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The National Ignition Facility (NIF) at Lawrence Livermore National Laboratory contains a 192-beam 4.2 MJ neodymium glass laser (around 1053 nm or 1w) that is frequency converted to 351nm light or 3w. It has been designed to support the study of Inertial Confinement Fusion (ICF) and High Energy Density Physics (HEDP). The NIF Precision Diagnostic System (PDS) was reactivated and new diagnostic packages were designed and fielded that offer a more comprehensive suite of high-resolution measurements. The current NIF laser performance will be presented as well as the preliminary results obtained with the various laser experimental campaigns using the new diagnostic tool suites.

Direct ink writing (DIW) three-dimensional (3D) printing provides a revolutionary approach to fabricating components with gradients in material properties. Herein, we report a method for generating colloidal germania feedstock and germania-silica inks for the production of optical quality germania-silica (GeO2-SiO2) glasses by DIW, making available a new material composition for the development of multimaterial and functionally graded optical quality glasses and ceramics by additive manufacturing. Colloidal germania and silica particles are prepared by a base-catalyzed sol-gel method and converted to printable shear-thinning suspensions with desired viscoelastic properties for DIW. The volatile solvents are then evaporated, and the green bodies are calcined and sintered to produce transparent, crack-free glasses. Chemical and structural evolution of GeO2-SiO2 glasses is confirmed by nuclear magnetic resonance, X-ray diffraction, and Raman spectroscopy. UV-vis transmission and optical homogeneity measurements reveal comparable performance of the 3D printed GeO2-SiO2 glasses to glasses produced using conventional approaches and improved performance over 3D printed TiO2-SiO2 inks. Moreover, because GeO2-SiO2 inks are compatible with DIW technology, they offer exciting options for forming new materials with patterned compositions such as gradients in the refractive index that cannot be achieved with conventional manufacturing approaches.

Sol–gel derived anti-reflective (AR) coatings, particularly those made by the Stober silica process, have been used on glass and crystal optics in high power and energy laser systems for >30 years, employed on over 100,000 half-meter-scale optics. Sol–gel’s advantages include an appropriate refractive index, which provides high-efficiency anti-reflection, high chemical purity, which leads to high laser-damage resistance, and relatively low cost synthesis and coating processes. This chapter reviews the requirements and design for AR coatings, the sol–gel synthesis process (including reaction rates, surface chemistry, and particle-size and porosity controls), coating methods and post treatments, coating stability, and laser-damage performance.

A lack of predictive methodology is frequently a major bottleneck in materials development for additive manufacturing. Hence, exploration of new printable materials often relies on the serendipity ...

Particle adsorption was explored in a model optical polishing system, consisting of silica colloids and like-charged silica surfaces. The adsorption was monitored in situ under various suspension conditions, in the absence of surfactants or organic modifiers, using a quartz crystal microbalance with dissipation monitoring (QCM-D). Changes in surface coverage with particle concentration, particle size, pH, ionic strength and ionic composition were quantified by QCM-D and further characterized ex situ by atomic force microscopy (AFM). A Monte Carlo model was used to describe the kinetics of particle deposition and provide insights on scaling with particle concentration. Transitions from near-zero adsorption to measurable adsorption were compared with equilibrium predictions made using the Deraguin-Verwey-Landau-Overbeek (DLVO) theory. In addition, the impact of silica surface roughness on the propensity for particle adsorption was studied on various spatial scale lengths by intentionally roughening the QCM sensor surface using polishing methods. It was found that a change in silica surface roughness at the AFM scale from 1.3 nm root-mean-square (rms) to 2.7 nm rms resulted in an increase in silica particle adsorption of 3-fold for 50-nm diameter particles and 1.3-fold for 100-nm diameter particles—far exceeding adsorption observed by altering suspension conditions alone, potentially because roughness at the proper scale reduces the total separation distance between particle and surface.

