Soubelet, Pedro I. (2019) Dinámica vibracional de nanoestructuras semiconductoras bidimensionales: superredes y dicalcogenuros de metales de transición. / Vibrational dynamics of two-dimensional semiconductor nanoestructures: superlattices and transition metal dichalcogenides. Tesis Doctoral en Física, Universidad Nacional de Cuyo, Instituto Balseiro.
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Resumen en español
Las propiedades vibracionales tienen una participación fundamental en la determinaci ón de las propiedades físicas de los materiales en general. En particular, en materiales semiconductores, los fonones (cuantos de vibración) son los principales portadores de calor y su interacción con los portadores de carga define gran parte de sus propiedades, como por ejemplo la conductividad térmica y eléctrica. Por esta razón, el estudio de los modos vibracionales y su interacción con los portadores de carga en estructuras fabricadas con estos materiales tiene un gran interés, no sólo desde el punto de vista de su física fundamental, sino también desde el punto de vista tecnológico. A lo largo de este trabajo de tesis se estudió exhaustivamente la dinámica vibracional de dos tipos diferentes de sistemas semiconductores, los cuales permiten, bajo determinadas circunstancias, ejercer control sobre sus diferentes excitaciones elementales como ser excitones y fonones, y la interacción de estos con fotones. Estos sistemas son, por un lado, las superredes semiconductoras del tipo III-V y, por otro, los semiconductores de multicapas moleculares. El primer caso analizado corresponde al de heteroestructuras de GaAs/AlAs crecidas epitaxialmente, en las cuales se ven fuertemente modificadas las densidades de estados electrónica y vibracional. En esta clase de estructuras se basan una gran cantidad de dispositivos optoelectrónicos actuales (diodos emisores, láseres de estados sólido, etc.). El segundo sistema semiconductor lo constituyen los dicalcogenuros de metales de transición. Esta novedosa clase de materiales está formada por capas moleculares bidimensionales y, mediante exfoliación, es posible aislar monocapas de dimensiones atómicas, cuyas propiedades mecánico-estructurales, ópticas y electrónicas han despertado un interés sin precedentes en la comunidad científica y tecnológica. Su utilización en combinación con otros calcogenuros ha impulsado nuevas escalas de miniaturización de diferentes dispositivos multifuncionales. En este trabajo nos hemos centrado en el estudio de un dicalcogenuro en particular, el diseleniuro de molibdeno (MoSe2). Ambos sistemas se estudiaron por medio de la técnica de espectroscopía Raman, una técnica que ha demostrado, a lo largo de las últimas cinco décadas, ser muy adecuada para acceder a la información espectral de los modos acústicos presentes en estas estructuras. Para el caso de las superredes, mediante esta técnica, se propuso la utilizaci ón de esquemas de dispersión novedosos y diferentes a los usuales. Se propuso una estructura de guía de onda híbrida, acústica y óptica a la vez, en la cual los modos vibracionales que se generan poseen un vector de onda en el plano de la superred y se encuentran guiados a través de la misma. Estas geometrías de dispersión permiten tener acceso a modos acústicos transversales que están prohibidos bajo geometrías de dispersión usuales. En los semiconductores multicapa la espectroscopía Raman permitió la caracterizaci ón exhaustiva de los modos vibracionales de muestras de MoSe2, en función del número de capas moleculares (desde una única monocapa hasta el caso masivo), hall ándose características espectrales no informadas hasta la fecha en la literatura. Finalmente, se hicieron experimentos de espectroscopía Raman resonante con los distintos estados electrónicos del material permitiendo, de este modo, el estudio del acoplamiento fotón-excitón. La dinámica de estos fonones, directamente en el espacio temporal, fue estudiada por medio de la técnica de espectroscopía ultrarrápida. El método utilizado fue el de "bombeo y sondeo" (comúnmente denominado pump-probe), donde se estudia la evolución de fonones acústicos, generados coherentemente por medio de una excitación impulsiva de la muestra provista por pulsos láser ultracortos. En el caso de las superredes, estos experimentos permitieron poner a prueba la estructura de guía de onda acústica. Por otro lado, al realizar experimentos sintonizando la energía del láser de excitación en torno a la energía de los estados electrónicos confinados, fue posible evaluar y estudiar directamente en el espacio temporal el acoplamiento entre los estados electrónicos y vibracionales, así como los efectos de generación resonante de fonones acústicos coherentes. Para el caso de los semiconductores multicapa, la técnica de pump-probe permitió realizar un estudio detallado de la vida media de uno de los modos vibracionales propios de esta clase de sistemas, el modo de "respiración intercapa" (breathing mode). Finalmente, analizando este modo particular que evidencia directamente el acoplamiento intercapa, se estudiaron los efectos de adhesión de estas muestras al substrato. Al ser sometidos a la condición de contorno del substrato, se observaron cambios muy signifi- cativos respecto a las muestras suspendidas, no sólo en la parte fonónica sino, también, sobre sus estados excitónicos. Si bien el trabajo tiene su foco principalmente en el área de la física experimental, presentamos diversos modelos teóricos fenomenológicos que explican conceptualmente gran parte de las observaciones realizadas.
