Semiclassical theories have proven to be a versatile tool in ultrafast strong field science. In this thesis, the power of classical trajectory Monte Carlo (CTMC) and quantum trajectory Monte Carlo (QTMC) simulations is celebrated by applying them in various strong field ionization settings. One question to be addressed concerns the way nonadiabaticity in the ionization process manifests itself. It will be shown how the assumption of a vanishing initial longitudinal momentum is the reason for the strong broadening of the initial time spread claimed in a popular nonadiabatic theory. Moreover, it will become clear how the broader time spread of this theory and the non-zero initial longitudinal momenta of another widely applied nonadiabatic theory approximately compensate each other during propagation for typically studied nonadiabatic parameters. However, parameters in the nonadiabatic but still experimentally relevant regime will be found where this approximation breaks down and the two different theories lead to distinguishably different momentum distributions at the detector after all, thus allowing to test which theory describes the situation at the tunnel exit more accurately.
After having tunneled through the barrier formed by the laser and Coulomb poten-tial, the electron does not necessarily leave the atom for good but can be captured in a Rydberg state. A study of the intensity-dependence of the Rydberg yield will reveal, among other things, nonadiabatic effects that can be used as an independent test of nonadiabaticity in strong field ionization. Moreover, it will be shown that the duration of the laser pulse can be used to control both the yield and principal quantum number distribution of Rydberg atoms. The highly enhanced and spatially inhomogeneous fields close to a nanostructure are another setting in which atoms can be ionized. Here, the emergence of a prominent higher energy structure (HES) in the spectrum of photoelectrons will be reported.
The narrow time-window in which the corresponding electrons are released suggests a promising method for creating a localized source of electron pulses of attosecond duration using tabletop laser technology. Having such potential applications in mind, analytical expressions are derived to describe the electrons’ motion in the inhomogeneous field, thus being able to control the spectral position and width of the HES.
Moreover, a unifying theory will be developed in which the recently reported experimental finding of a low-energy peak (LEP) can be understood to arise due to the same mechanism as the theoretically predicted HES, despite those two effects having been found in different energy regimes so far. This unifying theory will show how the well-established experimental technique in which the LEP was reported, i.e. ionization directly from the nanotip rather than from atoms in its vicinity, should allow the realization of a prominent and narrow peak at higher energies as it was theoretically described in the framework of the HES.
Despite being much weaker, the spatial inhomogeneity of the Coulomb potential can influence the photoelectron spectrum as well. It will be shown how the asymmetric Coulomb potential of a tilted diatomic molecule introduces an asymmetry in the photoelectron momentum distribution at the detector. The degree of asymmetry depends on whether the electron is born at the up- or downfield atom. This information is then used to quantify the ratio of ionization from the up- and downfield site from experimental photoelectron momentum distributions.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa:de:qucosa:88377 |
| Date | 30 November 2023 |
| Creators | Ortmann, Lisa |
| Contributors | Lein, Manfred, Rost, Jan-Michael, Strunz, Walter, Technische Universität Dresden |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | doc-type:doctoralThesis, info:eu-repo/semantics/doctoralThesis, doc-type:Text |
| Rights | info:eu-repo/semantics/openAccess |
| Relation | urn:nbn:de:bsz:14-qucosa2-367823, qucosa:36782 |
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