During optical glass polishing, a number of interactions between the workpiece (i.e., glass), polishing slurry, and pad can influence the resulting workpiece roughness at different spatial scale lengths. In our previous studies, the particle size distribution of the slurry, the pad topography, and the amount of material removed by a single particle on the workpiece were shown to strongly correlate with roughness at AFM scale lengths (nm-μm) and weakly at μ-roughness scale lengths (μm-mm). In this study, the polishing slurry pH and the generation of glass removal products are shown to influence the slurry particle spatial and height distribution at the polishing interface and the resulting μ-roughness of the glass workpiece. A series of fused silica and phosphate glass samples were polished with various ceria and colloidal silica slurries over a range of slurry pH, and the resulting AFM roughness and μ-roughness were measured. The AFM roughness was largely invariant with pH, suggesting that the removal function of a single particle is unchanged with pH. However, the μ-roughness changed significantly, increasing linearly with pH for phosphate glass and having a maximum at an intermediate pH for fused silica. In addition, the spatial and height distribution of slurry particles on the pad (as measured by laser confocal microscopy) was determined to be distinctly different at low and high pH during phosphate glass polishing. Also, the zeta potential as a function of pH was measured for the workpiece, slurry, and pad with and without surrogate glass products (K3PO4 for phosphate glass and Si(OH)4 for silica) to assess the role of interfacial charge during polishing. The addition of K3PO4 significantly raised the zeta potential, whereas addition of Si(OH)4 had little effect on the zeta potential. An electrostatic DLVO three-body force model, using the measured zeta potentials, was used to calculate the particle–particle, particle–workpiece, and particle–pad attractive and repulsive forces as a function of pH and the incorporation of glass products at the interface. The model predicted an increase in particle–pad attraction with an increase in pH and phosphate glass products consistent with the measured slurry distribution on the pads during phosphate glass polishing. Finally, a slurry “island” distribution gap (IDG) model has been formulated which utilizes the measured interface slurry distributions and a load balance to determine the interface gap, the contact area fraction, and the load on each slurry “island”. The IDG model was then used to simulate the workpiece surface topography and μ-roughness; the results show an increase in roughness with pH similar to that observed experimentally.

The final optics in the National Ignition Facility (NIF) are protected from target debris by sacrificial (disposable) debris shields (DDS) comprised of 3-mm thick Borofloat. While relatively inexpensive, Borofloat has been found to have bulk inclusions which, under UV illumination, damage, grow, and occasional erupt though the surface of the DDS. We have shown previously that debris generated from Input Surface Bulk Eruptions (ISBE) are a significant source of damage on NIF. Inclusion-free fused silica debris shield (FSDS) have been installed in between the DDS and the final optics on some NIF beam lines to test their efficacy in mitigating damage initiation. We will show results of the damage performance of the FSDS and its role in protecting the final optics. These results will help in our economic analysis of the potential benefits of using FSDS to protect NIF final optics.

We explored templating effects of various materials for hydrogen (H2 and D2) solidification by measuring the degree of supercooling required for liquid hydrogen to solidify below each triple point....

The National Ignition Facility (NIF) laser with its 192 independent laser beams is not only the world’s largest laser but also the largest optical system ever built. With its 192 independent laser ...

The National Ignition Facility (NIF) at Lawrence Livermore National Laboratory (LLNL) houses the world’s largest laser system, composed of 192 individual, 40-cm-aperture beamlines. The NIF laser ro...

Complex and precise research targets are required for the inertial confinement fusion (ICF) experiments conducted at the National Ignition Facility. During the National Ignition Campaign (NIC) the ...

The National Ignition Facility (NIF) regularly operates at fluences above the onset of laser-induced optics damage. To do so, it is necessary to routinely recycle the NIF final optics, which involves removing an optic from a beamline, inspecting and repairing the laser-induced damage sites, and re-installing the optic. The inspection and repair takes place in our Optics Mitigation Facility (OMF), consisting of four identical processing stations for performing the repair protocols. Until recently, OMF has been a labor-intensive facility, requiring 10 skilled operators over two shifts to meet the throughput requirements. Here we report on the implementation of an automated control system—informed by machine learning— that significantly improves the throughput capability for recycling of NIF optics while reducing staffing requirements. Performance metrics for mid-2018 show that approximately 85% of all damage sites can be automatically inspected and repaired without any required operator input. Computer keystrokes have been reduced from about 6000 per optic to under 300.

Operating the National Ignition Facility (NIF) near its power and energy performance limits has revealed a new damage initiation mechanism in the final UV optics. The typical damage event involves the last three optics in the NIF beamline: the final focusing lens, the grating debris shield, and the target debris shield. It occurs on high power shots from intensifications from small phase defects (pits) on the exit surface of the focusing lens that travel through the grating debris shield before reflecting off the AR-coated target debris shield about 75 cm downstream, then propagate back upstream and damage the input surface of the grating debris shield optic which is 15 cm downstream of the focusing lens. Ray tracing has firmly established the direct relationship between the phase defects on the final focusing lens and the damage on grating debris via the reflection from the target debris shield. In some cases, bulk filamentary damage is also observed in the 1-cm thick fused silica grating debris shield. It is not fully understood at this point how there can be enough energy from the reflected beam to cause damage where the forward-going beam did not. It does not appear that interaction between the forward-going beam and the backward-going reflected beam is necessary for damage to occur. It does appear necessary that the target debris shield be previously exposed to laser shots and/or target debris. Furthermore, there is no evidence of damage imparted to the target debris shield or the final focusing lens. We will describe all the conditions under which we have (and have not) observed these relatively rare events, and the steps we have taken to mitigate their occurrence, including identification and elimination of the source phase defects.

