Orientadores: Alberto Vazquez Saa, Amir Ordacgi Caldeira / Tese (doutorado) - Universidade Estadual de Campinas, Instituto de Física Gleb Wataghin / Made available in DSpace on 2018-08-17T18:21:33Z (GMT). No. of bitstreams: 1 Richartz_Mauricio_D.pdf: 3399746 bytes, checksum: 3da68926653d0bbb338f76240696b246 (MD5) Previous issue date: 2011 / Resumo: A Conjectura da Censura Cosmica, proposta por Roger Penrose em 1969, afirma que singularidades resultantes de um colapso gravitacional estão sempre envolvidas pelo horizonte de eventos de um buraco negro. O objetivo desse trabalho é investigar processos de tunelamento quântico que visam violar essa conjectura. Através do formalismo de Newman-Penrose, é feita, inicialmente, uma análise de perturbações escalares, de neutrinos, eletromagneticas e gravitacionais nas métricas de Kerr e de Reissner-Nordstr om. Processos de espalhamento ondulatorio nessas métricas são estudados e coeficientes de transmissão e reflexão para ondas incidentes são calculados nos limites de baixas energias. A partir desses resultados, experimentos imaginários com o intuito de destruir o horizonte de eventos de um buraco negro e expor sua singularidade para um observador externo são propostos e analisados. A superradiância, fenômeno no qual ondas incidentes são amplificadas ao serem refletidas por um potencial espalhador, se manifesta nesses experimentos e, por isso, é tratada com detalhes e de uma forma bastante geral nesse trabalho. Por fim, experimentos que visam detectar a radiação Hawking e o fenômeno da superradiância em modelos análogos de gravitação são analisados. Em particular, um experimento proposto por mim, em colaboração com Silke Weinfurtner, cujo objetivo e investigar a possibilidade de obtenção de superradiância em laboratório, é discutido / Abstract: The Cosmic Censorship Conjecture, proposed by Roger Penrose in 1969, asserts that singularities arising from the gravitational collapse of a body are always encompassed by the event horizon of a black hole. The main purpose of this work is to investigate quantum tunneling processes whose objetive is to violate this conjecture. Using the Newman-Penrose formalism, scalar, neutrino, electromagnetic and gravitational perturbations in both Kerr and Reissner-Nordstr om metrics are analysed. Wave scattering processes in these metrics are studied and transmission and reflection coecients for incident waves are calculated in the limit of small energies. From these results, gedanken experiments with the purpose of destroying the event horizon of a black hole and exposing its inner singularity to an external observer are proposed and analysed. Superradiance, phenomenum in which incident waves are amplified when reflected by a scattering potential, manifests itself in these thought experiments and, therefore, is also treated in detail in this work. Finally, some experiments with the purpose of detecting Hawking radiation and superradiance in analogue models of gravity are analysed. In particular, an experiment proposed by me, in collaboration with Silke Weinfurtner, whose aim is to investigate the possibility of superradiance detection in laboratory, is discussed / Doutorado / Física das Particulas Elementares e Campos / Doutor em Ciências

A series of para-substituted phenylethylamine analogues bound to the enzyme aromatic amine dehydrogenase have been simulated using quantum mechanical electronic structure calculations and molecular mechanical molecular dynamics simulations. Trends have been verified connecting bond dissociation energy (and thus driving force) to observed rate constants and activation enthalpy. Trends have been identified in connecting statistics drawn from molecular dynamics simulations and the temperature dependence of the kinetic isotope effect, notably that as the temperature dependence of the kinetic isotope effect increases the flexibility of the promoting vibration decreases. This is explained as being more effected by thermal energy put into the system, and therefore more affected by temperature.

There is a movement in the electronic industry toward building electronic devices with dimensions smaller than is currently possible. Atomically thin 2D material, such as graphene, bilayer graphene, hBN and MoS2 are great candidate for this goal and they have a potential set of novel electronic properties compare to their bulk counterparts due to the exhibition of quantum confinement effects. To this goal, we have investigated the electric field screening of multilayer 2D materials due to the presence of impurity charge in the interface and vertical electric fifield from back gate. Our result shows a dramatic difference of screening behavior in high and low charging limit, which depends on the number of layers as well. We also have an extensive study on quantum tunneling effect in graphene and bilayer graphene heterojunctions. The peculiar electronic properties of graphene lead to an unusual scattering effect of electron in graphene n-p junction. We implement the cohesive tunneling effect to explain the nonlinear electron transport in ultrashort channel graphene devices. This nonlinear behavior could make them tremendously useful for ultra-fast electronic applications.

