Salmaan Baxamusa

High fluence laser damage precursors and their mitigation in fused silica

The use of any optical material is limited at high fluences by laser-induced damage to optical surfaces. In many optical materials, the damage results from a series of sources which initiate at a large range of fluences and intensities. Much progress has been made recently eliminating silica surface damage due to fracture-related precursors at relatively low fluences (i.e., less than 10 J/cm(2), when damaged by 355 nm, 5 ns pulses). At higher fluence, most materials are limited by other classes of damage precursors which exhibit a strong threshold behavior and high areal density (>10(5) cm(-2)); we refer to these collectively as high fluence precursors. Here, we show that a variety of nominally transparent materials in trace quantities can act as surface damage precursors. We show that by minimizing the presence of precipitates during chemical processing, we can reduce damage density in silica at high fluence by more than 100 times while shifting the fluence onset of observable damage by about 7 J/cm(2). A better understanding of the complex chemistry and physics of cleaning, rinsing, and drying will likely lead to even further improvements in the damage performance of silica and potentially other optical materials.

Enhanced Delamination of Ultrathin Free-Standing Polymer Films via Self-Limiting Surface Modification

Free-standing polymer thin films are typically fabricated using a sacrificial underlayer (between the film and its deposition substrate) or overlayer (on top of the film to assist peeling) in order to facilitate removal of the thin film from its deposition substrate. We show the direct delamination of extraordinarily thin (as thin as 8 nm) films of poly(vinyl formal) (PVF), polystyrene, and poly(methyl methacrylate). Large (up to 13 cm diameter) films of PVF could be captured on wire supports to produce free-standing films. By modifying the substrate to lower the interfacial energy resisting film-substrate separation, the conditions for spontaneous delamination are satisfied even for very thin films. The substrate modification is based on the electrostatic adsorption of a cationic polyelectrolyte. Eliminating the use of sacrificial materials and instead relying on naturally self-limiting adsorption makes this method suitable for large areas. We have observed delamination of films with aspect ratios (ratio of lateral dimension between supports to thickness) of 10(7) and have captured dry, free-standing films with aspect ratios >10(6). Films with an aspect ratio of 10(5) can bear loads up to 10(6) times the mass of the film itself. The presence of the adsorbed layer can be observed using X-ray photoelectron spectroscopy, and this layer is persistent through multiple uses. In the system studied, elimination of sacrificial materials leads to an enhancement in the failure strength of the free-standing thin film. The robustness, persistence, and the self-optimizing nature distinguish this method from various fabrication methods utilizing sacrificial materials and make it a potentially scalable process for the fabrication of ultrathin free-standing or transferrable films for filtration, MEMS, or tissue engineering applications.

Mitigation of organic laser damage precursors from chemical processing of fused silica

Increases in the laser damage threshold of fused silica have been driven by the successive elimination of near-surface damage precursors such as polishing residue, fractures, and inorganic salts. In this work, we show that trace impurities in ultrapure water used to process fused silica optics may be responsible for the formation of carbonaceous deposits. We use surrogate materials to show that organic compounds precipitated onto fused silica surfaces form discrete damage precursors. Following a standard etching process, solvent-free oxidative decomposition using oxygen plasma or high-temperature thermal treatments in air reduced the total density of damage precursors to as low as <50 cm(-2). Finally, we show that inorganic compounds are more likely to cause damage when they are tightly adhered to a surface, which may explain why high-temperature thermal treatments have been historically unsuccessful at removing extrinsic damage precursors from fused silica.

Silica laser damage mechanisms, precursors, and their mitigation

Controlling laser damage is essential for reliable and cost-effective operation of high energy laser systems. We will review important optical damage precursors in silica up to UV fluences as high as 45J/cm2 (3ns) along with studies of the damage mechanisms involved and processes to mitigate damage precursors. We have found that silica surface damage is initiated by nano-scale precursor absorption followed by thermal coupling to the silica lattice and formation of a laser-supported absorption front. Residual polishing compound and defect layers on fracture surfaces are primarily responsible for optic damage below about 10J/cm2; they can be mitigated by an optimized oxide etch processes. At fluences above about 10J/cm2, precipitates of trace impurities are responsible for damage; they can be mitigated by eliminating the chances of impurity precipitation following wet chemical processing. Using these approaches, silica damage densities can be reduced by many orders of magnitude allowing large increases in the maximum operating fluences these optics see.

