Ramsey et al. [Nature Phys. 4, 277-281 (2008)] report the observation of quantum interference associated with tunnelling trajectories between states of different total spin length in a dimeric molecular nanomagnet. They argue that the interference is a consequence of the unique characteristics of a molecular Mn12 wheel, which behaves as a molecular dimer with weak ferromagnetic exchange coupling.
We show here that the data published by Ramsey et al. are not consistent and unfortunately mostly wrong. We show further that the Landau-Zener (LZ) formula, which links the tunnel probability with the tunnel splitting, can only be applied in a well-defined experimental region, which lays outside the region accessed by Ramsey and colleagues. Only a lower-limit estimate of the tunnel splitting can be obtained, showing that the observed transition cannot be explained with the dimer model. We also present other shortcomings of the paper questioning the dimer model, and that the alignment of the magnetic field is crucial for observing quantum interference.
We present here an exact version of our response (dated April 27) to Wernsdorfer's correspondence submitted to Nature Physics on March 31, 2008. After consultation with a referee, Nature Physics chose not publish any part of this exchange. We would therefore like to point out that our original study has now been considered favorably by four separate referees chosen by Nature Physics. Unfortunately, Wernsdorfer subsequently posted two further variations of his correspondence on this archive (arXiv:0804.1246v1 and arXiv:0804.1246v2). We note that aspects of the most recent posting (dated after s…
We study the phase transition of the escape rate of exchange-coupled dimer of single-molecule magnets which are coupled either ferromagnetic ally or antiferromagnetically in a staggered magnetic field and an easy $z$-axis anisotropy. The Hamiltonian for this system has been used to study molecular dimer nanomagnets [Mn$_4$]$_2$. We generalize the method of mapping a single-molecule magnetic spin problem onto a quantum-mechanical particle to dimeric molecular nanomagnets. The problem is mapped to a single particle quantum-mechanical Hamiltonian in terms of the relative coordinate and a coordina…
We present magnetization measurements on the single molecule magnet Mn6, revealing various tunnel transitions inconsistent with a giant-spin description. We propose a dimeric model of the molecule with two coupled spins S=6, which involves crystal-field anisotropy, symmetric Heisenberg exchange interaction, and antisymmetric Dzyaloshinskii-Moriya exchange interaction. We show that this simplified model of the molecule explains the experimentally observed tunnel transitions and that the antisymmetric exchange interaction between the spins gives rise to tunneling processes between spin states be…
We study spin tunneling in a magnetic nanoparticle with biaxial anisotropy that is free to rotate about its anisotropy axis. Exact instanton of the coupled equations of motion is found that connects degenerate classical energy minima. We show that mechanical freedom of the particle renormalizes magnetic anisotropy and increases the tunnel splitting.
Time-dependent specific heat experiments on the molecular nanomagnet Fe8 and the isotopic enriched analogue 57Fe8 are presented. The inclusion of the 57Fe nuclear spins leads to a huge enhancement of the specific heat below 1 K, ascribed to a strong increase in the spin-lattice relaxation rate Gamma arising from incoherent, nuclear-spin-mediated magnetic quantum tunneling in the ground-doublet. Since Gamma is found comparable to the expected tunneling rate, the latter process has to be inelastic. A model for the coupling of the tunneling levels to the lattice is presented. Under transverse fie…
We show that direct current in a tantalum microstrip can induce steady-state magnetic oscillations in an adjacent nanomagnet through spin torque from the spin Hall effect (SHE). The oscillations are detected electrically via a magnetic tunnel junction (MTJ) contacting the nanomagnet. The oscillation frequency can be controlled using the MTJ bias to tune the magnetic anisotropy. In this 3-terminal device the SHE torque and the MTJ bias therefore provide independent controls of the oscillation amplitude and frequency, enabling new approaches for developing tunable spin torque nano-oscillators.
