Three-dimensional modeling of electric-field enhancement in multilayer dielectric gratings arising from inadvertent flaws.

Pulse-compression gratings for high-power, short-pulse laser systems are exposed to high electric fields that are further enhanced locally due to their 2D nanostructured surface. This makes them vulnerable to laser-induced damage. The present work considers the effect on electric-field modulation caused by an array of commonly found inadvertent flaws in gratings including fabrication defects, contamination particles, and laser-induced-damage initiation. These defects affect the laser-damage performance characteristics of the grating. To understand the local field-enhancement distribution due these imperfections, 3D modeling of the electric-field distribution is performed with a sufficiently high resolution of 1/74 of the laser wavelength (λ) while considering a volume of ≈489 λ3. The results provide estimates for the ensuing electric-field intensification and projected reduction of the laser-damage thresholds, as well as the anticipated pattern of damage growth initiation.

Striated composite layers of silica and hafnia offering advantageous properties for short-pulse optical coatings.

Monolayers containing subnanometer striations of silica and hafnia to form composite materials at varying ratios are explored as a method to develop high-index dielectric layers with increased laser-induced-damage thresholds (LIDTs). These layers can then be used in multilayer dielectric coatings for short-pulse, high-peak-power laser applications, particularly in regions of the highest electric-field intensity. Fabrication is achieved by means of exposure to two different evaporant vapor plumes, where local exposure to each plume is controlled via shielding to prevent simultaneous exposure. The LIDT of the resulting layers has been evaluated at 1053 nm with 600-fs pulses. The results indicate that such hafnia/silica layers exhibit LIDTs similar to silica for a refractive index of ≤1.65. These results suggest that the use of these layers in locations subjected to high electric-field intensity within multilayer dielectric coatings may significantly improve the LIDT, with this deposition process providing particular benefit for scaling to large-aperture, high-fluence components.

Manufacturing-induced contamination in common multilayerdielectric gratings.

Contamination of pulse compression gratings during the manufacturing process is known to give rise to reduced laser damage performance and represents an issue that has not yet been adequately resolved. The present work demonstrates that the currently used etching methods introduce carbon contamination inside the etched region extending to a 50- to 80-nm layer below the surface. This study was executed using custom samples prepared in both, a laboratory setting and by established commercial vendors, showing results that are very similar. The laser-induced-damage performance of the etched and unetched regions in the grating-like samples suggest that contaminants introduced by etching process are contributing to the reduction of the laser-induced damage threshold.

Mechanisms governing the interaction of metallic particles with nanosecond laser pulses.

The interaction of nanosecond laser pulses at 1064- and 355-nm with micro-scale, nominally spherical metallic particles is investigated in order to elucidate the governing interaction mechanisms as a function of material and laser parameters. The experimental model used involves the irradiation of metal particles located on the surface of transparent plates combined with time-resolved imaging capable of capturing the dynamics of particle ejection, plume formation and expansion along with the kinetics of the dispersed material from the liquefied layer of the particle. The mechanisms investigated in this work are informative and relevant across a multitude of materials and irradiation geometries suitable for the description of a wide range of specific applications. The experimental results were interpreted using physical models incorporating specific processes to assess their contribution to the overall observed behaviors. Analysis of the experimental results suggests that the induced kinetic properties of the particle can be adequately described using the concept of momentum coupling introduced to explain the interaction of plane metal targets to large-aperture laser beams. The results also suggest that laser energy deposition on the formed plasma affects the energy partitioning and the material modifications to the substrate.

Damage on fused silica optics caused by laser ablation of surface-bound microparticles.

High peak power laser systems are vulnerable to performance degradation due to particulate contamination on optical surfaces. In this work, we show using model contaminant particles that their optical properties decisively determine the nature of the optical damage. Borosilicate particles with low intrinsic optical absorption undergo ablation initiating in their sub-surface, leading to brittle fragmentation, distributed plasma formation, material dispersal and ultimately can lead to micro-fractures in the substrate optical surface. In contrast, energy coupling into metallic particles is highly localized near the particle-substrate interface leading to the formation of a confined plasma and subsequent etching of the substrate surface, accompanied by particle ejection driven by the recoil momentum of the ablation plume. While the tendency to create fractured surface pitting from borosilicate is stochastic, the smooth ablation pits created by metal particles is deterministic, with pit depths scaling linearly with laser fluence. A simple model is employed which predicts ~3x electric field intensity enhancement from surface-bound fragments. In addition, our results suggest that the amount of energy deposited in metal particles is at least twice that in transparent particles.

