Dynamics of electronic excitations involved in laser-induced damage in HfO2 and SiO2 films.

The dynamics of electron excitations associated with the initiation of laser-induced damage in hafnia and silica monolayer films are investigated using time-resolved damage testing involving a pair of 0.7 ps pulses with adjustable delay and laser pulse fluences. Results in hafnia indicate that the relaxation profile depends on the pump-pulse fluence (initial excitation), and as a result, it exhibits an effective lifetime that is variable. Analogous experiments in silica form two different types of damage morphologies that are observed on different ranges of delay times.

Mechanisms of picosecond laser-induced damage in common multilayer dielectric gratings.

The modifications of multilayer dielectric (MLD) gratings arising from laser-induced damage using 0.6-ps and 10-ps laser pulses at 1053 nm are investigated to better understand the damage-initiation mechanisms. Upon damage initiation, sections of the affected grating pillars are removed, thereby erasing the signature of the underlying mechanisms of laser damage. To address this issue, we performed paired studies using macroscopic grating-like features that are 5 mm in width to reveal the laser-damage morphology of the different grating sections: pillar side wall, sole, and pillar top. The results suggest that, similarly to MLD coatings, there are two damage-initiation mechanisms corresponding to the different pulse durations.

Mechanisms of laser-induced damage in absorbing glasses with nanosecond pulses.

The propagation of 355-nm, nanosecond pulses in absorbing glasses is investigated for the specific case examples of the broadband absorbing glass SuperGrey and the Ce3+-doped silica glass. The study involves different laser irradiation conditions and material characterization methods to capture the transient material behaviors leading to laser-induced damage. Two damage-initiation mechanisms were identified: (1) melting of the surface as a result of increased temperature; and (2) self-focusing caused by a transient change in the index of refraction. Population of excited states greatly affects both mechanisms by increasing the transient absorption cross section via excited-state absorption and introducing a change of the refractive index to support the formation of graded-index lensing and self-focusing of the beam inside the material. The governing damage-initiation mechanism depends on the thermodynamic properties of the host glass, the electronic structure characteristics of the doped ion, and the laser-spot size.

Influence of absorption-edge properties on subpicosecond intrinsic laser-damage threshold at 1053 nm in hafnia and silica monolayers.

Owing to their relatively high resistance to laser-induced damage, hafnia and silica are commonly used in multilayered optical coatings in high-power laser facilities as high- and low-refractive-index materials, respectively. Here, we quantify the laser-induced-damage threshold (LIDT) at 1053 nm in the short-pulse regime of hafnia and silica monolayers deposited by different fabrication methods, including electron-beam evaporation, plasma ion-assisted deposition and ion-assisted deposition. The results demonstrate that nominally identical coatings fabricated by different deposition techniques and/or vendors can exhibit significantly different damage thresholds. A correlation of the LIDT performance of each material with its corresponding absorption edge is investigated. Our analysis indicates a weak correlation between intrinsic LIDT and the optical gap of each material (Tauc gap) but a much better correlation when considering the spectral characteristics in the Urbach tail spectral range. Spectrophotometry and photothermal absorption were used to provide evidence of the correlation between the strength of the red-shifted absorption tail and reduced LIDT at 1053 nm.

Optical properties of oxygen vacancies in HfO2 thin films studied by absorption and luminescence spectroscopy.

Hafnium oxide thin films with varying oxygen content were investigated with the goal of finding the optical signature of oxygen vacancies in the film structure. It was found that a reduction of oxygen content in the film leads to changes in both, structural and optical characteristics. Optical absorption spectroscopy, using nanoKelvin calorimetry, revealed an enhanced absorption in the near-ultraviolet (near-UV) and visible wavelength ranges for films with reduced oxygen content, which was attributed to mid-gap electronic states of oxygen vacancies. Absorption in the near-infrared was found to originate from structural defects other than oxygen vacancy. Luminescence generated by continuous-wave 355-nm laser excitation in e-beam films showed significant changes in the spectral profile with oxygen reduction and new band formation linked to oxygen vacancies. The luminescence from oxygen-vacancy states was found to have microsecond-scale lifetimes when compared with nanosecond-scale lifetimes of luminescence attributed to other structural film defects. Laser-damage testing using ultraviolet nanosecond and infrared femtosecond pulses showed a reduction of the damage threshold with increasing number of oxygen vacancies in hafnium oxide films.