Study on the interaction of intense femtosecond laser pulses with nanometre-sized hydrogen clusters

The interaction of intense femtosecond laser pulses with hydrogen clusters has been experimentally studied. The hydrogen clusters were produced from expansion of high-pressure hydrogen gas (backed up to 8x10(6)Pa) into vacuum through a conical nozzle cryogenically cooled by liquid nitrogen. The average size of hydrogen clusters was estimated by Rayleigh scattering measurement and the maximum proton energy of up to 4.2keV has been obtained from the Coulomb explosion of hydrogen clusters under 2 x 10(16)W/cm(2) laser irradiation. Dependence of the maximum proton energy on cluster size and laser intensity was investigated, indicating the correlation between the laser intensity and the cluster size. The maximum proton energy is found to be directly proportional to the laser intensity, which is consistent with the theoretical prediction.

The ultrafast excitation processes in femtosecond laser-induced damage in dielectric omnidirectional reflectors

A pump and probe system is developed, where the probe pulse duration tau is less than 60 fs while the pump pulse is stretched up to 150-670 fs. The time-resolved excitation processes and damage mechanisms in the omnidirectional reflectors SiO2/TiO2 and ZnS/MgF2 are studied. It is found that as the pump pulse energy is higher than the threshold value, the reflectivity of the probe pulse decreases rapidly during the former half, rather than around the peak of the pump pulse. A coupled dynamic model based on the avalanche ionization (AI) theory is used to study the excitation processes in the sample and its inverse influences on the pump pulse. The results indicate that as pulse duration is longer than 150 fs, photoionization (PI) and AI both play important roles in the generation of conduction band electrons (CBEs); the CBE density generated via AI is higher than that via PI by a factor of 10(2)-10(4). The theory explains well the experimental results about the ultrafast excitation processes and the threshold fluences. (c) 2006 American Institute of Physics.

Transverse evolution of a plasma channel in air induced by a femtosecond laser

We investigate the evolution of filamentation in air by using a longitudinal diffraction method and a plasma fluorescence imaging technique. The diameter of a single filament in which the intensity is clamped increases as the energy of the pump light pulse increases, until multiple filaments appear. (c) 2006 Optical Society of America.

ZnSe nanowires grown on the crystal surface by femtosecond laser ablation in air

Uniform ZnSe nanowires are observed on the ablation crater on ZnSe crystal surface irradiated by femtosecond lasers in air, while other parts of the sample surface are not polluted. The nanowire growth rate is about 5 mu m/s, it is higher than that fabricated by chemical vapor deposition method by a factor of 10(4). The nanowire length and diameter can be controlled by varying laser pulse energy and pulse number. The formation mechanism is studied and found to be self-catalyzed vapor-liquid-solid process. (c) 2006 American Institute of Physics.

Coulomb explosion of hydrogen clusters irradiated by an ultrashort intense laser pulse

The explosion dynamics of hydrogen clusters driven by an ultrashort intense laser pulse has been analyzed analytically and numerically by employing a simplified Coulomb explosion model. The dependence of average and maximum proton kinetic energy on cluster size, pulse duration, and laser intensity has been investigated respectively. The existence of an optimum cluster size allows the proton energy to reach the maximum when the cluster size matches with the intensity and the duration of the laser pulse. In order to explain our experimental results such as the measured proton energy spectrum and the saturation effect of proton energy, the effects of cluster size distribution as well as the laser intensity distribution on the focus spot should be considered. A good agreement between them is obtained.

Development of high-power OPCPA laser at 1064 and 780 nm

A compact 10-TW/100-fs level ultrashort-pulse and ultra-intense laser system at 1064 nm based on optical parametric chirped pulse amplification (OPCPA) scheme is described, at which the pump and seed for the optical parametric amplification (OPA) process is optically synchronized. We investigated the output stability and the conversion efficiency of the system. Moreover, a design toward higher peak power output is given and an optically synchronized amplifier based on the concept of OPCPA at 800 nm is preliminarily explored.

