J. J. Parks

Mechanical Control of Spin States in Spin-1 Molecules and the Underscreened Kondo Effect

Spin Control Through Molecular Stretching Molecules with high symmetry, such as metal complexes with several equivalent ligands, can, in principle, have this symmetry broken by stresses that lengthen bonds in one direction. Parks et al. (p. 1370; see the Perspective by Jarillo-Herrero) placed cobalt complexes in a break-junction contact and then applied a mechanical force to slowly open the contact. Low-temperature measurement of differential conductance revealed a splitting of the Kondo peak at zero-applied voltage into two features, which occurred by breaking the degeneracy of S = 1 triplet states. This assignment of the spin state was confirmed by the evolution of splitting with magnetic field and by comparison to theory for a case where the conduction electrons only partially screen the spin states. Controlled stretching of individual transition-metal complexes enables direct manipulation of the molecule’s spin states. The ability to make electrical contact to single molecules creates opportunities to examine fundamental processes governing electron flow on the smallest possible length scales. We report experiments in which we controllably stretched individual cobalt complexes having spin S = 1, while simultaneously measuring current flow through the molecule. The molecule’s spin states and magnetic anisotropy were manipulated in the absence of a magnetic field by modification of the molecular symmetry. This control enabled quantitative studies of the underscreened Kondo effect, in which conduction electrons only partially compensate the molecular spin. Our findings demonstrate a mechanism of spin control in single-molecule devices and establish that they can serve as model systems for making precision tests of correlated-electron theories.

Tuning the Kondo Effect with a Mechanically Controllable Break Junction

We study electron transport through C(60) molecules in the Kondo regime using a mechanically controllable break junction. By varying the electrode spacing, we are able to change both the width and the height of the Kondo resonance, indicating modification of the Kondo temperature and the relative strength of coupling to the two electrodes. The linear conductance as a function of T/T(K) agrees with the scaling function expected for the spin-1/2 Kondo problem. We are also able to tune finite-bias Kondo features which appear at the energy of the first C(60) intracage vibrational mode.

Single-Molecule Conductance of Pyridine-Terminated Dithienylethene Switch Molecules

We have investigated the conductance of individual optically switchable dithienylethene molecules in both their conducting closed configuration and nonconducting open configuration, using the technique of repeatedly formed break-junctions. We employed pyridine groups to link the molecules to gold electrodes in order to achieve relatively well-defined molecular contacts and stable conductance. For the closed form of each molecule, we observed a peak in the conductance histogram constructed without any data selection, allowing us to determine the conductance of the fully stretched molecules. For two different dithienylethene derivatives, these closed-configuration conductances were (3.3 ± 0.5) × 10(-5)G(0) and (1.5 ± 0.5) × 10(-6)G(0), where G(0) is the conductance quantum. For the open configuration of the molecules, the existence of electrical conduction via the molecule was evident in traces of conductance versus junction displacement, but the conductance of the fully stretched molecules was less than the noise floor of our measurement. We can set a lower limit of 30 for the on/off ratio for the simplest dithienylethene derivative we have investigated. Density functional theory calculations predict an on/off ratio consistent with this result.

Tunnelling spectra of individual magnetic endofullerene molecules

The manipulation of single magnetic molecules may enable new strategies for high-density information storage and quantum-state control. However, progress in these areas depends on developing techniques for addressing individual molecules and controlling their spin. Here, we report success in making electrical contact to individual magnetic N@C(60) molecules and measuring spin excitations in their electron tunnelling spectra. We verify that the molecules remain magnetic by observing a transition as a function of magnetic field that changes the spin quantum number and also the existence of non-equilibrium tunnelling originating from low-energy excited states. From the tunnelling spectra, we identify the charge and spin states of the molecule. The measured spectra can be reproduced theoretically by accounting for the exchange interaction between the nitrogen spin and electron(s) on the C(60) cage.

Quantum confinement and coherence in a two-dimensional electron gas in a carbon-face 3C-SiC/6H-SiC polytype heterostructure

We report the observation of the quantum coherence in a two-dimensional electron gas (2DEG) at a C-face 3C-/6H-SiC polytype heterostructure. Electronic confinement and coherence were observed at 1.5 K and high magnetic fields, indicating the presence and confinement of a 2DEG. The measured mobility of the 2DEG is 2000 cm2/V s and the electron sheet density is 2.7×1012/cm2.