Laser damage mechanisms in conductive widegap semiconductor films.

Laser damage mechanisms of two conductive wide-bandgap semiconductor films - indium tin oxide (ITO) and silicon doped GaN (Si:GaN) were studied via microscopy, spectroscopy, photoluminescence (PL), and elemental analysis. Nanosecond laser pulse exposures with a laser photon energy (1.03 eV, 1064 nm) smaller than the conductive films bandgaps were applied and radically different film damage morphologies were produced. The laser damaged ITO film exhibited deterministic features of thermal degradation. In contrast, laser damage in the Si:GaN film resulted in highly localized eruptions originating at interfaces. For ITO, thermally driven damage was related to free carrier absorption and, for GaN, carbon complexes were proposed as potential damage precursors or markers.

Characterization of laser-induced plasmas associated with energetic laser cleaning of metal particles on fused silica surfaces.

Time-resolved plasma emission spectroscopy was used to characterize the energy coupling and temperature rise associated with single, 10-ns pulsed laser ablation of metallic particles bound to transparent substrates. Plasma associated with Fe(I) emission lines originating from steel microspheres was observed to cool from >24,000 to ~15,000 K over ~220 ns as τ(-0.28), consistent with radiative losses and adiabatic gas expansion of a relatively free plasma. Simultaneous emission lines from Si(II) associated with the plasma etching of the SiO(2) substrate were observed yielding higher plasma temperatures, ~35,000 K, relative to the Fe(I) plasma. The difference in species temperatures is consistent with plasma confinement at the microsphere-substrate interface as the particle is ejected, and is directly visualized using pump-probe shadowgraphy as a function of pulsed laser energy.

Origins of optical absorption characteristics of Cu(2+) complexes in aqueous solutions.

Many transition metal complexes exhibit infrared or visible optical absorption arising from d-d transitions that are the key to functionality in technological applications and biological processes. The observed spectral characteristics of the absorption spectra depend on several underlying physical parameters whose relative contributions are still not fully understood. Although conventional arguments based on ligand-field theory can be invoked to rationalize the peak absorption energy, they cannot describe the detailed features of the observed spectral profile such as the spectral width and shape, or unexpected correlations between the oscillator strength and absorption peak position. Here, we combine experimental observations with first-principles simulations to investigate origins of the absorption spectral profile in model systems of aqueous Cu(2+) ions with Cl(-), Br(-), NO2(-) and CH3CO2(-) ligands. The ligand identity and concentration, fine structure in the electronic d-orbitals of Cu(2+), complex geometry, and solvation environment are all found to play key roles in determining the spectral profile. Moreover, similar physiochemical origins of these factors lead to interesting and unexpected correlations in spectral features. The results provide important insights into the underlying mechanisms of the observed spectral features and offer a framework for advancing the ability of theoretical models to predict and interpret the behavior of such systems.

Estimation of excited-state absorption and photobleaching in Fe²âº-doped lithium sodium silicate glass under exposure to high-power nanosecond laser pulses.

Fe-doped lithium sodium silicate glasses codoped with Sn and C to promote the Fe²âº redox state are investigated under simultaneous excitation at the first and third harmonics of a nanosecond Nd:YAG laser. The aim is to evaluate critical parameters associated with the potential use of this material as an optical filter that transmits the third harmonic but blocks the fundamental frequency. Estimations of the excited-state absorption coefficient and photobleaching (reduction of absorption at the fundamental) are provided. The results provide insight on the design and expected operational parameters of this type of Fe-doped materials.

Dynamics of defects in Ce³âº doped silica affecting its performance as protective filter in ultraviolet high-power lasers.

We investigate defects forming in Ce³âº-doped fused silica samples following exposure to nanosecond ultraviolet laser pulses and their relaxation as a function of time and exposure to low intensity light at different wavelengths. A subset of these defects are responsible for inducing absorption in the visible and near infrared spectral range, which is of critical importance for the use of this material as ultraviolet light absorbing filter in high power laser systems. The dependence of the induced absorption as a function of laser fluence and methods to most efficiently mitigate this effect are presented. Experiments simulating the operation of the material as a UV protection filter for high power laser systems were performed in order to determine limitations and practical operational conditions.

