Rozas, Guillermo (2011) Estudio Raman de ultra-alta resolución de la dinámica de fonones acústicos confinados en cavidades. / Ultra-high resolution Raman investigation of the dynamics of cavity-confined acoustic phonons. Tesis Doctoral en Física, Universidad Nacional de Cuyo, Instituto Balseiro.
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Resumen en español
Los fonones en el rango de frecuencias de terahertz (THz), con longitudes de onda de pocos nanómetros y energías del orden de algunos meV, son de gran interés tanto desde el punto de vista básico como aplicado. Las propiedades de los fonones a estas frecuencias tienen un rol importante en el transporte eléctrico y la propagación del calor, y su interacción con los electrones y los fotones los hace candidatos para aplicaciones en optoelectrónica y nanoscopía. Sin embargo, existe poca información sobre cómo las limitaciones intrínsecas asociadas a los fonones de alta frecuencia, como la anarmonicidad y los defectos en interfaces, afectan la eficiencia de los dispositivos acústicos de THz. En este trabajo, presentamos un estudio por dispersión Raman de nanocavidades acústicas de THz basadas en multicapas semiconductoras. Los dispositivos acústicos analizados están embebidos dentro de microcavidades ópticas planas, a fin de aprovechar los efectos de amplificación y cambio de reglas de selección asociados a ellas. Utilizamos para estudiar las cavidades acústicas una nueva técnica de espectroscopía Raman de ultra-alta resolución, desarrollada especificamente durante esta tesis, alcanzando resoluciones de hasta 0,008 cm"-1 sobre rangos espectrales de más de 5 cm"-1. En primer lugar, investigamos tanto teórica como experimentalmente cómo las cavidades ópticas afectan las propiedades ópticas, electrónicas y de dispersión Raman del sistema. En el caso de los efectos puramente fotónicos, utilizamos un modelo macroscópico completo de la sección eficaz Raman, que considera el cálculo exacto de los modos vibracionales y electromagnéticos de la estructura. El mismo nos permite describir en detalle la intensidad de la dispersión y las reglas de selección Raman a energías y geometrías arbitrarias, incluyendo la fuerte amplificación de la señal en el modo óptico de cavidad y los efectos presentes en el borde del gap óptico. En el caso de los efectos electrónicos, estudiamos la interacción fuerte entre el modo óptico confinado y los estados excitónicos, analizando la formación de polaritones de cavidad y los cambios que estos producen sobre el proceso Raman para fonones acústicos. La utilización de fonones acústicos nos permite trabajar experimentalmente en doble resonancia con un mismo estado polaritónico y sobre todas las ramas polaritónicas, incluyendo la rama inferior, que es la relevante para la dinámica de polaritones en estados condensados. Los perfiles de amplificación Raman correspondientes son reproducidos correctamente utilizando un modelo de factorización de la dispersión Raman mediada por polaritones, que considera fenomenológicamente las vidas medias de los estados involucrados. En segundo lugar, la novedosa técnica de espectroscopía Raman de ultra-alta resolución desarrollada nos permite estudiar las cavidades acústicas de THz con un detalle sin precedentes. Midiendo el ancho de línea del modo acústico confinado de cavidad, demostramos por primera vez en forma experimental que el factor de calidad de estas nanoestructuras fonónicas puede ser controlado sistemáticamente por diseño. Experimentos en función de la temperatura muestran que el efecto de la anarmonicidad es marginal, aún a temperatura ambiente y frecuencias de THz. Basados en simulaciones de la dispersión Raman, mostramos que la eficiencia de estas cavidades acústicas de THz está limitada por el ensanchamiento inhomogéneo originado en fluctuaciones sub-monocapa en las interfaces. Sin embargo, los resultados presentados establecen claramente el potencial de las nanocavidades acústicas semiconductoras como resonadores para fonones de alta energía, con factores de calidad medidos de Q ~ 260 a 1 THz y de ~ 1200 a 237 GHz.
Resumen en inglés
Acoustic phonons in the terahertz (THz) frequency range, with wavelengths of a few nanometers and energies of the order of a few meV, have great importance both in basic research and applications. The properties of phonons at these frequencies have an important role in electric transport and heat propagation, and their interaction with electrons and photons make them candidates for optoelectronic and nanoscopy applications. However, there is little information on how the intrinsic limitations associated with high frequency phonons, like anharmonicity and interface defects, affect the effciency of THz acoustic devices. We present in this work a Raman scattering study of THz acoustic nanocavities based on semiconductor multilayers. The studied acoustic devices are embedded inside planar optical microcavities, to take advantage of the amplification effects and the change in selection rules associated to them. To study the acoustic cavities we use a new ultra-high resolution Raman scattering technique specically developed during this thesis, reaching resolutions down to 0.008 cm"-1 over spectral ranges of more than 5 cm"-1. First, we investigate both theoretically and experimentally how the optical cavity affects the optical, electronic, and Raman scattering properties of the system. In the case of the purely photonic effects, we use a complete macroscopic model of the Raman cross section, which considers the exact calculation of the structure's vibrational and electromagnetic modes. This model allows us to describe in detail the scattering intensity and the Raman selection rules at arbitrary energies and geometries, including the strong signal amplification in the optical cavity mode and the effects present at the edge of the optical gap. In the case of the electronic effects, we study the strong interaction between the confined optical mode and the excitonic states, analysing the formation of cavity polaritons and the changes they produce on the Raman process for acoustic phonons. The use of acoustic phonons allows us to work experimentally in double resonance with a single polaritonic state and over all the powhich is relevant for the dynamics of polaritons in condensed states. The corresponding Raman amplification profiles are correctly reproduced using a factorization model of the polariton-mediated Raman scattering, which considers the lifetimes of the involved states in a phenomenological way. On the other hand, the newly developed ultra-high resolution Raman scattering technique allows us to study the THz acoustic cavities with unprecedented detail. By measuring the line-width of the cavity-confined acoustic mode we experimentally demonstrate for the first time that the quality factor for these phononic nanostructures can be systematically controlled by design. Temperature dependent experiments show that the effect of anharmonicity is marginal, even at room temperature and THz frequencies. Based on Raman scattering simulations, we show that the quality factor is limited by inhomogeneous broadening originated on sub-monolayer interface fluctuations. However, the presented results clearly establish the potential of semiconductor acoustic nanocavities as resonators for high energy phonons, with measured quality factors of Q ~ 260 at 1 THz and ~ 1200 at 237 GHz.
| Tipo de objeto: | Tesis (Tesis Doctoral en Física) |
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| Materias: | Física > Nanotecnología Física > Óptica |
| Divisiones: | Investigación y aplicaciones no nucleares > Física > Laboratorio de propiedades ópticas de los materiales |
| Código ID: | 370 |
| Depositado Por: | Marisa G. Velazco Aldao |
| Depositado En: | 05 Nov 2012 09:36 |
| Última Modificación: | 13 Nov 2012 13:42 |
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