Additive manufacturing offers new routes to lightweight optics inaccessible by conventional methods by providing a broader range of reconciled functionality, form factor, and cost. Predictive lattice design combined with the ability to 3D print complex structures allows for the creation of low-density metamaterials with high global and local stiffness and tunable response to static and dynamic loading. This capacity provides a path to fabrication of lightweight optical supports with tuned geometries and mechanical properties. Our approach involves the simulation and optimization of lightweight lattices for anticipated stresses due to polishing and mounting loads via adaptive mesh refinement. The designed lattices are 3D printed using large area projection microstereolithography (LAPuSL), coated with a metallic plating to improve mechanical properties, and bonded to a thin (1.25 mm) fused silica substrate. We demonstrate that this lightweight assembly can be polished to a desired flatness using convergent polishing, and subsequently treated with a reflective coating. *This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344 within the LDRD program. LLNL-ABS-738806.

The chemical characteristics and the proposed formation mechanisms of the modified surface layer (called the Beilby layer) on polished fused silica glasses are described. Fused silica glass samples were polished using different slurries, polyurethane pads, and at different rotation rates. The concentration profiles of several key contaminants, such as Ce, K, and H, were measured in the near surface layer of the polished samples using Secondary Ion Mass Spectroscopy (SIMS). The penetration of K, originating from KOH used for pH control during polishing, decreased with increase in polishing material removal rate. In contrast, penetration of the Ce and H increased with increase in polishing removal rate. In addition, Ce penetration was largely independent of the other polishing parameters (e.g., particle size distribution and the properties of the polishing pad). The resulting K concentration depth profiles are described using a two-step diffusion process: (1) steady-state moving boundary diffusion (due to material removal during polishing) followed by (2) simple diffusion during ambient postpolishing storage. Using known alkali metal diffusion coefficients in fused silica glass, this diffusion model predicts concentration profiles that are consistent with the measured data at various polishing material removal rates. On the other hand, the observed Ce profiles are inconsistent with diffusion based transport. Rather we propose that Ce penetration is governed by the ratio of Ce–O–Si and Si–O–Si hydrolysis rates; where this ratio increases with interface temperature (which increases with polishing material removal rate) resulting in greater Ce penetration into the Beilby layer. Calculated Ce surface concentrations using this mechanism are in good agreement to the observed change in measured Ce surface concentrations with polishing material removal rate. These new insights into the chemistry of the Beilby layer, combined together with details of the single particle removal function during polishing, are used to develop a more detailed and quantitative picture of the polishing process and the formation of the Beilby layer.

The primary sources of damage on the National Ignition Facility (NIF) Grating Debris Shield (GDS) are attributed to two independent types of laser-induced particulates. The first comes from the eruptions of bulk damage in a disposable debris shield downstream of the GDS. The second particle source comes from stray light focusing on absorbing glass armor at higher than expected fluences. We show that the composition of the particles is secondary to the energetics of their delivery, such that particles from either source are essentially benign if they arrive at the GDS with low temperatures and velocities.

Large laser systems that deliver optical pulses with peak powers exceeding one Petawatt (PW) have been constructed at dozens of research facilities worldwide and have fostered research in High-Energy-Density (HED) Science, High-Field and nonlinear physics [1]. Furthermore, the high intensities exceeding 1018W/cm2 allow for efficiently driving secondary sources that inherit some of the properties of the laser pulse, e.g. pulse duration, spatial and/or divergence characteristics. In the intervening decades since that first PW laser, single-shot proof-of-principle experiments have been successful in demonstrating new high-intensity laser-matter interactions and subsequent secondary particle and photon sources. These secondary sources include generation and acceleration of charged-particle (electron, proton, ion) and neutron beams, and x-ray and gamma-ray sources, generation of radioisotopes for positron emission tomography (PET), targeted cancer therapy, medical imaging, and the transmutation of radioactive waste [2, 3]. Each of these promising applications requires lasers with peak power of hundreds of terawatt (TW) to petawatt (PW) and with average power of tens to hundreds of kW to achieve the required secondary source flux.

Overview of progress in construction and testing of the laser systems of ELI-Beamlines, accomplished since 2015, is presented. Good progress has been achieved in construction of all four lasers based largely on the technology of diode-pumped solid state lasers (DPSSL). The first part of the L1 laser, designed to provide 200 mJ

We have demonstrated the world's highest average power, fully diode-pumped, petawatt-class peak power laser, the High-repetition-rate Advanced Petawatt Laser System (HAPLS) [1-3]. These first commissioning results at 16J (stretched) at 3%Hz fully validate projected performance of 30J/30fs (>1PW) at 10Hz. The laser has been operated at this intermediate level at Lawrence Livermore National Laboratory to demonstrate integrated performance of all subsystems and provide benchmarking data to laser performance models before further increasing energy and peak power. Data was obtained during multiple campaigns, exceeding several hours of run time, and a snapshot of 60min of data is shown in Fig. 1. The average pump laser 1ω (1053nm) energy was 97J with an rms stability of 0.7%, 2ω (527nm) energy at the Ti:sapphire power amplifier was 62J, and the average stretched short pulse energy was 16J. A full-aperture diagnostic suite allows simultaneous, single-shot measurement of energy, spectrum, beam quality, and pulse duration at full repetition rate. Single-shot SPIDER retrieved pulse shapes (Fig. 1 inset) with an average pulse duration over 12000 consecutive shots of 28.6fs (rms=1.4fs). The mean pulse duration is consistent with the measured spectral bandwidth and is ∼1.2× the transform limit. All results shown are raw data without filtering or averaging, demonstrating the exceptional pulse characteristics, repeatability, and stability of the entire laser system.

