Dorner-Kirchner, M. (2022). Applications of intense laser pulses to the control of attosecond processes in gas-phase atoms and dimers [Dissertation, Technische Universität Wien]. reposiTUm. https://doi.org/10.34726/hss.2022.68536
When a laser pulse interacts with a physical system, the laser electric field directly couples to the system’s electronic structure and allows to observe and, given sufficient field strength, steer processes therein. In this thesis intense ultrashort laser pulses are applied to the investigation and control of three specific processes in the electronic structure of gas-phase atoms and dimers on th...
When a laser pulse interacts with a physical system, the laser electric field directly couples to the system’s electronic structure and allows to observe and, given sufficient field strength, steer processes therein. In this thesis intense ultrashort laser pulses are applied to the investigation and control of three specific processes in the electronic structure of gas-phase atoms and dimers on their natural attosecond time scale. As properties of matter are ultimately determined by its electronic structure, these fundamental processes have implications for many important natural and technical mechanisms. The first process is the laser induced transfer and transient capture (LITE) of an electron from one atom across its system boundary to the other atom within an argon dimer. By reaction microscopy it is found that this electron transfer process triggers attosecond electron-electron interaction dynamics in the neighboring argon atom and that this is influenced by the carrier envelope phase (CEP) of the inducing laser pulse. Then, these findings are further investigated in the same sample system of argon dimers, where it is observed that also for the process of recapture of an electron into excited high lying Rydberg states, so-called frustrated field ionization (FFI), control can be exerted via CEP of ultrashort laser pulses. These findings disclose a strong-field route to controlling the dynamics in molecular compounds through the excitation of electronic dynamics on a distant molecule by driving inter-molecular electron-transfer processes. Distinct from these fundamental investigations on electronic processes, furthermore in this thesis a practical approach for driving the process of high-harmonic generation (HHG) is presented. It combines the high power scalability of an ytterbium based laser system with efficient spectral broadening and simultaneous red-shift by stimulated Raman scattering (SRS) in a long, stretched hollow core fiber (HCF) to significantly extend the achievable cutoff energy beyond previous limitations.