Sebastian Loth

Bistability in Atomic-Scale Antiferromagnets

Structured Memories High-density magnetic memory is generally produced by using ferromagnetic materials. As the density increases and the memory elements become closer together, stray fields can result in cross-talk and a corruption of the stored information. Antiferromagetic structures, however, are expected to be relatively insensitive to magnetic fields and so should, in principle, allow the elements to be packed in even closer. Loth et al. (p. 196) carried out low-temperature experiments to construct antiferromagnetic structures atom by atom. Electrical switching of the magnetic states was observed, and data could be robustly stored on the structure for several hours, albeit at low temperature. Atomically engineered antiferromagnets consisting of a few atoms exhibit stable magnetic states at low temperature. Control of magnetism on the atomic scale is becoming essential as data storage devices are miniaturized. We show that antiferromagnetic nanostructures, composed of just a few Fe atoms on a surface, exhibit two magnetic states, the Néel states, that are stable for hours at low temperature. For the smallest structures, we observed transitions between Néel states due to quantum tunneling of magnetization. We sensed the magnetic states of the designed structures using spin-polarized tunneling and switched between them electrically with nanosecond speed. Tailoring the properties of neighboring antiferromagnetic nanostructures enables a low-temperature demonstration of dense nonvolatile storage of information.

Measurement of fast electron spin relaxation times with atomic resolution.

In a Spin The relaxation dynamics of electron spins in solid-state systems is of crucial importance for their usage in quantum computation and information storage. The interaction of the spin with its local environment results in lifetimes in the pico- to microsecond range. Thus, high temporal and spatial resolutions are needed to measure the relaxation time with atomic precision. Loth et al. (p. 1628, see the cover; see the Perspective by Morgenstern) used a scanning tunneling microscope with a spin-polarized tip to monitor the electron spin relaxation times of individual atoms adsorbed on a surface. A spin was excited by a pump signal, and its state read out after a variable time delay with a weak probe pulse that produced a spin-sensitive tunneling current. This general technique may be applicable to other systems with fast dynamics. Scanning tunneling microscopy is used to monitor the fast relaxation dynamics of an atomic spin adsorbed on a surface. Single spins in solid-state systems are often considered prime candidates for the storage of quantum information, and their interaction with the environment the main limiting factor for the realization of such schemes. The lifetime of an excited spin state is a sensitive measure of this interaction, but extending the spatial resolution of spin relaxation measurements to the atomic scale has been a challenge. We show how a scanning tunneling microscope can measure electron spin relaxation times of individual atoms adsorbed on a surface using an all-electronic pump-probe measurement scheme. The spin relaxation times of individual Fe-Cu dimers were found to vary between 50 and 250 nanoseconds. Our method can in principle be generalized to monitor the temporal evolution of other dynamical systems.

Control of quantum magnets by atomic exchange bias

Mixing of discretized states in quantum magnets has a radical impact on their properties. Managing this effect is key for spintronics in the quantum limit. Magnetic fields can modify state mixing and, for example, mitigate destabilizing effects in single-molecule magnets. The exchange bias field has been proposed as a mechanism for localized control of individual nanomagnets. Here, we demonstrate that exchange coupling with the magnetic tip of a scanning tunnelling microscope provides continuous tuning of spin state mixing in an individual nanomagnet. By directly measuring spin relaxation time with electronic pump-probe spectroscopy, we find that the exchange interaction acts analogously to a local magnetic field that can be applied to a specific atom. It can be tuned in strength by up to several tesla and cancel external magnetic fields, thereby demonstrating the feasibility of complete control over individual quantum magnets with atomically localized exchange coupling.

Spin-polarized spin excitation spectroscopy

We report on the spin dependence of elastic and inelastic electron tunneling through transition metal atoms. Mn, Fe and Cu atoms were deposited onto a monolayer of Cu2N on Cu(100) and individually addressed with the probe tip of a scanning tunneling microscope. Electrons tunneling between the tip and the substrate exchange energy and spin angular momentum with the surface-bound magnetic atoms. The conservation of energy during the tunneling process results in a distinct onset threshold voltage above which the tunneling electrons create spin excitations in the Mn and Fe atoms. Here we show that the additional conservation of spin angular momentum leads to different cross-sections for spin excitations depending on the relative alignment of the surface spin and the spin of the tunneling electron. For this purpose, we developed a technique for measuring the same local spin with a spin-polarized and a non-spin-polarized tip by exchanging the last apex atom of the probe tip between different transition metal atoms. We derive a quantitative model describing the observed excitation cross-sections on the basis of an exchange scattering process.

