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Sarang Dev Ganeshamandiram

Publications and source records attributed to Sarang Dev Ganeshamandiram.

3 recordsLinked to original sources

Impact of interference between two infrared pulses driving high harmonic generation

Extreme ultraviolet (XUV) interferometry is technically challenging to implement. One approach to generating interference between two XUV pulses relies on driving high-harmonic generation in a gas jet with two collinearly overlapping infrared laser pulses. We investigate this scheme through a combined experimental and theoretical study, with particular emphasis on the regime of temporal overlap between the driving pulses. A special phase-modulation interferometry technique is implemented to increase the sensitivity for the comprehensive mapping of the strong-field induced high-order nonlinear response. We find that the dynamics arising from the interference of the two electric fields can be adequately described by the non-perturbative model developed by Lewenstein and co-workers.

physics.optics↗

H2-roaming dynamics in the formation of H3+ following two-photon double ionization of ethanol and aminoethanol

Roaming reactions involving a neutral fragment of a molecule that transiently wanders around another fragment before forming a new bond are intriguing and peculiar pathways for molecular rearrangement. Such reactions can occur for example upon double ionization of small organic molecules, and have recently sparked much scientific interest. We have studied the dynamics of the H$_2$-roaming reaction leading to the formation of H$_3^+$ after two-photon double ionization of ethanol and 2-aminoethanol, using an XUV-UV pump-probe scheme. For ethanol, we find dynamics similar to previous studies employing different pump-probe schemes, indicating the independence of the observed dynamics from the method of ionization and the photon energy of the disruptive probe pulse. Surprisingly, we do not observe a kinetic isotope effect in ethanol-D$_6$, in contrast to previous experiments on methanol where such an effect was observed. This distinction indicates fundamental differences in the energetics of the reaction pathways as compared to the methanol molecule. The larger number of possible roaming pathways compared to methanol complicates the analysis considerably. In contrast to previous studies, we additionally analyze a broad range of dissociative ionization products, which feature distinct dynamics from that of H$_{3}^{+}$ and allow initial insight into the action of the disruptive UV-probe pulse.

physics.chem-ph↗

Strong-field quantum control in the extreme ultraviolet using pulse shaping

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. While 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, due to the lack of pulse shaping technologies in the extreme ultraviolet (XUV) and X-ray domain. Here, exploiting pulse shaping of the seeded free-electron laser (FEL) FERMI, we demonstrate the strong-field quantum control of ultrafast Rabi dynamics in helium atoms with high fidelity. Our approach unravels a strong dressing of the ionization continuum, otherwise elusive to experimental observables. The latter is exploited to achieve control of the total ionization rate, with prospective applications in many XUV and soft X-ray experiments. Leveraging recent advances in intense few-femtosecond to attosecond XUV to soft X-ray light sources, our results open an avenue to the efficient manipulation and selective control of core electron processes and electron correlation phenomena in real time.

physics.atom-ph↗