Landau-Zener tunneling of a single Tb3+ magnetic moment allowing the electronic read-out of a nuclear spin

A multi-terminal device based on a carbon nanotube quantum dot was used at very low tem- perature to probe a single electronic and nuclear spin embedded in a bis-phthalocyanine Terbium (III) complex (TbPc2). A spin-valve signature with large conductance jumps was found when two molecules were strongly coupled to the nanotube. The application of a transverse field separated the magnetic signal of both molecules and enabled single-shot read-out of the Terbium nuclear spin. The Landau-Zener (LZ) quantum tunneling probability was studied as a function of field sweep rate, establishing a good agreement with the LZ equation and yielding the tunnel splitting \Delta. It was found that ? increased linearly as a function of the transverse field. These studies are an essential prerequisite for the coherent manipulation of a single nuclear spin in TbPc2.Comment: 7 pages, 6 figures, to appear in PR

Spintronique moléculaire de la vanne de spin à la détection d'un spin unique

Spintronique moléculaire : de la vanne de spin à la détection d'un spin unique. Parmi les thématiques qui ont émergé ces dix dernières années, la spintronique moléculaire est intéressante de par son caractère hybride, à la croisée entre l'électronique de spin, l'électronique moléculaire et le magnétisme moléculaire. Dans ce nouveau domaine, on cherche à exploiter les propriétés magnétiques et quantiques des aimants moléculaires pour créer des dispositifs originaux, utiles en spintronique ou en information quantique. Mon projet de thèse s'inscrit dans cette perspective en voulant combiner un transistor à nanotube de carbone avec des aimants à molécule unique, en les couplant par des interactions supramoléculaires. L'objectif est d'observer le renversement magnétique d'une seule molécule par des mesures de transport électronique à travers le nanotube. En effet, le diamètre de ce dernier étant comparable aux dimensions d'un aimant moléculaire, le couplage devrait être suffisamment fort pour en permettre la détection. La réalisation d'un tel dispositif, un défi technique, et la question de savoir s'il était réellement possible de détecter et de caractériser le moment d'une seule molécule ont constitué les deux enjeux majeurs de cette thèse. Une grande partie du travail réalisé porte sur la fabrication du dispositif expérimental par des techniques de micro- et nano-fabrication, ainsi que sur l'optimisation du greffage des aimants moléculaires sur la surface du nanotube. Dans un second temps, nous nous intéressons à l'étude du système et à son comportement à très basse température (100 mK). En effet, la proximité des aimants moléculaires TbPc2 modifie de façon spectaculaire les propriétés de transport d'un nanotube. En particulier, nous présentons la réalisation d'un dispositif dont la réponse est analogue à une vanne de spin classique, où les molécules magnétiques jouent le rôle de polariseur ou d'analyseur de spin. Grâce à ce système, nous avons réussi à affiner nos connaissances sur TbPc2. Entre autres résultats, nous sommes parvenus à isoler et à caractériser le retournement du moment magnétique d'un seul ion de terbium. Enfin, la dernière partie de cette thèse est consacrée à l'étude de l'interaction hyperfine au sein du terbium. En réalisant un dispositif qui n'est couplé qu'à deux molécules, nous avons mis en évidence qu'il est possible de réaliser une lecture directe de l'état d'un spin nucléaire unique.Nowadays, new directions in quantum spintronics aim at transposing the existing concepts and at developing alternative ones with various types of materials, from inorganic to -conjugated organic semiconductors. In this context, single molecule-magnets (SMMs) are interesting candidates to be integrated in molecular spintronics devices. Such devices lead the way for the electronic detection and coherent manipulation of SMMs spin states, exploitable in quantum computation schemes. We developed for this purpose an innovative multi-terminals device based on a carbon nanotube quantum dot, laterally coupled to few SMMs through supramolecular interaction. The conductance of the nanotube is measured at very low temperature (40 mK) and each time one of the SMM magnetic moment reverses, the conductance changes. The latters act on the conduction electron through the QD as spin polarizer and analyzer. This spin-valve effect gives access to the behavior of a single localized spin by standard electrometry We report a full magnetic characterization of a single bis-phthalocyaninato terbium complex (TbPc2). In particular, we performed a detailed study of quantum tunnelling of the magnetization of the Tb electronic moment and we present a read-out technic of the Tb nuclear spin state. These results open up strong perspectives for a coherent manipulation of a single nuclear spin in TbPc2.SAVOIE-SCD - Bib.électronique (730659901) / SudocGRENOBLE1/INP-Bib.électronique (384210012) / SudocGRENOBLE2/3-Bib.électronique (384219901) / SudocSudocFranceF