Effect of THz-bandwidth incoherent laser radiation on bulk damage in potassium dihydrogen phosphate crystals.

The laser-damage performance characteristics of potassium dihydrogen phosphate (KDP) samples under exposure to a distinctive broadband incoherent laser pulse are investigated. A laser system providing such pulses is intended to explore improved energy-coupling efficiency on the target in direct-drive inertial confinement fusion experiments and provides incoherent bandwidths as large as 10 THz in a nanosecond pulse. A consequence of this bandwidth is very rapid fluctuations in intensity capable of reaching maxima much larger than the average intensity within the pulse. A custom damage-test station has been built to perform measurements with broadband incoherent pulses in order to determine what effect these fast and high-intensity oscillations have on laser damage. A set of experiments under different bandwidth and beam configurations shows the effect to be minimal when probing bulk damage in KDP. Modeling indicates this behavior is supported by long electron-relaxation times compared to the source-field fluctuations, following excitation of individual electrons in the conduction band. The results help better understand the laser-induced-damage mechanisms in KDP, and its ability to operate in broadband temporally incoherent high-energy lasers that may be particularly suitable for future laser-fusion energy systems.

Time-resolved imaging of processes associated with exit-surface damage growth in fused silica following exposure to nanosecond laser pulses.

We study the dynamics of energy deposition and subsequent material response associated with exit surface damage growth in fused silica using a time resolved microscope system. This system enables acquisition of two transient images per damage event with temporal resolution of 180 ps and spatial resolution on the order of 1 µm. The experimental results address important issues in laser damage growth that include: a) the specific structural features within a damage site where plasma formation initiates; b) the subsequent growth of the plasma regions; c) the formation and expansion of radial and circumferential cracks; d) the kinetics and duration of material ejection; e) the characteristics of the generated shockwave.

Change of self-focusing behavior of phosphate glass resulting from exposure to ultraviolet nanosecond laser pulses.

The self-focusing characteristic of 355 nm, 3.3 ns pulses propagating through phosphate glass samples is found to significantly change during repeated exposure. The results indicate this change is related to the formation of color centers in the material as well as the generation of a transient defect population during exposure to the laser pulses. A model is used to fit the experimental data and obtain an estimated range of values for the modified linear and nonlinear indices of refraction.

Monolayer organic thin films as particle-contamination-resistant coatings.

Three organic monolayers coatings were developed and tested for their effectiveness to increase cleaning efficiency of attached microscale particles by air flows. The experiments were performed using silica substrates coated with these organic thin films and subsequently exposed to stainless-steel and silica microparticles as a model of contamination. Laser-induced-damage tests confirmed that the coatings do not affect the laser-induced-damage threshold values. The particle exposure results suggest that although the accumulation of particles is not significantly affected under the experimental conditions used in this work, the coated substrates exhibit significantly improved cleaning efficiency with a gas flow. A size-distribution analysis was conducted to study the adsorption and cleaning efficiency of particles of different sizes. It was observed that larger size (> 5-µm) particles can be removed from coated substrates with almost 100% efficiency. It was also determined that the coatings improve the cleaning efficiency of the smaller particles (≤ 5 µm) by 17% to 30% for the stainless steel metal and 19% to 38% for the silica particles.

Performance characterization of freeform finished surfaces of potassium dihydrogen phosphate using fluid jet polishing with a nonaqueous slurry.

Potassium dihydrogen phosphate (KDP) and its deuterated analog (DKDP) are unique nonlinear optical materials for high power laser systems. They are used widely for frequency conversion and polarization control by virtue of the ability to grow optical-quality crystals at apertures suitable for fusion-class laser systems. Existing methods for freeform figuring of KDP/DKDP optics do not produce surfaces with sufficient laser-induced-damage thresholds (LIDT's) for operation in the ultraviolet portion of high-peak-power laser systems. In this work, we investigate fluid jet polishing (FJP) using a nonaqueous slurry as a sub-aperture finishing method for producing freeform KDP surfaces. This method was used to selectively polish surface areas to different depths on the same substrate with removals ranging from 0.16 µm to 5.13 µm. The finished surfaces demonstrated a slight increase in roughness as the removal depth increased along with a small number of fracture pits. Laser damage testing with 351 nm, 1 ns pulses demonstrated excellent surface damage thresholds, with the highest values in areas devoid of fracture pits. This work demonstrates, for the first time, a method that enables fabrication of a waveplate that provides tailored polarization randomization that can be scaled to meter-sized optics. Furthermore, this method is based on FJP technology that incorporates a nonaqueous slurry specially designed for use with KDP. This novel nonaqueous FJP process can be also used for figuring other types of materials that exhibit similar challenging inherent properties such as softness, brittleness, water-solubility, and temperature sensitivity.