The effects of temperature and material deposit on workpiece material removal spatial uniformity during optical pad polishing are described. Round and square-fused silica workpieces (25–265 mm in size) were polished on a polyurethane pad using ceria slurry under various conditions. Using a nonrotated workpiece on a rotating lap, elevated temperatures (as measured by IR imaging), due to frictional heating at the workpiece–lap interface, were observed having a largely radial symmetric profile (relative to the lap center) on both the workpiece and lap with a peak temperature corresponding to the workpiece center. A 3D steady-state thermal model of the polishing process, which accounts for the frictional heating and effective heat transfer from various surfaces, quantitatively describes the observed thermal profiles. The temperature spatial uniformity, which affects the material removal spatial uniformity, can be significantly improved using a rotated workpiece and a specially designed compensating septum during polishing. Next, using a rotating workpiece and lap, the workpiece surface develops two types of mid-range structure: (1) fine ripples (sub-mm scale length) that run circumferentially with respect to the lap, which have been attributed to microscopic islands of slurry on the lap leading to radial material removal nonuniformities; and (2) a center depression (cm scale length) which has been attributed to nonlinear slurry & glass products buildup at a specific radial lap location. A polishing simulator model (called Surface Figure or SurF), which accounts for workpiece wear, pad wear, and now deposition on the pad, correctly simulates the preferential material deposit on the pad and the center depression structure developed on the workpiece. Strategies, such as time averaging through kinematics and diamond conditioning, for preventing both these nonuniformities are demonstrated.

A method for chemically stabilizing metal oxide polishing slurries to prevent their agglomeration while maintaining their surface activity is demonstrated experimentally. Negatively charged ceria, zirconia, and alumina particles are reversibly size-stabilized under low ionic strength conditions at and above their isoelectric points using anionic surfactants. Stability is imparted only at surfactant concentrations above the critical micelle concentration and when the particle and the micelle have like-signed charges. Zeta potential measurements demonstrate that little adsorption of anionic surfactant occurs under conditions where the particles are negatively charged. Changes to pH, hydrophobicity, and ionic strength disrupt the surfactant's ability to size-stabilize the slurries. These results suggest that the charged micelles electrosterically hinder the agglomeration of oxide particles. Because the stabilization method does not rely on adsorption, the particle surface remains accessible for chemical reactions, such as those involved in polishing. Metal oxide slurries stabilized by this method remove material at a rate comparable to that of unstabilized slurry. In addition, stabilized slurry is easier to filter, which improves the quality of the polished surface. Stabilizing colloids by this method may prove valuable for systems where particle surface functionality is important, such as those used in ceramics processing, optical polishing, and chemical-mechanical planarization.

This guest editorial introduces the Special Section on Ultraprecision Optics Fabrication and Characterization.

Loose abrasive grinding was performed on a wide range of optical workpiece materials [single crystals of Al2O3 (sapphire), SiC, Y3Al5O12 (YAG), CaF2, and LiB3O5 (LBO); a SiO2-Al2O3-P2O5-Li2O glass-ceramic (Zerodur); and glasses of SiO2 : TiO2 (ULE), SiO2 (fused silica), and P2O5-Al2O3-K2O-BaO (phosphate)]. Using the magneto rheological finishing (MRF) taper wedge technique (where a wedge was polished on each of the ground workpieces and the resulting samples were appropriately chemically etched), the subsurface mechanical damage (SSD) characteristics were measured. The SSD depth for most of the workpiece materials was found to scale as E11/2 / H1, where E1 is the elastic modulus and H1 is the hardness of the workpiece. This material scaling is the same as that for the growth of lateral cracks, suggesting that lateral cracks are a dominant source for SSD rather than radial/median cracks, as previously proposed. Utilizing the SSD depth data from both this study and others, semiempirical relationships have been formulated, which allows for estimating the SSD depth as a function of workpiece material and important grinding parameters (such as abrasive size and applied pressure).

