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The generation of coherent light pulses in the extreme ultraviolet (XUV) spectral region with attosecond pulse durations constitutes the foundation of the field of attosecond science. Twenty years after the first demonstration of isolated attosecond pulses, they continue to be a unique tool enabling the observation and control of electron dynamics in atoms, molecules and solids. It has long been identified that an increase in the repetition rate of attosecond light sources is necessary for many applications in atomic and molecular physics, surface science, and imaging. Although high harmonic generation (HHG) at repetition rates exceeding 100 kHz, showing a continuum in the cut-off region of the XUV spectrum was already demonstrated in 2013, the number of photons per pulse was insufficient to perform pulse characterisation via attosecond streaking, let alone to perform a pump-probe experiment. Here we report on the generation and full characterisation of XUV attosecond pulses via HHG driven by near-single-cycle pulses at a repetition rate of 100 kHz. The high number of 10^6 XUV photons per pulse on target enables attosecond electron streaking experiments through which the XUV pulses are determined to consist of a dominant single attosecond pulse. These results open the door for attosecond pump-probe spectroscopy studies at a repetition rate one or two orders of magnitude above current implementations., Comment: 27 Pages, 4 figures, supplementary information

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 $\times 10^{-4}$, low enough to provide almost a factor of two improvement 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 and Virgo detectors.

High finesse optical cavities of current interferometric gravitational-wave detectors are significantly limited in sensitivity by laser quantum noise and coating thermal noise. The thermal noise is associated with internal energy dissipation in the materials that compose the test masses of the interferometer. Our understanding of how the internal friction is linked to the amorphous material structure is limited due to the complexity of the problem and the lack of studies that span over a large range of materials. We present a systematic investigation of amorphous metal oxide and Ta$_2$O$_5$-based mixed oxide coatings to evaluate their suitability for low Brownian noise experiments. It is shown that the mechanical loss of metal oxides is correlated to their amorphous morphology, with continuous random network materials such as SiO$_2$ and GeO$_2$ featuring the lowest loss angles. We evaluated different Ta$_2$O$_5$-based mixed oxide thin films and studied the influence of the dopant in the optical and elastic properties of the coating. We estimated the thermal noise associated with high-reflectance multilayer stacks that employ each of the mixed oxides as the high index material. We concluded that the current high index material of TiO$_2$-doped Ta$_2$O$_5$ is the optimal choice for reduced thermal noise among Ta$_2$O$_5$-based mixed oxide coatings with low dopant concentrations.

Glasses are nonequilibrium solids with properties highly dependent on their method of preparation. In vapor-deposited molecular glasses, structural organization could be readily tuned with deposition rate and substrate temperature. Herein, we show the atomic arrangement of strong network forming GeO2 glass is modified at medium range (< 2 nm) through vapor deposition at elevated temperatures. Raman spectral signatures distinctively show the population of 6-membered GeO4 rings increases at elevated substrate temperatures. Deposition near the glass transition temperature is more efficient than post-growth annealing in modifying atomic structure at medium range. The enhanced medium range organization correlates with reduction of the room temperature internal friction. Identifying the microscopic origin of room temperature internal friction in amorphous oxides is paramount to design the next generation interference coatings for mirrors of the end test masses of gravitational wave interferometers, in which the room temperature internal friction is a main source of noise limiting their sensitivity.

Internal friction in oxide thin films imposes a critical limitation to the sensitivity and stability of ultra-high finesse optical cavities for gravitational wave detectors. Strategies like doping or creating nanolaminates are sought to introduce structural modifications that reduce internal friction. This work describes an investigation of the morphological changes SiO2/Ta2O5 and TiO2/Ta2O5 nanolaminates undergo with annealing and their impact on room temperature internal friction. It is demonstrated that thermal treatment results in a reduction of internal friction in both nanolaminates, but through different pathways. In the SiO2/Ta2O5 nanolaminate, which layers remain intact after annealing, the total reduction in internal friction follows the reduction in the composing SiO2 and Ta2O5 layers. Instead, interdiffusion initiated by annealing at the interface of the TiO2/Ta2O5 nanolaminate and the formation of a mixed phase dictate a more significant reduction in internal friction to ~ 2.6 * 10-4, a value lower than any other Ta2O5 mixture coating with similar cation concentration.

