Influence of defects on the femtosecond laser damage resistance of multilayer dielectric gratings.

Multilayer dielectric (MLD) gratings with high diffraction efficiency and a high laser-induced damage (LID) threshold for pulse compressors are key to scaling the peak and average power of chirped pulse amplification lasers. However, surface defects introduced by manufacturing, storage, and handling processes can reduce the LID resistance of MLD gratings and impact the laser output. The underlying mechanisms of such defect-initiated LID remain unclear, especially in the femtosecond regime. In this Letter, we model dynamic processes in interactions of a 20-fs near-infrared (NIR) laser pulse and a MLD grating design in the presence of cylindrically symmetrical nodules and particle contaminants and cracks at the surface. Utilizing a dynamic model based on a 2D finite difference in time domain (FDTD) field solver coupled with photoionization, electron collision, and refractive index modification, we study the simulation results for the damage site distribution initiated by defects of various types and sizes and its impact on the LID threshold of the grating design.

Isotopic Heterogeneity Imaged in a Uranium Fuel Pellet with Extreme Ultraviolet Laser Ablation and Ionization Time-of-Flight Mass Spectrometry.

We use extreme ultraviolet laser ablation and ionization time-of-flight mass spectrometry (EUV TOF) to map uranium isotopic heterogeneity at the nanoscale (≤100 nm). Using low-enriched uranium fuel pellets that were made by blending two isotopically distinct feedstocks, we show that EUV TOF can map the 235U/238U content in 100 nm-sized pixels. The two-dimensional (2D) isotope maps reveal U ratio variations in sub-microscale to ≥1 µm areas of the pellet that had not been fully exposed by microscale or bulk mass spectrometry analyses. Compared to the ratio distribution measured in a homogeneous U reference material, the ratios in the enriched pellet follow a ∼3× wider distribution. These results indicate U heterogeneity in the fuel pellet from incomplete blending of the different source materials. EUV TOF results agree well with those obtained on the same enriched pellets by nanoscale secondary ionization mass spectrometry (NanoSIMS), which reveals a comparable U isotope ratio distribution at the same spatial scale. EUV TOF's ability to assess and map isotopic heterogeneity at the nanoscale makes it a promising tool in fields such as nuclear forensics, geochemistry, and biology that could benefit from uncovering sub-microscale sources of chemical modifications.

Low Mechanical Loss TiO_{2}:GeO_{2} Coatings for Reduced Thermal Noise in Gravitational Wave Interferometers.

The sensitivity of current and planned gravitational wave interferometric detectors is limited, in the most critical frequency region around 100 Hz, by a combination of quantum noise and thermal noise. The latter is dominated by Brownian noise: thermal motion originating from the elastic energy dissipation in the dielectric coatings used in the interferometer mirrors. The energy dissipation is a material property characterized by the mechanical loss angle. We have identified mixtures of titanium dioxide (TiO_{2}) and germanium dioxide (GeO_{2}) that show internal dissipations at a level of 1×10^{-4}, low enough to provide improvement of almost a factor of 2 on the level of Brownian noise with respect to the state-of-the-art materials. We show that by using a mixture of 44% TiO_{2} and 56% GeO_{2} in the high refractive index layers of the interferometer mirrors, it would be possible to achieve a thermal noise level in line with the design requirements. These results are a crucial step forward to produce the mirrors needed to meet the thermal noise requirements for the planned upgrades of the Advanced LIGO (Laser Interferometer Gravitational-Wave Observatory) and Virgo detectors.

Single-shot large field of view Fourier transform holography with a picosecond plasma-based soft X-ray laser.

