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.

Ultrafast electronic excitation in CaF2 crystals

A new pump and probe experimental system was developed, the pump pulse duration of which is stretched and is much longer than that of the probe pulse. Using this system, time-resolved electronic excitation processes and damage mechanisms in CaF2 crystals were studied. The measured reflectivity of the probe pulse begins to increase at the peak of the pump pulse and increases rapidly in the latter half of the pump pulse, when the pump pulse duration is stretched to 580fs. Our experimental results indicate that both multiphoton ionization and impact ionization play important roles in the generation of conduction band electrons, at least they do so when the pump pulse durations are equal to or longer than 580fs.

Analysis of randomly time varying systems by gaussian closure technique

The Gaussian probability closure technique is applied to study the random response of multidegree of freedom stochastically time varying systems under non-Gaussian excitations. Under the assumption that the response, the coefficient and the excitation processes are jointly Gaussian, deterministic equations are derived for the first two response moments. It is further shown that this technique leads to the best Gaussian estimate in a minimum mean square error sense. An example problem is solved which demonstrates the capability of this technique for handling non-linearity, stochastic system parameters and amplitude limited responses in a unified manner. Numerical results obtained through the Gaussian closure technique compare well with the exact solutions.

Application of the Schwinger multichannel method to multichannel studies of electronically inelastic electron-molecule collisions

We have applied the Schwinger Multichannel Method(SMC) to the study of electronically inelastic, low energy electron-molecule collisions. The focus of these studies has been the assessment of the importance of multichannel coupling to the dynamics of these excitation processes. It has transpired that the promising quality of results realized in early SMC work on such inelastic scattering processes has been far more difficult to obtain in these more sophisticated studies.

We have attempted to understand the sources of instability of the SMC method which are evident in these multichannel studies. Particular instances of such instability have been considered in detail, which indicate that linear dependence, failure of the separable potential approximation, and difficulties in converging matrix elements involving recorrelation or Q-space terms all conspire to complicate application of the SMC method to these studies. A method involving singular value decomposition(SVD) has been developed to, if not resolve these problems, at least mitigate their deleterious effects on the computation of electronically inelastic cross sections.

In conjunction with this SVD procedure, the SMC method has been applied to the study of the H_2 , H_2O, and N_2 molecules. Rydberg excitations of the first two molecules were found to be most sensitive to multichannel coupling near threshold. The (3σ_g → 1π_g ) and (1π_u → 1π_g) valence excitations of the N_2 molecule were found to be strongly influenced by the choice of channel coupling scheme at all collision energies considered in these studies.

Mechanisms of femtosecond laser-induced breakdown and damage in MgO

Single-shot laser damage threshold of MgO for 40-986 fs, 800 nm laser pulses is reported. The pump-probe measurements with femtosecond pulses were carried out to investigate the time-resolved electronic excitation processes. A theoretical model including conduction band electrons (CBE) production and laser energy deposition was applied to discuss the roles of multiphoton ionization (MPI) and avalanche ionization in femtosecond laser-induced dielectric breakdown. The results indicate that avalanche ionization plays the dominant role in the femtosecond laser-induced breakdown in MgO near the damage threshold. (c) 2005 Elsevier B.V. All rights reserved.

飞秒激光作用下全向高反膜破坏的激发过程

设计和制备了全向高反膜SiO2／TiO2，研究了它在不同脉冲宽度、不同脉冲能量的飞秒激光作用下的破坏阈值和烧蚀深度．利用发展的抽运．探针方法，研究了抽运脉冲作用下材料中导带电子的超快激发和能量沉积过程，建立并求解了飞秒激光激发材料和材料的激发对抽运光自身反作用的耦合动力学模型．模型较好地揭示了材料破坏的激发过程．

Mechanisms of femtosecond laser-induced damage in magnesium fluoride

We studied the single-shot damage in magnesium fluoride irradiated by 800 nm femtosecond (fs) laser. The dependence of damage thresholds on the laser pulse durations from 60 to 750 fs was measured. The pump-probe measurements were carried out to investigate the time-resolved electronic excitation processes. A coupled dynamic model was applied to study the microprocesses in the interaction between fs laser and magnesium fluoride. The results indicate that both multiphoton ionization and avalanche ionization play important roles in the femtosecond laser-induced damage in MgF2. (C) 2006 Elsevier Ltd. All rights reserved.