We study the spin nutation effects of the molecular nanomagnet on the Josephson current through a superconductor$|$molecular nanomagnet$|$superconductor tunnel junction. We explicitly demonstrate that due to the spin nutation of the molecular nanomagnet two oscillatory terms emerge in the $ac$ Josephson current in addition to the conventional $ac$ Josephson current. Some resonances occur in the junction due to the interactions of the transported quasiparticles with the bias voltage and molecular nanomagnet spin dynamics. The appearance of them indicate that the energy exchanged during these in…
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 meso…
The Landau Zener method allows to measure very small tunnel splittings Δin molecular clusters Fe_8. The observed oscillations of Δas a function of the magnetic field applied along the hard anisotropy axis are explained in terms of topological quantum interference of two tunnel paths of opposite windings. Studies of the temperature dependence of the Landau Zener transition rate P gives access to the topological quantum interference between exited spin levels. The influence of nuclear spins is demonstrated by comparing P of the standard Fe_8 sample with two isotopically substituted samples. The …
A new mechanism is proposed for the magnetization reversal of molecular nanomagnets such as \Fe8. In this process the spin tunnels from the lowest state near one easy direction to the first excited state near the opposite easy direction, and subsequently decays to the second easy direction with the emission of a phonon, or it first emits a phonon and then tunnels to the final state. This mechanism is the simplest imaginable one that allows magnetization relaxation in the presence of a longitudinal magnetic field that is so large that the nuclear spin environment cannot absorb the energy requir…
The behavior of molecular nanomagnets in periodic magnetic field transverse to the easy axis direction is investigated. It is shown that at sufficiently strong field the tunneling time can be considerably reduced.
Single molecule magnets straddle the classical and quantum mechanical worlds, displaying many fascinating phenomena. They may have important technological applications in information storage and quantum computation. We review the physical properties of two prototypical molecular nanomagnets, Mn_12-acetate and Fe_8: each behaves as a rigid, spin-10 object, and exhibits tunneling between up and down directions. As temperature is lowered, the spin reversal process evolves from thermal activation to pure quantum tunneling. At low temperatures, magnetic avalanches occur in which the magnetization o…
The magnetization of the prototypical molecular magnet Mn12-acetate exhibits a series of sharp steps at low temperatures due to quantum tunneling at specific resonant values of magnetic field applied along the easy c-axis. An abrupt reversal of the magnetic moment of such a crystal can also occur as an avalanche, where the spin reversal proceeds along a "deflagration" front that travels through the sample at subsonic speed. In this article we review experimental results that have been obtained for the ignition temperature and the speed of propagation of magnetic avalanches in molecular nanomag…
We present details about an experimental method based on the Landau Zener model which allows to measure very small tunnel splittings $Δ$ in molecular clusters Fe8. The measurements are performed with an array of micro-SQUIDs. The observed oscillations of Delta as a function of the magnetic field applied along the hard anisotropy axis are explained in terms of topological quantum interference of two tunnel paths of opposite windings. Transitions between M = -S and (S - n), with n even or odd, revealed a parity (symmetry) effect which is analogous to the suppression of tunneling predicted for ha…
We demonstrate a possibility to manipulate the magnetic coupling between two nanomagnets with a help of ac electric field. In the scheme suggested the magnetic coupling in question is mediated by a magnetic particle contacting with both of the nanomagnets through the tunnel barriers. The electric field providing a successive suppression of the barriers leads to pumping of magnetization through the mediating particle. Time dependent dynamics of the particle magnetization allows to to switch between ferro- and antiferromagnetic couplings.
We report the possibility of achieving an order of magnitude reduction in the energy dissipation needed to write bits in perpendicular magnetic tunnel junctions (p-MTJs) by simulating the magnetization dynamics under a combination of resonant surface acoustic waves (r-SAW) and spin-transfer-torque (STT). The magnetization dynamics were simulated using the Landau-Lifshitz-Gilbert equation under macrospin assumption with the inclusion of thermal noise. The resonant magnetization dynamics in the magnetostrictive nanomagnet build over few 10s of cycles of SAW application that drives the magnetizat…
We study Landau-Zener macroscopic quantum transitions in ferromagnetic metal nanoparticles containing on the order of 100 atoms. The model that we consider is described by an effective giant-spin Hamiltonian, with a coupling to a random transverse magnetic field mimicking the effect of quasiparticle excitations and structural disorder on the gap structure of the spin collective modes. We find different types of time evolutions depending on the interplay between the disorder in the transverse field and the initial conditions of the system. In the absence of disorder, if the system starts from a…
Magnetization measurements of Mn12 molecular nanomagnets with spin ground states of S = 10 and S = 19/2 showresonance 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. Spin-parity dependent tunneling is established by comparing the quantum phase interference of integer and half-integer spin systems.