It is challenging to obtain nanoscale resolution images in a single ultrafast shot because a large number of photons, greater than 1011, are required in a single pulse of the illuminating source. We demonstrate single-shot high resolution Fourier transform holography over a broad 7 µm diameter field of view with ∼ 5 ps temporal resolution. The experiment used a plasma-based soft X-ray laser operating at 18.9 nm wavelength with nearly full spatial coherence and close to diffraction-limited divergence implemented utilizing a dual-plasma amplifier scheme. A Fresnel zone plate with a central aperture is used to efficiently generate the object and reference beams. Rapid numerical reconstruction by a 2D Fourier transform allows for real-time imaging. A half-pitch spatial resolution of 62 nm was obtained. This single-shot nanoscale-resolution imaging technique will allow for real-time ultrafast imaging of dynamic phenomena in compact setups.

Demonstration of a kilowatt average power, 1 J, green laser.

A λ=515nm laser generating joule-level pulses at 1 kHz repetition rate was demonstrated by frequency doubling 1.2 J, 2 ns temporally shaped square pulses from a cryogenically cooled Yb:YAG laser in an LBO crystal. A doubling efficiency of 78% resulted in 0.94 J second-harmonic pulses at 1 kHz. The unconverted light interacted with a second LBO crystal to generate >100mJ second-harmonic pulses to reach a total green average power of 1.04 kW. A conversion efficiency of 89% was achieved for 0.58 J green pulses at 1 kHz. These results open the possibility to pump high energy femtosecond lasers at kilohertz repetition rates.

Laser induced damage in coatings for cryogenic Yb:YAG active mirror amplifiers.

We report results of a study of the laser induced damage threshold (LIDT) behavior of ion beam sputtered HfO2/SiO2 multilayer coatings on Yb:YAG using 1-on-1 and N-on-1 test protocols. The tests were conducted at ambient, vacuum, and cryogenic conditions using 280 ps pulses at λ=1030nm. The 1-on-1 LIDT of antireflection (AR) stacks is found to be only slightly reduced under vacuum and cryogenic conditions, while that of high reflectivity (HR) stacks is insensitive to environmental conditions within the uncertainty of the measurements. Cryogenic N-on-1 tests show the LIDT of the HR coating is almost the same as in the 1-on-1 tests. Conversely, the cryogenic N-on-1 test of the AR coating shows damage at ∼13J/cm2, a fluence lower than the 20.4J/cm2 of 1-on-1 tests. The AR damage behavior is found to be affected by imperfections at the Yb:YAG surface. These findings show that high surface quality is required to increase energy extraction from active mirror laser amplifiers.

Comparison of damage and ablation dynamics of multilayer dielectric films initiated by few-cycle pulses versus longer femtosecond pulses.

The importance of high intensity few- to single-cycle laser pulses for applications such as intense isolated attosecond pulse generation is constantly growing, and with the breakdown of the monochromatic approximation in field ionization models, the few-cycle pulse (FCP) interaction with solids near the damage threshold has ushered a new paradigm of nonperturbative light-matter interaction. In this Letter, we systematically study and contrast how femtosecond laser-induced damage and ablation behaviors of SiO2/HfO2-based reflective multilayer dielectric thin film systems vary between FCP and 110 fs pulses. With time-resolved surface microscopy and ex situ analysis, we show that there are distinct differences in the interaction depending on the pulse duration, specifically in the "blister" morphology formation at lower fluences (damage) as well as in the dynamics of debris formation at higher fluences (ablation).

1.1 J Yb:YAG picosecond laser at 1 kHz repetition rate.

We demonstrate the generation of 1.1 J pulses of picosecond duration at 1 kHz repetition rate (1.1 kW average power) from a diode-pumped chirped pulse amplification Yb:YAG laser. The laser employs cryogenically cooled amplifiers to generate λ=1030nm pulses with average power of up to 1.26 kW prior to compression with excellent beam quality. Pulses are compressed to 4.5 ps duration with 90% efficiency. This compact picosecond laser will enable a variety of applications that require high energy ultrashort pulses at kilohertz repetition rates.

Ultra-low stress SiO2 coatings by ion beam sputtering deposition.