Surface oxygen micropatterns on glow discharge polymer targets by photo irradiation

Recent simulations predict surface oxygen may be a significant source of disruptive perturbations in the implosion process of glow-discharge polymers (GDP) ablators at the National Ignition Facility. GDP material held in ambient atmospheric conditions showed an increase in mass when stored in light transparent containers, which suggests that photo exposure is a driving force for oxygen absorption. To investigate if surface oxygen is a contributing factor of disruptive perturbations during implosion, a method to imprint a periodic micropattern of oxygen on the surface of GDP was developed and used to fabricate a flat sample for empirical testing. Photo exposure using collimated blue light was used to generate micropatterns of surface oxygen on the GDP material. The periodic oxygen micropattern was confirmed by secondary ion mass spectrometry (SIMS) and energy dispersive spectroscopy. A SIMS depth profile showed the atomic percent of oxygen ranged from 8 at. % near the surface to 1 at. % at a depth of 2 μm ...

Update 2015 on Target Fabrication Requirements for NIF Layered Implosions, with Emphasis on Capsule Support and Oxygen Modulations in GDP

Abstract Experiments and analysis in the 3 years since the 2012 Target Fabrication Meeting have resulted in significant improvement in understanding of the requirements for high-performance layered implosions. Three issues have been identified that significantly degrade the performance of the implosions as they were originally configured for National Ignition Facility experiments: capsule support system, time-dependent radiation asymmetry, and transverse oxygen nonuniformity in the glow discharge polymer (GDP) ablator. Analyses suggest that the shortfalls in these three areas can explain the degraded performance of the National Ignition Campaign implosions. We present the status of work toward curing these three problems in the standard GDP ablator/gold hohlraum configuration as they affect target fabrication priorities. We also summarize the prospects for alternate ablators that might reduce these degradation mechanisms.

Fabrication of Large-area Free-standing Ultrathin Polymer Films

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.

Supercooling of Hydrogen on Template Materials to Deterministically Seed Ignition-Quality Solid Fuel Layers

Abstract 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 results show high supercooling (>100 mK) for most metallic, covalent, and ionic solids, and low supercooling (<100 mK) for van der Waals (vdW) solids. We attribute the low supercooling of vdW solids to the weak interaction of the substrate and hydrogen. Highly ordered pyrolytic graphite showed the lowest supercooling among materials that are solid at room temperature, but did not exhibit a templating effect within a fill-tube and capsule assembly.

Update 2017 on Target Fabrication Requirements for High-Performance NIF Implosion Experiments

Abstract Experiments and analysis in the 2 years since the 2015 Target Fabrication Meeting have resulted in further evolution of the requirements for high-performance layered implosions. This paper is a status update on the experimental program and supporting modeling, with emphasis on the implications for fabrication requirements. Previous work on the capsule support has continued, with various other support options being explored in experiments and modeling. Work also continues on ablator composition nonuniformities, with important new results from CH experiments on Omega, and the first three-dimensional X-ray transmission measurements of Be capsules on the National Ignition Facility. Work on hohlraums continues to include near-vacuum hohlraums and U hohlraums without a gold lining. Overall, the understanding that has been achieved, along with the progress in fabrication technology, represents good continuing progress toward the goal of fusion in the laboratory.

Ultralow stress, thermally stable cross-linked polymer films of polydivinylbenzene (PDVB)

Although closely related to polystyrene, poly(divinylbenzene) (PDVB) has found limited utility due to the difficulties associated with its synthesis. As a highly cross-linked polymer, PDVB is infusible and insoluble and thus nearly impossible to shape into films by either melt or solvent-based processes. Here, we report the initiated chemical vapor deposition (iCVD) of nearly stress-free, highly transparent, free-standing films of PDVB up to 25 μm thick. Films initially grow under tensile intrinsic stress but become more compressive with thickness and eventually converge to zero-stress values once they reach ≥10 μm in thickness. Upon initial heating, the evaporative loss of unreacted monomer left in the polymer matrix induces between 35 and 45 MPa of tensile stress in the films. Afterward, subsequent heating cycles induce reversible stress and film expansion behaviors. We estimate the degree of cross-linking to be 44%, resulting in high thermal stability (up to 300 °C) and mechanical stiffness (Youngs modulus of 5.2 GPa). The low stress combined with high cross-linking makes iCVD PDVB an excellent candidate for protective coatings in harsh environments.