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Register a new userPerturbation-Assisted Laser-Induced Atomic Fragment Fluorescence Spectroscopy: A Facile Route to Spin-Forbidden States
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This paper has been withdrawn by the authors, because the authors have made abundant revisions and resubmitted the modified new version entitled Laser-induced atomic fragment fluorescence spectroscopy: A facile technique for molecular spectroscopy of spin-forbidden states to arXiv:0812.4554. Thanks for your attention.
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A laser-induced acoustic desorption source, developed for use at central facilities, such as free-electron lasers, is presented. It features prolonged measurement times and a fixed interaction point. A novel sample deposition method using aerosol spraying provides a uniform sample coverage and hence stable signal intensity. Utilizing strong-field ionization as a universal detection scheme, the produced molecular plume is characterized in terms of number density, spatial extend, fragmentation, temporal distribution, translational velocity, and translational temperature. The effect of desorption laser intensity on these plume properties is evaluated. While translational velocity is invariant for different desorption laser intensities, pointing to a non-thermal desorption mechanism, the translational temperature increases significantly and higher fragmentation is observed with increased desorption laser fluence.
We demonstrate the experimental realization of impulsive alignment of carbonyl sulfide (OCS) molecules at the Low Density Matter Beamline (LDM) at the free-electron laser FERMI. OCS molecules in a molecular beam were impulsively aligned using 200 fs pulses from a near-infrared laser. The alignment was probed through time-delayed ionization above the sulphur 2p edge, resulting in multiple ionization via Auger decay and subsequent Coulomb explosion of the molecules. The ionic fragments were collected using a time-of-flight mass spectrometer and the analysis of ion-ion covariance maps confirmed the correlation between fragments after Coulomb explosion. The analysis of the CO+ and S+ channels allowed us to extract the rotational dynamics, which is in agreement with our theoretical description as well as with previous experiments. This result opens the way for a new class of experiments at LDM within the field of coherent control of molecules with the possibilities that a precisely synchronized optical-pump XUV-probe laser setup like FERMI can offer.
A strong inhomogeneous static electric field is used to spatially disperse a rotationally cold supersonic beam of 2,6-difluoroiodobenzene molecules according to their rotational quantum state. The molecules in the lowest lying rotational states are selected and used as targets for 3-dimensional alignment and orientation. The alignment is induced in the adiabatic regime with an elliptically polarized, intense laser pulse and the orientation is induced by the combined action of the laser pulse and a weak static electric field. We show that the degree of 3-dimensional alignment and orientation is strongly enhanced when rotationally state-selected molecules, rather than molecules in the original molecular beam, are used as targets.
A strong inhomogeneous static electric field is used to spatially disperse a supersonic beam of polar molecules, according to their quantum state. We show that the molecules residing in the lowest-lying rotational states can be selected and used as targets for further experiments. As an illustration, we demonstrate an unprecedented degree of laser-induced 1D alignment $(<cos^2theta_{2D}>=0.97)$ and strong orientation of state-selected iodobenzene molecules. This method should enable experiments on pure samples of polar molecules in their rotational ground state, offering new opportunities in molecular science.
Dimers of carbon disulfide (CS$_2$) molecules embedded in helium nanodroplets are aligned using a moderately intense, 160ps, non-resonant, circularly polarized laser pulse. It is shown that the intermolecular carbon-carbon (C-C) axis aligns along the axis perpendicular to the polarization plane of the alignment laser pulse. The degree of alignment, quantified by $langle cos^2(theta_text{2D}) rangle$, is determined from the emission directions of recoiling CS$_2$$^+$ fragment ions, created when an intense 40fs probe laser pulse doubly ionizes the dimers. Here, $theta_text{2D}$ is the projection of the angle between the C-C axis on the 2D ion detector and the normal to the polarization plane. $langle cos^2(theta_text{2D}) rangle$ is measured as a function of the alignment laser intensity and the results agree well with $langle cos^2(theta_text{2D}) rangle$ calculated for gas-phase CS$_2$ dimers with a rotational temperature of 0.4K.
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