Nano-imprint lithography of broad-band and wide-angle antireflective structures for high-power lasers.

We demonstrate efficient anti reflection coatings based on adiabatic index matching obtained via nano-imprint lithography. They exhibit high total transmission, achromaticity (99.5% < T < 99.8% from 390 to 900 nm and 99% < T < 99.5% from 800 to 1600 nm) and wide angular acceptance (T > 99% up to 50 degrees). Our devices show high laser-induced damage thresholds in the sub-picosecond (>5 J/cm2 at 1030 nm, 500 fs), nanosecond (>150 J/cm2 at 1064 nm, 12 ns and >100 J/cm2 at 532 nm, 12 ns) regimes, and low absorption in the CW regime (<1.3 ppm at 1080 nm), close to those of the fused silica substrate.

Impact of the multilayer dielectric design on the laser-induced damage threshold of pulse compression gratings for petawatt-class lasers.

The peak-power of petawatt-class lasers is limited by laser-induced damage to final optical components, especially on the pulse compression gratings. Multilayer dielectric (MLD) gratings are widely used in compressor systems because they exhibit a high diffraction efficiency and high damage threshold. It is now well established that the etching profile plays a key role in the electric field distribution, which influences the laser damage resistance of MLD gratings. However, less attention has been devoted to the influence of the multilayer design on the laser damage resistance of MLD gratings. In this Letter, we numerically and experimentally evidence the impact of the dielectric stack design on the electric field intensity (EFI) and the laser-induced damage threshold (LIDT). Three different MLD gratings are designed and manufactured to perform laser damage tests. On the basis of the expected EFIs and diffraction efficiencies, the measured LIDTs show how the multilayer design influences the laser resistance of the MLD gratings. This result highlights the impact of the multilayer dielectric design on the electric field distribution and shows how to further improve the laser-induced damage threshold of pulse compression gratings.

Influence of the multilayer dielectric mirror design on the laser damage growth in the sub-picosecond regime.

The peak power of high-power laser facilities is limited by the laser-induced damage to the final optical components. Also, when a damage site is generated, the damage growth phenomenon limits the lifetime of the component. Many studies have been performed to improve the laser-induced damage threshold of these components. The question now arises as to whether improvement of the initiation threshold leads to a reduction of the damage growth phenomenon. To address this question, we performed damage growth experiments on three different multilayer dielectric mirror designs exhibiting different damage thresholds. We used classical quarter-wave designs and optimized designs. The experiments were carried out with a spatial top-hat beam, spectrally centered at 1053 nm with a pulse duration of 0.8 ps in s- and p-polarization. The results showed the impact of design on the improvement of the damage growth thresholds and a reduction of the damage growth rates. A numerical model was used to simulate damage growth sequences. The results reveal similar trends to those observed experimentally. On the basis of these three cases, we have shown that improvement of the initiation threshold through a modification of the mirror design can lead to the reduction of the damage growth phenomenon.

Investigation of the influence of a spatial beam profile on laser damage growth dynamics in multilayer dielectric mirrors in the near infrared sub-picosecond regime.

Laser-induced damage growth has often been studied with Gaussian beams in the sub-picosecond regime. However, beams generated by high-power laser facilities do not feature Gaussian profiles, a property that raises questions concerning the reliability of off-line laser-induced damage measurements. Here, we compare laser-induced damage growth dynamics as a function of beam profiles. Experiments on multilayer dielectric mirrors at 1053 nm have been carried out with squared top-hat and Gaussian beams. The results demonstrate that the laser-induced damage growth threshold does not depend on the incident beam profile. A higher damage growth rate, however, has been measured with the top-hat beam. In addition, three different regimes in the growth dynamics were identified above a given fluence. A numerical model has been developed to simulate a complete damage growth sequence for different beam profiles. The numerical results are in good agreement with the observations, three growth regimes were also revealed. These results demonstrate that a linear description of growth cannot be used for the whole growth domain.

Polarization dependence of laser damage growth features on multilayer dielectric mirrors for petawatt-class lasers.