Photoluminescence spectroscopy of sputtering Er-doped silicon-rich silicon nitride films

Er-doped silicon-rich silicon nitride (SRN) films were deposited on silicon substrate by an RF magnetron reaction sputtering system. After high temperature annealing, the films show intense photoluminescence in both the visible and infrared regions. Besides broad-band luminescence centered at 780 nm which originates from silicon nanocrystals, resolved peaks due to transitions from all high energy levels up to ~2H_(11/2) to the ground state of Er~(3+) are observed. Raman spectra and HRTEM measurements have been performed to investigate the structure of the films, and possible excitation processes are discussed.

Spectroscopic measurements of phase-resolved electron energy distribution functions in RF-excited discharges

The reliable measurement of the electron energy distribution function (EEDF) of plasmas is one of the most important subjects of plasma diagnostics, because this piece of information is the key to understand basic discharge mechanisms. Specific problems arise in the case of RF-excited plasmas, since the properties of electrons are subject to changes on a nanosecond time scale and show pronounced spatial anisotropy. We report on a novel spectroscopic method for phase- and space-resolved measurements of the electron energy distribution function of energetic (> 12 eV) electrons in RF discharges. These electrons dominate excitation and ionization processes and are therefore of particular interest. The technique is based on time-dependent measurements during the RF cycle of excited-state populations of rare gases admixed in small fractions. These measurements yield � in combination with an analytical model � detailed information on the excitation processes. Phase-resolved optical emission spectroscopy allows us to overcome the difficulties connected with the very low densities (107�109 cm�3) and the transient character of the electrons in the sheath region. The EEDF of electrons accelerated in the sheath region can be described by a shifted Maxwellian with a drift velocity component in direction of the electric field. The method yields the high-energy tail of the EEDF on an absolute scale. The applicability of the method is demonstrated at a capacitively coupled RF discharge in hydrogen.

Prospects of phase resolved optical emission spectroscopy as a powerful diagnostic tool for RF-discharges

Phase resolved optical emission spectroscopy (PROES) bears considerable potential for diagnostics of RF discharges that give detailed insight of spatial and temporal variations of excitation processes. Based on phase and space resolved measurements of the population dynamics of excited states several diagnostic techniques have been developed. Results for a hydrogen capacitively coupled RF (CCRF) discharge are discussed as an example. The gas temperature, the degree of dissociation and the temporally and spatially resolved electron energy distribution function (EEDF) of energetic electrons (>12eV) are measured. Furthermore, the pulsed electron impact excitation during the field reversal phase, typical for hydrogen CCRF discharges, is exploited for measurements of atomic and molecular data like lifetimes of excited states, coefficients for radiationless collisional de-excitation (quenching coefficients), and cascading processes from higher electronic states.

Realization of a Scanning Photoacoustic Technique: Thermal properties of Bulk and Film Samples