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The prominent features of single molecule magnets (SMMs), such as the quantum tunneling of the magnetization (QTM), are conventionally understood through the giant spin approximation (GSA) which considers the molecule as a single rigid spin. This model often requires the inclusion of high order anisotropy terms in the Hamiltonian, a manifestation of admixing of low lying excited states that can be more naturally understood by employing a multi-spin (MS) description i.e. considering the individual spins and the interactions between ions within the molecule. However, solving the MS Hamiltonian for high nuclearity molecules is not feasible due to the enormous dimensions of the associated Hilbert space that put it beyond the capability of existing computational resources. In contrast, low nuclearity systems permit the complete diagonalization of the MS Hamiltonian required to sample the effect of internal degrees of freedom, such as exchange interactions and single ion anisotropies, on the QTM. This dissertation focuses on the study of low nuclearity SMMs in view of understanding these subtle quantum effects. To accomplish this, we have developed a series of magnetic characterization techniques, such as integrated microchip sensors resulting from the combination of two dimensional electron gas (2DEG) Hall-Effect magnetometers and microstrip resonators, capable of performing measurements of magnetization and EPR spectroscopy simultaneously. The thesis bases on a comparative study of two low nuclearity SMMs with identical magnetic cores (Mn4 dicubane) but differing ligands. Notably, one of these SMMs lacked solvent molecules for crystallization; a characteristic that gives rise to extremely sharp resonances in the magnetization loops and whose basic QTM behavior can be well explained with the GSA. On the contrary, the second SMM exhibited mixed energy levels, making a MS description necessary to explain the observations. We have also examined the role of internal degrees of freedom on more subtle QTM phenomena, leading to the explanation of asymmetric Berry-phase interference patterns observed in a Mn4 SMM in terms of a competition between different intermolecular magnetic interactions, i.e. non-collinear zero-field splitting tensors and intramolecular dipolar iii interactions, resulting in astonishing manifestations of the structural molecular symmetry on the quantum dynamics of the molecular spin.

Detectors and sensors are an integral part of modern electronics and are crucial to highly sensitive applications. Metal-Insulator-Metal (MIM) tunnel junctions have been explored for the past five decades and are still being investigated due to its wide use of applications such as mixers, capacitors, detectors, rectifiers and energy conversion devices. In this research, various designs of thin film based tunnel junctions have been investigated and the optimum one picked for the purpose of a wide band detector up to 10GHz based on their sensitivities. A modified design with an isolation layer incorporating a self-aligning method to increase fabrication throughput was developed. A mask for the reliability testing of multiple devices with different areas was also developed. Nickel Oxide based insulators with different stoichiometries have been incorporated in the fabrication of the device to identify which stoichiometry gives the best performance for high frequency applications. Nickel Oxide (NiO), Zinc Oxide (ZnO) and the combination of the two have been deposited using reactive sputtering and investigated as insulator materials. The bilayer devices showed increased sensitivities at lower turn on voltages and very good efficiencies at 100MHz and 1GHz. Although, the MIM device provides a simple structure, some of the critical parameters required to quantify the device functionality are still being explored. Based on the parameters, a criterion was developed to help engineer a tunnel device for a desired detectivity.

The main body of this thesis describes how to calculate scanning tunneling microscopy (STM) images from first-principles methods. The theory is based on localized orbital density functional theory (DFT), whose limitations for large-vacuum STM models are resolved by propagating localized-basis wave functions close to the surface into the vacuum region in real space. A finite difference approximation is used to define the vacuum Hamiltonian, from which accurate vacuum wave functions are calculated using equations based on standard single-particle Green’s function techniques, and ultimately used to compute the conductance. By averaging over the lateral reciprocal space, the theory is compared to a series of high-quality experiments in the low- bias limit, concerning copper surfaces with adsorbed carbon monoxide (CO) species and adsorbate atoms, scanned by pure and CO-functionalized copper tips. The theory compares well to the experiments, and allows for further insights into the elastic tunneling regime. A second significant project in this thesis concerns first-principles calculations of a simple chemical reaction of a hydroxyl (oxygen-deuterium) monomer adsorbed on a copper surface. The reaction mechanism is provided by tunneling electrons that, via a finite electron-vibration coupling, trigger the deuterium atom to flip between two nearly identical configurational states along a frustrated rotational motion. The theory suggests that the reaction primarily occurs via nuclear tunneling for the deuterium atom through the estimated reaction barrier, and that over-barrier ladder climbing processes are unlikely.