We present an accurate way to detect spin dynamics of a nutating molecular nanomagnet by inserting it in a tunnel Josephson junction and studying the current voltage (I-V) characteristic. The spin nutation of the molecular nanomagnet is generated by applying two circularly polarized magnetic fields. We demonstrate that modulation of the Josephson current by the nutation of the molecular nanomagnet's spin appears as a stepwise structure like Shapiro steps in the I-V characteristic of the junction. Width and heights of these Shapiro-like steps are determined by two parameters of the spin nutatio…
In large magnetoresistance devices spin torque-induced changes in resistance can produce GHz current and voltage oscillations which can affect magnetization reversal. In addition, capacitive shunting in large resistance devices can further reduce the current, adversely affecting spin torque switching. Here, we simultaneously solve the Landau-Lifshitz-Gilbert equation with spin torque and the transmission line telegrapher's equations to study the effects of resistance feedback and capacitance on magnetization reversal of both spin valves and magnetic tunnel junctions. While for spin valves para…
We present an experimental study of the {\em nonlinear} susceptibility of Mn$_{12}$ single-molecule magnets. We investigate both their thermal-equilibrium and dynamical nonlinear responses. The equilibrium results show the sensitivity of the nonlinear susceptibility to the magnetic anisotropy, which is nearly absent in the linear response for axes distributed at random. The nonlinear dynamic response of Mn$_{12}$ was recently found to be very large and displaying peaks reversed with respect to classical superparamagnets [F. Luis {\em et al.}, Phys. Rev. Lett. {\bf 92}, 107201 (2004)]. Here we …
As an extension of two-level quantum bits (qubits), multilevel systems, so-called qudits, where d represents the Hilbert space dimension, have been predicted to reduce the number of iterations in quantum computation algorithms. This has been tested in the well-known [TbPc2]0 SMM, which allowed the implementation of the Grover algorithm in a single molecular unit. In the quest for molecular systems possessing an increased number of accessible nuclear spin states, we explore herein a dimeric Tb2-SMM via single crystal μ-SQUID measurements at sub-Kelvin temperatures. We observe ferromagnetic inte…
In the molecular nanomagnet Fe$_{8}$ tunneling can occur from a metastable state to an excited state followed by a transition to the ground state. This transition is accompanied by an energy release of $115.6$GHz. We constructed an experimental setup to measure whether this energy is released in the form of thermal or electromagnetic energy. Contrary to a previous publication we find no evidence for release of electromagnetic radiation. Our results for transitions between the first and second excited states to the ground state are consistent with a release of only thermal energy. This energy r…
A P-N junction engineered within a Dirac cone system acts as a gate tunable angular filter based on Klein tunneling. For a 3D topological insulator with substantial bandgap, such a filter can produce a charge-to-spin conversion due to the dual effects of spin-momentum locking and momentum filtering. We analyze how spins filtered at an in-plane topological insulator PN junction (TIPNJ) interact with a nanomagnet, and argue that the intrinsic charge-to-spin conversion does not translate to an external gain if the nanomagnet also acts as the source contact. Regardless of the nanomagnet's position…
We show that the dynamic magnetic susceptibility and the superparamagnetic blocking temperature of an Fe8 single molecule magnet oscillate as a function of the magnetic field Hx applied along its hard magnetic axis. These oscillations are associated with quantum interferences, tuned by Hx, between different spin tunneling paths linking two excited magnetic states. The oscillation period is determined by the quantum mixing between the ground S=10 and excited multiplets. These experiments enable us to quantify such mixing. We find that the weight of excited multiplets in the magnetic ground stat…
