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Register a new userSub-femtosecond tracing of molecular dynamics during strong-field interaction
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Added by
Markus Kitzler-Zeiler
Publication date
2019
fields
Physics
and research's language is
English
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We introduce and experimentally demonstrate a method, where the two intrinsic time scales of a molecule, the slow nuclear motion and the fast electronic motion, are simultaneously measured in a photo-electron photo-ion coincidence experiment. In our experiment, elliptically polarized, 750~nm, 4.5~fs laser pulses were focused to an intensity of $9times10^{14}mathrm{W/cm}^2$ onto H$_2$. Using coincidence imaging, we directly observe the nuclear wavepacket evolving on the ssg{} state of H$_2^+$ during its first roundtrip with attosecond temporal and picometer spatial resolution. The demonstrated method should enable insight into the first few femtoseconds of the vibronic dynamics of ionization-induced unimolecular reactions of larger molecules.
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A nonlinear interferometry scheme is described theoretically to induce and resolve electron wave- function beating on time scales shorter than the optical cycle of the time-delayed pump and probe pulses. By employing two moderately intense few-cycle laser fields with a stable carrier-envelope phase, a large range of the entire electronic level structure of a quantum system can be retrieved. In contrast to single-photon excitation schemes, the retrieved electronic states include levels that are both dipole- and non-dipole-accessible from the ground electronic state. The results show that strong-field interferometry can reveal both high-resolution and broad-band spectral information at the same time with important consequences for quantum-beat spectroscopy on attosecond or even shorter time scales.
We compare femtosecond pump-probe experiments in Ni and micromagnetic modelling based on the Landau-Lifshitz-Bloch equation coupled to a two-temperature model, revealing a predominant thermal ultrafast demagnetization mechanism. We show that both spin (femtosecond demagnetization) and electron-phonon (magnetization recovery) rates in Ni increase as a function of the laser pump fluence. The slowing down for high fluences arises from the increased longitudinal relaxation time.
Coherent light pulses of few to hundreds of femtoseconds (fs) duration have prolifically served the field of ultrafast phenomena. While fs pulses address mainly dynamics of nuclear motion in molecules or lattices in the gas, liquid or condensed matter phase, the advent of attosecond pulses has in recent years provided direct experimental access to ultrafast electron dynamics. However, there are processes involving nuclear motion in molecules and in particular coupled electronic and nuclear motion that possess few fs or even sub-fs dynamics. In the present work we have succeeded in addressing simultaneously vibrational and electronic dynamics in molecular Hydrogen. Utilizing a broadband extreme-ultraviolet (XUV) continuum the entire, Frank-Condon allowed spectrum of H2 is coherently excited. Vibrational, electronic and ionization 1fs scale dynamics are subsequently tracked by means of XUV-pump-XUV-probe measurements. These reflect the intrinsic molecular behavior as the XUV probe pulse hardly distorts the molecular potential.
In strong field ionization, the pump pulse not only photoionizes the molecule, but also drives efficient population exchanges between its ionic ground and excited states.In this study, we investigated the population dynamics accompanying strong field molecular photoionization, using angular distribution of dissociative fragments after ionization.Our results reveal that the first and higher order processes of the post-ionization population redistribution mechanism (PPRM) in the ion core can be disentangled and classified by {its} angle-resolved kinetic energy release (KER) spectra.We demonstrate that the imprints of PPRM in the KER spectra can be used to determine the branching ratio of the population exchange pathways of different orders, by exploiting the pump intensity dependent variation of the spectra.
We report on the unambiguous observation of the sub-cycle ionization bursts in sequential strong-field double ionization of H$_2$ and their disentanglement in molecular frame photoelectron angular distributions. This observation was made possible by the use of few-cycle laser pulses with a known carrier-envelope phase in combination with multi-particle coincidence momentum imaging. The approach demonstrated here will allow sampling of the intramolecular electron dynamics and the investigation of charge-state specific Coulomb-distortions on emitted electrons in polyatomic molecules.
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