Magnetic fingerprint of individual Fe4 molecular magnets under compression by a scanning tunnelling microscope

Single-molecule magnets (SMMs) present a promising avenue to develop spintronic technologies. Addressing individual molecules with electrical leads in SMM-based spintronic devices remains a ubiquitous challenge: interactions with metallic electrodes can drastically modify the SMMs properties by charge transfer or through changes in the molecular structure. Here, we probe electrical transport through individual Fe4 SMMs using a scanning tunnelling microscope at 0.5 K. Correlation of topographic and spectroscopic information permits identification of the spin excitation fingerprint of intact Fe4 molecules. Building from this, we find that the exchange coupling strength within the molecules magnetic core is significantly enhanced. First-principles calculations support the conclusion that this is the result of confinement of the molecule in the two-contact junction formed by the microscope tip and the sample surface.

Connection of anisotropic conductivity to tip-induced space-charge layers in scanning tunneling spectroscopy of p-doped GaAs

The electronic properties of shallow acceptors in p-doped GaAs{110} are investigated with scanning tunneling microscopy at low temperature. Shallow acceptors are known to exhibit distinct triangular contrasts in STM images for certain bias voltages. Spatially resolved I(V)-spectroscopy is performed to identify their energetic origin and behavior. A crucial parameter - the STM tips work function - is determined experimentally. The voltage dependent potential configuration and band bending situation is derived. Ways to validate the calculations with the experiment are discussed. Differential conductivity maps reveal that the triangular contrasts are only observed with a depletion layer present under the STM tip. The tunnel process leading to the anisotropic contrasts calls for electrons to tunnel through vacuum gap and a finite region in the semiconductor.

The emergence of classical behaviour in magnetic adatoms

A wide class of nanomagnets shows striking quantum behaviour, known as quantum spin tunnelling (QST): instead of two degenerate ground states with opposite magnetizations, a bonding-antibonding pair forms, resulting in a splitting of the ground-state doublet with wave functions linear combination of two classically opposite magnetic states, leading to the quenching of their magnetic moment. Here we study how QST is destroyed and classical behaviour emerges in the case of magnetic adatoms, where, contrary to larger nanomagnets, the QST splitting is in some instances bigger than temperature and broadening. We analyze two different mechanisms for the renormalization of the QST splitting: Heisenberg exchange between different atoms, and Kondo exchange interaction with the substrate electrons. Sufficiently strong spin-substrate and spin-spin coupling renormalize the QST splitting to zero allowing the environmental decoherence to eliminate superpositions between classical states, leading to the emergence of spontaneous magnetization. Importantly, we extract the strength of the Kondo exchange for various experiments on individual adatoms and construct a phase diagram for the classical to quantum transition.

Quantitative mapping of fast voltage pulses in tunnel junctions by plasmonic luminescence

An optical read-out technique is demonstrated that enables mapping the time-dependent electrostatic potential in the tunnel junction of a scanning tunneling microscope with millivolt and nanosecond accuracy. We measure the time-dependent intensity of plasmonic light emitted from the tunnel junction upon excitation with a nanosecond voltage pulse. The light intensity is found to be a quantitative measure of the voltage between tip and sample. This permits non-invasive mapping of fast voltage transients directly at the tunnel junction. Knowledge of the pulse profile reaching the tunnel junction is applied to optimize the experiments time response by actively shaping the incident pulses.

Spin Polarization of the Split Kondo State

Spin-resolved scanning tunneling microscopy is employed to quantitatively determine the spin polarization of the magnetic field-split Kondo state. Tunneling conductance spectra of a Kondo-screened magnetic atom are evaluated within a simple model taking into account inelastic tunneling due to spin excitations and two Kondo peaks positioned symmetrically around the Fermi energy. We fit the spin state of the Kondo-screened atom with a spin Hamiltonian independent of the Kondo effect and account for Zeeman splitting of the Kondo peak in the magnetic field. We find that the width and the height of the Kondo peaks scales with the Zeeman energy. Our observations are consistent with full spin polarization of the Kondo peaks, i.e., a majority spin peak below the Fermi energy and a minority spin peak above.

Measuring the Three-Dimensional Structure of Ultrathin Insulating Films at the Atomic Scale

The increasing technological importance of thin insulating layers calls for a thorough understanding of their structure. Here we apply scanning probe methods to investigate the structure of ultrathin magnesium oxide (MgO) which is the insulating material of choice in spintronic applications. A combination of force and current measurements gives high spatial resolution maps of the local three-dimensional insulator structure. When force measurements are not available, a lower spatial resolution can be obtained from tunneling images at different voltages. These broadly applicable techniques reveal a previously unknown complexity in the structure of MgO on Ag(001), such as steps in the insulator-metal interface.