Engineering topics

Yuen, C. H.

Publications and source records attributed to Yuen, C. H..

4 records

DOE OSTI2024

Theory of strong-field sequential double ionization of polyatomic molecules

Understanding of strong-field sequential double ionization (SDI) of molecules by a highly intense infrared laser pulse could be the key to observing electron motion in molecules in the attosecond to femtosecond timescale. Based on a novel density matrix approach for SDI (DM-SDI), a recent theoretical study has shown that SDI can be used as a probe to monitor the changes in vibronic coherence in homonuclear diatomic molecules. In this article, we extend the DM-SDI model to general molecules that could possess permanent dipole moments and arbitrary symmetry. We apply the model to SDI of a water molecule and identify the formation pathway of individual dication states. We further deduce that kinetic energy release spectra from two- and three-body fragments could carry the signature of vibronic coherence between the lowest two states of the water cation. Furthermore, our results suggest that observables from the SDI probe can be interpreted intuitively with only the knowledge of electronic structures of populated ionic states, making the SDI probe to be a highly desirable probing scheme for vibronic coherence in generic molecules.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2024

Probing vibronic coherence in charge migration in molecules using strong-field sequential double ionization

We propose a scheme for probing vibronic coherence in charge migration in molecules utilizing strong-field sequential double ionization. To demonstrate the feasibility of this approach, we perform full simulations of a pump-probe scheme employing few-cycle intense infrared pulses for N 2 and O 2 . We predict that the vibronic coherence between the pumped states will be directly imprinted in experimental observables such as kinetic energy release spectra and branching ratios of the dissociative dications. Our simulations are based on the recently developed density matrix approach for sequential double ionization model, which is capable of efficiently accounting for molecular orientations and enabling direct comparison with experimental results. Lastly, our findings strongly encourage the use of this probing scheme in future charge migration experiments.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2023

Modeling the sequential dissociative double ionization of O 2 by ultrashort intense infrared laser pulses

A density matrix approach for sequential double ionization (DM-SDI) of molecules has been developed recently and was applied to the N 2 molecule. In this article, we extended the DM-SDI model to O 2 , which is a more complicated system to model than N 2 , due to its electronic structures and spin-orbit and laser couplings in the manifold of doubly charged states. We obtained a good agreement on the kinetic energy release spectrum of O + + O + from previous experiments. Thanks to the low computational cost of the model, we explored the mechanism behind the ionization and dissociation dynamics as well as the effects of lasers on the spectrum. Furthermore, this work will pave the way to model sequential dissociative double ionization of larger molecules and to probe molecular dynamics by measuring kinetic energy release spectra from this process.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2022

Density-matrix approach for sequential dissociative double ionization of molecules

Intense femtosecond infrared (IR) laser pulses have been used in recent years to study the breakup dynamics of molecules. However, observables such as kinetic energy release and branching ratios of molecular fragments are often difficult to predict by theory, making information of the molecular dynamics difficult to retrieve. In this work, we develop a simple model for sequential double ionization of molecules based on a density-matrix approach. The model describes tunneling ionization of the neutral and the ion as well as laser couplings between the ionic states simultaneously. Population of different doubly charged states can be obtained at a low computational cost. Furthermore, we applied our model to N 2 and obtained a good agreement on the kinetic energy release spectrum with a previous experiment. This theoretical development could open up the opportunities to use intense short IR laser pulses with coincidence measurement to probe molecular dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