Through the use of the technique of time-of-flight mass spectroscopy, we obtain strong-field ionization yields for randomly oriented 1,2-dichloroethylene (1,2-DCE) (CHCl) and 2-butene (CH). We are interested in studying the effect of conformal structure in strong-field ionization and, in particular, the role of molecular polarity. That is, we can perform strong-field ionization studies in polar vs non-polar molecules that have the same chemical composition. We report our findings through the ionization yields and the ratio (trans/cis) of each stereoisomer pair as a function of intensity.
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http://dx.doi.org/10.1038/srep42149 | DOI Listing |
Nature
December 2024
Institute of Physics, University of Freiburg, Freiburg, Germany.
Tailored light-matter interactions in the strong coupling regime enable the manipulation and control of quantum systems with up to unit efficiency, with applications ranging from quantum information to photochemistry. Although strong light-matter interactions are readily induced at the valence electron level using long-wavelength radiation, comparable phenomena have been only recently observed with short wavelengths, accessing highly excited multi-electron and inner-shell electron states. However, the quantum control of strong-field processes at short wavelengths has not been possible, so far, because of the lack of pulse-shaping technologies in the extreme ultraviolet (XUV) and X-ray domain.
View Article and Find Full Text PDFPhys Chem Chem Phys
December 2024
JEOL Ltd, Akishima, Tokyo, 196-8558, Japan.
The McLafferty rearrangement (McLR) of the methyl valerate molecular ion has been comprehensively studied from the standpoints of the timescale for the keto-enol transformation and the change of the configuration of intermediates and transition state (TS), using mass spectrometry with electron ionization, strong-field tunnel ionization and collision-induced dissociation methods, and the global reaction route mapping (GRRM) program with quantum chemical calculations (QCCs). The timescales estimated from mass spectrometric results suggested that the McLR starts at 100 fs after ionization and is completed at least within 100 ns in the ion source. Whereas the timescales are consistent with a stepwise mechanism of fast (100 fs) and slow (10 ps) steps presented by Stamm , the QCCs put forth the possibility that an unanticipated, rapid, concerted process may be involved in completing the McLR reaction.
View Article and Find Full Text PDFRev Sci Instrum
December 2024
LaserLaB, Department of Physics and Astronomy, Vrije Universiteit Amsterdam, De Boelelaan 1105, 1081HV Amsterdam, The Netherlands.
We present a simple and easy-to-implement Graphics Processing Unit (GPU)-accelerated routine to numerically simulate the propagation of ultrashort and intense laser pulses as they interact with a medium. The routine is based on the solution of Maxwell's wave equation in the frequency domain with an extended Crank-Nicolson algorithm implemented in the Nvidia CUDA C++ programming language. The main advantages of our method are its significant speed-up factor and its ease of implementation, requiring only basic knowledge of CUDA and C++.
View Article and Find Full Text PDFJ Phys Chem Lett
December 2024
J. R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, Kansas 66506, United States.
Velocity-map imaging (VMI) is a key tool for studying outgoing electrons or ions following optical strong-field interactions of atoms and molecules and provides good momentum resolution even if the source volume of the fragments extends along a laser beam path. Here, we demonstrate within an enhancement cavity how, independently of the focal Rayleigh length, counter-propagating pulses longitudinally compress the ionization volume down to few tens of micrometers. We observe nonlinear above-threshold ionization (ATI) processes confined to the spatial overlap of femtosecond pulses, whereas the shortened ionization volume makes an electrostatic lens unnecessary for VMI.
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