Intense laser beam guiding in self-induced electron cavitation channel in underdense plasmas

In underdense plasmas, the transverse ponderomotive force of an intense laser beam with Gaussian transverse profile expels electrons radially, and it can lead to an electron cavitation. An improved cavitation model with charge conservation constraint is applied to the determination of the width of the electron cavity. The envelope equation for laser spot size derived by using source-dependent expansion method is extended to including the electron cavity. The condition for self-guiding is given and illuminated by an effective potential for the laser spot size. The effects of the laser power, plasma density and energy dissipation on the self-guiding condition are discussed.

Formation mechanisms of uniform arrays of periodic nanoparticles and nanoripples on 6H-SiC crystal surface induced by femtosecond laser ablation

Uniform arrays of periodic nanoparticles with 80-nm period are formed on 6H-SiC crystal irradiated by circularly polarized 400-nm femtosecond laser pulses. In order to understand the formation mechanism, the morphology evolvement as a function of laser pulse energy and number is studied. Periodic nanoripples are also formed on the sample surface irradiated by linearly polarized 400-, 510- and 800-nm femtosecond laser pulses. All these results support well the mechanism that second-harmonic generation plays an important role in the formation of periodic nanostructures.

Self-assembled quasi-periodic voids in glass induced by a tightly focused femtosecond laser

Multiple refocusing of a tightly focused femtosecond laser due to the dynamic transformation between self-focusing and self-defocusing is employed to provide a novel method to produce quasi-periodic voids in glass. It is found that the diameter or the interval of the periodic voids increases with the increasing pulse energy of the laser. The detailed course for producing periodic voids is discussed by analysing the damaged track induced by the tightly focused femtosecond laser pulses. It is suggested that this periodic structure has potential applications in fabrication of three-dimensional optical devices.

Standing electron plasma wave mechanism of void array formation inside glass by femtosecond laser irradiation

We investigate the mechanism of formation of periodic void arrays inside fused silica and BK7 glass irradiated by a tightly focused femtosecond (fs) laser beam. Our results show that the period of each void array is not uniform along the laser propagation direction, and the average period of the void array decreases with increasing pulse number and pulse energy. We propose a mechanism in which a standing electron plasma wave created by the interference of a fs-laser-driven electron wave and its reflected wave is responsible for the formation of the periodic void arrays.

Effects on the proton production from explosions of hydrogen clusters subjected to intense femtosecond laser fields

The dependence of the maximum and average energies of protons, which were produced in the interaction of an intense laser pulse (similar to 1 x 10(16) W cm(-2), 65 fs) with hydrogen clusters in a gas jet backed up to 80 bar at liquid nitrogen temperature (similar to 80 K), on the backing pressure has been studied. The general trend of the proton energy dependence on the square of the average cluster radius, which is determined by a calibrated Rayleigh scattering measurement, is similar to that described by theory under the single size approximation. Calculations are made to fit the experimental results under a simplified model by taking into account both a log-normal cluster size distribution and the laser intensity attenuation in the interaction volume. A very good agreement between the experimental proton energy spectra and the calculations is obtained in the high- energy part of the proton energy distributions, but a discrepancy of the fits is revealed in the low-energy part at higher backing pressures which are associated with denser flows. A possible mechanism which would be responsible for this discrepancy is discussed. Finally, from the fits, a variation of the cluster size distributions was revealed to be dependent on the gas backing pressure as well as on the evolving time of the gas flow of clusters.

Intense local plasma heating by stopping of ultrashort ultraintense laser pulse in dense plasma

Self-trapping, stopping, and absorption of an ultrashort ultraintense linearly polarized laser pulse in a finite plasma slab of near-critical density is investigated by particle-in-cell simulation. As in the underdense plasma, an electron cavity is created by the pressure of the transmitted part of the light pulse and it traps the latter. Since the background plasma is at near-critical density, no wake plasma oscillation is created. The propagating self-trapped light rapidly comes to a stop inside the slab. Subsequent ion Coulomb explosion of the stopped cavity leads to explosive expulsion of its ions and formation of an extended channel having extremely low plasma density. The energetic Coulomb-exploded ions form shock layers of high density and temperature at the channel boundary. In contrast to a propagating pulse in a lower density plasma, here the energy of the trapped light is deposited onto a stationary and highly localized region of the plasma. This highly localized energy-deposition process can be relevant to the fast ignition scheme of inertial fusion.