PETAL (Petawatt Aquitaine Laser) is an ultrahigh-power laser dedicated to academic research that delivers sub-picosecond pulses. One of the major issues of these facilities is the laser damage on optical components located at the final stage. Transport mirrors of the PETAL facility are illuminated under different polarization directions. This configuration motivates a thorough investigation of the dependency of the laser damage growth features (thresholds, dynamics, and damage site morphologies) on the incident polarization. Damage growth experiments were carried out in s- and p-polarization at 0.8 ps and 1053 nm on multilayer dielectric mirrors with a squared top-hat beam. Damage growth coefficients are determined by measuring the evolution of the damaged area for both polarizations. In this Letter, we report higher damage growth threshold in p-polarization together with higher damage initiation threshold in s-polarization. We also report faster damage growth dynamics in p-polarization. The damage site morphologies and their evolution under successive pulses are found to strongly depend on polarization. A numerical model in 3D was developed to assess experimental observations. This model shows the relative differences in damage growth threshold even if it is not able to reproduce the damage growth rate. Numerical results demonstrate that damage growth is mainly driven by the electric field distribution which depends on the polarization.

Multipass lock-in thermography for the study of optical coating absorption.

The development of high-power lasers requires optics with very low absorption to avoid detrimental thermal effects. In this work, we discuss our recent developments on the use of lock-in thermography to measure absorption. We apply this technique in a multipass configuration to increase the effective power on the tested samples. We present a system based on a kW-class ytterbium fiber laser operating at 1.07 µm wavelength, which enables exposing samples to 5 kW effective power and measuring absorption in the ppm range. The implementation, calibration procedure, and obtained performance are discussed with some applications to single-layer coatings of HfO2,Ta2O5,TiO2,Nb2O5, and SiO2 deposited by plasma-assisted electron beam deposition.

3D printing of silica glass through a multiphoton polymerization process.

We introduce a laser-based process relying on multiphoton-induced polymerization to produce complex three-dimensional (3D) glass parts. A focused, intense laser beam is used to polymerize a transparent resin, loaded with additives and silica nanoparticles, at the wavelength of the laser beam through nonlinear absorption processes. The object is created directly in the volume, overcoming the limitation of the layer-by-layer process. The process enables the production of silica parts with consecutive debinding and sintering processes. With bulk silica density and a resolution that depends on the laser spot size, 3D objects of centimetric dimensions are obtained.

Beam-size effects on the measurement of sub-picosecond intrinsic laser induced damage threshold of dielectric oxide coatings.

Laser-induced damage experiments on HfO2 and Nb2O5 thin films were performed with 500 fs pulse duration at 1030 nm wavelength. Threshold fluences as a function of beam size have been determined for effective beam diameters ranging from 40 to 220 µm, in a single shot regime. The results suggest no beam-size effect related to material properties in the investigated range, but size effects related to the metrology. The results indicate the importance of appropriate focusing conditions and beam measurement to qualify the optics for use in lasers with large beam sizes.

Temporal dependency in the picosecond regime of laser damage growth.

Based on squared top-hat beam irradiations, we investigate how a change of the pulse duration in the picosecond regime affects the phenomenon of laser damage growth on dielectric mirrors. We first confirm two major previously reported experimental results with a Gaussian beam that are the existence of a growth threshold fluence smaller than the laser-induced damage threshold (LIDT) and the linear evolution, characterized by a growth coefficient, of the damage area with the number of irradiations when growth occurs. We then express the growth coefficient with the fluence and the growth threshold in particular. Changing the pulse duration ultimately allows us to refine this expression a step further which leads us to establish an empirical growth law for the damage area. The temporal dependency displayed within this law appears to be very close to the one found for the LIDT which evidences the deterministic nature of laser damage growth in short pulse regimes.

Polarization dependent laser damage growth of optical coatings at sub-picosecond regime.