High mechanical stress can affect the performance of multilayer thin film optical coatings, causing wavefront aberrations. This is particularly important if the multilayer stack is deposited onto thin substrates, such as those used in adaptive optics. Stress in thin film coatings is dependent on the deposition process, and ion beam sputtering (IBS) thin films are known to have high compressive stress. In the present work, we show that stress in IBS $ {{\rm SiO}_2} $SiO2 thin films can be reduced from 490 MPa to 48 MPa using high-energy $ {{\rm O}_2} $O2 assist ion bombardment during deposition while maintaining high optical quality. A comparison of the reduction of stress in $ {{\rm SiO}_2} $SiO2 deposited from oxide and metal targets is provided.

Growth and characterization of Sc2O3 doped Ta2O5 thin films.

We present the optical and structural characterization of films of Ta2O5, Sc2O3, and Sc2O3 doped Ta2O5 with a cation ratio around 0.1 grown by reactive sputtering. The addition of Sc2O3 as a dopant induces the formation of tantalum suboxide due to the "oxygen getter" property of scandium. The presence of tantalum suboxide greatly affects the optical properties of the coating, resulting in higher absorption loss at λ=1064nm. The refractive index and optical band gap of the mixed film do not correspond to those of a mixture of Ta2O5 and Sc2O3, given the profound structural modifications induced by the dopant.

Investigation of laser annealing mechanisms in thin film coatings by photothermal microscopy.

We study the evolution of the absorptance of amorphous metal oxide thin films when exposed to intense CW laser radiation measured using a photothermal microscope. The evolution of the absorptance is characterized by a nonexponential decay. Different models that incorporate linear and nonlinear absorption, free carrier absorption, and defect diffusion are used to fit the results, with constraints imposed on the fit parameters to scale with power and intensity. The model that best fits is that two types of interband defects are passivated independently, one by a one-photon process and the other one by a two-photon process.

Characterization of absorptance homogeneity in thin-film coatings for high-power lasers by thermal lensing microscopy.

A focus error method photothermal microscope was designed for the characterization of absorptance homogeneity in thin-film coatings for high-power lasers. The technique relies on the detection of the thermal lens induced by the local absorption of a light power focused laser. The detailed design of the instrument is presented. The resolution of the system is better than 0.1 ppm and allows the realization of spatial sweeps and even measurements of the evolution of absorption as a function of time with a spatial resolution of 1 µm. These capabilities allow the location of defects and their characterization.

Depth-Profiling Microanalysis of CoNCN Water-Oxidation Catalyst Using a λ = 46.9 nm Plasma Laser for Nano-Ionization Mass Spectrometry.

Nanoscale depth profiling analysis of a CoNCN-coated electrode for water oxidation catalysis was carried out using table-top extreme ultraviolet (XUV) laser ablation time-of-flight mass spectrometry. The self-developed laser operates at λ = 46.9 nm and represents factor of 4 reduction in wavelength with respect to the 193 nm excimer laser. The reduction of the wavelength is an alternative approach to the reduction of the pulse duration, to enhance the ablation characteristics and obtain smaller quasi-nondestructive ablation pits. Such a XUV-laser ablation method allowed distinguishing different composite components of the catalyst-Nafion blend, used to modify a screen-printed carbon electrode surface. Chemical information was extracted by fragment assignment and relative amplitude analysis of the mass spectrometry peaks. Pure Nafion and the exposed carbon substrate were compared as references. Material specific fragments were clearly identified by the detected nonoverlapping mass-to-charge peaks of Nafion and CoNCN. Three dimensional mapping of relevant mass peak amplitudes was used to determine the lateral distribution and to generate depth profiles from consecutive laser pulses. Evaluating the profiles of pristine electrodes gave insight into fragmentation behavior of the catalyst in a functional ionomer matrix and comparison of post-catalytic electrodes revealed spots of thin localized Co residues.