Studies of phonon anharmonicity in solids

Today our understanding of the vibrational thermodynamics of materials at low temperatures is emerging nicely, based on the harmonic model in which phonons are independent. At high temperatures, however, this understanding must accommodate how phonons interact with other phonons or with other excitations. We shall see that the phonon-phonon interactions give rise to interesting coupling problems, and essentially modify the equilibrium and non-equilibrium properties of materials, e.g., thermodynamic stability, heat capacity, optical properties and thermal transport of materials. Despite its great importance, to date the anharmonic lattice dynamics is poorly understood and most studies on lattice dynamics still rely on the harmonic or quasiharmonic models. There have been very few studies on the pure phonon anharmonicity and phonon-phonon interactions. The work presented in this thesis is devoted to the development of experimental and computational methods on this subject.

Modern inelastic scattering techniques with neutrons or photons are ideal for sorting out the anharmonic contribution. Analysis of the experimental data can generate vibrational spectra of the materials, i.e., their phonon densities of states or phonon dispersion relations. We obtained high quality data from laser Raman spectrometer, Fourier transform infrared spectrometer and inelastic neutron spectrometer. With accurate phonon spectra data, we obtained the energy shifts and lifetime broadenings of the interacting phonons, and the vibrational entropies of different materials. The understanding of them then relies on the development of the fundamental theories and the computational methods.

We developed an efficient post-processor for analyzing the anharmonic vibrations from the molecular dynamics (MD) calculations. Currently, most first principles methods are not capable of dealing with strong anharmonicity, because the interactions of phonons are ignored at finite temperatures. Our method adopts the Fourier transformed velocity autocorrelation method to handle the big data of time-dependent atomic velocities from MD calculations, and efficiently reconstructs the phonon DOS and phonon dispersion relations. Our calculations can reproduce the phonon frequency shifts and lifetime broadenings very well at various temperatures.

To understand non-harmonic interactions in a microscopic way, we have developed a numerical fitting method to analyze the decay channels of phonon-phonon interactions. Based on the quantum perturbation theory of many-body interactions, this method is used to calculate the three-phonon and four-phonon kinematics subject to the conservation of energy and momentum, taking into account the weight of phonon couplings. We can assess the strengths of phonon-phonon interactions of different channels and anharmonic orders with the calculated two-phonon DOS. This method, with high computational efficiency, is a promising direction to advance our understandings of non-harmonic lattice dynamics and thermal transport properties.

These experimental techniques and theoretical methods have been successfully performed in the study of anharmonic behaviors of metal oxides, including rutile and cuprite stuctures, and will be discussed in detail in Chapters 4 to 6. For example, for rutile titanium dioxide (TiO₂), we found that the anomalous anharmonic behavior of the B_1g mode can be explained by the volume effects on quasiharmonic force constants, and by the explicit cubic and quartic anharmonicity. For rutile tin dioxide (SnO₂), the broadening of the B_2g mode with temperature showed an unusual concave downwards curvature. This curvature was caused by a change with temperature in the number of down-conversion decay channels, originating with the wide band gap in the phonon dispersions. For silver oxide (Ag₂O), strong anharmonic effects were found for both phonons and for the negative thermal expansion.

Multistaged acceleration of ions by circularly polarized laser pulse: Monoenergetic ion beam generation

A multiple-staged ion acceleration mechanism in the interaction of a circularly polarized laser pulse with a solid target is studied by one-dimensional particle-in-cell simulation. The ions are accelerated from rest to several MeV monoenergetically at the front surface of the target. After all the plasma ions are accelerated, the acceleration process is repeated on the resulting monoenergetic ions. Under suitable conditions multiple repetitions can be realized and a high-energy quasi-monoenergetic ion beam can be obtained.

Electron acceleration by a propagating laser pulse in vacuum

Electrons accelerated by a propagating laser pulse of linear or circular polarization in vacuum have been investigated by one-dimensional particle-in-cell simulations and analytical modeling. A stopping target is used to stop the laser pulse and extract the energetic electrons from the laser field. The effect of the reflected light is taken into account. The maximum electron energy depends on the laser intensity and initial electron energy. There is an optimal acceleration length for electrons to gain maximum energy where electrons meet the peak of the laser pulse. The optimal acceleration length depends strongly on the laser pulse duration and amplitude. (C) 2007 American Institute of Physics.