In this thesis, I will present the experimental results of the dynamics of superconducting single electron transistors (sSETs), under the influence of tunable dissipation. The sSET, consisting of two dc SQUIDs in series and the third gate electrode, is deposited onto a GaAs/AlGaAs heterostructure which contains a two dimensional electron gas plane 100nm beneath the substrate surface. The Josephson coupling energy, charging energy and dissipation related Hamiltonian can all be tuned in situ, while keeping others unchanged. We measured the switching current statistics and the transport properties, as a function of the dissipation and gate charge at different temperatures. If the sSET is in the classical regime where phase is a good quantum variable, we found that the switching current and corresponding Josephson energy decrease as dissipation increases. Our observation agrees qualitatively with the theoretical calculation of a single Josephson junction with dominant Josephson energy, in a frequency dependent dissipative environment where energy barrier decreases as dissipation increases in thermally activated escape regime. This dissipation dependence result can be understood as the consequence of a reduced quantum fluctuations in the charge numbers. Whereas in the charging regime, the switching current shows a 1e periodicity with respect to gate charge, indicating a pronounced charging effect. At a specific gate charge number, quantum fluctuations of the phase variable are compressed as dissipation increases, resulting in an enhanced switching current and Josephson energy. This result matches the theory of a sSET capacitively coupled to a dissipative environment qualitatively. The temperature dependence of the switching current histogram indicates the existence of both quantum and classical thermal phase diffusion. Moreover, quantum charge fluctuations are minimized at the degeneracy point, causing a sharp dip on the width of the switching current histogram. For a sSET with comparable Josephson energy and charging energy, quantum fluctuations of both phase and charge variables are significant. The influence of dissipation on the dynamics of the device is distinct in the classical and charging regimes. Dissipation compresses quantum phase fluctuations in the charging regime, whereas reduces the quantum charge fluctuations in the classical regime. The transition between these two regimes is found to be determined by the tunnel resistance of the SQUID. The competition between Josephson and charging energies, however, is not the intrinsic parameter of this transition. Our results imply that a detailed theoretical calculation of a sSET with comparable Josephson coupling energy and charging energy under the influence of dissipation is needed.

Zugl.: Wien, Techn. University, Diss., 1997.

Un effort mondial existe actuellement dans le but de réaliser un ordinateur quantique. Un tel dispositif permettrait d'implémenter des algorithmes plus rapides que les algorithmes classiques pour certaines tâches (recherche dans des bases de données, factorisation d'entiers). Il permettrait également de simuler des systèmes quantiques de manière beaucoup plus efficace qu'un ordinateur classique. L'obtention de ce gain en puissance nécessite d'intriquer un grand nombre de bits quantiques (qubits). Celle ci suppose de pouvoir déplacer un qubit d'un point à un autre de l'espace. Dans cette thèse, nous démontrons une première étape vers le déplacement d'un qubit de spin électronique : un électron unique est déplacé, à la demande, entre deux boîtes quantiques distantes de quelques microns. Le transport est réalisé à l'aide d'une onde acoustique de surface qui entraîne l'électron. Le transfert a été réalisé avec une efficacité de 90 % et déclenché à la nanoseconde. Ces résultats ouvrent la voie à la réalisation d'expériences d'optique quantique électronique avec une détection évènement par évènement. L'envoi d'un électron sur deux initialement présents ouvre la voie à la génération de paires d'électrons distants et intriqués. / A global effort is pursued to realise a quantum computer. Such a dispositive will allow to implement faster algorithms for tasks like integer factoring and database search. It will also allow to simulate quantum system much more efficiently. than a classical system. This power gain necessitates to entangle a large number of qubits. This in turn requires the ability to transport a qubit in space. In this thesis, we demonstrate a first step: a single electron is transported on demand from one quantum dot to another quantum dot, micrometers away. The transport is realised thanks to a Surface Acoustic Wave (SAW) that drags the electron. The transfer is realised with an efficiency of 90 % and triggered within one nanosecond. These results open the way to the realisation of electron quantum optics experiments with an event per event detection. A work on the separation of two electron initially present in the quantum dot will lead to the generation of distant entangled particles.