The genomics approach to materials, heralded by increasingly accurate density functional theory (DFT) calculations conducted on thousands of crystalline compounds, has led to accelerated material discovery and property predictions. However, so far amorphous materials have been largely excluded from this as these systems are notoriously difficult to simulate. Here we study amorphous Ta$_2$O$_5$ thin films mixed with Al$_2$O$_3$, SiO$_2$, Sc$_2$O$_3$, TiO$_2$, ZnO, ZrO$_2$, Nb$_2$O$_5$ and HfO$_2$ to identify their crystalline structure upon post-deposition annealing in air both experimentally and with simulations. Using the Materials Project open database, phase diagrams based on DFT calculations are constructed for the mixed oxide systems and the annealing process is evaluated via grand potential diagrams with varying oxygen chemical potential. Despite employing calculations based on crystalline bulk materials, the predictions agree well with the experimentally observed crystallized phases of the amorphous films. Only in two cases the database leads to incorrect predictions: in TiO$_2$-doped Ta$_2$O$_5$ because it does not contain a ternary compound found experimentally, and in Sc$_2$O$_3$-doped Ta$_2$O$_5$ because DFT overestimates the formation enthalpy difference between Sc$_2$O$_3$ and Ta$_2$O$_5$ and thus does not reproduce observed oxygen competition effects. In the absence of ternary phases, the dopant acts as an amorphizer agent increasing the thermal stability of Ta$_2$O$_5$. These results show that DFT calculations can be applied for the prediction of crystallized structures of annealed amorphous materials. This could pave the way for accelerated \textit{in silico} material discovery and property predictions using the powerful genomic approach for amorphous oxide coatings employed in a wide range of applications such as optical coatings, energy storage and electronic devices.

Amorphous oxide thin films play a fundamental role in state-of-the art interferometry experiments, such as gravitational wave detectors where these films compose the high reflectance mirrors of end and input masses. The sensitivity of these detectors is affected by thermal noise in the mirrors with its main source being the mechanical loss of the high index layers. These thermally driven fluctuations are a fundamental limit to optical interferometry experiments and there is a pressing need to understand the underlying processes that lead to mechanical dissipation in materials at room temperature. Two strategies are known to lower the mechanical loss: employing a mixture of Ta$_2$O$_5$ with $\approx$ 20\% of TiO$_2$ and post-deposition annealing, but the reasons behind this are not completely understood. In this work, we present a systematic study of the structural and optical properties of ion beam sputtered TiO$_2$-doped Ta$_2$O$_5$ films as a function of the annealing temperature. We show for the first time that low mechanical loss is associated with a material morphology that consists of nanometer sized Ar-rich bubbles embedded into an atomically homogeneous mixed titanium-tantalum oxide. When the Ti cation ratio is high, however, phase separation occurs in the film which leads to increased mechanical loss. These results indicate that for designing low mechanical loss mixed oxide coatings for interferometry applications it would be beneficial to identify materials with the ability to form ternary compounds while the dopant ratio needs to be kept low to avoid phase separation.

Brownian thermal noise is a limiting factor for the sensitivity of many high precision metrology applications, among other gravitational-wave detectors. The origin of Brownian noise can be traced down to internal friction in the amorphous materials that are used for the high reflection coatings. To properly characterize the internal friction in an amorphous material, one needs to consider separately the bulk and shear losses. In most of previous works the two loss angles were considered equal, although without any first principle motivation. In this work we present a method that can be used to extract the material bulk and shear loss angles, based on current state-of-the-art coating ring-down measurement systems. We also show that for titania-doped tantala, a material commonly used in gravitational-wave detector coatings, the experimental data strongly favor a model with two different and distinct loss angles, over the simpler case of one single loss angle.

Many experiments in attosecond science will benefit from attosecond pulses at high repetition rates with sufficient photon flux for pump-probe experiments. We use 7fs, 800nm pulses from a non-collinear optical parametric chirped pulse amplification (NOPCPA) laser system to generate few-pulse attosecond pulse trains (APTs) in the extreme ultraviolet (XUV) at a repetition rate of 100kHz. The pulse trains have been fully characterized by recording FROG-CRAB (Frequency-Resolved Optical Gating for Complete Reconstruction of Attosecond Bursts) traces with a velocity map imaging spectrometer., Comment: 7 pages, 4 figures, submitted version