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• W91119982 abstract "Orbit-based theoretical approaches to modelling strong eld phenomena allow physicalintuition to be extracted from complex multi-dimensional quantum processes. Highorderharmonic generation (HHG) has been interpreted relatively successfully for almosttwo decades as a three step process in which an ionized electron is accelerated by theeld and recombines with its parent ion, resulting in high-order multiples of the laserfrequency. This process is often modelled within the strong-eld approximation (SFA),where the eect of the Coulomb potential on the electron is neglected while the electronis accelerated by the eld, and the single-active electron (SAE) approximation. The SFAprovides an appealing interpretation of HHG in terms of interfering electron trajectories.Although successful in reproducing experimental observables in atomic systems, inrecent years the importance of multi-electron eects, molecular orbital symmetry andthe Coulomb potential in atoms and diatomic molecules have been seen experimentallyand theoretically. These eects, neglected by the original SFA formulation, mean thateither modications to the original SFA, or new trajectory based theories, are essentialfor a more complete physical understanding of the HHG phenomenon.This thesis investigates these eects in HHG from homonuclear and heteronuclear diatomicmolecules in strong elds. We model and assess the importance of multiplemolecular orbital contributions, molecular orbital geometry and two-centre interferenceon the HHG spectrum. These problems are approached within a semi-analytical, SFA,framework and with a static core. It is found that these eects can be seen in the HHGspectrum. By predicting novel features in the spectrum arising from such eects we obtainnot only a better understanding and interpretation of current experimental results,but also new insight and applicability to molecular imaging.In addition to these modications, a new theoretical approach, the coupled coherentstate (CCS) method is used to model Hydrogen in an intense eld, although it can beextended to multi-electron systems and diatomic molecules. In the CCS method, theCoulomb potential is fully included at all stages in the HHG process, and most notably,during the electron propagation, where it is neglected by the SFA. The CCS method hasfavourable scaling with dimensionality, compared to other numerical approaches, as wellas being fully quantum. It is trajectory based, facilitating comparison with the threestep model and the strong eld approximation. Therefore we benet from the physicalintuition of semi-classical approaches but within a fully quantum framework and withoutthe approximations of semi-analytical methods." @default.
• W91119982 created "2016-06-24" @default.
• W91119982 creator A5072279835 @default.
• W91119982 date "2012-06-28" @default.
• W91119982 modified "2023-09-23" @default.
• W91119982 title "Orbit based treatments of quantum interference in atomic and molecular high-order harmonic generation." @default.
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