In this thesis I present a complete and detailed guide for the development process and fabrication of efficient single-electron transistors (SETs) and a better single-molecule magnets (SMMs) deposition yield. Starting from a commercial Si/SiO2 wafer I show the steps for the deposition of different layers to fabricate a SET as well as the improvements achieved in those for a completely functional SET device. The development process is based on a combination of optical lithography and e-beam lithography with metal deposition in ultra-high vacuum. The improvements involve a better conductance in the Al gate component, with a controlled formation of the superficial oxide layer and a faster feedback electromigration-induced breaking of Au nanowires for the creation of nanogaps at room temperature. The gate component is improved by increasing its thickness and exposing it to plasma oxidation for the complete oxidation of its surface. The nanowire breaking is realized at room temperature to make use of the surface tension of Au, which, after a previous feedback procedure, eventually opens the final gap in the nanowire. Finally, I demonstrate a new technique that allows increasing the yield of having a SMM connected in the nanowire gap. This new technique is based on monitoring the resistance of the broken nanowires during the SMM deposition from a controlled liquid solution at room temperature. When the resistance ( > GΩ for open gaps) drops to values below Mega-ohms (characteristic resistance of a molecule bridging the gap) for a number of nanowires in the chip, the device is then ready for low temperature measurements.

In this dissertation, we study the most important microscopic aspects that grant molecules such as Single Molecule Magnets (SMMs) their preferential spin direction. We do so by proposing and solving a model that includes correlations between electrons occupying atomic orbitals. In addition, we study the relation between the non-equilibrium electronic transport signatures in a SMM model weakly coupled to a three-terminal single electron transistor device, and the interference features of the SMM model in the presence of a magnetic field. Finally, we investigate the equilibrium transport features in a giant-spin model of a SMM in the Kondo regime. We study how the magnetic field modulation of the energy in a highly anisotropic molecule can affect the conductance of the molecule in the Kondo regime.

The flavin-containing monoamine oxidases (MAO) A and B catalyze the oxidative deamination of primary and secondary amines. The overall process involves a two electron oxidation of the amine to the iminium with concomitantreduction of the flavin. Based on extensive studies with a variety of chemical probes, Silverman and colleagues have proposed a catalytic pathway for the processing of amine substrates and inactivators by MAO-B that is initiated by a single electron transfer (SET) step from the nitrogen lone pair to the oxidized flavin followed by α-proton loss from the resulting amine radical cation that leads to a carbon radical. Subsequent transfer of the second electron leads to the reduced flavin and the iminium product. In the case of N-cyclopropylamines, the initially formed amine radical cation is proposed to undergo rapid ring opening to form a highly reactive primary carbon centered radical that is thought to be responsible for inactivation of the enzyme. In this thesis we have exploited the unique substrate and inactivator properties of 1,4-disubstituted tetrahydropyridine derivatives to probe the mechanism of MAO-B catalysis. Reports of the parkinsonian inducing neurotoxin 1-methyl-4-phenyl-1,2,3,6-tetrahydropyridine (MPTP) as a structurally unique substrate of MAO-B initiated these studies. Consistent with the SET pathway, the N-cyclopropyl analog of MPTP proved to be an efficient time and concentration dependent inactivator but not a substrate of MAO-B. On the other hand, the 4-benzyl-1-cyclopropyl analog is both a substrate and inactivator of MAO-B. These properties may not be consistent with the obligatory formation of a cyclopropylaminyl radicalcation intermediate. In an attempt to gain further insight into the mechanism associated with the MAO catalyzed oxidation of 1,4-disubstituted tetrahydropyridines, deuterium isotope effects studies on both the substrate and inactivation properties of the 4-benzyl-1- cyclopropyl derivative were undertaken. A series of 1-methyl- and 1-cyclopropyltetrahydropyridine derivatives bearing various heteroaro-matic groups at C-4 also have been examined. The MAO-B substrate properties, inactivator properties and partition ratios for these compounds together with preliminary results from chemical model studies are discussed in terms of the MAO-B catalytic pathway. / Ph. D.