Characterization of ejected fused silica particles following surface breakdown with nanosecond pulses.

The light emission produced near the surface of fused silica following laser-induced breakdown on the exit surface was spatially and spectrally resolved. This signal is in part generated by ejected particles while traveling outside the hot ionized region. The thermal emission produced by the particles can be separated from the plasma emission near the surface and its spectral characteristics provide information on the temperature of the particles after ejection from the surface. Assuming the emission is thermal in origin, data suggest an initial average temperature on the order of at least 0.5 eV.

Multiparameter laser performance characterization of liquid crystals for polarization control devices in the nanosecond regime.

Interactions of liquid crystals (LC's) with polarized light have been studied widely and have spawned numerous device applications, including the fabrication of optical elements for high-power and large-aperture laser systems. Currently, little is known about both the effect of incident polarization state on laser-induced-damage threshold (LIDT) and laser-induced functional threshold (LIFT) behavior at sub-LIDT fluences under multipulse irradiation conditions. This work reports on the first study of the nanosecond-pulsed LIDT's dependence on incident polarization for several optical devices employing oriented nematic and chiral-nematic LC's oriented by surface alignment layers. Accelerated lifetime testing was also performed to characterize the ability of these devices to maintain their functional performance under multipulse irradiation as a function of the laser fluence at both 1053 nm and 351 nm. Results show that the LIDT varies as a function of input polarization by 30-80% within the same device, while the multipulse LIFT (which can differ from the nominal LIDT) depends on irradiation conditions such as laser fluence and wavelength.

Measurement of the Raman scattering cross section of the breathing mode in KDP and DKDP crystals.

The spontaneous Raman scattering cross sections of the main peaks (related to the A1 vibrational mode) in rapid and conventional grown potassium dihydrogen phosphate and deuterated crystals are measured at 532 nm, 355 nm, and 266 nm. The measurement involves the use of the Raman line of water centered at 3400 cm-1 as a reference to obtain relative values of the cross sections which are subsequently normalized against the known absolute value for water as a function of excitation wavelength. This measurement enables the estimation of the transverse stimulated Raman scattering gain of these nonlinear optical materials in various configurations suitable for frequency conversion and beam control in high-power, large-aperture laser systems.

Investigation of the electronic and physical properties of defect structures responsible for laser-induced damage in DKDP crystals.

Laser-induced damage at near operational laser excitation conditions can limit the performance of potassium dihydrogen phosphate (KH(2)PO(4), or KDP) and its deuterated analog (DKDP) which are currently the only nonlinear optical materials suitable for use in large-aperture laser systems. This process has been attributed to pre-existing damage precursors that were incorporated or formed during growth that have not yet been identified. In this work, we present a novel experimental approach to probe the electronic structure of the damage precursors. The results are modeled assuming a multi-level electronic structure that includes a bottleneck for 532 nm excitation. This model reproduces our experimental observations as well as other well-documented behaviors of laser damage in KDP crystals. Comparison of the electronic structure of known defects in KDP with this model allows for identification of a specific class that we postulate may be the constituent defects in the damage precursors. The experimental results also provide evidence regarding the physical parameters affecting the ability of individual damage precursors to initiate damage, such as their size and defect density; these parameters were found to vary significantly between KDP materials that exhibit different damage performance characteristics.

Monitoring annealing via CO(2) laser heating of defect populations on fused silica surfaces using photoluminescence microscopy.

Photoluminescence (PL) microscopy and spectroscopy under 266 nm and 355 nm laser excitation are explored as a means of monitoring defect populations in laser-modified sites on the surface of fused silica and their subsequent response to heating to different temperatures via exposure to a CO(2) laser beam. Laser-induced temperature changes were estimated using an analytic solution to the heat flow equation and compared to changes in the PL emission intensity. The results indicate that the defect concentrations decrease significantly with increasing CO(2) laser exposure and are nearly eliminated when the peak surface temperature exceeds the softening point of fused silica (approximately 1900K), suggesting that this method might be suitable for in situ monitoring of repair of defective sites in fused silica optical components.