Laser temperature programmed desorption: A flexible technique to study ion-surface interaction.

Understanding the physical-chemical processes ruling the interaction of particles (atoms, molecules, and ions) with surfaces is fundamental in several research fields, such as heterogeneous catalysis, astrochemistry, and nuclear fusion. In particular, the interaction of hydrogen isotopes with plasma facing materials represents a high-priority research task in the fusion community. Such studies are essential to ensure the successful operation of experimental fusion reactors, such as the tokamak ITER. In this work, we present a surface science apparatus developed to study ion-surface interaction in fusion relevant systems. It combines laser-based techniques with contaminant-free ion/molecular beams, mass spectrometry, and surface science tools such as low-energy electron diffraction and Auger electron spectroscopy. It allows to cover a wide range of sample temperatures, from 130 to 2300 K, by changing the heating rate of samples from 0.1 to 135 K/s and maintaining the linearity of the heating ramps, a powerful feature to gain insight on adsorption, absorption, and desorption mechanisms. Experimental calibration and performance are presented in detail. Moreover, to provide a factual overview of the experimental capabilities, we focus on two different applications: the protocol used to clean a W(110) single crystal sample and the development of laser temperature programmed desorption to study helium retention in tungsten.

A laser-based system to heat nuclear fuel pellets at high temperature.

Annealing tests are of utmost importance in nuclear fuel research, particularly to study the thermophysical properties of the material, microstructure evolution, or the released gas as a function of temperature. As an alternative to conventional furnace or induction annealing, we report on a laser-heating experiment allowing one to heat a nuclear fuel pellet made of uranium dioxide, UO2, or potentially other nuclear fuel pellets in an isothermal and controlled manner. For that purpose, we propose to use an indirect heating method based on a two compartment tungsten crucible, one containing the sample and the other acting as a laser susceptor for efficient and homogeneous heating of the assembly. With this concept, we demonstrate the heating of UO2 samples up to 1500 °C at a maximum heating rate of 30 °C/s with the use of two 500 W lasers. The system is, however, scalable to higher heating rates or higher temperatures by increasing the laser power up to few kW. The experiment has been designed to heat a pressurized water reactor fuel pellet, but the concept could be easily applied to other sample geometries or materials.

A high power laser facility to conduct annealing tests at high temperature.

The knowledge of material properties and their behavior at high temperatures is of crucial importance in many fields. For instance, annealing phenomena occurring during the thermomechanical processing of materials, such as recrystallization, have long been recognized as being both of scientific interest and technological importance. Different methods are currently used to study annealing phenomena and submit metals to heat loads. In this work, we present the design and the development of a laser-based facility for annealing tests. This experimental setup enables studies at the laboratory scale with great flexibility to submit samples to various spatial and temporal heating profiles. Due to the possibility of having optical access to the sample, laser heating can be combined with several non-contact diagnostics such as infrared imaging to control and analyze the temperature gradients. As a case study, we present a set of experiments performed to study the recrystallization kinetics of tungsten. We demonstrate that samples can be heated linearly with heating rate up to ∼2000 K/s, at temperatures above 2000 K, for seconds or hours, with typical errors in the temperature measurement of around 1% that depend mainly on the determination of sample emissivity. Such studies are of crucial interest in the framework of nuclear fusion since the international thermonuclear experimental reactor nuclear reactor will operate with a full-W divertor.

Implications of laser beam metrology on laser damage temporal scaling law for dielectric materials in the picosecond regime.

We report on the implications that the temporal and spatial beam metrologies have on the accuracy of temporal scaling laws of Laser Induced Damage Threshold (LIDT) for dielectric materials in the picosecond regime. Thanks to a specific diagnostic able to measure the temporal pulse shape of subpicosecond and picosecond pulses, we highlight through simulations and experiments how the temporal shape has to be taken into account first in order to correctly understand the temporal dependency of dielectrics LIDT. This directly eases the interpretation of experimental temporal scaling laws of LIDT and improves their accuracy as a prediction means. We also give numerically determined benchmark temporal scaling laws of intrinsic LIDT for SiO2 (thin film) based on the model developed for this work. Finally, we show as well what kind of spatial metrology is needed during any temporal scaling law determination to take into account potential variations of the spatial profile.

Wavefront sensing applied to determine the temperature dependence of the refractive index of liquids.

A method based on wavefront sensing is described to determine the temperature dependence of the refractive index of liquids. The technique only implies measuring the wavefront of a light beam passing through a micro-vessel containing the liquid. Here, this vessel is a crater made by CO2 laser processing in a fused silica plate. From the wavefront analysis, the optical path that is related to the refractive index of the liquid can be determined. This measurement can be done at different temperatures to obtain the temperature dependence of the refractive index. This method is applied to three liquids: water, ethanol, and cyclohexane at λ=630 nm. The results show a linear dependence in the range of 17°C-50°C and give coefficients dndT that are in good agreement with values from the literature.

An experimental platform for real-time measurement of the deformation of nuclear fuel rod claddings submitted to thermal transients.

We report on experimental development and qualification of a system developed to detect and quantify the deformations of the cladding surface of nuclear fuel pellet assemblies submitted to heat transient conditions. The system consists of an optical instrument, based on 2 wavelengths speckle interferometry, associated with an induction furnace and a model pellet assembly used to simulate the radial thermal gradient experienced by fuel pellets in pressurized water reactors. We describe the concept, implementation, and first results obtained with this system. We particularly demonstrate that the optical system is able to provide real time measurements of the cladding surface shape during the heat transients from ambient to high temperatures (up to a cladding surface temperature of 600 °C) with micrometric resolution.

Direct comparison of kilohertz- and megahertz-repetition-rate femtosecond damage threshold.