Although scalingof CMOS technology has been predicted to continue for another decade, novel technological solutions are required to overcome the fundamental limitations of the decananometer MOS transistors. Single Electron Transistor (SET) has attracted attention mainly because of its unique Coulomb blockade oscillations characteristics, ultra low power dissipation and nanoscale feature size. Despite the high potential, due to some intrinsic limitations (e.g., very low current drive) it will be very difficult for SET to compete head-to-head with CMOS’s large-scale infrastructure, proven design methodologies, and economic predictability. Nevertheless, the characteristics of SET and MOS transistors are quite complementary. SET advocates low-power consumption and new functionality (related to the Coulomb blockade oscillations), while CMOS has advantages like high-speed driving and voltage gain that can compensate the intrinsic drawbacks of SET. Therefore, although a complete replacement of CMOS by single-electronics is unlikely in the near future, it is also true that combining SET and CMOS one can bring out new functionalities, which are unmirrored in pure CMOS technology. As the hybridization of CMOSand SET is gaining popularity, silicon SETs are appearing to be more promising than metallic SETs for their possible integration with CMOS. SETs are normally studied on the basis of the classical Orthodox Theory, where quantization of energy states in the island is completely ignored. Though this assumption greatly simplifies the physics involved, it is valid only when the SET is made of metallic island. As one cannot neglect the quantization of energy states in a semi conductive island, it is extremely important to study the effects of energy quantization on hybrid CMOSSET integrated circuits. The main objectives of this thesis are: (1) understand energy quantization effects on SET by numerical simulations; (2) develop simple analytical models that can capture the energy quantization effects; (3)analyze the effects of energy quantization on SET logic inverter, and finally; (4)developa CAD framework for CMOS-SETco-simulation and to study the effects of energy quantization on hybrid circuits using that framework. In this work the widely accepted SIMON Monte Carlo (MC) simulator for single electron devices and circuits is used to study the effects of energy quantization. So far SIMON has been used to study SETs having metallic island. In this work, for the first time, we have shown how one can use SIMON to analyze SET island properties having discrete energy states.It is shown that energy quantization mainly changes the Coulomb Blockade region and drain current of SET devices and thus affects the noise margin, power dissipation, and the propagation delay of SET logic inverter. Anew model for the noise margin of SET inverter is proposed, which includes the energy quantization term. Using the noise margin as a metric, the robustness of SET inverter is studied against the effects of energy quantization. An analytical expression is developed, which explicitly defines the maximum energy quantization (termedas “Quantization Threshold”)that an SET inverter logic circuit can withstand before its noise margin upper bound crosses the acceptable tolerance limit. It is found that SET inverter designed with CT : CG =0.366 (where CT and CG are tunnel junction and gate capacitances respectively) offers maximum robustness against energy quantization. Then the effects of energy quantization are studied for Current biased SET (CBS), which is an integral part of almost all hybrid CMOS-SET circuits. It is demonstrated that energy quantization has no impact on the gain of the CBS characteristics though it changes the output voltage levels and oscillation periodicity. The effects of energy quantization are further studied for two circuits: Negative Differential Resistance (NDR) and Neurone Cell, which use CBS. A new model for the conductance of NDR characteristics is also formulated that includes the energy quantization term. A novel CAD framework is then developed for CMOS-SET co-simulation, whichuses MCsimulator for SET devices alongwithconventional SPICE. Using this framework, the effects of energy quantization are studied for some hybrid circuits, namely, SETMOS, multiband voltage filter, and multiple valued logic circuits. It is found that energy quantization degrades the performance of hybrid circuit, which could be compensated by properly tuning the bias current of SET devices. Though this study is primarily done by exhaustive MC simulation, effort has also been put to develop first order compact model for SET that includes energy quantization effects. Finally it has been demonstrated that the SET behavior under energy quantization can be predicted byslightlymodifyingthe existing SETcompact models that are valid for metallic devices having continuous energy states.

