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E. del Barco

Publications and source records attributed to E. del Barco.

At least 19 recordsLinked to original sources
arXiv2024

Cooperative quantum tunneling of the magnetization in Fe-doped Li$_3$N

The spin-reversal in dilute Li$_2$(Li$_{1-x}$Fe$_{x}$)N with $x < 1$ % is dominated by resonant quantum tunneling of spatially well-separated states. We report on the effect of finite couplings between those states that give rise to cooperative, simultaneous quantum tunneling of two spins. This phenomenon, known as spin-spin cross relaxation, effectively elucidates the fine-structure observed in isothermal magnetization loops, a previously unresolved aspect. Temperature and field-dependent magnetization measurements were conducted over a range from T = 2 K to 300 K in applied fields of up to $μ_0H$ = 7 T. Magnetic dipole fields are computed numerically. Our findings affirm the absence of stoichiometric defects in Li$_2$(Li$_{1-x}$Fe$_{x}$)N and underscore its exemplary suitability as a model system for investigating spin-reversal processes at the microscopic level. This is attributed to its comparatively simple crystal structure, the availability of large single crystals, elevated characteristic energies, and well-defined energy levels

cond-mat.str-el↗
arXiv2018

Extreme field-sensitivity of the magnetic tunneling in Fe-doped Li$_3$N

The magnetic properties of dilute Li$_2$(Li$_{1-x}$Fe$_x$)N with $x \sim 0.001$ are dominated by the spin of single, isolated Fe atoms. Below $T = 10$ K the spin-relaxation times become temperature-independent indicating a crossover from thermal excitations to the quantum tunneling regime. We report on a strong increase of the spin-flip probability in $\textit{transverse}$ magnetic fields that proves the resonant character of this tunneling process. $\textit{Longitudinal}$ fields, on the other hand, lift the ground-state degeneracy and destroy the tunneling condition. An increase of the relaxation time by four orders of magnitude in applied fields of only a few milliTesla reveals exceptionally sharp tunneling resonances. Li$_2$(Li$_{1-x}$Fe$_x$)N represents a comparatively simple and clean model system that opens the possibility to study quantum tunneling of the magnetization at liquid helium temperatures.

cond-mat.mtrl-sci↗
arXiv2015

Dynamical spin injection at a quasi-one-dimensional ferromagnet-graphene interface

We present a study of dynamical spin injection from a three-dimensional ferromagnet into two-dimensional single-layer graphene. Comparative ferromagnetic resonance (FMR) studies of ferromagnet/graphene strips buried underneath the central line of a coplanar waveguide show that the FMR linewidth broadening is the largest when the graphene layer protrudes laterally away from the ferromagnetic strip, indicating that the spin current is injected into the graphene areas away from the area directly underneath the ferromagnet being excited. Our results confirm that the observed damping is indeed a signature of dynamical spin injection, wherein a pure spin current is pumped into the single-layer graphene from the precessing magnetization of the ferromagnet. The observed spin pumping efficiency is difficult to reconcile with the expected backflow of spins according to the standard spin pumping theory and the characteristics of graphene, and constitutes an enigma for spin pumping in two-dimensional structures.

cond-mat.mes-hall↗
arXiv2012

Dynamic Spin Injection into Chemical Vapor Deposited Graphene

We demonstrate dynamic spin injection into chemical vapor deposition (CVD) grown graphene by spin pumping from permalloy (Py) layers. Ferromagnetic resonance measurements at room temperature reveal a strong enhancement of the Gilbert damping at the Py/graphene interface, exceeding that observed in even Py/platinum interfaces. Similar results are also shown on Co/graphene layers. This enhancement in the Gilbert damping is understood as the consequence of spin pumping at the interface driven by magnetization dynamics. Our observations suggest a strong enhancement of spin-orbit coupling in CVD graphene, in agreement with earlier spin valve measurements.

cond-mat.mes-hall↗
arXiv2011

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↗
arXiv2010

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↗
arXiv2010

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↗
arXiv2009

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↗
arXiv2008

High-Frequency Microstrip Cross Resonators for Circular Polarization EPR Spectroscopy

In this article we discuss the design and implementation of a novel microstrip resonator which allows for the absolute control of the microwaves polarization degree for frequencies up to 30 GHz. The sensor is composed of two half-wavelength microstrip line resonators, designed to match the 50 Ohms impedance of the lines on a high dielectric constant GaAs substrate. The line resonators cross each other perpendicularly through their centers, forming a cross. Microstrip feed lines are coupled through small gaps to three arms of the cross to connect the resonator to the excitation ports. The control of the relative magnitude and phase between the two microwave stimuli at the input ports of each line allows for tuning the degree and type of polarization of the microwave excitation at the center of the cross resonator. The third (output) port is used to measure the transmitted signal, which is crucial to work at low temperatures, where reflections along lengthy coaxial lines mask the signal reflected by the resonator. EPR spectra recorded at low temperature in an S= 5/2 molecular magnet system show that 82%-fidelity circular polarization of the microwaves is achieved over the central area of the resonator.

cond-mat.mes-hall↗
arXiv2008

Geometrical control of the magnetization direction in high aspect-ratio PdNi ferromagnetic nano-electrodes

We present a study of electron-beam evaporated Pd0.4Ni0.6 alloy thin films by means of ferromagnetic resonance measurements on extended films of varying thickness and anisotropic magnetoresistance measurements of lithographically patterned high aspect-ratio ferromagnetic electrodes, respectively. The results reveal that the direction of the magnetization strongly depends on the electrode lateral dimensions, transitioning from in-plane magnetization for extended films to out-of-the-plane magnetization for electrode widths below 2-3 microns, reaching 58 degrees off-plane for 100 nm-wide nanoelectrodes.

cond-mat.str-el↗
arXiv2008

On-chip Integration of High-Frequency Electron Paramagnetic Resonance Spectroscopy and Hall-Effect Magnetometry

A sensor that integrates high sensitivity micro-Hall effect magnetometry and high-frequency electron paramagnetic resonance spectroscopy capabilities on a single semiconductor chip is presented. The Hall-effect magnetometer was fabricated from a two dimensional electron gas GaAs/AlGaAs heterostructure in the form of a cross, with a 50x50 um2 sensing area. A high-frequency microstrip resonator is coupled with two small gaps to a transmission line with a 50 Ohms impedance. Different resonator lengths are used to obtain quasi-TEM fundamental resonant modes in the frequency range 10-30 GHz. The resonator is positioned on top of the active area of the Hall-effect magnetometer, where the magnetic field of the fundamental mode is largest, thus optimizing the conversion of microwave power into magnetic field at the sample position. The two gaps coupling the resonator and transmission lines are engineered differently. The gap to the microwave source is designed to optimize the loaded quality factor of the resonator (Q = 150) while the gap for the transmitted signal is larger. This latter gap minimizes losses and prevents distortion of the resonance while enabling measurement of the transmitted signal. The large filling factor of the resonator permits sensitivities comparable to that of high-quality factor resonant cavities. The integrated sensor enables measurement of the magnetization response of micron scale samples upon application of microwave fields. In particular, the combined measurement of the magnetization change and the microwave power under cw microwave irradiation of single crystal of molecular magnets is used to determine of the energy relaxation time of the molecular spin states. In addition, real time measurements of the magnetization dynamics upon application of fast microwave pulses are demonstrated

cond-mat.str-el↗
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↗
arXiv2006

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↗
arXiv2005

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↗
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↗
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↗