We report the influence of polarization on the damage mechanism of oxide thin films submitted to multiple pulses in the sub-picosecond regime. We have exposed single layer coatings of oxide materials and multilayer stacks (mirrors) to multiple laser pulses at 1030nm, 500fs, and the events on the tested sample sites were recorded in situ with high resolution microscopy. For multiple shots while keeping the fluence below the single shot threshold, damage on the film begins to form and for some of the samples the damage growth follows polarization dependent patterns. This damage growth was investigated and our results match with the assumption that the existence of nano-defects contributes to the early stage of the formation of damage, in which the energy absorption in a defect site causes local nanoablation at a laser fluence under the intrinsic ablation threshold and nanovoid formation. Based on the simulation of the interference of the scattered wave by the nanovoid with the incident wave, we obtain good correlation between simulated and observed damage growth behavior. This process leads to the formation of specific damage morphology that is strongly dependent on the polarization of the incident wave.

Sub-picosecond laser damage growth on high reflective coatings for high power applications.

Growth of laser damage on High Reflection (HR) thin film coatings is investigated at the wavelength of 1.030µm in the sub-picosecond regime. An experimental laser damage setup in a pump / probe configuration is used to study the growth behavior of engineered damage sites as well as laser damage sites. Results demonstrate that engineered sites and laser damage sites grow identically which indicates that the growth phenomenon is intrinsic to materials and stack design. In order to analyze the experimental results, we have developed a numerical model to simulate growth. Using FEM simulations, we demonstrate that growth is governed by the evolution of the electric field distribution in the mirror stack under the successive laser shots, which is supported by time-resolved observations of damage growth events. Eventually the results are compared to laser damage observations made on of full scale PETAL mirrors, which fully support the approach.

Tunable optical properties of amorphous Tantala layers in a quantizing structure.

Plasma deposition techniques like ion-beam-sputtering (IBS) are state of the art to manufacture high quality optical components for laser applications. Besides the well optimized process and monitoring systems, the coating material selection is integral to achieve optimum optical performances. Applying the IBS technology, an approach is presented to create novel materials by the direct application of binary oxides in a quantizing structure. By reducing the physical thickness of the high refractive index material to a few nm, within a classical high-low index stack, the electron confinement can be changed. Optical characterizations of the manufactured samples with decreasing quantum well thicknesses result in an increasing blue shift of the absorption gap and offer a method to approximate the effective mass of the high refractive index material in conjunction with theoretical models. Laser-induced damage threshold tests of coating samples prepared with different well thicknesses indicate an increase of the measured threshold values with optical gap energy.

Laser-induced birefringence measurements by quantitative polarized-phase microscopy.

A technique that provides quantitative and spatially resolved retardance measurement is studied for application to laser-induced modification in transparent materials. The method is based on the measurement of optical path differences between two wavefronts carrying different polarizations, measured by a wavefront sensor placed in the image plane of a microscope. We have applied the technique to the investigation of stress distribution induced by CO2 laser processing of fused silica samples. By comparing experiments to the results of thermomechanical simulations we demonstrate quantitative agreement between measurements and simulations of optical retardance. The technique provides an efficient and simple way to measure retardance of less than 1 nm with a diffraction-limited spatial resolution in transparent samples, and coupled to thermomechanical simulations it gives access to birefringence distribution in the sample.

Absorption measurements in optical coatings by lock-in thermography.

We evaluate and apply lock-in thermography as a method to quantitatively evaluate absorption losses of optical coatings. The principle of the method consists of applying periodically modulated laser intensity on the coatings and to monitor the periodic surface temperature evolution with an infrared camera. By application of a lock-in correlation procedure and using calibrated absorption samples, it is possible to obtain quantitative absorption values and to obtain absorption mappings with spatial resolution that depends on the optical configuration. Numerical simulations and experiments were performed in the case of 10-60 W laser irradiation at 1060 nm on different single layer coatings and highly reflective mirrors. In the tested conditions, the measurement of absorption down to 1 ppm level could be reached. The advantages, limitations, and potential applications of the technique are discussed.