0.85 PW laser operation at 3.3 Hz and high-contrast ultrahigh-intensity λ = 400 nm second-harmonic beamline.

We demonstrate the generation of 0.85 PW, 30 fs laser pulses at a repetition rate of 3.3 Hz with a record average power of 85 W from a Ti:sapphire laser. The system is pumped by high-energy Nd:glass slab amplifiers frequency doubled in LiB3O5 (LBO). Ultrahigh-contrast λ=400 nm femtosecond pulses were generated in KH2PO4 (KDP) with >40% efficiency. An intensity of 6.5×1021 W/cm2 was obtained by frequency doubling 80% of the available Ti:sapphire energy and focusing the doubled light with an f/2 parabola. This laser will enable highly relativistic plasma experiments to be conducted at high repetition rate.

Strategies to increase laser damage performance of Ta2O5/SiO2 mirrors by modifications of the top layer design.

Ta2O5/SiO2 high reflection (HR) interference coatings for λ∼1 µm offer superior performance at high irradiance conditions. However, these coatings are not good candidates for high peak power conditions in comparison to HfO2/SiO2 multilayer stacks. Here we show that the modification of the top layers design of a quarter wave Ta2O5/SiO2 high reflector leads to 4-5 fold increase in the laser damage fluence compared to a quarter wave (Ta2O5/SiO2)15 when tested at λ=1.03 µm using pulse durations of 0.19 and 4 ns and peak power densities of 43.5 and 216 GW/cm2. One of the designs achieved a laser damage threshold fluence of 174 J/cm2 at 4 ns, which is 10% higher than that of a HfO2/SiO2 quarter wave design.

1 J, 0.5 kHz repetition rate picosecond laser.

We report the demonstration of a diode-pumped chirped pulse amplification Yb:YAG laser that produces λ=1.03 µm pulses of up to 1.5 J energy compressible to sub-5 ps duration at a repetition rate of 500 Hz (750 W average power). Amplification to high energy takes place in cryogenically cooled Yb:YAG active mirrors designed for kilowatt average power laser operation. This compact laser system will enable new advances in high-average-power ultrashort-pulse lasers and high-repetition-rate tabletop soft x-ray lasers. As a first application, the laser was used to pump a 400 Hz λ=18.9 nm laser.

Relative intersection of confidence intervals rule for sharper restoration of soft x-ray images.

We present a novel method for restoration of images of nanostructures obtained with a soft-ray microscope that uses a 46.9 nm soft x-ray laser microscope for illumination. To suppress the noise and to preserve the image sharpness, we develop a method based on pixel adaptive zero-order modeling of the observed object. Neighboring areas of each pixel are selected using the relative intersection of confidence intervals rule and used for restoration. Due to the non-uniform distribution of noise in the images, we use robust spatial noise modeling. The method provides sharp restored images-sharper than competitive approaches. The sharpness is measured using local phase coherence in the complex wavelet transform domain and shows visible improvement of the novel method.

Restoration of soft x-ray laser images of nanostructures.

We present advanced techniques for the restoration of images obtained by soft x-ray laser microscopy. We show two methods. One method is based on adaptive thresholding, while the other uses local Wiener filtering in the wavelet domain to achieve high noise gains. These wavelet based denoising techniques are improved using spatial noise modeling. The accurate noise model is built up from two consecutive images of the object and respective background images. To our knowledge, the results of both proposed approaches over-perform competitive methods. The analysis is robust to enable image acquisition with significantly lower exposure times, which is critical in samples that are sensitive to radiation damage as is the case of biological samples imaged by SXR microscopy.

High laser-resistant multilayer mirrors by nodular defect planarization [invited].

Substrate defect planarization has been shown to increase the laser resistance of 1053 nm mirror coatings to greater than 100 J/cm2, an increase of 20-fold, when tested with 10 ns laser pulses. Substrate surface particles that are overcoated with optical interference mirror coatings become nodular defects, which behave as microlenses intensifying light into the defect structure. By a discrete process of angle-dependent ion etching and unidirectional ion-beam deposition, substrate defects can be reduced in cross-sectional area by over 90%.