In a nanomagnet (whose total spin S< 1000), very small polarized currents can lead to magnetic reversal. Treating on the same footing the transport and magnetic properties of a nanomagnet connected to magnetic leads via tunneling barriers, we derive a closed equation for the time evolution of the magnetization. The interplay between Coulomb blockade phenomena and magnetism gives some additional structure to the current induced spin torque. In addition to the possibility of stabilizing uniform spin waves, we find that the system is highly hysteretic: up to three different magnetic states can be…
This mini-review presents a simple and accessible summary on the fascinating physics of quantum nanomagnets coupled to a nuclear spin bath. These chemically synthesized systems are an ideal test ground for the theories of decoherence in mesoscopic quantum degrees of freedom, when the coupling to the environment is local and not small. We shall focus here on the most striking quantum phenomenon that occurs in such nanomagnets, namely the tunneling of their giant spin through a high anisotropy barrier. It will be shown that perturbative treatments must be discarded, and replaced by a more sophis…
We study electromagnetic interaction of a nanomagnet with a weak superconducting link. Equations that govern coupled dynamics of the two systems are derived and investigated numerically. We show that the presence of a small magnet in the proximity of a weak link may be detected through Shapiro-like steps caused by the precession of the magnetic moment. Despite very weak magnetic field generated by the weak link, a time-dependent bias voltage applied to the link can initiate a non-linear dynamics of the nanomagnet that leads to the reversal of its magnetic moment. We also consider quantum probl…
We present a complete theory of the spin torque phenomena in a ultrasmall nanomagnet coupled to non-collinear ferromagnetic electrodes through tunnelling junctions. This model system can be described by a simple microscopic model which captures many physical effects characteristic of spintronics: tunneling magneto resistance, intrinsic and transport induced magnetic relaxation, current induced magnetization reversal and spin accumulation. Treating on the same footing the magnetic and transport degrees of freedom, we arrive at a closed equation for the time evolution of the magnetization. This …
In recent years, studies on cyclic molecular nanomagnets have captivated the attention of researchers. These magnets are finite in size and contain very large spins. They are interesting because they possess macroscopic quantum tunneling of Néel vectors. For antiferromagnetic molecular nanomagnets with finite number of even-numbered coupled spins, tunneling involves two classical localized Néel ground states separated by a magnetic energy barrier. The question is: can such phenomena be observed in nano magnets with odd number of magnetic ions? The answer is not directly obvious because cyclic …
Quantum simulators are controllable systems that can be used to simulate other quantum systems. Here we focus on the dynamics of a chain of molecular qubits with interposed antiferromagnetic dimers. We theoretically show that its dynamics can be controlled by means of uniform magnetic pulses and used to mimic the evolution of other quantum systems, including fermionic ones. We propose two proof-of-principle experiments, based on the simulation of the Ising model in transverse field and of the quantum tunneling of the magnetization in a spin-1 system.
At low temperature, information can be stored in the orientation of the localized magnetic moment of an adatom. However, scattering of electrons and phonons with the nanomagnet leads its state to have incoherent classical dynamics and might cause fast loss of the encoded information. Recently, it has been understood that such scattering obeys certain selection rules due to the symmetries of the system. By analyzing the point-group symmetry of the surface, the time-reversal symmetry and the magnitude of the adatom effective spin, we identify which nanomagnets configurations are to be avoided an…
In a recent letter Alonso et al. (Phys. Rev. Lett. 87, 097205 (2001)) present Monte Carlo simulations for interacting dipoles. Short-time relaxation was caused by a simple noise field, acting uniformly over an "energy window" of small width (to simulate the fluctuating nuclear spin bias). However, the physics of the tunneling relaxation of an ensemble of tunneling nanomagnets or magnetic molecules (as well as of the "tunneling hole" formation) is different and here we discuss this point.