SOUSA, Ariel Adorno de. Vazamentos de corrente e ineficiência de transporte em nanoestruturas semicondutoras investigadas através de propagação de pacotes de onda. 2015. 149 f. Tese (Doutorado em Física) - Programa de Pós-Graduação em Física, Departamento de Física, Centro de Ciências, Universidade Federal do Ceará, Fortaleza, 2015. / Submitted by Edvander Pires (edvanderpires@gmail.com) on 2015-06-11T18:23:58Z No. of bitstreams: 1 2015_tese_aasousa.pdf: 11602478 bytes, checksum: 96b288e68aacaf0da271842e48706b70 (MD5) / Approved for entry into archive by Edvander Pires(edvanderpires@gmail.com) on 2015-06-11T18:24:41Z (GMT) No. of bitstreams: 1 2015_tese_aasousa.pdf: 11602478 bytes, checksum: 96b288e68aacaf0da271842e48706b70 (MD5) / Made available in DSpace on 2015-06-11T18:24:41Z (GMT). No. of bitstreams: 1 2015_tese_aasousa.pdf: 11602478 bytes, checksum: 96b288e68aacaf0da271842e48706b70 (MD5) Previous issue date: 2015 / Advances in growth techniques have made possible the fabrication of quasi one-dimensional semiconductor structures on nanometric scales, called quantum dots, wires, wells and rings. Interest in these structures has grown considerably not only due to their possible applications in electronic devices and to their easy chemical manipulation, but also because they offer the possibility of experimentally exploring several aspects of quantum confinement, scattering and interference phenomena. In particular, in this work, we investigate the electronic and transport properties in quantum wells, wires and rings, whose dimensions can be achieved experimentally. For this purpose, we solve the time-dependent Schrödinger equation using the split-operator method in two dimensions. We address four different problems: in the first one, the electronic transport properties of a mesoscopic branched out quantum ring are discussed in analogy to the Braess Paradox of game theory, which, in simple words, states that adding an extra path to a traffic network does not necessarily improves its overall flow. In this case, we consider a quantum ringindex{Quantum ring} with an extra channel in its central region, aligned with the input and output leads. This extra channel plays the role of an additional path in a similar way as the extra roads in the classical Braess paradox. Our results show that in this system, surprisingly the transmission coefficient decreases for some values of the extra channel width, similarly to the case of traffic networks in the original Braess problem. We demonstrate that such transmission reduction in our case originates from both quantum scattering and interference effects, and is closely related to recent experimental results in a similar mesoscopic system. In the second work of this thesis, we extend the first system by considering different ring geometries, and by investigating the effects of an external perpendicular magnetic field and of obstructions to the electrons pathways on the transport properties of the system. For narrow widths of the extra channel, it is possible to observe Aharonov-Bohm oscillations in the transmission probability. More importantly, the Aharonov-Bohm phase acquired by the wave function in the presence of the magnetic field allows one to verify in which situations the transmission reduction induced by the extra channel is purely due to interference. We simulate a possible closure of one of the paths by applying a local electrostatic potential, which can be seen as a model for the charged tip of an atomic force microscope (AFM). We show that positioning the AFM tip in the extra channel suppresses the transmission reduction due to the Braess paradox, thus demonstrating that closing the extra path improves the overall transport properties of the system. In the third work, we analyze the tunneling of wave packets between two semiconductor quantum wires separated by a short distance. We investigate the smallest distance at which a significant tunneling between the semiconduting wires still occur. This work is of fundamental importantance for the manufacturing of future nanostructured devices, since it provides information on the minimum reasonable distances between the electron channels in miniaturized electronic circuits, where quantum tunnelling and interference effects will start to play a major role. In the last work of this thesis, we investigate the binding energy of the electron-impurity pair in a GaN/HfO2 quantum well. We consider simultaneously the contributions of all interactions in the self-energy due to the dielectric constant mismatch between materials. We investigate the electron-impurity bound states in quantum wells of several widths, and compared the results for different impurity positions. / Os avanços nas técnicas de crescimento tornaram possível a fabricação de estruturas semicondutoras quase-unidimensionais em escalas nanométricas, chamadas pontos, fios, poços e anéis quânticos. Interesse nessas estruturas tem crescido consideravelmente, não só devido às suas possíveis aplicações em dispositivos eletrônicos e à sua manipulação química fácil, mas também porque eles oferecem a possibilidade de explorar experimentalmente vários aspectos de confinamento quântico, espalhamento e fenômenos de