A series of controlled grinding experiments, utilizing loose or fixed abrasives of either alumina or diamond at various particle sizes, were performed on a wide range of optical workpiece materials [single crystals of Al2O3 (sapphire), SiC, Y3Al5O12 (YAG), CaF2, and LiB3O5 (LBO); a SiO2−Al2O3−P2O5−Li2O glass ceramic (Zerodur); and glasses of SiO2:TiO2 (ULE), SiO2 (fused silica), and P2O5−Al2O3−K2O−BaO (phosphate)]. The material removal rate, surface roughness, and morphology of surface fractures were measured. Separately, Vickers indentation was performed on the workpieces, and the depths of various crack types as a function of applied load was measured. Single pass grinding experiments showed distinct differences in the spatial pattern of surface fracturing between the loose alumina abrasive (isolated indent-type lateral cracking) and the loose or fixed diamond abrasive (scratch-type elongated lateral cracking). Each of the grinding methods had a removal rate and roughness that scaled with the lateral crack slope, s l (i.e., the rate of increase in lateral crack depth with the applied load) of the workpiece material. A grinding model (based on the volumetric removal of lateral cracks accounting for neighboring lateral crack removal efficiency and the fraction of abrasive particles leading to fracture initiation) and a roughness model (based on the depth of lateral cracks or the interface gap between the workpiece and lap) are shown to quantitatively describe the material removal rate and roughness as a function of workpiece material, abrasive size, applied pressure, and relative velocity. This broad, multiprocess variable grinding model can serve as a predictive tool for estimating grinding rates and surface roughness for various grinding processes on different workpiece materials.

Various ceria and colloidal silica polishing slurries were used to polish fused silica glass workpieces on a polyurethane pad. Characterization of the slurries’ particle size distribution (PSD) (using both ensemble light scattering and single particle counting techniques) and of the polished workpiece surface (using atomic force microscopy) was performed. The results show the final workpiece surface roughness is quantitatively correlated with the logarithmic slope of the distribution function for the largest particles at the exponential tail end of the PSD. Using the measured PSD, fraction of pad area making contact, and mechanical properties of the workpiece, slurry, and pad as input parameters, an Ensemble Hertzian Gap (EHG) polishing model was formulated to estimate each particle’s penetration, load, and contact zone. The model is based on multiple Hertzian contact of slurry particles at the workpiece–pad interface in which the effective interface gap is determined through an elastic load balance. Separately, ceria particle static contact and single pass sliding experiments were performed showing ~1-nm depth removal per pass (i.e., a plastic type removal). Also, nanoindentation measurements on fused silica were made to estimate the critical load at which plastic type removal starts to occur (Pcrit~5 3 10 � 5 N). Next the EHG model was extended to create simulated polished surfaces using the Monte Carlo method where each particle (with the calculated characteristics described above) slides and removes material from the silica surface in random directions. The polishing simulation utilized a constant depth removal mechanism (i.e., not scaling with particle size) of the elastic deformation zone cross section between the particle and silica surface, which was either 0.04 nm (for chemical removal) at low loads ( Pcrit). The simulated surfaces quantitatively compare well with the measured rms roughness, power spectra, surface texture, absolute thickness material removal rate, and load dependence of removal rate.

In the follow study, we have developed a detailed understanding of the chemical and mechanical microscopic interactions that occur during polishing affecting the resulting surface microroughness of the workpiece. Through targeted experiments and modeling, the quantitative relationships of many important polishing parameters & characteristics affecting surface microroughness have been determined. These behaviors and phenomena have been described by a number of models including: (a) the Ensemble Hertzian Multi Gap (EHMG) model used to predict the removal rate and roughness at atomic force microscope (AFM) scale lengths as a function of various polishing parameters, (b) the Island Distribution Gap (IDG) model used to predict the roughness at larger scale lengths, (c) the Deraguin-Verwey-Landau-Overbeek (DLVO) 3-body electrostatic colloidal model used to predict the interaction of slurry particles at the interface and roughness behavior as a function of pH, and (d) a diffusion/chemical reaction rate model of the incorporation of impurities species into the polishing surface layer (called the Bielby layer). Based on this improved understanding, novel strategies to polish the workpiece have been developed simultaneously leading to both ultrasmooth surfaces and high material removal rates. Some of these strategies include: (a) use of narrow PSD slurries, (b) a novel diamond conditioning recipemore » of the lap to increase the active contact area between the workpiece and lap without destroying its surface figure, (c) proper control of pH for a given glass type to allow for a uniform distribution of slurry particles at the interface, and (d) increase in applied load just up to the transition between molecular to plastic removal regime for a single slurry particle. These techniques have been incorporated into a previously developed finishing process called Convergent Polishing leading to not just economical finishing process with improved surface figure control, but also simultaneously leading to low roughness surface with high removal rates.« less

Modeling of laser-induced optics damage has been introduced to benchmark existing optic usage at the National Ignition Facility (NIF) which includes the number of optics exchanged for damage repair. NIF has pioneered an optics recycle strategy to allow it to run the laser at capacity since fully commissioned in 2009 while keeping the cost of optics usage manageable. We will show how the damage model is being used to evaluate strategies to streamline our optics loop efficiency, as we strive to increase the laser shot rate without increasing operating costs.

