By Malte Oppermann
This thesis offers an experimental research of the ultrafast molecular dynamics of CO_2^+ which are brought on via a powerful, near-infrared, femtosecond laser pulse. specifically, normal robust box phenomena corresponding to tunneling ionisation, nonsequential double ionisation and photo-induced dissociation are investigated and regulated by means of utilizing an experimental approach referred to as impulsive molecular alignment. the following, a primary laser pulse fixes the molecule in house, such that the molecular dynamics could be studied as a functionality of the molecular geometry with a moment laser pulse. The experiments are positioned in the context of the research and keep an eye on of ultrafast molecular dynamics, the place sub-femtosecond (10^-15 seconds) solution in ever higher molecular platforms represents the present frontier of study. The thesis provides the mandatory history in powerful box and molecular physics, femtosecond laser structure and experimental thoughts in a transparent and available language that doesn't require any earlier wisdom in those fields.
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Extra info for Resolving Strong Field Dynamics in Cation States of CO_2 via Optimised Molecular Alignment
This leads to excitation and deexcitation of the ion and is associated with the electron hole moving to another orbital during TI . This mechanism is thus sometimes referred to as inelastic tunneling. It is illustrated for the XA channel in inset (b) in Fig. 14. Here, TI from HOMO takes place initially. During tunneling, the hole moves to HOMO-1 leaving the ion in the first excited state A. In this way, the correlation channel does not possess the full exponential suppression of the direct channel (TI from HOMO-1, AA).
38) A long laser pulse (>10 fs at 800 nm) may be assumed to consist of many identical cycles. Thus the dipole interaction with the molecule will also be approximately periodic with the laser frequency. As in the context of HHG (see Sect. 5), a periodically driven process in time is related to a spectrum of harmonics of the driving field via Fourier transformation . In the energy domain, this corresponds to an infinite set of coherent states spaced by the photon energy ωL of the laser field.
This means that recollision may take place at higher ellipticities. In the case of atoms, this effect has thus far only been suggested to be significant in Mg . In the case of molecules, their orbital structure may increase the transverse velocity spread of the tunneled electron. This can then lead to a maximum recollision probability for non-zero ellipticity. This effect is discussed in detail in Chap. 6. Second, when the electron gets close to the parent ion upon its return, it may be attracted by its Coulomb potential.