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Title: Charge transfer of Rydberg hydrogen molecules and atoms at doped silicon surfaces
Author: Ganeshalingam, Sashikesh
ISNI:       0000 0004 2722 3116
Awarding Body: University of Oxford
Current Institution: University of Oxford
Date of Award: 2012
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The work of this thesis focuses on the interaction of high Rydberg states of hydrogen molecules and atoms with various doped Si semiconductor surfaces with the results compared with those obtained with an atomically flat gold surface. The major part of the thesis was carried out using para-H₂ molecular Rydberg states with principal quantum number n = 17 - 21 and core rotational quantum number N⁺ = 2. Subsequently, this study was continued using H atomic Rydberg states with principal quantum number n = 29 - 34. The high Rydberg states have been produced using two-step laser excitation. For close Rydberg surface separation (< 6 n² a.u.), the Rydberg states may be ionized due to an attractive surface potential experienced by the Rydberg electron, and the remaining ion core may be detected by applying an external electric field. An efficient ion detectability method is introduced to compare the many surface ionization profiles quantitatively. The p-type doped Si surfaces enhance the detected ion-signal more than the n-type doped Si surfaces due to the presence of widely distributed positive dopant charge fields in the p-type doped Si surfaces. As the dopant density increases, the area sampled by the resultant ions becomes effectively more neutral, and the decay rate of the potential from the surface dopant charge with distance from the surface becomes more rapid. Therefore, the minimum ionization distance is also reduced with increasing dopant density. It is found that the detected ion-signal decreases with increasing dopant density of both p- and n- type doped Si surfaces. The higher-n Rydberg states have shown higher ion detectability than that of lower-n Rydberg states and this variation also becomes smaller when increasing the dopant density. Experiments involving H2 Rydberg molecules incident on various doped Si surfaces in the presence of a Stark field at the point of excitation are also presented here. The surface ionization profiles produced via both electron and ion detection schemes are measured by changing the Stark polarization. Positive surface dopant charges oppose production of backscattered electrons and negative surface dopant charges enhance the electron-signal. For the electron detection scheme, lightly doped n-type Si surfaces show higher detectability but in the case of p-type Si surfaces the more heavily doped Si surfaces give a higher detected signal. This different behaviour of the detected ion or electron signal implies a different production mechanism. Theoretical trajectory simulations were also carried out based on a new 2D surface potential model. The results qualitatively agree with the experimental results and explain the changes of the surface ionization profiles between the various dopant types and dopant densities of the Si surfaces.
Supervisor: Timothy P., Softley Sponsor: Clarendon Fund ; Magdalen College Perkin Research Studentship
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available
Keywords: Physical & theoretical chemistry ; Spectroscopy and molecular structure ; Surface chemistry ; Molecular Physics ; Rydberg ; Jellium ; image-charge