Optical fabrication Science & Technology (specifically sub-surface damage, surface figure, & roughness) and its impact on fabricating economical high quality, laser damage resistant optics for use in high energy, high power lasers are reviewed.

A new method (a variant of tumble finishing) for polishing and achieving local planarization on precision spherical, plastic capsules is described. Such capsules have niche applications, such as ablators used in high-peak-power laser targets for fusion energy research. The as-manufactured ablators contain many shallow domes (many 100's of nm high and a few 10's of μm wide) on the outer surface which are undesirable due to contributions to instabilities during implosion. These capsules were polished (i.e., tumble finished) by rotating a cylindrical vial containing the capsule, many borosilicate glass or zirconia media, and an aqueous-based colloidal silica polishing slurry. During tumble finishing, the relative media/capsule motions cause multiple, random sliding spherical–spherical Hertzian contacts, resulting in material removal, and possibly plastic deformation, on the capsule. As a result, the domes were observed to locally planarize (i.e., converge to lower heights). Utilizing the correct kinematics (i.e., the characteristics of the media/capsule motions), as controlled by the vial rotation rate and the fill fraction of media and slurry, the high velocity downward circumferential media motions were avoided, preventing fracturing of the fragile capsules. Also, the resulting post-polished surface roughness on the capsule was found to scale with the initial media surface roughness. Hence, pre-polishing the media greatly reduced the roughness of the media and thus the roughness of the polished capsule. A material removal model is described based on the Preston model and spherical–spherical Hertzian contacts which shows reasonable agreement with measured average removal rates of 35 ± 15 nm/day and which serves as a valuable tool to scale the polishing behavior with changes in process variables. Narrow domes were observed to planarize more rapidly than wider domes. A local planarization convergence model is also described, based on the concept of workpiece–lap mismatch where the local pressure, and hence removal, varies with the gap at the interface contact. The calculated rate and shape evolution of various size isolated domes compares well with the experimental data.

A new method of optical polishing termed “Convergent Polishing” is demonstrated where a workpiece, regardless of its initial surface figure, will converge to the lap shape in a single iteration. This method of polishing is accomplished by identifying the phenomena that contribute to non-uniform spatial material removal, and mitigating the non-uniformity for each phenomenon (except for the workpiece-lap mismatch due to the workpiece surface shape). The surface mismatch at the interface between the workpiece and lap causes a spatial and time varying pressure differential which decreases with removal, thus allowing the workpiece to converge to the shape of the lap. In this study, fused (amorphous) silica workpieces are polished using ceria slurry on various polyurethane pads. Polishing parameters were systematically controlled to prevent various sources of non-uniform material removal which include: (i) moment force, (ii) viscoelastic lap relaxation, (iii) kinematics, (iv) pad wear, and (v) workpiece bending. The last two are described herein. With these mitigations, removal uniformity has been demonstrated to within 1.0 μm over the surface after 83 μm of material removal corresponding to a within workpiece non-uniformity (WIWNU) of

The effect of various HF-based etching processes on the laser damage resistance of scratched fused silica surfaces has been investigated. Conventionally polished and subsequently scratched fused silica plates were treated by submerging in various HF-based etchants (HF or NH4F:HF at various ratios and concentrations) under different process conditions (e.g., agitation frequencies, etch times, rinse conditions, and environmental cleanliness). Subsequently, the laser damage resistance (at 351 or 355 nm) of the treated surface was measured. The laser damage resistance was found to be strongly process dependent and scaled inversely with scratch width. The etching process was optimized to remove or prevent the presence of identified precursors (chemical impurities, fracture surfaces, and silica-based redeposit) known to lead to laser damage initiation. The redeposit precursor was reduced (and hence the damage threshold was increased) by: (1) increasing the SiF62− solubility through reduction in the NH4F concentration and impurity cation impurities, and (2) improving the mass transport of reaction product (SiF62−) (using high-frequency ultrasonic agitation and excessive spray rinsing) away from the etched surface. A 2D finite element crack-etching and rinsing mass transport model (incorporating diffusion and advection) was used to predict reaction product concentration. The predictions are consistent with the experimentally observed process trends. The laser damage thresholds also increased with etched amount (up to ∼30 μm), which has been attributed to: (1) etching through lateral cracks where there is poor acid penetration, and (2) increasing the crack opening resulting in increased mass transport rates. With the optimized etch process, laser damage resistance increased dramatically; the average threshold fluence for damage initiation for 30 μm wide scratches increased from 7 to 41 J/cm2, and the statistical probability of damage initiation at 12 J/cm2 of an ensemble of scratches decreased from ∼100 mm−1 of scratch length to ∼0.001 mm−1.