We performed femtosecond laser-induced damage threshold (fs LIDT) measurements with substantially different repetition rate Ti:sapphire laser systems: a 1 kHz regenerative amplifier and a 4.3 MHz long-cavity oscillator. All other pulse parameters are kept the same. Comparative measurements of a dielectric high reflector, a chirped mirror, and metallic mirrors show at least a factor of 2.7 lower fs LIDT at megahertz repetition rates. We attribute this to thermally assisted damage mechanisms supported by complex heat transfer simulations.

Removal of scratches on fused silica optics by using a CO2laser.

We investigate the efficiency of local CO2laser processing of scratches on silica optics in order to enhance the nanosecond UV-laser damage resistance. The surface deformations induced by the process have been measured for different CO2laser parameters and then the pulse duration and the beam diameter have been chosen accordingly to limit those deformations below 1 µm. From the study of the laser damage resistance as a function of different material modifications we identify a range of optimal radiation parameters allowing a complete elimination of scratches associated with a high threshold of laser damage. Calculation of the temperature of silica using a two-dimensional axi-symmetric code was compared with experiment, supporting an optimization of the laser parameter as a function of the maximal dimensions of scratches that could be removed by this process.

Investigation of the distribution of laser damage precursors at 1064 nm, 12 ns on niobia-silica and zirconia-silica mixtures.

Simple Nb(2)O(5), ZrO(2), SiO(2) oxide coatings and their mixtures with SiO(2) have been prepared by the Ion Beam Sputtering (IBS) technique. The Laser-Induced Damage of these samples has been studied at 1064 nm, 12 ns. The laser induced damage threshold (LIDT) decreases in both sets of the mixtures with the volumetric fraction of high index material. We find that the nanosecond LIDT of the mixtures is related to the band gap of the material as it has been widely observed in the subpicosecond regime. The laser damage probability curves have been fitted firstly by a statistical approach, i.e. direct calculation of damage precursor density from damage probability and secondly by a thermal model based on absorption of initiator. The distributions of damage precursors versus fluence extracted from these fittings show a good agreement. The thermal model makes it possible to connect damage probability to precursor physical properties. A metallic defect with a maximum radius of 18 nm was proposed to the interpretation. The critical temperature in the laser damage process exhibited a dependence on the band-gap of the material.

A high accuracy femto-/picosecond laser damage test facility dedicated to the study of optical thin films.

A laser damage test facility delivering pulses from 100 fs to 3 ps and designed to operate at 1030 nm is presented. The different details of its implementation and performances are given. The originality of this system relies the online damage detection system based on Nomarski microscopy and the use of a non-conventional energy detection method based on the utilization of a cooled CCD that offers the possibility to obtain the laser induced damage threshold (LIDT) with high accuracy. Applications of this instrument to study thin films under laser irradiation are presented. Particularly the deterministic behavior of the sub-picosecond damage is investigated in the case of fused silica and oxide films. It is demonstrated that the transition of 0-1 damage probability is very sharp and the LIDT is perfectly deterministic at few hundreds of femtoseconds. The damage process in dielectric materials being the results of electronic processes, specific information such as the material bandgap is needed for the interpretation of results and applications of scaling laws. A review of the different approaches for the estimation of the absorption gap of optical dielectric coatings is conducted and the results given by the different methods are compared and discussed. The LIDT and gap of several oxide materials are then measured with the presented instrument: Al(2)O(3), Nb(2)O(5), HfO(2), SiO(2), Ta(2)O(5), and ZrO(2). The obtained relation between the LIDT and gap at 1030 nm confirms the linear evolution of the threshold with the bandgap that exists at 800 nm, and our work expands the number of tested materials.

Impact of two CO(2) laser heatings for damage repairing on fused silica surface.

CO(2) laser is an interesting tool to repair defects on silica optics. We studied UV nanosecond laser-induced damage in fused silica after CO(2) laser heating. The localization of damage sites and the laser damage threshold are closely related to stress area in silica induced by heating. By applying a suitable second laser heating, we managed to eliminate the debris issued from redeposited silica and to modify the stress area. As a consequence, a significant increase of laser resistance has been observed. This process offers the possibility to improve damage repairing sufficiently to extend the lifetime of the silica components.

Impact of storage induced outgassing organic contamination on laser induced damage of silica optics at 351 nm.

The impact of storage conditions on laser induced damage density at 351 nm on bare fused polished silica samples has been studied. Intentionally outgassing of polypropylene pieces on silica samples was done. We evidenced an important increase of laser induced damage density on contaminated samples demonstrating that storage could limit optics lifetime performances. Atomic Force Microscopy (AFM) and Gas Chromatography -Mass Spectrometry (GC-MS) have been used to identify the potential causes of this effect. It shows that a small quantity of organic contamination deposited on silica surface is responsible for this degradation. Various hypotheses are proposed to explain the damage mechanism. The more likely hypothesis is a coupling between surface defects of optics and organic contaminants.

Statistical study of single and multiple pulse laser-induced damage in glasses.

Single and multiple pulse laser damage studies are performed in Suprasil silica and BK-7 borosilicate glasses. Experiments are made in the bulk of materials at 1.064microm with nanosecond pulses, using an accurate and reliable measurement system. By means of a statistical study on laser damage probabilities, we demonstrate that the same nano-precursors could be involved in the multiple shot and single shot damage process. A damage mechanism with two stages is then proposed to explain the results. Firstly, a pre-damage process, corresponding to material changes at a microscopic level, leads the precursor to a state that can induce a one-pulse damage. And secondly a final damage occurs, with a mechanism identical to the single shot case. For each material, a law is found to predict the precursor life-time. We can then deduce the long term life of optical elements in high-power laser systems submitted to multipulse irradiation.