Toyo Kazu Yamada

Robust spin crossover and memristance across a single molecule

A nanoscale molecular switch can be used to store information in a single molecule. Although the switching process can be detected electrically in the form of a change in the molecules conductance, adding spin functionality to molecular switches is a key concept for realizing molecular spintronic devices. Here we show that iron-based spin-crossover molecules can be individually and reproducibly switched between a combined high-spin, high-conduction state and a low-spin, low-conduction state, provided the individual molecule is decoupled from a metallic substrate by a thin insulating layer. These results represent a step to achieving combined spin and conduction switching functionality on the level of individual molecules.

Giant magnetoresistance through a single molecule

Magnetoresistance is a change in the resistance of a material system caused by an applied magnetic field. Giant magnetoresistance occurs in structures containing ferromagnetic contacts separated by a metallic non-magnetic spacer, and is now the basis of read heads for hard drives and for new forms of random access memory. Using an insulator (for example, a molecular thin film) rather than a metal as the spacer gives rise to tunnelling magnetoresistance, which typically produces a larger change in resistance for a given magnetic field strength, but also yields higher resistances, which are a disadvantage for real device operation. Here, we demonstrate giant magnetoresistance across a single, non-magnetic hydrogen phthalocyanine molecule contacted by the ferromagnetic tip of a scanning tunnelling microscope. We measure the magnetoresistance to be 60% and the conductance to be 0.26G(0), where G(0) is the quantum of conductance. Theoretical analysis identifies spin-dependent hybridization of molecular and electrode orbitals as the cause of the large magnetoresistance.

Magnetoelectric coupling at metal surfaces

Magnetoelectric coupling allows the magnetic state of a material to be changed by an applied electric field. To date, this phenomenon has mainly been observed in insulating materials such as complex multiferroic oxides. Bulk metallic systems do not exhibit magnetoelectric coupling, because applied electric fields are screened by conduction electrons. We demonstrate strong magnetoelectric coupling at the surface of thin iron films using the electric field from a scanning tunnelling microscope, and are able to write, store and read information to areas with sides of a few nanometres. Our work demonstrates that high-density, non-volatile information storage is possible in metals.

Single molecule magnetoresistance with combined antiferromagnetic and ferromagnetic electrodes.

The magnetoresistance of a hydrogen-phthalocyanine molecule placed on an antiferromagnetic Mn(001) surface and contacted by a ferromagnetic Fe electrode is investigated using density functional theory based transport calculations and low-temperature scanning tunneling microscopy. A large and negative magnetoresistance ratio of ~50% is observed in combination with a high conductance. The effect originates from a lowest unoccupied molecular orbital (LUMO) doublet placed almost in resonance with the Fermi energy. As a consequence, irrespective of the mutual alignment of magnetizations, electron transport is always dominated by resonant transmission of Mn-majority charge carries going through LUMO levels.

Use of voltage pulses to detect spin-polarized tunneling

The present letter describes a method to make a spin-polarized scanning tunneling microscopy tip by applying voltage pulses between a W tip and a magnetic sample. This spin-polarized tip has the similar characteristics as an Fe-coated W tip, which was confirmed by observations of antiferromagnetically coupled ferromagnetic Mn(001) layers (>3 ML) grown on an Fe(001) whisker at 370 K. Furthermore, we demonstrate that these voltage pulses can vary the tip magnetization direction.

Method for Controlling Electrical Properties of Single-Layer Graphene Nanoribbons via Adsorbed Planar Molecular Nanoparticles

A simple method for fabricating single-layer graphene nanoribbons (sGNRs) from double-walled carbon nanotubes (DWNTs) was developed. A sonication treatment was employed to unzip the DWNTs by inducing defects in them through annealing at 500 °C. The unzipped DWNTs yielded double-layered GNRs (dGNRs). Further sonication allowed each dGNR to be unpeeled into two sGNRs. Purification performed using a high-speed centrifuge ensured that more than 99% of the formed GNRs were sGNRs. The changes induced in the electrical properties of the obtained sGNR by the absorption of nanoparticles of planar molecule, naphthalenediimide (NDI), were investigated. The shape of the I-V curve of the sGNRs varied with the number of NDI nanoparticles adsorbed. This was suggestive of the existence of a band gap at the narrow-necked part near the NDI-adsorbing area of the sGNRs.

Spin configuration in a frustrated ferromagnetic/antiferromagnetic thin-film system

We have studied the magnetic configuration in ultrathin antiferromagnetic Mn films grown around monoatomic steps on an Fe( 001) surface by spin-polarized scanning tunnelling microscopy/spectroscopy ...

Spin polarization vectors of field emitted electrons from Fe/W tips

The atomic and electronic structures at the apex of W tips were studied by means of field ion microscopy and field emission microscopy, before and after the thermal deposition of a 5 nm Fe film. Two geometries of W tip, a conventional hemi-spherical type and a chisel (flat needle) type, were prepared. The hemispherical and the chisel W tips had a 110 direction parallel and perpendicular to the tip axis, respectively. The coated Fe films were found to be most likely in a non-crystalline phase, and to have a lower work function leading to a drastic change in electron emission from the apexes. The spin-polarization vectors of field-emitted electrons from these Fe/W tips were investigated with a Mott detector with a rotatable mechanism of tips. A similar absolute value of the spin-polarization vector was obtained for each Fe/W, while the direction of the spin-polarization vector was dependent on the shape of the apex. The angle from the tip axis was θ=45° for the hemispherical apex and θ=66° for the chisel apex. A spin-polarized scanning tunneling microscopy setup with a rotation mechanism of such Fe/W tips made it possible to detect both the in-plane and the out-of-plane spin component of a sample magnetization.

Origin of Magnetic Contrast in Spin-Polarized Scanning Tunneling Spectroscopy: Experiments on Ultra-Thin Mn Films

Normalized differential tunneling conductivities obtained with Fe-coated W tips show a spin-polarized peak around +0.8 V on ultrathin bct Mn films grown on Fe(001)-whiskers. This spin-polarized peak results in a clear magnetic contrast in spectroscopic images. Our normalization removes the influence of the tunneling probability and makes the spectroscopic curves most reliable for a derivation of the spin-resolved sample density of states (DOS) at positive voltages. From this analysis we conclude that the magnetic contrast in our spectroscopic maps is caused by a highly polarized DOS. Furthermore, a tip polarization of about 15% is found.

Electron-bombarded 〈110〉-oriented tungsten tips for stable tunneling electron emission

A clean tungsten (W) tip apex with a robust atomic plane is required for producing a stable tunneling electron emission under strong electric fields. Because a tip apex fabricated from a wire by aqueous chemical etching is covered by impurity layers, heating treatment in ultra-high vacuum is experimentally known to be necessary. However, strong heating frequently melts the tip apex and causes unstable electron emissions. We investigated quantitatively the tip apex and found a useful method to prepare a tip with stable tunneling electron emissions by controlling electron-bombardment heating power. Careful characterizations of the tip structures were performed with combinations of using field emission I-V curves, scanning electron microscopy, X-ray diffraction (transmitted Debye-Scherrer and Laue) with micro-parabola capillary, field ion microscopy, and field emission microscopy. Tips were chemically etched from (1) polycrystalline W wires (grain size ∼1000 nm) and (2) long-time heated W wires (grain size larger than 1 mm). Heating by 10-40 W (10 s) was found to be good enough to remove oxide layers and produced stable electron emission; however, around 60 W (10 s) heating was threshold power to increase the tip radius, typically +10 ± 5 nm (onset of melting). Further, the grain size of ∼1000 nm was necessary to obtain a conical shape tip apex.