The effects of HF/NH4F, wet chemical etching on the morphology of individual surface fractures (indentations, scratches) and of an ensemble of surface fractures (ground surfaces) on fused silica glass has been characterized. For the individual surface fractures, a series of static or dynamic (sliding) Vickers and Brinnell indenters were used to create radial, lateral, Hertzian cone and trailing indentation fractures on a set of polished fused silica substrates which were subsequently etched. After short etch times, the visibility of both surface and subsurface cracks is significantly enhanced when observed by optical microscopy. This is attributed to the increased width of the cracks following etching, allowing for greater optical scatter at the fracture interface. The removal of material during etching was found to be isotropic except in areas where the etchant has difficulty penetrating or in areas that exhibit significant plastic deformation/densification. Isolated fractures continue to etch, but will never be completely removed since the bottom and top of the crack both etch at the same rate. The etching behavior of ensembles of closely spaced cracks, such as those produced during grinding, has also been characterized. This was done using a second set of fused silica samples that were ground using either fixed or loose abrasives. The resulting samples were etched and both the etch rate and the morphology of the surfaces were monitored as a function of time. Etching results in the formation of a series of open cracks or cusps, each corresponding to the individual fractures originally on the surface of the substrate. During extended etching, the individual cusps coalesce with one another, providing a means of reducing the depth of subsurface damage and the peak-to-valley roughness. In addition, the material removal rate of the ground surfaces was found to scale with the surface area of the cracks as a function of etch time. The initial removal rate for the ground surface was typically 3.5× the bulk etch rate. The evolving morphology of ground surfaces during etching was simulated using an isotropic finite difference model. This model illustrates the importance that the initial distributions of fracture sizes and spatial locations have on the evolution of roughness and the rate at which material is removed during the etching process. The etching of ground surfaces can be used during optical fabrication to convert subsurface damage into surface roughness thereby reducing the time required to produce polished surfaces that are free of subsurface damage.

The distribution and characteristics of surface cracks (i.e., sub-surface damage or scratching) on fused silica formed during grinding/polishing resulting from the addition of rogue particles in the base slurry has been investigated. Fused silica samples (10 cm diameter × 1 cm thick) were: (1) ground by loose abrasive grinding (alumina particles 9–30 μm) on a glass lap with the addition of larger alumina particles at various concentrations with mean sizes ranging from 15 to 30 μm, or (2) polished (using 0.5 μm cerium oxide slurry) on various laps (polyurethane pads or pitch) with the addition of larger rogue particles (diamond (4–45 μm), pitch, dust, or dried Ceria slurry agglomerates) at various concentrations. For the resulting ground samples, the crack distributions of the as-prepared surfaces were determined using a polished taper technique. The crack depth was observed to: (1) increase at small concentrations (>10 −4 fraction) of rogue particles; and (2) increase with rogue particle concentration to crack depths consistent with that observed when grinding with particles the size of the rogue particles alone. For the polished samples, which were subsequently etched in HF:NH 4 F to expose the surface damage, the resulting scratch properties (type, number density, width, and length) were characterized. The number density of scratches increased exponentially with the size of the rogue diamond at a fixed rogue diamond concentration suggesting that larger particles are more likely to lead to scratching. The length of the scratch was found to increase with rogue particle size, increase with lap viscosity, and decrease with applied load. At high diamond concentrations, the type of scratch transitioned from brittle to ductile and the length of the scratches dramatically increased and extended to the edge of the optic. The observed trends can be explained semi-quantitatively in terms of the time needed for a rogue particle to penetrate into a viscoelastic lap. The results of this study provide useful insights and ‘rules-of-thumb’ relating scratch characteristics observed on surfaces during optical glass fabrication to the characteristics of the rogue particles causing them and their possible source.

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.

This procedure describes a method for the fabrication of large-area and ultrathin free-standing polymer films. Typically, ultrathin films are prepared using either sacrificial layers, which may damage the film or affect its mechanical properties, or they are made on freshly cleaved mica, a substrate that is difficult to scale. Further, the size of ultrathin film is typically limited to a few square millimeters. In this method, we modify a surface with a polyelectrolyte that alters the strength of adhesion between polymer and deposition substrate. The polyelectrolyte can be shown to remain on the wafer using spectroscopy, and a treated wafer can be used to produce multiple films, indicating that at best minimal amounts of the polyelectrolyte are added to the film. The process has thus far been shown to be limited in scalability only by the size of the coating equipment, and is expected to be readily scalable to industrial processes. In this study, the protocol for making the solutions, preparing the deposition surface, and producing the films is described.

Fe-doped lithium sodium silicate glasses codoped with Sn and C to promote the Fe²⁺ 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.