interferência. Em particular, neste trabalho, investigamos as propriedades eletrônicas e de transporte em poços quânticos, fios e anéis, cujas dimensões podem ser alcançados experimentalmente. Para isto, resolvemos a equação de Schrödinger dependente do tempo utilizando o método Split-operator em duas dimensões. Nesta tese, abordamos quatro trabalhos, sendo o primeiro uma analogia ao Paradoxo de Braess para um sistema mesoscópico. Para isso, utilizamos um anel quântico com um canal adicional na região central, alinhado com os canais de entrada e saída. Este canal extra faz o papel do caminho adicional em uma rede de tráfego na teoria dos jogos, similar ao caso do paradoxo de Braess. Calculamos as auto-energias e a evolução temporal para o anel quântico. Surpreendentemente, o coeficiente de transmissão para algumas larguras do canal extra diminuiu, semelhante ao que acontece com redes de tráfego, onde a presença de uma via extra não necessariamente melhora o fluxo total. Com a analise dos resultados obtidos, foi possível determinar que neste sistema o paradoxo ocorre devido a efeitos de interferência e de espalhamento quântico. No segundo trabalho, foi feita uma extensão do primeiro, (i) aplicando-se um campo magnético, onde foi possível obter o efeito Aharonov-Bohm para pequenos valores do canal extra e controlar efeitos de interferência responsáveis pelo paradoxo mencionado, e (ii) fazendo também a aplicação de um potencial que simula a ponta de um microscópio de força atômica (AFM) interagindo com a amostra - este potencial é repulsivo e simula um possível fechamento do caminho em que o pacote de onda se propaga. Assim, neste trabalho, realizamos uma contra-prova do primeiro, onde observamos que com o posicionamento da ponta do AFM sobre canal extra, se diminui o efeito de redução de corrente devido ao paradoxo de Braess. No terceiro trabalho, realizamos uma análise de tunelamento entre dois fios quânticos separados por uma certa distância e calculamos qual a menor distância para qual ocorre tunelamento significativo nesse sistema eletrônico. Este trabalho é de fundamental importância para o manufaturamento de dispositivos nanoestruturados, porque nos permite investigar qual a distância mínima para a construção de um circuito eletrônico sem que haja interferências nas transmissões das informações. No quarto e último trabalho desta tese, investigamos a energia de ligação do elétron-impureza em GaN/HfO2 para um poço quântico. Consideramos simultaneamente as contribuições de todas as interações das auto-energias devido ao descasamento das constantes dielétricas entre os materiais. Foram estudados poços largos e estreitos, comparando os resultados para diferentes posições da impureza e a contribuição da auto-energia para o sistema.

Dans ce manuscrit, nous présentons d'abord le bloc de construction moléculaire ultime pour les dispositifs de spintronique, les aimants à molécule unique (Chapitre 2). En particulier, nous nous concentrerons sur une molecule de TbPc2 et différentes approches pour sonder son aimantation à l'aide de détecteurs a base de nanotubes de carbone et de mécanismes de couplage différents (flux magnétique, couplage électronique et mécanique). Dans le but de construire un detecteur de torque supramoléculaire capable de sonder le moment magnétique d'un aimant moléculaire, nous allons décrire dans le chapitre 3 un candidat très prometteur, un système nanoélectromécanique (NEMS) à base d'un nanotube de carbone. Nous décrirons d'abord les avantages de NEMS à base de carbone par rapport aux résonateurs classiques à base de silicium. Par la suite, nous présenterons l'état de l'art des NEMS à base de nanotubes de carbone, en nous focalisant en particulier sur deux différents mouvements nanomécaniques, un mode de flexion transverse et un mode de compression longitudinal. Dans le chapitre 4, nous présenterons la mise en oeuvre expérimentale d'un detecteur de torque supramoléculaire basé sur NEMS à nanotubes de carbone et des aimants à molécule unique. Nous décrirons d'abord le processus de fabrication ultra propre et les étapes de la caractérisation d'un NEMS à nanotubes de carbone à températures ambiante et cryogénique. Nous allons ensuite démontrer un procédé de greffage d'une molécule aimants de TbPc2 sur un tel NEMS à nanotube de carbone, qui conserve à la fois les propriétés magnétiques de la molécule et les propriétés mécaniques du résonateur. Dans le chapitre 5, nous allons ensuite procéder à une étude systématique du mode de flexion transverse dans un NEMS à nanotube de carbone. Nous montrerons, que la dissipation de ce mode de vibration induit par l'effet tunnel d'électron unique à travers le nanotube de carbone (considére comme point quantique) dépend essentiellement de l'environnement électronique du nanotube, c'est à dire de la capacité, du couplage entre le nanotube de carbone et les electrodes métalliqes, du courant et de la température. Les résultats indiquent que l'on pourrait atteindre des facteurs de qualité de 10^6 ou plus en choisissant un diélectrique de grille appropriées et/ou en améliorant le couplage entre le nanotube de carbone et les electrodes, ce qui permettrait notamment d'augmenter la sensibilité du NEMS nanotubes de carbone