Transient Optical Nonlinearities Engendered by Femtosecond Laser Filamentation in Gases

In an intense, ultrashort laser pulse, the electric field magnitude can reach and exceed characteristic atomic values to produce a partially ionized, nonequilibrium plasma in the pulse wake. Interaction of such pulses with gas media offers an opportunity to take direct control of electrons in the system, and to engage the system in highly nonlinear processes with lasting outcomes.

This research project addresses the transitional regime in which the electrons released by the strong-field ionization during the laser pulse become actively interacting with neighbor atoms. The project will concentrate on transient nonlinear optics in the controllable filament-wake channels; the expected results will be linked to a number of current and upcoming experimental activities.

The research will advance knowledge of intense laser-matter interactions, a topic of considerable interest for physics, chemistry, and coherent control communities. It also has many technological applications, such as remote lasing in the atmosphere, and developing new sources of attosecond and X-ray pulses. The research activity at the Center for Advanced Photonics Research (CAPR) at Temple University attracts a large number of students at graduate and undergraduate levels, including broad participation of underrepresented groups.

These students receive training in high-technology areas of femtosecond laser systems and the related fields of high-volume parallel computations.

The project aims at exploring and harnessing the physical mechanisms that create and control a transient alternative state of medium in a filament wake channel and thus determine its nonlinear-optical manifestations. Delayed nonlinear effects are manifest in many recent measurements, including higher harmonics generation, igniter-heater processes, and giant Rabi sideband emission from the channels.

The task will be addressed using a combination of ab initio calculations for the nonlinear response of individual ions, kinetic description of the evolution of the inhomogeneous excited medium, and density matrix calculations for probe laser coupling with this medium. The objectives include: (i) developing a predictive description of filament channel formation in a relatively dense gas medium, as driven by the competing processes of inverse Bremsstrahlung on neutrals, impact ionization, and collisional excitation, toward exploring pulse-shape control of the resulting excited system; (ii) tracing evolution of electronic degrees of freedom in the filament wake channels, including structured channels with finite ionization/excitation gratings, as driven by thermalized electrons engaged in collisional processes and affected by Penning ionization and also by dissociative recombination and vibrational excitation in the case of molecular gases; the expected output being the spatio-temporal patterns of the evolving ion density profiles and molecular/atomic excitation; (iii) calculating dynamic polarizability and hyperpolarizability coefficients of ions in the wake of the laser pulse (when perturbative approaches become applicable) by implementing the auxiliary-field approach and ab initio calculations to obtain the evolving dynamic quadratic and quartic nonlinear refractive indices in filament wake channels and ionization gratings; and (iv) investigating hallmark nonlinear interactions of probe pulses with the wake channels and predicting the patterns of molecular rotational revival induced via the transient nonadiabatic charge redistribution mechanism, the patterns of frequency-domain mapping of ionic rotational revivals, and controllable spatial-spectral patterns of dynamic Rabi sideband emission from structured channels.

This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.