The distribution and characteristics of surface cracking (i.e., sub-surface damage or SSD) formed during standard grinding processes have been measured on fused silica glass using a surface taper polishing technique. The measured SSD depth distributions are described by a single exponential followed by an asymptotic cutoff in depth. The observed surface cracks are characterized as near-surface lateral and deeper trailing indent type fractures (i.e., chatter marks). The length of the trailing indent is strongly correlated with a given grinding process. It is shown that only a small fraction of the abrasive particles are being mechanically loaded and causing fracture, and most likely it is the larger particles in the abrasive particle size distribution that bear the higher loads. The SSD depth increased with load and with a small amount of larger contaminant particles. Using a simple brittle fracture model for grinding, the SSD depth distribution has been related to the SSD length distribution to gain insight into ‘effective’ size distribution of particles participating in the fracture. Both the average crack length and the surface roughness were found to scale linearly with the maximum SSD depth. These relationships can serve as useful rules-of-thumb for non-destructively estimating SSD depth and for identifying the process that caused the SSD.

For experimental campaigns on the National Ignition Facility (NIF) to be successful, they must obtain useful data without causing unacceptable impact on the facility. Of particular concern is excessive damage to optics and diagnostic components. There are 192 fused silica main debris shields (MDS) exposed to the potentially hostile target chamber environment on each shot. Damage in these optics results either from the interaction of laser light with contamination and pre-existing imperfections on the optic surface or from the impact of shrapnel fragments. Mitigation of this second damage source is possible by identifying shrapnel sources and shielding optics from them. It was recently demonstrated that the addition of 1.1-mm thick borosilicate disposable debris shields (DDS) blocks the majority of debris and shrapnel fragments from reaching the relatively expensive MDS's. However, DDS's cannot stop large, fast moving fragments. We have experimentally demonstrated one shrapnel mitigation technique showing that it is possible to direct fast moving fragments by changing the source orientation, in this case a Ta pinhole array. Another mitigation method is to change the source material to one that produces smaller fragments. Simulations and validating experiments are necessary to determine which fragments can penetrate or break 1-3 mm thick DDS's. Three-dimensional modeling of complex target-diagnostic configurations is necessary to predict the size, velocity, and spatial distribution of shrapnel fragments. The tools we are developing will be used to assure that all NIF experimental campaigns meet the requirements on allowed level of debris and shrapnel generation.

The effects of residual polishing slurry on the surface topology of highly polished, Nd-doped meta-phosphate laser glasses are reported. Glass samples were pitched polished using cerium oxide or zirconium oxide slurry at different pHs and then washed by different methods that allowed varying amounts of residual slurry to ‘dry’ on the surface. Upon rewashing with water, some of the samples showed surface haze (scatter), which scaled with the amount of residual slurry. Profilometry measurements showed that the haze is the result of shallow surface pits (100 nm–20 μm wide × ∼15 nm deep). Chemical analyses of material removed during rewashing, confirmed the removal of glass components as well as the preferential removal of modifier ions (e.g., K 1+ and Mg 2+ ). The surface pits appear to result from reaction of the glass with condensed liquid at the slurry particle–glass interface that produces water-soluble phosphate products that dissolves away with subsequent water contact. Aggressive washing, to remove residual slurry immediately following polishing, can minimize surface haze on phosphate glasses. It is desirable to eliminate haze from glass used in high-peak-power lasers, since it can cause scatter-induced optical modulation that can cause damage to downstream optics.

The rate of subcritical crack growth in a metaphosphate Nd-doped laser glass was measured using the double-cleavage-drilled compression (DCDC) method. The crack velocity is reported as a function of stress intensity at temperatures ranging from 296 to 573 K and in nitrogen with water vapor pressures ranging from 40 Pa (0.3 mmHg) to 4.7 × 104 Pa (355 mmHg). The measured crack velocities follow region I, II, and III behavior similar to that reported for silicate glasses. A chemical and mass-transport-limited reaction rate model explains the behavior of the data except at high temperatures and high water vapor pressures where crack tip blunting is observed. Blunting is characterized by an arrest in the crack growth followed by the inability to reinitiate slow crack growth at higher stresses. A dynamic crack tip blunting mechanism is proposed to explain the deviation from the reaction rate model.

Various silica sols (varying in surface chemistry and solvent) were synthesized by the Stober process and then subsequently coated on substrates at various humidities. For ethanol-based sols, films prepared by spin or dip coating at low humidities had a higher refractive index, lower thickness, and greater microcracking than those prepared at high humidities. The change in film properties followed an abrupt, instead of a gradual, change with humidity. This change in film microstructure can be explained by the ability/inability of capillary condensed liquid in the micropores of the colloid to evaporate prior to achieving full film strength and hence allowing the micropores to collapse. The magnitude of the shrinkage and the relative humidity at which the pores collapsed were found to depend on the colloid surface chemistry and the coating method. In contrast to the ethanol-based sols, humidity during spin coating had a negligible effect on film properties for sec-butanol and decane-based sols. This is likely due to the lower vapor pressure and/or lower water solubility of these solvents such that the pores in the latter stages of drying the films did not contain much water. Understanding this behavior has been important for improving the performance and process repeatability of using these films as anti-reflective coatings in high-peak-power laser systems.