arXiv subjects

Vaibhav S. Prabhudesai

Publications and source records attributed to Vaibhav S. Prabhudesai.

10 recordsLinked to original sources

arXiv2026

Inelastic electron scattering induced quantum coherence: isotope effect

Recent discoveries of electron-induced coherence in both resonant and non-resonant interactions have introduced new perspectives in the field. In non-resonant processes, coherence has been observed in dipolar dissociation, where electron-induced excitation forms a coherent superposition of states of opposite parities, resulting in asymmetry in the angle-differential cross-section of the process relative to the incident electron beam. Notably, an isotope effect has been observed in $D_2$ at 50 eV, where heavier isotopes exhibit diminished asymmetry due to their longer dissociation times. Here, we report the isotope effect on quantum coherence in $D_2$ across different electron energies. Additionally, we investigate the role of coherence in the isotopologue HD. Our findings reveal that the asymmetric masses in HD do not influence electron-impact excitation, leading to similar asymmetry in the angular distributions of $H^-$ and $D^-$ ions. This observation is explained by the homonuclear-like behavior of HD within the Franck-Condon region.

physics.chem-ph↗

arXiv2024

Quantum coherence in dissociative electron attachment: isotope effect

Dissociative electron attachment (DEA) is one of the processes that shows a strong coupling between the nuclear and electronic degrees of freedom in a molecule. This coupling results in an efficient transformation of the kinetic energy of attaching free electrons into the chemical energy of the compound molecule. A recent discovery of quantum coherence in this process has opened a whole new dimension in its description. On the other hand, the mass variation in isotopes of the constituent atoms has a profound effect on DEA. In quantum coherence observed in DEA, the isotope effect depicts itself in terms of change in the phase and the amplitude of the interfering dissociation paths. Here, we report the quantum coherence observed in DEA to HD, an isotopologue of H$_2$. In this isotopologue, both H$^-$ and D$^-$ show identical forward-backward asymmetry in the angular distribution. We explain these findings using the interference between two quantum paths, with the permanent dipole moment of the asymmetric mass playing no role in the process.

physics.chem-ph↗

arXiv2023

Dynamics of Dissociative Electron Attachment to Aliphatic Thiols

Dissociative electron attachment (DEA) shows functional group-dependent site selectivity in the $H^-$ ion channel. In this context, the thiol functional group has yet to be studied in great detail, although this functional group carries importance in radiation damage studies where the low-energy secondary electrons are known to induce damage through the DEA process. We report detailed measurements of absolute cross-sections and momentum images of various anion fragments formed in the DEA process in simple aliphatic thiols. We also compare the observed dynamics with that reported earlier in hydrogen sulphide, the precursor molecule for this functional group and also with aliphatic alcohols. Our findings show substantial resemblance in the underlying dynamics in these compounds and point to a possible generalisation of these features in the DEA to thiols. We also identify various pathways that contribute to the $S^-$ and $SH^-$ channels.

physics.chem-ph↗

arXiv2023

Dynamics of the dissociative electron attachment to Ethanol

We report the detailed dynamics of the site selectivity observed in the dissociative electron attachment (DEA) process in ethanol based on the momentum images obtained using the velocity slice imaging technique. The H- dissociation channel shows the site selectivity where the anion signal from the O-H site peaks at 6.5 eV and 8 eV, and that from the C-H site peaks at 9.5 eV. The momentum images also show the two-body dissociation dynamics for the O-H site break-up. This dissociation channel shows a substantial effect of the torsion mode of vibrations on the electron attachment process. In contrast, the C-H site dissociation results from the many-body break-up consistent with the earlier reports of DEA dynamics from organic molecules. We have also found that the OH- channel has a resonance at 9.3eV and is produced with very little kinetic energy. Using the isotope substitution, we show the role of H atom scrambling in the C-O bond dissociation leading to the OH- channel. This channel shows a substantial deviation from the corresponding photodissociation dynamics.

physics.chem-ph↗

arXiv2023

Effect of Background Signal on Momentum Imaging

The velocity Slice Imaging technique has revolutionised electron molecule interaction studies. Multiple electrostatic lens assemblies are often used in spectrometers for resolving low kinetic energy fragments. However, in a crossed-beam experiment with an effusive molecular beam, the extended source of ion generation due to the presence of the background gas creates artefacts on the momentum images as we try to magnify them beyond a certain size. Here, we present a systematic study of this effect on momentum imaging and the solutions to address this issue by background subtraction with suitable magnification. Additionally, we demonstrated that a supersonic molecular beam target helps minimise these artefacts in the image magnification by reducing the background signal. These systematic findings may bring valuable insight into the investigation of low kinetic energy release processes involving electron impact, ion impact, and merge beam experiments with large interaction volumes where high magnification is needed.