par rapport à un torque magnétique générer par le retournement d'un aimant moléculaire. Dans le chapitre 6, nous démontrons la présence d'un mode de vibration longitudinal quantique dans un NEMS à base de nanotube de carbon fonctionnalisé avec des aimants moléculaires de TbPc2. Nous allons en particulier montrer que la nature quantique des deux systèmes, se traduit par un fort couplage entre le mode de compression longitudinal et l'aimantation d'un aimant moléculaire TbPc2 unique greffé sur la parois du nanotube de carbone. Ce fort couplage permet par la suite de détecter les états de spin nucléaire dans la molécule de TbPc2. Enfin, nous présenterons dans la conclusion de ce manuscrit quelques perspectives pour la détection et la manipulation (coherente) d'un seul spin (nucléaire) à l'aide d'un système mécanique quantique. / In this manuscript, we will first present the ultimate molecular building block for spintronic devices, so called single-molecule magnets (Chapter 2). In particular we will focus on a TbPc2 complex and various approaches of probing its magnetization using carbon nanotube detectors and different coupling mechanisms (magnetic flux, electronic and mechanical coupling). With the aim of building a supramolecular torque magnetometer capable of probing the magnetic moment of a molecular magnet, we will describe in Chapter 3 a promising candidate, a carbon nanotube nanoelectromechanical system (NEMS). We will first describe the advantages of carbon based NEMS over classical Si based resonators. Subsequently we will present the state of art of carbon nanotube NEMS and focus in particular on two different nanomechanical motions, a transverse bending mode and a longitudinal stretching mode. In Chapter 4, we present the experimental implementation of a supramolecular torque magnetometer based on carbon nanotube NEMS and single molecule magnets. We first describe the ultraclean bottom-up fabrication process and the extensive characterisation steps of carbon nanotube NEMS at room and cryogenic temperatures. We will finally demonstrate a method of grafting a TbPc2 single molecules magnet on such a carbon nanotube NEMS, that conserves both the magnetic properties of the molecule and the mechanical properties of the resonator. In Chapter 5, we will then perform a systematic study of the transverse bending mode vibration in a carbon nanotube NEMS. We demonstrate for instance, that the dissipation of a carbon nanotube's bending mode vibration to single electron tunneling through the carbon nanotube NEMS-quantum dot critically depends on the dot's electronic environment, i.e. the capacitance, the tunnel coupling to the metal leads, the current and temperature. The findings suggest that one could achieve quality factors of 10^6 or higher by choosing appropriate gate dielectrics and/or by improving the tunnel coupling to the leads, which would notably increase the sensitivity of the carbon nanotube NEMS with respect to a magnetic torque generate by a rotating molecular magnet. In Chapter 6, we demonstrate the presence of a quantized longitudinal stretching mode vibration in a carbon nanotube NEMS functionnalized with TbPc2 single molecule quantum magnets. We will in particular demonstrate that the quantum mechanical nature of both systems, results in a strong coupling between the longitudinal stretching mode and the magnetization of an individual TbPc2 single molecule magnet grafted to the carbon nanotube's sidewall. The strong coupling in fact enables the detection of the nuclear spin states in the TbPc2 molecule. Finally, we present in the conclusion of this manuscript some future prospects for the detection and (coherent) manipulation of a single (nuclear) spin using a mechanical quantum system.

Indiana University-Purdue University Indianapolis (IUPUI) / Based on plane wave DFT calculation, we carried out micro level investigation of hydrogen storage in nanoporous silicon (npSi). One quarter of a hexagonal pore with Palladium catalyst placed at the surface has been studied for hydrogen dissociation, spillover, bond hopping, and diffusion for both single catalyst atom and small catalyst cluster consisting of multiple catalyst atoms. All the DFT computations were done in one of the biggest research supercomputer facilities of the world, Big Red II. We opted ABINIT, an open source DFT tool for our computations. Our calculation revealed low dissociation, spillover, and bond hoping energy barrier. The energy required to be provided from external sources to fully recharge the storage medium from a gaseous source at a completely empty state has also been evaluated. Hydrogen diffusion along the inner surface of the pore as a means of bond hopping and the possibility of quantum tunneling, a low temperature phenomena used to spontaneously go over an otherwise less likely high energy barrier have been studied as well. Using these micro level parameter values evaluated from the DFT study, the performance of any potential hydrogen storage material can be compared to a set of characteristics sought in an efficient storage media. Thus, the micro scale feasibility of this novel npSi material based hydrogen storage technology was studied as a part of a STTR Phase I project.