Resumen en inglés
The vibrational properties have a fundamental role in the determination of the physical properties of materials in general. In particular, in semiconductor materials, phonons (quanta of vibration) are the main heat carriers, and their interaction with charge carriers defines a large part of their properties, such as thermal and electrical conductivity. For this reason, the study of vibrational modes and their interaction with charge carriers in structures made of these materials is of great interest, not only from the point of view of their fundamental physics, but also from a technological perspective. In this thesis we thoroughly study the vibrational dynamics of two different types of semiconductor systems, which enable, under certain conditions, the control of their different elementary excitations such as excitons and phonons, and their interaction with light (photons). These systems are, on the one hand, semiconductor superlattices of type III-V and, on the other hand, multilayered molecular semiconductors. The first analyzed case corresponds to epitaxially grown GaAs/AlAs heterostructures, in which the densities of electronic and vibrational states are strongly modified. A large number of optoelectronic devices are based on this class of structures (emitting diodes, solid state lasers, etc.) The second system consists of semiconductor transition metal dichalcogenides. These novel class of materials is made up of two-dimensional molecular layers and, by exfoliation, it is possible to isolate monolayers of atomic dimensions, whose mechanostructural, optical, and electronic properties have aroused unprecedented interest in the scientific and technological communities. Its use, in combination with other chalcogenides with different characteristics, has promoted new scales of miniaturization of different multifunctional devices. In this work we have focus on the study of a particular dichalcogenide: molybdenum diselenide (MoSe2). Both systems were studied using Raman spectroscopy, a technique that has proven over the last five decades to be very suitable for accessing the spectral information of acoustic modes present in these structures. A key point of this technique is the experimental geometry, which dictates the selection rules for sensing the mechanical motion. In the case of superlattices, we proposed novel dispersion schemes. These dispersion geometries allow access to transverse acoustic modes that are forbidden under usual dispersion geometries. In this context, we proposed a hybrid, acoustic and optical waveguide structure, in which the vibrational modes that are generated have a wave vector in the superlattice plane and are guided through it. In multilayered semiconductors, Raman spectroscopy enabled an exhaustive characterization of the vibrational modes of MoSe2 samples as a function of the number of molecular layers (from a single monolayer to bulk), finding spectral features that were not yet reported in the literature. Finally, resonant Raman spectroscopy experiments were made with different electronic states of the material, allowing the study of the photon-exciton coupling. The temporal dynamics of phonons was studied by means of ultrafast optical spectroscopy. The method used was the "pump-probe", where the excitation of coherent acoustic phonons in the structures was investigated by means of the impulsive absorption of ultra-short laser pulses. In the case of the superlattices these experiments enabled to test the acoustic waveguide structure. On the other hand, when performing experiments tuning the energy of the excitation laser around the energy of the confined electronic states, it was possible to evaluate and study directly in the time domain the coupling between electronic and vibrational states, as well as the effects of resonant generation of coherent acoustic phonons. In the case of multilayered semiconductors, the pump-probe technique allowed a detailed study of the lifetime of one of the characteristic vibrational mode of this class of systems, the "breathing mode", which demonstrates the interlayer coupling. Finally, analyzing this mode, the adhesion effects of these samples to the substrate were studied. Very significant changes were observed, when comparing a substrate boundary condition to suspended samples, not only on the phonons, but also on their excitonic states. Although this thesis is mainly focused on the experimental results, we present several phenomenological models that conceptually explain most of the observed underlying physics we observed.
| Tipo de objeto: | Tesis (Tesis Doctoral en Física) |
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| Palabras Clave: | Raman Spectroscopy; Espectroscopía Raman; Superlattices; Superestructuras; [Vibrational dynamics; Dinámica vibracional; Untra-fast spectroscopy; Espectroscopía ultrarrápida] |
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| Materias: | Física > Fotónica |
| Divisiones: | Gcia. de área de Investigación y aplicaciones no nucleares > Gcia. de Física > Materia condensada > Laboratorio de fotónica y optoelectrónica |
| Código ID: | 812 |
| Depositado Por: | Tamara Cárcamo |
| Depositado En: | 01 Mar 2021 12:55 |
| Última Modificación: | 01 Mar 2021 12:55 |
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