physics.chem-ph↗

arXiv2023

Predissociation dynamics of negative ion resonances of H$_2$ near 12 eV and 14.5 eV using velocity slice imaging technique

Dissociative electron attachment (DEA) is an important tool for investigating negative ion resonances. We have studied the negative ion resonances of H2 at 10 eV and 14 eV using the improved velocity slice imaging technique. We obtained modulations in the kinetic energy spectrum of H$^-$ ions obtained at 12 eV and 14.5 eV electron energy, consistent with the earlier reported vibrational state contributions from the higher lying bound resonances. We show that structures obtained at 12 eV are due to predissociation of the $C^2Σ_g^+$ resonance consistent with the current understanding. However, based on our angular distribution measurements, we propose that the structures obtained at 14.4 eV are due to predissociation of bound resonance of $^2Σ_g^+$ symmetry as against $δ_g$ that was proposed earlier. We also report that the bound $^2Σ_g^+$ resonance contributes to the observed inversion symmetry breaking near 14 eV.

physics.chem-ph↗

arXiv2022

Quantum coherence in molecular dynamics induced by inelastic free electron scattering

This paper presents the inversion symmetry breaking observed in ion-pair formation from molecular hydrogen on electron impact. We explain these observations using quantum interference of two dissociation paths coherently accessed by multiple angular momentum transfer channels. The results point to the generic nature of quantum coherence induced into the molecular dynamics by single electron non-resonant scattering ubiquitous in a plasma environment, planetary atmosphere, astrochemistry, etc.

physics.chem-ph↗

arXiv2016

Observation of Quantum Interferences via Light Induced Conical Intersections in Diatomic Molecules

We observe energy-dependent angle-resolved diffraction patterns in protons from strong-field dissociation of the molecular hydrogen ion H$_2^+$. The interference is a characteristic of dissociation around a laser-induced conical intersection (LICI), which is a point of contact between two surfaces in the dressed 2-dimensional Born-Oppenheimer potential energy landscape of a diatomic molecule in a strong laser field. The interference magnitude and angular period depend strongly on the energy difference between the initial state and the LICI, consistent with coherent diffraction around a cone-shaped potential barrier whose width and thickness depend on the relative energy of the initial state and the cone apex. These findings are supported by numerical solutions of the time-dependent Schrödinger equation for similar experimental conditions.

physics.atm-clus↗

arXiv2012

Quantum Control of Photodissociation via Manipulation of Bond Softening

We present a method to control photodissociation by manipulating the bond softening mechanism occurring in strong shaped laser fields, by varying the chirp sign and magnitude of an ultra-short laser pulse. Manipulation of bond-softening is experimentally demonstrated for strong field (795 nm, 10^12 - 10^13 W/cm^2) photodissociation of H2+, exhibiting substantial increase of dissociation by positively chirped pulses with respect to both negatively chirped and transform limited pulses. The measured kinetic energy release and angular distributions are used to quantify the degree of control of dissociation. The control mechanism is attributed to the interplay of dynamic alignment and chirped light induced potential curves.

physics.optics↗

arXiv2008

Electric-field-induced change of alkali-metal vapor density in paraffin-coated cells

Alkali vapor cells with antirelaxation coating (especially paraffin-coated cells) have been a central tool in optical pumping and atomic spectroscopy experiments for 50 years. We have discovered a dramatic change of the alkali vapor density in a paraffin-coated cell upon application of an electric field to the cell. A systematic experimental characterization of the phenomenon is carried out for electric fields ranging in strength from 0-8 kV/cm for paraffin-coated cells containing rubidium and cells containing cesium. The typical response of the vapor density to a rapid (duration < 100 ms) change in electric field of sufficient magnitude includes (a) a rapid (duration of < 100 ms) and significant increase in alkali vapor density followed by (b) a less rapid (duration of ~ 1 s) and significant decrease in vapor density (below the equilibrium vapor density), and then (c) a slow (duration of ~ 100 s) recovery of the vapor density to its equilibrium value. Measurements conducted after the alkali vapor density has returned to its equilibrium value indicate minimal change (at the level of < 10%) in the relaxation rate of atomic polarization. Experiments suggest that the phenomenon is related to an electric-field-induced modification of the paraffin coating.

physics.atom-ph↗