Le contrôle du nombre et de l'état quantique d'électrons individuels est un élément clé pour la construction d'applications innovantes comme les sources à un électron ou les standards métrologiques de courant. La difficulté d'atteindre la précision métrologique pour une source de courant alimente la recherche fondamentale sur le transport individuel d'électrons dans les structures mésoscopiques. Un candidat prometteur combine le concept de quantification de la charge dans un transistor à un électron et la bande interdite de la densité d'états d'électrodes supraconductrices. Le transport corrélé en temps d'électrons entre les électrodes supraconductrices est alors assuré par la densité d'états continue de l'ilot métallique central. Le grand nombre d'états électroniques disponibles dans l'ilot, bien que favorable en termes de couplage tunnel, a néanmoins deux conséquences importantes que sont les fluctuations thermiques et des processus parasites d'ordre supérieur, ce qui limite la performance de ces dispositifs. Dans ce contexte, nous explorons le transport de charges dans un tourniquet à électrons hybride basé sur une boîte quantique en lieu et place de l'ilot métallique. Les dispositifs sont réalisés par l'électromigration contrôlée de constrictions d'Aluminium précédée par le dépôt aléatoire de nano-particules d'or. Ce procédé in-situ (réalisé à 4 K) permet l'obtention de jonctions tunnel entre des électrodes supraconductrices d'aluminium et nano-particules d'or avec un taux de succès de l'ordre de 4%. Nous caractérisons le transport statique et en fréquence dans ces nanostructures par la mesure statique du courant à une température de 100 mK dans un environnement fortement filtré, mais néanmoins compatible avec l'électro-migration, d'un réfrigérateur à dilution. L'analyse des cartes de conductance en fonction des tensions drain-source et de grille révèle une énergie de charge très élevée de l'ordre de 10 meV et un écart entre niveaux discrets d'énergie de l'ordre de 1 meV. Par une étude détaillée de l'élargissement des pics de cohérence au seuil du blocage de Coulomb, nous montrons que le transport électronique est assuré par un niveau unique dans la boîte quantique. Bien que le couplage tunnel soit faible, le temps de vie d'un électron dans un niveau donné est dominé par l'hybridation des états électroniques entre les électrodes et la boîte quantique. En effet, les fluctuations thermiques et les processus inélastiques sont inopérants du fait du grand écart d'énergie entre niveaux et de la bande interdite supraconductrice dans les électrodes. L'observation de résonances sous le seuil imposé par le blocage de Coulomb est décrite par des processus de cotunneling de type paire de Cooper-électron. Lorsqu'un signal radio-fréquence de forme sinusoïdale ou carrée est ajouté à la tension de grille, un fonctionnement de tourniquet à électron est montré. Nous obtenons un courant quantifié jusqu'à une fréquence de 200 MHz, au delà de laquelle la précision se dégrade à cause d'évènements tunnel manqués. Le couplage à un niveau unique dans la boîte quantique est clairement démontré par l'apparition d'effets de transport tunnel inversé à grande tension drain-source ainsi que l'insensibilité à la température jusqu'à environ 300 mK. Enfin, nous observons une suppression systématique du courant uniquement à basse fréquence et avec un signal r.f. sinusoïdal. En accord avec une prédiction théorique, nous montrons que les effets tunnel manqués sont causés par un processus adiabatique au travers l'anti-croisement d'un niveau quantique sur la boîte quantique avec la densité d'états des électrodes supraconductrices. Nos expériences fournissent la première démonstration expérimentale de la répulsion de niveaux entre un niveau discret et un semi-continuum, illustrant ainsi l'évolution cohérente de nos tourniquets hybrides à électron dans un régime adiabatique. / Accurate control over the state and motion of single individual electrons would enable a variety of appealing applications reaching from quantized to quantum coherent electron sources. Realizing the accuracy of quantized current sources required for a metrological standard is however extremely challenging and has naturally fuelled fundamental research into single electron transport through mesoscopic structures. A promising candidate, foreseen to meet the demand, combines the concept of quantized charge in single electron transistors (SETs) and the gapped density of states in superconducting metals (hence called hybrid electron turnstile), to produce a quantized current. The time-correlated electron transport (sub-poissonian) between the superconducting leads is conveyed by the continuous density of states of the central normal island. The large amount of available states at the normal island, although favorable in terms of tunnel coupling, has nevertheless two important ramifications i.e. 1) thermal fluctuations and 2) adverse higher-order processes, which limit the performance of hybrid electron turnstiles. Inspired by this ingenious application and the advances in quantum dot trans- port, we explore the operation of a hybrid electron turnstile embodying a bottom-up quantum dot instead of the usual metallic island. The desired devices are obtained by controlled electromigration of aluminium nano-wires preceded by the deposition of gold nano-particles. This in-situ process (conducted at 4 K) produces pristine tunnel junctions between aluminium leads and gold nano-particles with a yield of about 4%. We characterize the stationary and turnstile operation by direct current measurements at 100 mK, in a heavily filtered, but electromigration compatible, inverse dilution refrigerator. Analysis of the acquired conductance maps under stationary conditions, reveal a large charging energy (> 10 meV) and mean level spacing (> 1 meV). With a detailed study of the coherence peak broadening at the Coulomb blockade (CB) threshold, we show that electron transport through the quantum dot is conveyed by a single quantum level. Although the tunnel coupling is weak, the single level life-time is dominated by the lead - quantum dot hybridization as thermal energy fluctuation and in-elastic scattering are suppressed by the large single level spacing on the quantum dot and the superconducting gap in the leads. The observation of sub-threshold resonances parallel to the CB diamond edges are consistent with earlier predicted higher-order Cooper-pair - electron (CPE) cotunneling processes. Under turnstile operation a periodic modulation signal (sine or square wave) is added to the static gate potential. We demonstrate quantized current up to 200 MHz at which its accuracy starts to worsen due to missed tunnel events. Strong experimental evidence of the single quantum dot level nature of our turnstile device is provided by a sharp onset of backtunneling processes and the temperature-robust operation beyond 300 mK. Finally we observe a systematic current suppression unique to the low frequency sine wave operation. Supported by theoretical work, we show that the underlying missed tunnel events are caused by adiabatic traverses across the avoided crossing of a quantum dot level and superconducting gap edges. These experiments deliver the first experimental observation of the level repulsion between an electronic discrete state and a semi-continuum and demonstrate the quantum coherent evolution of our devices under adiabatic operation conditions.

