Vladimir P. Zhukov

Modification of transparent materials with ultrashort laser pulses: What is energetically and mechanically meaningful?

A comprehensive analysis of laser-induced modification of bulk glass by single ultrashort laser pulses is presented which is based on combination of optical Maxwell-based modeling with thermoelastoplastic simulations of post-irradiation behavior of matter. A controversial question on free electron density generated inside bulk glass by ultrashort laser pulses in modification regimes is addressed on energy balance grounds. Spatiotemporal dynamics of laser beam propagation in fused silica have been elucidated for the regimes used for direct laser writing in bulk glass. 3D thermoelastoplastic modeling of material relocation dynamics under laser-induced stresses has been performed up to the microsecond timescale when all motions in the material decay. The final modification structure is found to be imprinted into material matrix already at sub-nanosecond timescale. Modeling results agree well with available experimental data on laser light transmission through the sample and the final modification structure.

Impacts of Ambient and Ablation Plasmas on Short- and Ultrashort-Pulse Laser Processing of Surfaces

In spite of the fact that more than five decades have passed since the invention of laser, some topics of laser-matter interaction still remain incompletely studied. One of such topics is plasma impact on the overall phenomenon of the interaction and its particular features, including influence of the laser-excited plasma re-radiation, back flux of energetic plasma species, and massive material redeposition, on the surface quality and processing efficiency. In this paper, we analyze different plasma aspects, which go beyond a simple consideration of the well-known effect of plasma shielding of laser radiation. The following effects are considered: ambient gas ionization above the target on material processing with formation of a “plasma pipe”; back heating of the target by both laser-driven ambient and ablation plasmas through conductive and radiative heat transfer; plasma chemical effects on surface processing including microstructure growth on liquid metals; complicated dynamics of the ablation plasma flow interacting with an ambient gas that can result in substantial redeposition of material around the ablation spot. Together with a review summarizing our main to-date achievements and outlining research directions, we present new results underlining importance of laser plasma dynamics and photoionization of the gas environment upon laser processing of materials.

Ultrashort-pulse laser processing of transparent materials: insight from numerical and semi-analytical models

Interaction of ultrashort laser pulses with transparent materials is a powerful technique of modification of material properties for various technological applications. The physics behind laser-induced modification phenomenon is rich and still far from complete understanding. We present an overview of our models developed to describe processes induced by ultrashort laser pulses inside and on the surface of bulk glass. The most sophisticated model consists of two parts. The first part solves Maxwell’s equations supplemented by the rate and hydrodynamics equations for free electrons. The model resolves spatiotemporal dynamics of free-electron population and yields the absorbed energy map. The latter serves as an initial condition for thermoelastoplastic simulations of material redistribution. The simulations performed for a wide range of irradiation conditions have allowed to clarify timescales at which modification occurs after single laser pulses. Simulations of spectrum of laser light scattered by laser-generated plasma revealed considerable blueshifting which increases with pulse energy. To gain insight into temperature evolution of a glass material under the surface irradiation conditions, we employ a model based on the rate equation describing free electron generation coupled with the energy equations for electrons and lattice. Swift heating of electron and lattice subsystems to extremely high temperatures at fs timescale has been found at laser fluences exceeding the threshold fluence by 2-3 times that can result in efficient bremsstrahlung emission from the irradiation spot. The mechanisms of glass ablation with ultrashort laser pulses are discussed by comparing with the experimental data. Finally, a model is outlined, developed for multi-pulse irradiation regimes, which enables gaining insight into the roles of defects and heat accumulation.

Continuum Models of Ultrashort Laser–Matter Interaction in Application to Wide-Bandgap Dielectrics

This chapter is aimed to provide a basic introduction into the principles of modeling approaches which have been developed for getting insight into various interconnected processes initiated inside transparent materials under the action of ultrashort laser pulses with consequences in volumetric modification of material structure. In view of extreme complexity of the problem, modification mechanisms and their driving processes are still far from complete understanding and require further considerable research efforts. Here we focus our consideration on established approaches that treat matter as a continuum medium. They include models describing laser beam propagation through a non-linear transparent glass or crystal with kinetics of electron plasma generation upon beam focusing and attempts to consider further material evolution with insights into thermodynamic state, stress dynamics, and plastic deformations. We underline that the quality of the final structures is determined by the synergetic action of laser excitation/relaxation kinetics, thermodynamics, and mechanics. The chapter does not pretend to completeness and aims to outline main ideas, achievements, and most intriguing findings which are still waiting for explanations and theoretical treatments.

