190 p.The ability of materials to transfer electrons is a basic property controlling the functionality and performance of devices at the nanoscale. Of particular importance is the tranfor of electros at surfaces as a fundamental process in catalytic and photocatalytic applications. This work aims along these lines at a theoretical description of resonant charge injection at surfaces using a combination of density functional theory and Green's functions. A close comparison with available data from core-hole-clock experiments is maintained throughout the work and confirms the validity and predictive power of our first-principles approach. This is demonstrated on the basis of three prototypical systems where we study fundamental aspects of charge transfer, providing additional, often complementary information to the interpretation of the experiments. First, we present a detailed study of the effects of structural fluctuations on elastic charge transfer for isonicotinic acid adsorbed on rutile (110) in relation to photovoltaic applications. Second we explore spin-dependent charge injection from core-excited argon resonances on Co(0001) and Fe(110), with possible implications for spintronics. Third, we examine the directionality of charge transfer from sulfur related resonances at surfaces of layered 1T-TaS2 in the commensurate charge density wave phase.DIPC
CSIC
CICnanoGune
CFM
Marie Curie Action

Müller, Moritz

English

Doctoral Thesis Submitted to the University of the Basque Country for the Degree of Doctor in Physics.[EN]: The ability of materials to transfer electrons is a basic property controlling the functionality and performance of devices at the nanoscale. Of particular importance is the tranfor of electros at surfaces as a fundamental process in catalytic and photocatalytic applications. This work aims along these lines at a theoretical description of resonant charge injection at surfaces using a combination of density functional theory and Green's functions. A close comparison with available data from core-hole-clock experiments is maintained throughout the work and confirms the validity and predictive power of our first-principles approach. This is demonstrated on the basis of three prototypical systems where we study fundamental aspects of charge transfer, providing additional, often complementary information to the interpretation of the experiments. First, we present a detailed study of the effects of structural fluctuations on elastic charge transfer for isonicotinic acid adsorbed on rutile (110) in relation to photovoltaic applications. Second we explore spin-dependent charge injection from core-excited argon resonances on Co(0001) and Fe(110), with possible implications for spintronics. Third, we examine the directionality of charge transfer from sulfur related resonances at surfaces of layered 1T-TaS2 in the commensurate charge density wave phase.[ES]: Los procesos de transferencia de electrones son fundamentales tanto en la Naturaleza y como para gran cantidad de aplicaciones tecnológicas. Una comprensión detallada de su funcionamiento en la escala atómica es de gran importancia para el diseño de nuevos materiales y dispositivos. En particular, la transferencia de electrones tiene lugar en reacciones catalíticas y foto-catalíticas, así como en celdas electroquímicas y
distintos dispositivos generadores de energía solar como las células solares “sensibilizadas” por colorantes (en inglés “dye-sensitized solar cells”, DSSCs). En este tipo de situaciones, con frecuencia la transferencia electrónica tiene lugar en una superficie o a través de una interfase, mientras el electrón transferido normalmente procede de una unidad química donora, como un átomo o una molécula absorbidos sobre o
cercanos a dicha superficie. Las técnicas experimentales modernas son capaces de estudiar estos procesos en detalle, accediendo a sus escalas espaciales y temporales fundamentales (el nanometro y el femtosegundo). Sin embargo, en sistemas grandes y/o complejos diversos procesos pueden interferir, complicando la descripción. Por dicha razón es preferible estudiar sistemas sencillos que pueden ser estudiados tanto de forma teórica como experimental y comprendidos con modelos relativamente simples. 
La presente Tesis se ocupa de describir procesos elásticos de transferencia electrónica en superficies utilizando cálculos de primeros principios. En particular, desarrollamos un método que combina el uso funciones de Green con la información obtenida a partir de cálculos del funcional de la densidad (en inglés “density functional theory”, DFT) para realizar una descripción realista de los procesos de transferencia electrónica resonante en superficies. Los tiempos de transferencia de carga así calculados son comparados, con frecuencia de forma muy favorable, con los extraídos de experimentos que utilizan la técnica de espectroscopía “con cronometraje por hueco interno” (en inglés “core-hole-clock spectroscopy”).I gratefully acknowledge the EU-FP7 project THINFACE (grant No. 607232) for
financial support through Nanogune and training, the Spanish MINECO (grant No. MAT2016-78293-C6-4-R) for funding, the Centro de Física de Materiales (CFM) for
providing work space, and the Donostia International Physics Center (DIPC) for
financial support as well as computational time at the DIPC computing center and
Daniel Franco as well as Diego Lasa for expert computational support.Peer reviewe

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Theory of ultrafast electron transfer from localized quantum states at surfaces

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Theory of ultrafast electron transfer from localized quantum states at surfaces .

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Theory of ultrafast electron transfer from localized quantum states at surfaces .

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