Table of contents

This paper reviews results of experimental and theoretical studies of surface micro- and nanostructuring of metals and other materials irradiated directly by short and ultrashort laser pulses. Special attention is paid to direct laser action involving melting of the material (with or without ablation), followed by ultrarapid surface solidification, which is an effective approach to producing surface nanostructures. Theoretical analysis of recrystallisation kinetics after irradiation by ultrashort laser pulses makes it possible to determine the volume fraction of crystallised phase and the average size of forming crystalline structures as functions of laser treatment regime and thermodynamic properties of the material. The present results can be used to optimise pulsed laser treatment regime in order to ensure control nanostructuring of metal surfaces.

This paper considers nanostructuring of solid surfaces by nano-optical techniques, primarily by laser particle nanolithography. Threshold processes are examined that can be used for laser structuring of solid surfaces, with particular attention to laser swelling of materials. Fundamental spatial resolution issues in three-dimensional (3D) laser nanostructuring are analysed with application to laser nanopolymerisation and 3D optical information recording. The formation of nanostructures in the bulk of solids due to their structural instability under irradiation is exemplified by photoinduced formation of nanocomposites.

We analyse the processes taking place in transparent crystals and glasses irradiated by ultrashort laser pulses in the regimes typical of various applications in optoelectronics and photonics. We consider some phenomena, which have been previously described by the authors within the different model representations: charging of the dielectric surface due to electron photoemission resulting in a Coulomb explosion; crater shaping by using an adaptive control of the laser pulse shape; optimisation of the waveguide writing in materials strongly resistant to laser-induced compaction under ordinary irradiation conditions. The developed models and analysis of the processes relying on these models include the elements of the solid-state physics, plasma physics, thermodynamics, theory of elasticity and plasticity. Some important experimental observations which require explanations and adequate description are summarised.

The works devoted to the formation and modification of nanoparticles using laser ablation of solid targets in liquids are reviewed. Several approaches to implement laser ablation in liquids, aimed at synthesising nanoparticles of complex composition, are considered: direct laser ablation of a target of corresponding composition, laser ablation of a combined target composed of two different metals, laser irradiation of a mixture of two or more colloidal solutions, and laser ablation in reactive liquids. The properties of two-component bimetallic systems (Ag — Cu, Ag — Au), semiconductor nanocrystals (ZnO, CdSe), chalcopyrite nanoparticles, and doped oxide nanoparticles (ZnO:Ag, Gd₂O₂:Tb³⁺) formed as a result of single- and double-pulse laser ablation in different liquids (water, ethanol, acetone, solutions of polysaccharides) are discussed.

The boundary problem of light reflection and transmission by a film with chaotically distributed nanoinclusions is considered. Based on the proposed microscopic approach, analytic expressions are derived for distributions inside and outside the nanocomposite medium. Good agreement of the results with exact calculations and (at low concentrations of nanoparticles) with the integral Maxwell-Garnett effective-medium theory is demonstrated. It is shown that at high nanoparticle concentrations, averaging the dielectric constant in volume as is done within the framework of the effective-medium theory yields overestimated values of the optical film density compared to the values yielded by the proposed microscopic approach. We also studied the dependence of the reflectivity of a system of gold nanoparticles on their size, the size dependence of the plasmon resonance position along the wavelength scale, and demonstrated a good agreement with experimental data.

Surface nanostructuring of titanium, nickel, molybdenum, and tungsten by ablation with pico- and femtosecond laser pulses in liquids is studied experimentally for the first time. The morphology and properties of obtained nanostructures are investigated using a field emission scanning electron microscope and Raman spectroscopy. The size of nanostructures depends on the laser pulse duration and energy density and on the target material. As a rule, the size distribution of structures is bimodal. Potential applications of such nanostructured substrates are discussed.

Formation of small clusters during pulsed ablation of two binary semiconductors, zinc oxide and indium phosphide, in vacuum by UV, visible, and IR laser radiation is comparatively studied. The irradiation conditions favourable for generation of neutral and charged Zn_nO_m and In_nP_m clusters of different stoichiometry in the ablation products are found. The size and composition of the clusters, their expansion dynamics and reactivity are analysed by time-of-flight mass spectrometry. A particular attention is paid to the mechanisms of ZnO and InP ablation as a function of laser fluence, with the use of different ablation models. It is established that ZnO evapourates congruently in a wide range of irradiation conditions, while InP ablation leads to enrichment of the target surface with indium. It is shown that this radically different character of semiconductor ablation determines the composition of the nanostructures formed: zinc oxide clusters are mainly stoichiometric, whereas In_nP_m particles are significantly enriched with indium.

The ejection of ultradispersed diamond from a metallised target surface irradiated by nano- and subnanosecond laser pulses is experimentally investigated. Several targets with different transparent bases (quartz, polymethylmethacrylate) and absorbing metal coatings (titanium, aluminium) are investigated. The effect of the metal layer thickness and pulse width on the range of energy densities in which the ejection of diamond nanopowder is due to the transverse strain of metal layer is analysed. The heating of the target rear surface from which transfer occurs, in dependence of the target and laser pulse parameters, is estimated.

We set forth the data of experiments involving direct microtarget irradiation by the 12 second-harmonic beams (λ = 0.66 μm) of iodine laser radiation carried out on the Iskra-5 facility. For microtargets we employed glass shells ∼500 μm in diameter with ∼1-μm thick walls, which were filled with a DT mixture at a pressure p_DT ≈ 3-4 atm. In one of these experiments, a tomographic image of the microtarget was recorded from the images obtained using pinhole cameras, which were arranged along seven different directions. The pinhole images were acquired in the X-ray radiation with photon energies above 1.5 keV. The procedure used for reconstructing the volume luminosity of the microtarget is described. An analysis of the tomographic image suggests that the compressed microtarget domain possesses a complex asymmetric shape; 20–30 μm sized structural elements being clearly visible. The resultant data set allowed us to estimate the initial nonuniformity of microtarget surface irradiation by the laser radiation. The rms nonuniformity of microtarget irradiance was estimated at ∼60 %.

The possibility of unique reconstruction of the spatial profile of the cubic nonlinear susceptibility tensor component of a one-dimensionally inhomogeneous plate whose medium has a symmetry plane perpendicular to its surface is proved for the first time and the unique reconstruction algorithm is proposed. The amplitude complex coefficients of reflection and transmission (measured in some range of angles of incidence) as well as of conversion of an -polarised plane signal monochromatic wave into two waves propagating on both sides of the plate make it possible to reconstruct the profile. These two waves result from nonlinear interaction of a signal wave with an intense plane wave incident normally on the plate. All the waves under consideration have the same frequency , and so its variation helps study the frequency dispersion of the cubic nonlinear susceptibility tensor component . For media with additional symmetry axes , , , or that are perpendicular to the plate surface, the proposed method can be used to reconstruct the profile and to examine the frequency dispersion of about one third of all independent complex components of the tensor .