Molecular Quantum Spintronics: Supramolecular Spin Valves Based on Single-Molecule Magnets and Carbon Nanotubes

We built new hybrid devices consisting of chemical vapor deposition (CVD) grown carbon nanotube (CNT) transistors, decorated with TbPc2 (Pc = phthalocyanine) rare-earth based single-molecule magnets (SMMs). The drafting was achieved by tailoring supramolecular π-π interactions between CNTs and SMMs. The magnetoresistance hysteresis loop measurements revealed steep steps, which we can relate to the magnetization reversal of individual SMMs. Indeed, we established that the electronic transport properties of these devices depend strongly on the relative magnetization orientations of the grafted SMMs. The SMMs are playing the role of localized spin polarizer and analyzer on the CNT electronic conducting channel. As a result, we measured magneto-resistance ratios up to several hundred percent. We used this spin valve effect to confirm the strong uniaxial anisotropy and the superparamagnetic blocking temperature (TB ~ 1 K) of isolated TbPc2 SMMs. For the first time, the strength of exchange interaction between the different SMMs of the molecular spin valve geometry could be determined. Our results introduce a new design for operable molecular spintronic devices using the quantum effects of individual SMMs

Generation of a single-cycle acoustic pulse: a scalable solution for transport in single-electron circuits

The synthesis of single-cycle, compressed optical and microwave pulses sparked novel areas of fundamental research. In the field of acoustics, however, such a generation has not been introduced yet. For numerous applications, the large spatial extent of surface acoustic waves (SAW) causes unwanted perturbations and limits the accuracy of physical manipulations. Particularly, this restriction applies to SAW-driven quantum experiments with single flying electrons, where extra modulation renders the exact position of the transported electron ambiguous and leads to undesired spin mixing. Here, we address this challenge by demonstrating single-shot chirp synthesis of a strongly compressed acoustic pulse. Employing this solitary SAW pulse to transport a single electron between distant quantum dots with an efficiency exceeding 99%, we show that chirp synthesis is competitive with regular transduction approaches. Performing a time-resolved investigation of the SAW-driven sending process, we outline the potential of the chirped SAW pulse to synchronize single-electron transport from many quantum-dot sources. By superimposing multiple pulses, we further point out the capability of chirp synthesis to generate arbitrary acoustic waveforms tailorable to a variety of (opto)nanomechanical applications. Our results shift the paradigm of compressed pulses to the field of acoustic phonons and pave the way for a SAW-driven platform of single-electron transport that is precise, synchronized, and scalable.Comment: To be published in Physical Review

Coulomb-mediated antibunching of an electron pair surfing on sound

Electron flying qubits are envisioned as potential information link within a quantum computer, but also promise -- alike photonic approaches -- a self-standing quantum processing unit. In contrast to its photonic counterpart, electron-quantum-optics implementations are subject to Coulomb interaction, which provide a direct route to entangle the orbital or spin degree of freedom. However, the controlled interaction of flying electrons at the single particle level has not yet been established experimentally. Here we report antibunching of a pair of single electrons that is synchronously shuttled through a circuit of coupled quantum rails by means of a surface acoustic wave. The in-flight partitioning process exhibits a reciprocal gating effect which allows us to ascribe the observed repulsion predominantly to Coulomb interaction. Our single-shot experiment marks an important milestone on the route to realise a controlled-phase gate for in-flight quantum manipulations