Guerra Hernández, Luis A. (2019) Antenas ópticas en la nano y microescala. / Optical antennas at the nano and microscale. Tesis Doctoral en Física, Universidad Nacional de Cuyo, Instituto Balseiro.
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Resumen en español
Los resultados del presente trabajo de tesis doctoral sientan bases para la comprensión de fenómenos plasmónicos, asociados a la espectroscopia Raman amplificada por superficie (SERS) para el desarrollo de nuevos métodos de detección molecular. La sistemática de estudio consisti_o en evaluar la respuesta plasmonica y SERS de cinco tipos de sistemas metalicos nanoestructurados: i) superficies rugosas de Au, ii) cavidades esfericas de Au, iii) sistemas de film de Au (o Ag) sobre nanoesferas (AuFON o AgFON), iv) nanopartículas triangulares de Au (AuNPS) y v) un substrato comercial Klarite. En los sistemas mencionados se abordaron estudios del acoplamiento de la luz con plasmones, a través de mecanismos resonantes poco frecuentes en la literatura. Así mismo, se presentan resultados de modelados numéricos para comprender y reforzar la interpretación de los resultados experimentales. Se estableció también una correlación entre estos plasmones y la respuesta SERS de moléculas sonda absorbidas covalentemente en la superficie del sistema. En las superficies rugosas de Au, se presentan resultados de la respuesta SERS en función del grado de rugosidad para nanoestructuras con relajación natural de la rugosidad y congelada artificialmente. Esto se hizo mediante un control no del grado de rugosidad, desde valores muy pequeños a valores grandes. Este estudio de rugosidad finamente controlado se realizó como insumo para luego poder estudiar el efecto de la rugosidad en substratos plasmonicos ordenados, fabricados por métodos de litografía con esferas de látex. La inhibición de la relajación de la superficie se realizó con métodos químicos produciendo mayor señal SERS en comparación con las superficies relajadas. En los sistemas de cavidades con rugosidad superficial adaptada o incrementada se estudió el efecto de esta rugosidad sobre la eficiencia SERS. Se demostró que este sistema híbrido cavidad + rugosidad funciona como una antena sinérgica multiescala donde la cavidad esférica cumple la función de incrementar el modo plasmonico cerca de la superficie rugosa, permitiendo un mejor acoplamiento de la radiación del campo lejano, a campos cercanos mejorados localmente. Otro resultado en este sistema híbrido, está relacionado con el acoplamiento resonante selectivo de modos plasmonicos de cavidad tipo P y D con diferente distribución espacial. El modo D espacialmente más connado a la superficie que el modo P, conduce a una canalización más eficiente de la energía desde el campo lejano a campos cercanos en la superficie. Otro de los resultados de la tesis está direccionado a estudios resonantes en sistemas AuFON y AgFON. En estos evaluamos y correlacionamos la respuesta SERS de tres modos plasmonicos (etiquetamos como M3, M2 y M1) con medidas de la reactividad óptica y modelado numérico de la mejora del campo en la superficie. Fundamentamos que los mecanismos de amplificación debido a los plasmones y la resonancia metal-ligando (M-L), muestran una relación con la amplificación SERS. Del modelado numérico en estos mismos sistemas mostramos que los modos plasmonicos M2 y M1 presentan similar distribución espacial de campo eléctrico pero distinta intensificación. En el caso de los AuFON, el modo M1 de mayor intensificación de campo eléctrico que M2 contribuye mas al rendimiento SERS cuando se cruza con la resonancia M-L. En los sistemas de AgFON fue posible incrementar los límites de detección molecular diez veces en comparación con los sistemas de AuFON. Además, se evidencio una nueva resonancia plasmonica (poco relevante en sistemas de AuFON) que contribuye significativamente a la respuesta SERS, generando un nuevo maximo en dicha respuesta. Por otro lado, los sistemas de AuNPS muestran señales SERS muy bajas en comparación con los otros sistemas estudiados. Esta baja amplificación esta relacionada con que, la superficie cubierta por estas AuNPS es mucho menor que la superficie total del substrato implicada en el proceso SERS. Finalmente, un último resultado hace referencia al estudio comparativo de los cinco sistemas mencionados. De esta comparación el sistema AuFON, resulto de mejores características en cuanto a valores de intensidad y homogeneidad de la señal SERS respecto a los demás sistemas estudiados. En general, determinamos que la contribución a la señal SERS proviene de los mecanismos plasmonicos, la resonancia M-L y la rugosidad superficial del sistema. Con los estudios de la tesis surgen posibilidades de desarrollo de sistemas de detección ultrasensible de moléculas en forma cuantitativa.