Time-resolved quantitative-phase microscopy of laser-material interactions using a wavefront sensor.

We report on a simple and efficient technique based on a wavefront sensor to obtain time-resolved amplitude and phase images of laser-material interactions. The main interest of the technique is to obtain quantitative self-calibrated phase measurements in one shot at the femtosecond time-scale, with high spatial resolution. The technique is used for direct observation and quantitative measurement of the Kerr effect in a fused silica substrate and free electron generation by photo-ionization processes in an optical coating.

Assessment of mono-shot measurement as a fast and accurate determination of the laser-induced damage threshold in the sub-picosecond regime.

Standard test protocols need several laser shots to assess the laser-induced damage threshold of optics and, consequently, large areas are necessary. Taking into account the dominating intrinsic mechanisms of laser damage in the sub-picosecond regime, a simple, fast, and accurate method, based on correlating the fluence distribution with the damage morphology after only one shot in optics is therein presented. Several materials and components have been tested using this method and compared to the results obtained with the classical 1/1 method. Both lead to the same threshold value with an accuracy in the same order of magnitude. Therefore, this mono-shot testing could be a straightforward protocol to evaluate damage threshold in short pulse regime.

Laser damage growth with picosecond pulses.

Laser-induced damage growth has been investigated in the subpicosecond regime at 1030 nm. We have herein studied the growth of damage sites initiated on a high-reflective dielectric coating under subsequent laser irradiations at a constant fluence. We show through an experimental approach that growth can be triggered for fluences as low as 50% of the intrinsic damage threshold of the mirror. Moreover, once growth starts, damage areas increase linearly with the number of laser shots. The behavior of defect-induced damage sites has been observed more extensively, and it appears that their growth probability depends on their initiation fluence.

Laser damage density measurement of optical components in the sub-picosecond regime.

A rasterscan procedure adapted to the sub-picosecond regime is set to determine laser-induced damage densities as function of fluences. Density measurement is carried out on dielectric high-reflective coatings operating at 1053 nm. Whereas laser-induced damage is usually considered deterministic in this regime, damage events occur on these structures for fluences significantly lower than their intrinsic damage threshold. Scanning electron microscope observations of these "under-threshold" damage sites evidence ejections of defects, embedded in the dielectric stack. This method brings a new viewpoint for the qualification of optical components and their optimization for a high resistance in the sub-picosecond regime.

Quantitative phase imaging applied to laser damage detection and analysis.

We investigate phase imaging as a measurement method for laser damage detection and analysis of laser-induced modification of optical materials. Experiments have been conducted with a wavefront sensor based on lateral shearing interferometry associated with a high-magnification optical microscope. The system has been used for the in-line observation of optical thin films and bulk samples, laser irradiated in two different conditions: 500 fs pulses at 343 and 1030 nm, and millisecond to second irradiation with a CO2 laser at 10.6 µm. We investigate the measurement of the laser-induced damage threshold of optical material by detection and phase changes and show that the technique realizes high sensitivity with different optical path measurements lower than 1 nm. Additionally, the quantitative information on the refractive index or surface modification of the samples under test that is provided by the system has been compared to classical metrology instruments used for laser damage or laser ablation characterization (an atomic force microscope, a differential interference contrast microscope, and an optical surface profiler). An accurate in-line measurement of the morphology of laser-ablated sites, from few nanometers to hundred microns in depth, is shown.

Direct holographic imaging of ultrafast laser damage process in thin films.

Dynamic process of femtosecond laser-induced damage formation in dielectric thin films is reconstructed from a series of time-resolved images. Ta2O5 single-layer coatings of four different thicknesses have been investigated in transmission mode by means of time-resolved off-axis digital holography. Different processes overlapped in time were found to occur; namely, the Kerr effect, free-electron generation, ultrafast lattice heating, and shockwave generation. The trends in contribution of these effects are qualitatively reproduced by numerical models based on electron-rate equations and Drude theory, which take into account transient changes in the films and interference effects of the pump and probe pulses.