line (${\bf B}_{irr}$), magneto-thermal instabilities are observed in the form of flux jumps. The abrupt cessation of these instabilities just below ${\bf B}_{irr}$ indicates a quantum melting transition from a quasi-two-dimensional vortex lattice phase to a quantum liquid phase.

cond-mat.supr-con↗

arXiv2000

Magneto-thermal instabilities in kappa-(BEDT-TTF)2Cu(NCS)2

Angle and temperature dependent torque magnetization measurements are reported for the organic superconductor kappa-(BEDT-TTF)2Cu(NCS)2, at extremely low temperatures (approx. Tc/10^3). Magneto-thermal instabilities are observed in the form of abrupt magnetization (flux) jumps. We carry out an analysis of the temperature and field orientation dependence of these flux jumps based on accepted models for layered type-II superconductors. Using a simple Bean model, we also find a critical current density of 4x10^8 A/m^2 from the remnant magnetization, in agreement with previous measurements.

cond-mat.supr-con↗

arXiv2000

Josephson plasma resonance in k-(BEDT-TTF)2Cu(NCS)2

A cavity perturbation technique is used to study the microwave response of the organic superconductor k-(BEDT-TTF)2Cu(NCS)2. Observation of a Josephson plasma resonance, below Tc (approx. 10 K), enables investigation of the vortex structure within the mixed state of this highly anisotropic, type-II, superconductor. Contrary to previous assumptions, frequency dependent studies (28 - 153 GHz) indicate that the squared plasma frequency depends exponentially on the magnetic field strength. Such behavior has been predicted for a weakly pinned quasi-two-dimensional vortex lattice [Bulaevskii et al. Phys. Rev. Lett. 74, 801 (1995)], but has not so far been observed experimentally. Our data also suggests a transition in the vortex structure near the irreversibility line not previously reported for an organic superconductor using this technique.

cond-mat.supr-con↗