The strong influence of nuclear spins on resonant quantum tunneling in the molecular cluster Fe_8 is demonstrated for the first time by comparing the relaxation rate of the standard Fe_8 sample with two isotopic modified samples: (i) 56_Fe is replaced by 57_Fe, and (ii) a fraction of 1_H is replaced by 2_H. By using a recently developed "hole digging" method, we measured an intrinsic broadening which is driven by the hyperfine fields. Our measurements are in good agreement with numerical hyperfine calculations. For T > 1.5 K, the influence of nuclear spins on the relaxation rate is less import…
Magnetization measurements of a truly axial symmetry Mn12-tBuAc molecular nanomagnet with a spin ground state of S = 10 show resonance tunneling. This compound has the same magnetic anisotropy as Mn12-Ac but the molecules are better isolated and the crystals have less disorder and a higher symmetry. Hysteresis loop measurements at several temperatures reveal a well-resolved step fine-structure which is due to level crossings of excited states. All step positions can be modeled by a simple spin Hamiltonian. The crossover between thermally assisted and pure quantum tunneling can be investigated …
The spin dynamics of all ferromagnetic materials are governed by two types of collective excitations: spin waves and domain walls. The fundamental processes underlying these collective modes, such as exchange interactions and magnetic anisotropy, all originate at the atomic scale; yet, conventional probing techniques, based on neutron and photon scattering, provide high resolution in reciprocal space, and thereby poor spatial resolution. Here we present direct imaging of spin waves in individual chains of ferromagnetically coupled $S=2$ Fe atoms, assembled one by one on a Cu$_2$N surface using…
Recent advances in nanoscience have raised interest in the minimum bit size required for classical information storage, i.e. for bistability with suppressed quantum tunnelling and energy barriers that exceed ambient temperatures. In the case of magnetic information storage much attention has centred on molecular magnets[1] with bits consisting of ~ 100 atoms, magnetic uniaxial anisotropy energy barriers ~ 50 K, and very slow relaxation at low temperatures. In this article we draw attention to the remarkable magnetic properties of some transition metal dimers which have energy barriers approach…
Molecular nanomagnets are among the first examples of spin systems of finite size and have been test-beds for addressing a range of elusive but important phenomena in quantum dynamics. In fact, for short-enough timescales the spin wavefunctions evolve coherently according to the an appropriate cluster spin-Hamiltonian, whose structure can be tailored at the synthetic level to meet specific requirements. Unfortunately, to this point it has been impossible to determine the spin dynamics directly. If the molecule is sufficiently simple, the spin motion can be indirectly assessed by an approximate…
We have investigated analytically quantum tunneling of large spin in the biaxial spin system with the magnetic field applied along the hard and medium anisotropy axes by using a purely quantum-mechanical approach. When the magnetic field parallels the hard axis, the tunnel splittings of all the energy level pairs are oscillatory as a function of the magnetic field. The quenching points are completely determined by the coexistence of solutions of the Ince's equation. When the magnetic field points the medium axis, the tunnel splitting oscillations disappear due to no coexistence of solutions. T…
The transfer of spin angular momentum to a nanomagnet from a spin polarized current provides an efficient means of controlling the magnetization direction in nanomagnets. A unique consequence of this spin torque is that the spontaneous oscillations of the magnetization can be induced by applying a combination of a dc bias current and a magnetic field. Here we experimentally demonstrate a different effect, which can drive a nanomagnet into spontaneous oscillations without the need of external spin torque injection. For the demonstration of this effect, we use a nano-pillar of magnetic tunnel ju…
Low barrier nanomagnets have attracted a lot of research interest for their use as sources of high quality true random number generation. More recently, low barrier nanomagnets with tunable output have been shown to be a natural hardware platform for unconventional computing paradigms such as probabilistic spin logic. Efficient generation and tunability of high quality random bits is critical for these novel applications. However, current spintronic random number generators are based on superparamagnetic tunnel junctions (SMTJs) with tunability obtained through spin transfer torque (STT), whic…
The ground state tunnel splitting for the biaxial spin model in the magnetic field, H = -D S_{x}^2 + E S_{z}^2 - g μ_B S_z H_z, has been investigated using an instanton approach. We find a new type of spin instanton and a new quantum interference phenomenon associated with it: at a certain field, H_2 = 2SE^{1/2}(D+E)^{1/2}/(g μ_B), the dependence of the tunneling splitting on the field switches from oscillations to a monotonic growth. The predictions of the theory can be tested in Fe_8 molecular nanomagnets.