Among the large number of photothcrmal techniques available, photoacoustics assumes a very significant place because of its essential simplicity and the variety of applications it finds in science and technology. The photoacoustic (PA) effect is the generation of an acoustic signal when a sample, kept inside an enclosed volume, is irradiated by an intensity modulated beam of radiation. The radiation absorbed by the sample is converted into thermal waves by nonradiative de-excitation processes. The propagating thermal waves cause a corresponding expansion and contraction of the gas medium surrounding the sample, which in tum can be detected as sound waves by a sensitive microphone. These sound waves have the same frequency as the initial modulation frequency of light. Lock-in detection method enables one to have a sufficiently high signal to noise ratio for the detected signal. The PA signal amplitude depends on the optical absorption coefficient of the sample and its thermal properties. The PA signal phase is a function of the thermal diffusivity of the sample.Measurement of the PA amplitude and phase enables one to get valuable information about the thermal and optical properties of the sample. Since the PA signal depends on the optical and thennal properties of the sample, their variation will get reflected in the PA signal. Therefore, if the PA signal is collected from various points on a sample surface it will give a profile of the variations in the optical/thennal properties across the sample surface. Since the optical and thermal properties are affected by the presence of defects, interfaces, change of material etc. these will get reflected in the PA signal. By varying the modulation frequency, we can get information about the subsurface features also. This is the basic principle of PA imaging or PA depth profiling. It is a quickly expanding field with potential applications in thin film technology, chemical engineering, biology, medical diagnosis etc. Since it is a non-destructive method, PA imaging has added advantages over some of the other imaging techniques. A major part of the work presented in this thesis is concemed with the development of a PA imaging setup that can be used to detect the presence of surface and subsmface defects in solid samples.Determination of thermal transport properties such as thermal diffusivity, effusivity, conductivity and heat capacity of materials is another application of photothennal effect. There are various methods, depending on the nature of the sample, to determine these properties. However, there are only a few methods developed to determine all these properties simultaneously. Even though a few techniques to determine the above thermal properties individually for a coating can be found in literature, no technique is available for the simultaneous measurement of these parameters for a coating. We have developed a scanning photoacoustic technique that can be used to determine all the above thermal transport properties simultaneously in the case of opaque coatings such as paints. Another work that we have presented in this thesis is the determination of thermal effusivity of many bulk solids by a scanning photoacoustic technique. This is one of the very few methods developed to determine thermal effiisivity directly.

A new interpretation of the bonding properties and UV–vis spectra of [M3(CO)12] clusters (M = Ru, Os): a TD-DFT study

DFT and TD-DFT calculations (ADF program) were performed in order to analyze the electronic structure of the [M-3(CO)(12)] clusters (M = Ru, Os) and interpret their electronic spectra. The highest occupied molecular orbitals are M-M bonding (sigma) involving different M-M bonds, both for Ru and Os. They participate in low-energy excitation processes and their depopulation should weaken M-M bonds in general. While the LUMO is M-NI and M-CO anti-bonding (sigma*), the next, higher-lying empty orbitals have a main contribution from CO (pi*) and either a small (Ru) or an almost negligible one (Os) from the metal atoms. The main difference between the two clusters comes from the different nature of these low-energy unoccupied orbitals that have a larger metal contribution in the case of ruthenium. The photochemical reactivity of the two clusters is reexamined and compared to earlier interpretations.

Infrared-to-visible frequency upconversion in transparent glass ceramics containing trivalent-rare-earth-doped nanocrystals

In this work we report on visible upconversion emission in Er 3+-, and Ho3+-doped PbGeO3-PbF 2-CdF2-based transparent glass ceramics under 980 nm infrared excitation. In erbium-doped vitroceramic samples, blue(410 ran), green(530, and 550 nm) and red(660 nm) emission signals were generated, which were identified as due to the 2H9/2, 2H 11/2, 4S3/2, and 4F9/2 transitions to the 4I15/2 ground-state, respectively. Intense red(650 nm) upconversion emission corresponding to the 5F5 - 5I8 transition and very small blue(490 nm) and green(540 nm) signals assigned to the 5F 2,3 - 5I8 and 4S2, 5F4 - 5I8 transitions, respectively, were observed in the holmium-doped samples. The 540 nm is the dominant upconversion signal in Ho3+-doped vitroceramics under 850 nm excitation. The dependence of the upconversion processes upon pump power and doping concentration are also investigated, and the main routes for the upconversion excitation processes are also identified. The comparison of the upconversion process in transparent glass ceramics and the precursor glass was also examined and the results revealed that the former present higher upconversion efficiencies.