Insights into Laser-Materials Interaction Through Modeling on Atomic and Macroscopic Scales

Computer simulations and theoretical analysis of laser-materials interactions are playing an increasingly important role in the advancement of modern laser technologies and broadening the range of laser applications. In this chapter, we first provide an overview of the current understanding of the laser coupling and transient variation of optical properties in metals, semiconductors and dielectrics, with the focus on the practical implications on the energy deposition and distribution in the irradiated targets. The continuum-level modeling of the dynamic evolution of laser-induced stresses, nonequilibrium phase transformations, and material redistribution within the laser spot are then discussed, and the need for the physical insights into the mechanisms and kinetics of highly nonequilibrium processes triggered by the laser excitation is highlighted. The physical insights can be provided by atomistic modeling, and several examples are discussed where large-scale molecular dynamics simulations are used for investigation of the mechanisms of the generation of crystal defects (vacancies, interstitials, dislocations, and twin boundaries) and the material redistribution responsible for the formation of laser-induced periodic surface structures in the single-pulse ablative regime. The need for the integrated computational approach fully accounting for the strong coupling between processes occurring at different time- and length-scales is highlighted.

Asymmetry of light absorption upon propagation of focused femtosecond laser pulses with spatiotemporal coupling through glass materials

Ultrashort laser pulses are usually described in terms of temporal and spatial dependences of their electric field, assuming that the spatial dependence is separable from time dependence. However, in most situations this assumption is incorrect as generation of ultrashort pulses and their manipulation lead to couplings between spatial and temporal coordinates resulting in various effects such as pulse front tilt and spatial chirp. One of the most intriguing spatiotemporal coupling effects is the so-called “lighthouse effect”, the phase front rotation with the beam propagation distance [Akturk et al., Opt. Express 13, 8642 (2005)]. The interaction of spatiotemporally coupled laser pulses with transparent materials have interesting peculiarities, such as the effect of nonreciprocal writing, which can be used to facilitate microfabrication of photonic structures inside optical glasses. In this work, we make an attempt to numerically investigate the influence of the pulse front tilt and the lighthouse effect on the absorption of laser energy inside fused silica glass. The model, which is based on nonlinear Maxwell’s equations supplemented by the hydrodynamic equations for free electron plasma, is applied. As three-dimensional solution of such a problem would require huge computational resources, a simplified two-dimensional model has been proposed. It has enabled to gain a qualitative insight into the features of propagation of ultrashort laser pulses with the tilted front in the regimes of volumetric laser modification of transparent materials, including directional asymmetry upon direct laser writing in glass materials.

Nonlinear effects during interaction of femtosecond doughnut-shaped laser pulses with glasses: overcoming intensity clamping

Interaction of femtosecond laser pulses with a bulk glass (fused silica as an example) has been studied numerically based on non-linear Maxwell’s equations supplemented by the hydrodynamics-type equations for free electron plasma for the cases of Gaussian linearly-polarized and doughnut-shaped radially-polarized laser beams. For Gaussian pulses focused inside glass (800 nm wavelength, 45 fs duration, numerical aperture of 0.25), the free electron density in the laser-excited region remains subcritical while the locally absorbed energy density does not exceed ~2000 J/cm3 in the range of pulse energies of 200 nJ – 2 μJ. For doughnut-shaped pulses, the initial high-intensity ring of light is shrinking upon focusing. Upon reaching a certain ionization level on its way, the light ring splits into two branches, one of which shrinks swiftly toward the beam axis well before the geometrical focus, leading to generation of supercritical free electron density. The second branch represents the laser light scattered by the electron plasma away from the beam axis. The final laserexcited volume represents a tube of 0.5–1 μm in radius and 10-15 μm long. The local maximum of absorbed energy can be more than 10 times higher compared to the case of Gaussian beams of the same energy. The corresponding pressure levels have been evaluated. It is anticipated that, in the case of doughnut-shaped pulses, the tube-like shape of the deposited energy should lead to implosion of material that can be used for improving the direct writing of high-refractive index optical structures inside glass or for achieving extreme thermodynamic states of matter.