Molecular Spin Qudits for Quantum Algorithms

Presently, one of the most ambitious technological goals is the development of devices working under the laws of quantum mechanics. One prominent target is the quantum computer, which would allow the processing of information at quantum level for purposes not achievable with even the most powerful computer resources. The large-scale implementation of quantum information would be a game changer for current technology, because it would allow unprecedented parallelised computation and secure encryption based on the principles of quantum superposition and entanglement. Currently, there are several physical platforms racing to achieve the level of performance required for the quantum hardware to step into the realm of practical quantum information applications. Several materials have been proposed to fulfil this task, ranging from quantum dots, Bose-Einstein condensates, spin impurities, superconducting circuits, molecules, amongst others. Magnetic molecules are among the list of promising building blocks, due to (i) their intrinsic monodispersity, (ii) discrete energy levels (iii) the possibility of chemical quantum state engineering, and (iv) their multilevel characteristics, leading to the so called Qudits (d > 2), amongst others. Herein we review how a molecular multilevel nuclear spin qubit (or qudit, where d = 4), known as TbPc2, gathers all the necessary requirements to perform as a molecular hardware platform with a first generation of molecular devices enabling even quantum algorithm operations.Comment: Chem. Soc. Rev., 2017, Advance Articl

Cotunneling through a magnetic single-molecule transistor based on N\atC60

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.Comment: Accepted for publication in PRB Rapid Com, 4 pages, 4 figures, with supplementary information (6 pages, 3 figures

Universal transport signatures in two-electron molecular quantum dots: gate-tunable Hund's rule, underscreened Kondo effect and quantum phase transitions

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 dots experiments have shown that an electrostatic backgate could be used to control the energy dispersion of magnetic levels. We discuss how the generically 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 to fine-tune 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, taylored to capture sharp finie-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.Comment: Review article. 16 pages, 17 figures. Minor corrections and extra references added in V

Out-of-equilibrium singlet-triplet Kondo effect in a single C_60 quantum dot

We have used an electromigration technique to fabricate a $\rm{C_{{60}}}$ 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.Comment: 6 pages, 4 figure

Field-Tunable 0-pi-Transitions in SnTe Topological Crystalline Insulator SQUIDs.

Schonle J, Borisov K, Klett R, et al. Field-Tunable 0-pi-Transitions in SnTe Topological Crystalline Insulator SQUIDs. Scientific reports. 2019;9(1): 1987.The manifestation of spin-orbit interactions, long known to dramatically affect the band structure of heavy-element compounds, governs the physics in the surging class of topological matter. A particular example is found in the new family of topological crystalline insulators. In this systems transport occurs at the surfaces and spin-momentum locking yields crystal-symmetry protected spin-polarized transport. We investigated the current-phase relation of SnTe thin films connected to superconducting electrodes to form SQUID devices. Our results demonstrate that an assisting in-plane magnetic field component can induce 0-π-transitions. We attribute these findings to giant g-factors and large spin-orbit coupling of SnTe topological crystalline insulator, which provides a new platform for investigation of the interplay between spin-orbit physics and topological transport

Quantum phase transition in a single-molecule quantum dot

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, can be observed in several strongly correlated materials such as heavy fermion compounds or possibly high-temperature superconductors, and is believed to govern many of their fascinating, yet still unexplained properties. In contrast to these bulk materials with very complex electronic structure, artificial nanoscale devices could offer a new and simpler vista to the comprehension of quantum phase transitions. This long-sought possibility is demonstrated by our work in a fullerene molecular junction, where gate voltage induces a crossing of singlet and triplet spin states at zero magnetic field. Electronic tunneling from metallic contacts into the $\rm{C_{60}}$ quantum dot provides here the necessary many-body correlations to observe a true quantum critical behavior.Comment: 8 pages, 5 figure

Superconductivity in a single C60 transistor

Single molecule transistors (SMTs) are currently attracting enormous attention as possible quantum information processing devices. An intrinsic limitation to the prospects of these however is associated to the presence of a small number of quantized conductance channels, each channel having a high access resistance of at best $R_{K}/2=h/2e^{2}$=12.9 k$\Omega$. When the contacting leads become superconducting, these correlations can extend throughout the whole system by the proximity effect. This not only lifts the resistive limitation of normal state contacts, but further paves a new way to probe electron transport through a single molecule. In this work, we demonstrate the realization of superconducting SMTs involving a single C60 fullerene molecule. The last few years have seen gate-controlled Josephson supercurrents induced in the family of low dimensional carbon structures such as flakes of two-dimensional graphene and portions of one-dimensional carbon nanotubes. The present study involving a full zero-dimensionnal fullerene completes the picture.Comment: 12 pages, 3 figure

Dynamique quantique d'un SQUID-DC

A theoretical study that we went through predicted that a DC-SQUID, having a quality factor equals to 100 in its quantum macroscopic regime, permits one shot quantum measurement of the charge state of a qubit within an error of the order of 2%. This thesis work is then a study and an experimental development of a quantum measurement of a SQUID. We studied the escape dynamic from the zero voltage state of an inductif DC-SQUID as a function of flux and temperature. We showed up the macroscopic quantum regime and thermal activation regime, in the way of the escape of a fictive metastable particule from a bidimensionnal potential. The lifetime of the zero voltage state of a SQUID in its thermal activation regime was measured in the nano-seconde range using a flux pulses technique. Th euse of microwaves pulses permitted also to measure the plasma frequency of a SQUID using a resonante activation technique, and to measure a quality factor of the order of 100.Une étude théorique que nous avons menée prédit qu'un SQUID-DC, ayant un facteur de qualité égal à 100 dans son régime d'effet tunnel macroscopique, permet une mesure quantique en un coup l'état de charge d'un qubit avec une erreur de l'ordre de 2%. Ce travail de thèse s'inscrit donc dans l'étude et le développement expérimental d'un système de mesure quantIque d'un SQUID. Nous avons étudié la dynamique d'échappement de l'état de tension nulle d'un SQUID-DC inductif en fonction du flux et de la température. Nous avons mis en évidence le régime d'effet tunnel macroscopique et d'activation thermique, dans le cadre de l'échappement d'une particule fictive métastable d'un potentiel bi-dimensionnel. Le temps de vie de l'état de tension nulle d'un SQUID dans son régime d'activation thermique a été mesuré dans la gamme des nano-secondes grâce à une technique d'impulsions en flux. L'utilisation d'impulsions micro-ondes a également permis de mesurer la fréquence plasma d'un SQUID par une technique d'activation résonante, et de mesurer un facteur de qualité de l'ordre de 100

Dynamique quantique d'un SQUID-DC

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