Publication: Dinámica y Espectroscopía láser de agregados de van der Waals de moléculas de interés biológico y amoniaco en condiciones de microsolvatación
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2021-06-18
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Universidad Complutense de Madrid
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Abstract
Los compuestos no covalentes o clusters son agregados moleculares o atómicos, con estructuras únicas, a medio camino entre moléculas aisladas y materiales masivos [1]. Son los responsables de la misma existencia de la fase líquida, y determinan la estructura de biomoléculas como el ADN, el ARN y las proteínas, dotándolas de flexibilidad para permitir la transcripción de la información genética [2][3]. La estabilidad de las bases nucleicas bajo la acción de radiación ultravioleta es extremadamente importante, así como los mecanismos de distribución de energía disparados por la radiación ultravioleta. Domcke et al. han propuesto un mecanismo de relajación no radiativo entre los niveles excitados mediante radiación ultravioleta y el nivel fundamental, que tendría lugar en la escala de los picosegundos y, por tanto, suficientemente rápido para evitar procesos fotoquímicos en estados excitados, lo que constituiría la base de la foto estabilidad de estos sistemas [4]. Desde el trabajo de Domcke y colaboradores, este mecanismo se ha caracterizado para grannúmero de pequeños cromóforos y bases de ADN, fundamentalmente en fase gaseosa, o en disolución. En este proyecto de Tesis Doctoral se pretende dar un paso más en el estudio de la fotoestabilidad de estos sistemas, estudiando la fotoquímica y fotofísica de los clusters formados por moléculas similares a los cromóforos de bases de ADN y moléculas de amoniaco (NH3)...
Clusters are molecular or atomic aggregates with unique structures, halfway between isolated molecules and bulk materials [1]. They are responsible for the very existence of the liquid phase and determine the structure of large biomolecules such as DNA, RNA and proteins, providing them with the necessary flexibility to allow the transcription of genetic information[2][3]. The stability of the nuclear bases under the action of ultraviolet radiation is extremely important, as they are the mechanisms of energy redistribution triggered by ultraviolet radiation. Domcke et al. have proposed a non-radiative relaxation mechanism between those states excited by ultraviolet radiation and the fundamental level to happen on the picosecond time scale, which is fast enough to avoid any kind of photochemical dynamics in the excited states, the proposed relaxation mechanism should constitute the basis of the photostabilityof most biological systems [4]. Since Domcke's work, the relaxation mechanism has been characterized for a large number of small chromophores and DNA bases, primarily in the gas phase, or in solution. This Thesis constitutes, therefore, another step in the study of the photostability of systems of biological interest, through the study of the photochemistry and photophysics of clusters formed by ammonia molecules (NH3) and model systems specifically chosen to represent, in small scale, larger chromophores and DNA bases...
Clusters are molecular or atomic aggregates with unique structures, halfway between isolated molecules and bulk materials [1]. They are responsible for the very existence of the liquid phase and determine the structure of large biomolecules such as DNA, RNA and proteins, providing them with the necessary flexibility to allow the transcription of genetic information[2][3]. The stability of the nuclear bases under the action of ultraviolet radiation is extremely important, as they are the mechanisms of energy redistribution triggered by ultraviolet radiation. Domcke et al. have proposed a non-radiative relaxation mechanism between those states excited by ultraviolet radiation and the fundamental level to happen on the picosecond time scale, which is fast enough to avoid any kind of photochemical dynamics in the excited states, the proposed relaxation mechanism should constitute the basis of the photostabilityof most biological systems [4]. Since Domcke's work, the relaxation mechanism has been characterized for a large number of small chromophores and DNA bases, primarily in the gas phase, or in solution. This Thesis constitutes, therefore, another step in the study of the photostability of systems of biological interest, through the study of the photochemistry and photophysics of clusters formed by ammonia molecules (NH3) and model systems specifically chosen to represent, in small scale, larger chromophores and DNA bases...
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Tesis inédita de la Universidad Complutense de Madrid, Facultad de Ciencias Químicas, Departamento de Química Física, leída el 30/11/2020