The present dissertation contains the theoretical studies performed on the topic of a high energy deposition in matter. The work focuses on electronic excitation and relaxation processes on ultrafast timescales. Energy deposition by means of intense ultrashort (femtosecond) laser pulses or by means of swift heavy ions irradiation have a certain similarities: the final observable material modifications result from a number of processes on different timescales. First, the electronic excitation by photoabsorption or by ion impact takes place on subfemtosecond timescales. Then these excited electrons propagate and redistribute their energy interacting among themselves and exciting secondary generations of electrons. This typically takes place on femtosecond timescales. On the order of tens to hundreds femtoseconds the excited electrons are usually thermalized. The energy exchange with the lattice atoms lasts up to tens of picoseconds. The lattice temperature can reach melting point; then the material cools down and recrystalizes, forming the final modified nanostructures, which are observed experimentally. The processes on each previous step form the initial conditions for the following step. Thus, to describe the final phase transition and formation of nanostructures, one has to start from the very beginning and follow through all the steps.
The present work focuses on the early stages of the energy dissipation after its deposition, taking place in the electronic subsystems of excited materials. Different models applicable for different excitation mechanisms will be presented: in the thesis I will start from the description of high energy excitation (electron energies of \(\sim\) keV), then I shall focus on excitations to intermediate energies of electrons (\(\sim\) 100 eV), and finally coming down to a few eV electron excitations (visible light). The results will be compared with experimental observations.
For the high energy material excitation assumed to be caused by irradiation with swift heavy ions, the classical Asymptotical Trajectory Monte-Carlo (ATMC) is applied to describe the excitation of electrons by the impact of the projectile, the initial kinetics of electrons, secondary electron creation and Auger-redistribution of holes. I first simulate the early stage (first tens of fs) of kinetics of the electronic subsystem (in silica target, SiO\(_2\)) in tracks of ions decelerated in the electronic stopping regime. It will be shown that the well pronounced front of excitation in the electronic and ionic subsystems is formed due to the propagation of electrons, which cannot be described by models based on diffusion mechanisms (e.g. parabolic equations of heat diffusion). On later timescales, the thermalization time of electrons can be estimated as a time when the particle- and the energy propagation turns from the ballistic to the diffusive one. As soon as the electrons are thermalized, one can apply the Two Temperature Model. It will be demonstrated how to combine the MC output with the two temperature model. The results of this combination demonstrate that secondary ionizations play a very important role for the track formation process, leading to energy stored in the hole subsystem. This energy storage causes a significant delay of heating and prolongs the timescales of lattice modifications up to tens of picoseconds.
For intermediate energies of excitation (XUV-VUV laser pulse excitation of materials) I applied the Monte-Carlo simulation, modified where necessary and extended in order to take into account the electronic band structure and Pauli's principle for electrons within the conduction band. I apply the new method for semiconductors and for metals on examples of solid silicon and aluminum, respectively.
It will be demonstrated that for the case of semiconductors the final kinetic energy of free electrons is much less than the total energy provided by the laser pulse, due to the energy spent to overcome ionization potentials. It was found that the final total number of electrons excited by a single photon is significantly less than \(\hbar \omega / E_{gap}\). The concept of an 'effective energy gap' is introduced for collective electronic excitation, which can be applied to estimate the free electron density after high-intensity VUV laser pulse irradiation.
For metals, experimentally observed spectra of emitted photons from irradiated aluminum can be explained well with our results. At the characteristic time of a photon emission due to radiative decay of \(L-\)shell hole (\(t < 60\) fs), the distribution function of the electrons is not yet fully thermalized. This distribution consists of two main branches: low energy distribution as a distorted Fermi-distribution, and a long high energy tail. Therefore, the experimentally observed spectra demonstrate two different branches of results: the one observed with \(L-\)shell radiation emission reflects the low energy distribution, the Bremsstrahlung spectra reflects high energy (nonthermalized) tail. The comparison with experiments demonstrated a good agreement of the calculated spectra with the experimentally observed ones.
For the irradiation of semiconductor with low energy photons (visible light), a statistical model named the "extended multiple rate equation" is proposed. Based on the earlier developed multiple rate equation, the model additionally includes the interaction of electrons with the phononic subsystem of the lattice and allows for the direct determination of the conditions for crystal damage. Our model effectively describes the dynamics of the electronic subsystem, dynamical changes in the optical properties, and lattice heating, and the results are in very good agreement with experimental measurements on the transient reflectivity and the fluence damage threshold of silicon irradiated with a femtosecond laser pulse.
Ion energy spectra of a laser-produced Ta plasma have been investigated as a function of the flight distance from the focus. The laser (Nd:YAG, 20 ns, 210 mJ) is incident obliquely (45°) and focused to an intensity of about 10^11 W cm-2. The changes in the ion distributions have been analysed for the Ta+ to Ta6+ ions in an expansion range 64 - 220 cm. With increasing distance from the target, a weak but monotonic decrease is observed for the total number of ions, which is essentially due to the decrease in the number of the more highly charged species. For the Ta+ and Ta2+ ions the net changes approximately cancel. A more sophisticated picture of the recombination dynamics is obtained, however, if the changes within individual groups of ions expanding with different velocities are compared. Here, in the same spectrum, both increasing and decreasing ion numbers can be observed. This can be interpreted as direct evidence of recombination and its dependence on temperature, density and charge.
The particle flux produced by an obliquely incident Nd Q-switched pulse (20 ns) on a Ta target has been analysed with regard to its angular distribution resolved for both its neutral and ion components. The laser intensity has been varied in the range between about 10^10 - 10^11 W cm-2, which is appropriate for many low-irradiance applications. It is observed that, at all emission angles and for the whole range of laser intensities, the number of neutral species clearly dominates the composition of the particles. At 1.3 x 10^10 W cm-2 the total number of emitted particles is 4 x 10^14, scaling as E_L^¾ with the laser energy. While for relatively low laser energies the angular distribution shows the usual smooth cos-behaviour, an additional strong directive emission cone, superimposed upon the cos-distribution, develops if the laser energy is enhanced. Both the strength and the width strongly depend on the laser intensity. While at lower intensities a fit by a cos^n function with n ~ 10 seems appropriate, n increases to 26 at an intensity of 10^11 W cm-2 . It can be assumed that secondary energy transfer processes that are not yet fully understood are responsible for this anomalous emission.
Excitation and relaxation of the electronic subsystem in solids after high energy deposition
(2011)