Ce travail porte sur le développement d'un procédé de fabrication de transistor monoélectronique {single-electron transistor, SET). II dresse un portrait de l'état de l’art actuel et met en lumière un manque dramatique de marge d'opération dans le fonctionnement de ces dispositifs. Cette problématique est présentée comme une des limites majeures aux espoirs de développement commercial de cette technologie. La thèse propose d'aller chercher la marge de manoeuvre manquante par un procédé de fabrication qui exploite le contrôle des dimensions verticales des dispositifs. Les résultats montreront que si les approches actuelles 2D semblent avoir atteint leurs limites physiques, l'approche 3D permet d'accéder à des températures d'opération encore insoupçonnées jusqu'à présent. L'impact est important, puisqu'une analyse de la thèse conclura que, même en tenant compte des pires fluctuations du procédé de fabrication, les SETs issus du concept 3D conservent une marge d'opération appréciable. La gamme de température d'opération obtenue est semblable aux transistors à effet de champ conventionnels (field effect transistor, FET) et on peut penser qu'il serait ainsi possible d'utiliser les deux technologies simultanément sur un même substrat afin de créer de nouvelles fonctionnalités issues de cette technologie hybride SET/FET.

Selenium is a required trace element which was originally discovered by the Swedish chemist Jons Jacob Berzelius in 1817. It was initially believed to be a toxin as it was identified as being the cause of hoof maladies and excessive hair loss in horses that feed upon plants with high selenium content. It wasn’t until 1957 that the potential contributions of selenium to physiology were first demonstrated. Selenium is now known to play a critical role in the maintenance of human health. Interestingly, unlike other trace metals/semi-metals, selenium is directly incorporated into proteins in the form of the amino acid selenocysteine (Sec) in a very complicated and energetically costly fashion. Though rare, being found in only 25 human proteins, Sec proteins are involved in numerous vital biological processes including maintenance of redox homeostasis and anti-oxidant defense. Even though Sec is essential, the reason that Sec replaces its structural analog cysteine (Cys) in only 25 proteins is not widely agreed upon. A previous model suggests that the replacement of Cys with Sec provides enzymes with a type of catalytic advantage. The presence of Cys-containing orthologs of mammalian Sec-enzymes in other eukaryotes argues against this model. A newer model to explain the use of Sec is that the gain of function imparted to an enzyme by replacing Cys with Sec is the ability of Sec to impart chemical reversibility. Building on previous results from our lab demonstrating the ability of Sec to confer proteins with the ability to resist over oxidation we have elucidated the mechanism by which Sec containing thioredoxin reductase (TrxR) resists over oxidation. The ability of Sec-TrxR to resist oxidative inactivation is due to the greater electrophilicity of Sec relative to Cys. This allows for quicker resolution and prevents over oxidation. Based on these findings we also investigate the utility of the alkylating agent dimedone to probe the oxidation state of Sec. Interestingly, it was discovered that dimedone will react with seleneninic acid with the resulting adduct being labile. Additonally it was discovered that dimedone will also react with seleninic acid, resulting in the formation of a dimedone dimer. These results call into question the usefulness of dimedone in deteremining the oxidation state of Sec. Finally, we provide evidence that Sec-TrxR enzymes are able to catalyze single electron reductions. This is most likely due to the formation of a stable Sec radical intermediate. As a whole this project provides support for the theory that Sec was selected for due to its ability to convey chemical reversiablity to proteins.