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ABSTRACT: Quantum control of individual spins in condensed-matter devices is an emerging field with a wide range of applications, from nanospintronics to quantum computing. The electron, possessing spin and orbital degrees of freedom, is conventionally used as the carrier of quantum information in proposed devices. However, electrons couple strongly to the environment, and so have very short relaxation and coherence times. It is therefore extremely difficult to achieve quantum coherence and stable entanglement of electron spins. Alternative concepts propose nuclear spins as the building blocks for quantum computing, because such spins are extremely well isolated from the environment and less prone to decoherence. However, weak coupling comes at a price: it remains challenging to address and manipulate individual nuclear spins. Here we show that the nuclear spin of an individual metal atom embedded in a single-molecule magnet can be read out electronically. The observed long lifetimes (tens of seconds) and relaxation characteristics of nuclear spin at the single-atom scale open the way to a completely new world of devices in which quantum logic may be implemented.
Nature 08/2012; 488(7411):357-60. · 36.28 Impact Factor
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ABSTRACT: We review here some universal aspects of the physics of two-electron molecular transistors in the absence of strong spin-orbit effects. Several recent quantum dot experiments have shown that an electrostatic backgate could be used to control the energy dispersion of magnetic levels. We discuss how the generally asymmetric coupling of the metallic contacts to two different molecular orbitals can indeed lead to a gate-tunable Hund's rule in the presence of singlet and triplet states in the quantum dot. For gate voltages such that the singlet constitutes the (non-magnetic) ground state, one generally observes a suppression of low voltage transport, which can yet be restored in the form of enhanced cotunneling features at finite bias. More interestingly, when the gate voltage is controlled to obtain the triplet configuration, spin S = 1 Kondo anomalies appear at zero bias, with non-Fermi liquid features related to the underscreening of a spin larger than 1/2. Finally, the small bare singlet-triplet splitting in our device allows fine-tuning with the gate between these two magnetic configurations, leading to an unscreening quantum phase transition. This transition occurs between the non-magnetic singlet phase, where a two-stage Kondo effect occurs, and the triplet phase, where the partially compensated (underscreened) moment is akin to a magnetically 'ordered' state. These observations are put theoretically into a consistent global picture by using new numerical renormalization group simulations, tailored to capture sharp finite-voltage cotunneling features within the Coulomb diamonds, together with complementary out-of-equilibrium diagrammatic calculations on the two-orbital Anderson model. This work should shed further light on the complicated puzzle still raised by multi-orbital extensions of the classic Kondo problem.
Journal of Physics Condensed Matter 06/2011; 23(24):243202. · 2.55 Impact Factor
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ABSTRACT: We present an experimental and theoretical study of a magnetic
single-molecule transistor based on N@C60 connected to gold electrodes.
Particular attention is paid to the regime of intermediate molecule-lead
coupling, where cotunneling effects manifest themselves in the Coulomb-blockade
regime. The experimental results for the differential conductance as a function
of bias, gate voltage, and external magnetic field are in agreement with our
analysis of the tunneling rates and provide evidence of magnetic signatures in
single-N@C60 devices arising from an antiferromagnetic exchange interaction
between the C60 spin and the nitrogen spin.
01/2011;
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ABSTRACT: We present the first quantitative experimental evidence for the underscreened Kondo effect, an incomplete compensation of a quantized magnetic moment by conduction electrons, as originally proposed by Nozières and Blandin. The device consists of an even charge spin S=1 molecular quantum dot, obtained by electromigration of C60 molecules into gold nanogaps and operated in a dilution fridge. The persistence of logarithmic singularities in the low temperature conductance is demonstrated by a comparison to the fully screened configuration obtained in odd charge spin S=1/2 Coulomb diamonds. We also discover an extreme sensitivity of the underscreened Kondo resonance to the magnetic field that we confirm on the basis of numerical renormalization group calculations.
Physical Review Letters 11/2009; 103(19):197202. · 7.37 Impact Factor
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ABSTRACT: We have used an electromigration technique to fabricate a C60 single-molecule transistor(SMT). Besides describing our electromigration procedure, we focus and present an experimental
study of a single molecule quantum dot containing an even number of electrons, revealing, for two different samples, a clear
out-of-equilibrium Kondo effect. Low temperature magneto-transport studies are provided, which demonstrates a Zeeman splitting
of the finite bias anomaly.
Journal of Low Temperature Physics 11/2008; 153(5):350-358. · 1.19 Impact Factor
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ABSTRACT: Quantum criticality is the intriguing possibility offered by the laws of quantum mechanics when the wave function of a many-particle physical system is forced to evolve continuously between two distinct, competing ground states. This phenomenon, often related to a zero-temperature magnetic phase transition, is believed to govern many of the fascinating properties of strongly correlated systems such as heavy-fermion compounds or high-temperature superconductors. In contrast to bulk materials with very complex electronic structures, artificial nanoscale devices could offer a new and simpler means of understanding quantum phase transitions. Here we demonstrate this possibility in a single-molecule quantum dot, where a gate voltage induces a crossing of two different types of electron spin state (singlet and triplet) at zero magnetic field. The quantum dot is operated in the Kondo regime, where the electron spin on the quantum dot is partially screened by metallic electrodes. This strong electronic coupling between the quantum dot and the metallic contacts provides the strong electron correlations necessary to observe quantum critical behaviour. The quantum magnetic phase transition between two different Kondo regimes is achieved by tuning gate voltages and is fundamentally different from previously observed Kondo transitions in semiconductor and nanotube quantum dots. Our work may offer new directions in terms of control and tunability for molecular spintronics.
Nature 06/2008; 453(7195):633-7. · 36.28 Impact Factor
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