Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userProbing wave functions of molecular nuclei with high harmonic generation
138
0
0.0
(
0
)
Added by
Gerrit C. Groenenboom
Publication date
2011
fields
Physics
and research's language is
English
Ask ChatGPT about the research
No Arabic abstract
This paper has been withdrawn by the authors because the wave packet propagation used in the ion-dynamics calculation did not allow for electron-nuclei correlation. Hence, the conclusion that the ion-dynamics model is not in agreement with experiment is not substantiated.
rate research
Read More
High-order harmonic generation (HHG) in aligned linear molecules can offer valuable information about strong-field interactions in lower-lying molecular orbitals, but extracting this information is difficult for three-dimensional molecular geometries. Our measurements of the asymmetric top SO2 show large axis dependencies, which change with harmonic order. The analysis shows that these spectral features must be due to field ionization and recombination from multiple orbitals during HHG. We expect that HHG can probe orbital dependencies using this approach for a broad class of asymmetric-top molecules.
We investigate the orientation dependence of molecular high-order harmonic generation (HHG) both numerically and analytically. We show that the molecular recollision electronic wave packets (REWPs) in the HHG are closely related to the ionization potential as well as the particular orbital from which it ionized. As a result, the spectral amplitude of the molecular REWP can be significantly different from its reference atom (i.e., with the same ionization potential as the molecule under study) in some energy regions due to the interference between the atomic cores of the molecules. This finding is important for molecular orbital tomography using HHG[Nature textbf{432}, 867(2004)].
We produce oriented rotational wave packets in CO and measure their characteristics via high harmonic generation. The wavepacket is created using an intense, femtosecond laser pulse and its second harmonic. A delayed 800 nm pulse probes the wave packet, generating even-order high harmonics that arise from the broken symmetry induced by the orientation dynamics. The even-order harmonic radiation that we measure appears on a zero background, enabling us to accurately follow the temporal evolution of the wave packet. Our measurements reveal that, for the conditions optimum for harmonic generation, the orientation is produced by preferential ionization which depletes the sample of molecules of one orientation.
Asymmetric molecules look different when viewed from one side or the other. This difference influences the electronic structure of the valence electrons, thereby giving stereo sensitivity to chemistry and biology. We show that attosecond and re-collision science provides a detailed and sensitive probe of electronic asymmetry. On each 1/2 cycle of an intense light pulse, laser-induced tunnelling extracts an electron wave packet from the molecule. When the electron wave packet recombines, alternately from one side of the molecule or the other, its amplitude and phase asymmetry determines the even and odd harmonics radiation that it generates. This harmonic spectrum encodes three manifestations of asymmetry; an amplitude and phase asymmetry in electron tunneling; an asymmetry in the phase that the electron wave packet accumulates relative to the ion between the moment of ionization and recombination; and an asymmetry in the amplitude and phase of the transition moment. We report the first measurement of high harmonics from oriented gas samples. We determine the phase asymmetry of the attosecond XUV pulses emitted when an electron recollides from opposite sides of the CO molecule, and the phase asymmetry of the recollision electron just before recombination. We discuss how the various contributions to asymmetry can be isolated in future experiments.
We study high-order harmonic generation (HHG) resulting from the illumination of plasmonic nanostructures with a short laser pulse. We show that both the inhomogeneities of the local electric field and the confinement of the electron motion play an important role in the HHG process and lead to a significant increase of the harmonic cutoff. In order to understand and characterize this feature, we combine the numerical solution of the time dependent Schroedinger equation (TDSE) with the electric fields obtained from 3D finite element simulations. We employ time-frequency analysis to extract more detailed information from the TDSE results and to explain the extended harmonic spectra. Our findings have the potential to boost up the utilization of HHG as coherent extreme ultraviolet (XUV) sources.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