Resumen en inglés
The results presented on this Ph. D. thesis lay the foundation for the comprehension of plasmonic phenomena, associated with Surface Enhancement Raman Spectroscopy (SERS) for the development of new molecular detection methods. The study methodology consisted of evaluating the plasmonic response and SERS of five variety of nanostructured metallic systems: i) Au rough surface, ii) Au spherical cavities, iii) Au (orAg) film over nanospheres (AuFON or AgFON) systems, iv) Au triangular nanoparticles (AuNPS) and v) a commercial Klarite substrate. For the mentioned systems, studies of light coupling with plasmons were performed through resonant mechanisms, which are not frequently found in the literature. Likewise, numerical model results are presented for better comprehension and further interpretation of the experimental results. Also, it was stablished a correlation between these plasmons and the SERS response of probe molecules covalently attached to the surface of the system. For the Au rough surfaces, the SERS response is studied as a function of the degree of roughness. This is done for the nanostructures with natural relaxation of the roughness and for surfaces in which the relaxation is artificially freezed. This was done by fine control of the degree of roughness, from very small values to large values. This study of finely controlled roughness was performed as an input to then be able to study the effect of roughness in ordered plasmonic substrates, manufactured by lithography methods with latex spheres. The surface relaxation of the relaxation is stopped by means of chemical methods, producing a higher SERS signal in comparison to the relaxed surfaces. In the system of cavities with adapted superfficial roughness, it was studied the effect of this roughness on the SERS efficiency. It was demonstrated that the hybrid system cavity + roughness works as a synergic multiscale antenna, where the spherical cavity has the function of efficiently collecting the far field radiation, channelling the laser light, and enhancing the plasmonic mode close to the rough surface, allowing for a better coupling of the far field radiation, to the near field enhanced locally by roughness. An additional result of this hybrid system is related to the selective resonant coupling of plasmonic modes P and D with different spatial distribution. The mode D, with larger projection to the surface than mode P, conducts to a more efficient energy canalization rom the far field to near fields where the molecules reside. Another remarkable result of the present thesis is directed to resonant studies in AuFON and AgFON systems. For these substrates, we evaluated and correlated the SERS response of the three observed plasmonic modes (labeled as M3, M2 and M1) with optical reectivity measurements and numerical modelling for the improvement of the surface field. We demonstrate that the amplification mechanisms due both to the plasmons and the metal-ligand (M-L) resonance, show an association with the SERS intensity. From the numerical modelling of this system we show that the plasmonics modes M2 and M1 present a similar spatial distribution of the electric field but different intensification. For the case of the AuFON, the M1 mode, of higher intensification of electric field than M2, contributes more to the SERS efficiency and specifically when the resonance M-L is crossed. In AgFON systems, it was possible to enhance the detection limits up to ten times in comparison to the AuFON systems. Furthermore, a new plasmonic resonance at shorter wavelengths was evidenced (with no relevance in AuFON systems) that significantly contributes to the SERS response. On the other hand, AuNPS systems show very low SERS signals compared to the other studied systems. This low ampliffication is related to the fact that the covered surface is much smaller than the total surface of the substrate implied in the SERS process. Finally, the last result refers to the comparative study of the five mentioned systems. From this comparison, we conclude that the AuFON system shows the best characteristics referred to the intensity and homogeneity of the SERS signal, with respect to the other analyzed systems. In general, we determined that the contribution to the SERS signal comes from the combination of plasmonic mechanisms, the M-L resonance and the superfficial roughness of the system. From the studies performed in this thesis emerge valuable information of the development of improved ultrasensitive detection systems, for the quantitative detection of molecules.
| Tipo de objeto: | Tesis (Tesis Doctoral en Física) |
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| Palabras Clave: | Raman spectroscopy; Espectroscopía raman; [Plasmonics; Plasmónica; Optical Antennas; Antenas ópticas; Sers] |
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| Materias: | Física > Óptica |
| Divisiones: | Gcia. de área de Investigación y aplicaciones no nucleares > Gcia. de Física > Materia condensada > Laboratorio de fotónica y optoelectrónica |
| Código ID: | 867 |
| Depositado Por: | Tamara Cárcamo |
| Depositado En: | 26 Feb 2021 14:25 |
| Última Modificación: | 26 Feb 2021 14:27 |
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