All-electronic Nanosecond-resolved Scanning Tunneling Microscopy: Facilitating the Investigation of Single Dopant Charge Dynamics

The miniaturization of semiconductor devices to scales where small numbers of dopants can control device properties requires the development of new ...

Max Planck Institute for the Structure and Dynamics of Matter

Max Planck Institute for Solid State Research

Scanning probe microscopy: close-up on spin coherence.

Magnetic anisotropy plays a key role in the magnetic stability and spin-related quantum phenomena of surface adatoms. It manifests as angular variations of the atom's magnetic properties. We measure the spin excitations of individual Fe atoms on a copper nitride surface with inelastic electron tunneling spectroscopy. Using a three-axis vector magnet we rotate the magnetic field and map out the resulting variations of the spin excitations. We quantitatively determine the three-dimensional distribution of the magnetic anisotropy of single Fe atoms by fitting the spin excitation spectra with a spin Hamiltonian. This experiment demonstrates the feasibility of fully mapping the vector magnetic properties of individual spins and characterizing complex three-dimensional magnetic systems.

Three-dimensional mapping of single-atom magnetic anisotropy.

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.

Spin polarization of the split Kondo state.

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 SMM's 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 molecule's 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.

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

As the ultimate miniaturization of semiconductor devices approaches, it is imperative that the effects of single dopants be clarified. Beyond providing insight into functions and limitations of conventional devices, such information enables identification of new device concepts. Investigating single dopants requires sub-nanometre spatial resolution, making scanning tunnelling microscopy an ideal tool. However, dopant dynamics involve processes occurring at nanosecond timescales, posing a significant challenge to experiment. Here we use time-resolved scanning tunnelling microscopy and spectroscopy to probe and study transport through a dangling bond on silicon before the system relaxes or adjusts to accommodate an applied electric field. Atomically resolved, electronic pump-probe scanning tunnelling microscopy permits unprecedented, quantitative measurement of time-resolved single dopant ionization dynamics. Tunnelling through the surface dangling bond makes measurement of a signal that would otherwise be too weak to detect feasible. Distinct ionization and neutralization rates of a single dopant are measured and the physical process controlling those are identified.

Time-resolved single dopant charge dynamics in silicon.

The ability to sense the magnetic state of individual magnetic nano-objects is a key capability for powerful applications ranging from readout of ultradense magnetic memory to the measurement of spins in complex structures with nanometer precision. Magnetic nano-objects require extremely sensitive sensors and detection methods. We create an atomic spin sensor consisting of three Fe atoms and show that it can detect nanoscale antiferromagnets through minute, surface-mediated magnetic interaction. Coupling, even to an object with no net spin and having vanishing dipolar stray field, modifies the transition matrix element between two spin states of the Fe atom-based spin sensor that changes the sensor's spin relaxation time. The sensor can detect nanoscale antiferromagnets at up to a 3-nm distance and achieves an energy resolution of 10 μeV, surpassing the thermal limit of conventional scanning probe spectroscopy. This scheme permits simultaneous sensing of multiple antiferromagnets with a single-spin sensor integrated onto the surface.

Nonlocally sensing the magnetic states of nanoscale antiferromagnets with an atomic spin sensor.

The creation of molecule-like structures in which magnetic atoms interact controllably is full of potential for the study of complex or strongly correlated systems. Here, we create spin chains in which a strongly correlated Kondo state emerges from magnetic coupling of transition-metal atoms. We build chains up to ten atoms in length by placing Fe and Mn atoms on a Cu2N surface with a scanning tunneling microscope. The atoms couple antiferromagnetically via superexchange interaction through the nitrogen atom network of the surface. The emergent Kondo resonance is spatially distributed along the chain. Its strength can be controlled by mixing atoms of different transition metal elements and manipulating their spatial distribution. We show that the Kondo screening of the full chain by the electrons of the nonmagnetic substrate depends on the interatomic entanglement of the spins in the chain, demonstrating the prerequisites to build and probe spatially extended strongly correlated nanostructures.

Building Complex Kondo Impurities by Manipulating Entangled Spin Chains.

We present the appearance of negative differential resistance (NDR) in spin-dependent electron transport through a few-atom spin chain. A chain of three antiferromagnetically coupled Fe atoms (Fe trimer) was positioned on a Cu_{2}N/Cu(100) surface and contacted with the spin-polarized tip of a scanning tunneling microscope, thus coupling the Fe trimer to one nonmagnetic and one magnetic lead. Pronounced NDR appears at the low bias of 7 mV, where inelastic electron tunneling dynamically locks the atomic spin in a long-lived excited state. This causes a rapid increase of the magnetoresistance between the spin-polarized tip and Fe trimer and quenches elastic tunneling. By varying the coupling strength between the tip and Fe trimer, we find that in this transport regime the dynamic locking of the Fe trimer competes with magnetic exchange interaction, which statically forces the Fe trimer into its high-magnetoresistance state and removes the NDR.

Sebastian Loth

Max Planck Institute for the Structure and Dynamics of Matter

All-electronic Nanosecond-resolved Scanning Tunneling Microscopy: Facilitating the Investigation of Single Dopant Charge Dynamics