$^{57}$Fe and $^1$H relaxation measurements have been performed in single crystal and oriented powder of enriched $^{57}$Fe8 molecular cluster in the temperature range 0.05--1.7 K in zero external field and with small perturbing longitudinal field ($< 1$ T). On the basis of the experimental results it is argued that in zero external field the nuclear spin-lattice relaxation ($1/T_1$) mechanism is driven by a strong collision mechanism whereby $1/T_1$ is a direct measure of the incoherent tunneling probability in the low lying magnetic energy states of the molecular nanomagnet. The approximate …
The oscillation of tunnel splitting are obtained by geometrical analysis of the topological Wess-Zumino phase on the basis of tunneling paths in biaxial nanomagnetic particles with magnetic field along the hard anisotropy axis. This theory not only just yields the previous quantum interference results for the ground state tunneling, but also gives the excited level splittings, all of which agree well with the numerical diagonalization. Furthermore, the parity effect in the asymmetric system which was recently discovered in experiment can be derived by similar arguments, and is also certified b…
Forbidden transitions between energy levels typically involve violation of selection rules imposed by symmetry and/or conservation laws. A nanomagnet tunneling between up and down states violates angular momentum conservation because of broken rotational symmetry. Here we report observations of highly forbidden transitions between spin states in a Ni$_4$ single-molecule magnet in which a single photon can induce the spin to change by several times $\hbar$, nearly reversing the direction of the spin. These observations are understood as tunneling-assisted transitions that lift the standard $Δm …
We investigate scaling of technologically relevant magnetic tunnel junction devices in the trilayer and pentalayer configurations by varying the cross-sectional area along the transverse direction using the non-equilibrium Green's function spin transport formalism. We study the geometry dependence by considering square and circular cross-sections. As the transverse dimension in each case reduces, we demonstrate that the transverse mode energy profile plays a major role in the resistance-area product. Both types of devices show constant tunnel magnetoresistance at larger cross-sectional areas b…
The reversal of the magnetization of crystals of molecular magnets that have a large spin and high anisotropy barrier generally proceeds below the blocking temperature by quantum tunneling. This is manifested as a series of controlled steps in the hysteresis loops at resonant values of the magnetic field where energy levels on opposite sides of the barrier cross. An abrupt reversal of the magnetic moment of the entire crystal can occur instead by a process commonly referred to as a magnetic avalanche, where the molecular spins reverse along a deflagration front that travels through the sample …
The Landau Zener model has recently been used to measure very small tunnel splittings in molecular clusters of Fe8, which at low temperature behaves like a nanomagnet with a spin ground state of S = 10. The observed oscillations of the tunnel splittings as a function of the magnetic field applied along the hard anisotropy axis are due to topological quantum interference of two tunnel paths of opposite windings. Transitions between quantum numbers M = -S and (S - n), with n even or odd, revealed a parity effect which is analogous to the suppression of tunnelling predicted for half integer spins…
Triangular zigzag nanographenes, such as triangulene and its pi-extended homologues, have received widespread attention as organic nanomagnets for molecular spintronics, and may serve as building blocks for high-spin networks with long-range magnetic order - of immense fundamental and technological relevance. As a first step toward these lines, we present the on-surface synthesis and a proof-of-principle experimental study of magnetism in covalently bonded triangulene dimers. On-surface reactions of rationally-designed precursor molecules on Au(111) lead to the selective formation of triangule…
We analyze the statistics of charge and energy currents and spin torque in a metallic nanomagnet coupled to a large magnetic metal via a tunnel contact. We derive a Keldysh action for the tunnel barrier, describing the stochastic currents in the presence of a magnetization precessing with the rate $Ω$. In contrast to some earlier approaches, we include the geometric phases that affect the counting statistics. We illustrate the use of the action by deriving spintronic fluctuation relations, the quantum limit of pumped current noise, and consider the fluctuations in two specific cases: the situa…
We briefly review the oscillator and spin bath models of quantum environments, which can be used to describe the low-energy dynamics of open quantum systems. We then use them to discuss both the mechanisms causing decoherence at low $T$, and the dynamics of this decoherence. This is done first for a central 2-level system coupled to these environments- the results can be applied to the dynamics of quantum nanomagnets and superconducting SQUIDs, where large-scale tunneling of magnetisation and flux take place. Decoherence in these systems is caused principally by coupling to electrons and nucle…
We use neutron diffraction to probe the magnetization components of a crystal of Mn12 single-molecule magnets. Each of these molecules behaves, at low temperatures, as a nanomagnet with spin S = 10 and strong anisotropy along the crystallographic c axis. Application of a magnetic field perpendicular to c induces quantum tunneling between opposite spin orientations, enabling the spins to attain thermal equilibrium. Below approximately 0.9 K, intermolecular interactions turn this equilibrium state into a ferromagnetically ordered phase. However, long range ferromagnetic correlations nearly disap…
High energy resolution spectroscopic studies of quantum magnets have proven to be extremely valuable in directly accessing magnetodynamics quantities, such as energy barriers, magnetic interactions, lifetime of excited states and fluctuations at the most fundamental level. Here, we explore the existence of a new flavor of low-energy spin-excitations for quantum spins coupled to an electron bath. In sharp contrast to the usual tunneling signature of two steps symmetrically centered around the Fermi level, we find a single step in the conductance. Combining time-dependent and many-body perturbat…
