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

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 Added by Joshua Parks
 Publication date 2010
  fields Physics
and research's language is English




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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 stretch individual cobalt complexes having spin S = 1, while simultaneously measuring current flow through the molecule. The molecules 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.



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We analyze the low energy properties of a device with $N+1$ quantum dots in a star configuration. A central quantum dot is tunnel coupled to source and drain electrodes and to $N$ quantum dots. Extending previous results for the $N=2$ case we show that, in the appropriate parameter regime, the low energy Hamiltonian of the system is a ferromagnetic Kondo model for a $S=(N-1)/2$ impurity spin. For small enough interdot tunnel coupling, however, a two-stage Kondo effect takes place as the temperature is decreased. The spin $1/2$ in the central quantum dot is Kondo screened first and at lower temperatures the antiferromagnetic coupling to the side coupled quantum dots leads to an underscreened $S=N/2$ Kondo effect. We present numerical results for the thermodynamic and spectral properties of the system which show a singular behavior at low temperatures and allow to characterize the different strongly correlated regimes of the device.
We investigate the spin relaxation and Kondo resistivity caused by magnetic impurities in doped transition metal dichalcogenides monolayers. We show that momentum and spin relaxation times due to the exchange interaction by magnetic impurities, are much longer when the Fermi level is inside the spin split region of the valence band. In contrast to the spin relaxation, we find that the dependence of Kondo temperature $T_K$ on the doping is not strongly affected by the spin-orbit induced splitting, although only one of the spin species are present at each valley. This result, which is obtained using both perturbation theory and poor mans scaling methods, originates from the intervalley spin-flip scattering in the spin-split region. We further demonstrate the decline in the conductivity with temperatures close to $T_K$ which can vary with the doping. Our findings reveal the qualitative difference with the Kondo physics in conventional metallic systems and other Dirac materials.
The Kondo effect is a key many-body phenomenon in condensed matter physics. It concerns the interaction between a localised spin and free electrons. Discovered in metals containing small amounts of magnetic impurities, it is now a fundamental mechanism in a wide class of correlated electron systems. Control over single, localised spins has become relevant also in fabricated structures due to the rapid developments in nano-electronics. Experiments have already demonstrated artificial realisations of isolated magnetic impurities at metallic surfaces, nanometer-scale magnets, controlled transitions between two-electron singlet and triplet states, and a tunable Kondo effect in semiconductor quantum dots. Here, we report an unexpected Kondo effect realised in a few-electron quantum dot containing singlet and triplet spin states whose energy difference can be tuned with a magnetic field. This effect occurs for an even number of electrons at the degeneracy between singlet and triplet states. The characteristic energy scale is found to be much larger than for the ordinary spin-1/2 case.
We report the observation of Kondo physics in a spin- 3/2 hole quantum dot. The dot is formed close to pinch-off in a hole quantum wire defined in an undoped AlGaAs/GaAs heterostructure. We clearly observe two distinctive hallmarks of quantum dot Kondo physics. First, the Zeeman spin-splitting of the zero-bias peak in the differential conductance is independent of gate voltage. Second, this splitting is twice as large as the splitting for the lowest one-dimensional subband. We show that the Zeeman splitting of the zero-bias peak is highly-anisotropic, and attribute this to the strong spin-orbit interaction for holes in GaAs.
Kondo-type zero-bias anomalies have been frequently observed in quantum dots occupied by two electrons and attributed to a spin-triplet configuration that may become stable under particular circumstances. Conversely, zero-bias anomalies have been so far quite elusive when quantum dots are occupied by an even number of electrons greater than two, even though a spin-triplet configuration is more likely to be stabilized there than for two electrons. We propose as an origin of this phenomenon the spin-orbit interaction, and we show how it profoundly alters the conventional Kondo screening scenario in the simple case of a laterally confined quantum dot with four electrons.
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