We present a consistent model supported by experimental data of damage of dielectric films by
femtosecond to nanosecond pulses. Special emphasis is given to the role of defects and transient
processes in the material. New imaging and diagnostic techniques are discussed to characterize
the film performance.
We have investigated the role of native point defects in the laser damage behavior of amorphous thin films of Sc2O3 deposited by ion beam sputtering. Through systematic characterization and detailed modeling we show that native
defects influence the 1-on-1 laser induced damage threshold fluence of the Sc2O3. This effect, as shown by the model
and confirmed by experiments, is pulse duration dependent.
Scandium oxide is an attractive candidate for the engineering of interference coatings, although not widely explored.
This paper describes the ion beam sputtering of Sc2O3. It is shown that the structural properties of the material are
affected by the deposition conditions. Laser damage in different regimes of pulsewidths is investigated. These results
show that the 1-on-1 laser damage fluence, in both the thermal and deterministic regimes, varies with deposition
conditions but this is not the case for S-on-1, indicating that laser-induced defects are important.
The multiple-pulse laser-induced breakdown behavior of dielectrics is modeled. The model is based on a critical conduction
band (CB) electron density leading to dielectric breakdown. The evolution of the CB electron density during the
pulse train is calculated using rate equations for the occupation and ionization of band and midgap states (native and laser
induced). Using realistic estimations for the trap density and ionization cross-section, the model is able to reproduce
the experimentally observed drop in the multiple-pulse damage threshold relative to the single-pulse value, as long as the
CB electron density is controlled primarily by avalanche ionization seeded by multiphoton ionization of the traps and the
valence band. The model shows that at long pulse duration, the breakdown threshold becomes more sensitive to presence
of traps close (within one photon energy) to the conduction band. The effect of native and laser-induced defects can be
distinguished by their saturation behavior. The model explains the principal behavior of the LIDT of a pair of pulses as a
function of the temporal separation. Using the model, the observed transients can be related to rate constants of electrons
leaving the CB and midgap states.
A film of hafnium oxide, doped with 5 atomic % nitrogen, was prepared by dual-ion-beam-assisted deposition. The
properties were compared to a pure hafnium oxide film. The damage threshold is lower for the nitrogen-doped film.
However, the multiple-pulse damage threshold for a 1 kHz train of 800 fs pulses shows no drop relative to the singlepulse
value. These results are discussed within the context of a
multiple-damage model, based on midgap trapping states.
We discuss the physical and optical properties of Sc2O3 single layers deposited by the dual ion beam sputtering technique
at oxygen partial pressures ranging from 1.7×10-5 to 5.1×10-5 Torr. The films are amorphous with crystallite size ~10
nm and have surface roughness RMS values of 1.2±0.3 nm. The refractive index at 1 μm is 1.95. Absorption loss is shown
to be sensitive to the oxygen partial pressure during growth. Multiple-pulse damage experiments suggest that the scandia
film deposited at the higher oxygen partial pressure accumulates laser-induced trap defects more slowly than the scandia
film deposited in a lower oxygen partial pressure atmosphere.
In this contribution we will summarize the fundamental mechanisms that lead to subpicosecond laser
damage in dielectric films, discuss the resulting scaling laws of single pulse (1-on-1) damage with respect
to pulse duration and bandgap, of the multiple pulse (S-on-1) damage threshold as a function of pulse
number, and compare these findings to recent experimental results.
The single pulse femtosecond laser induced damage threshold (LIDT) of hafnia and silica films is not affected by the
ambient gas pressure. In vacuum, the multiple pulse LIDT drops to ~10% (~10%) of its atmospheric value for hafnia
(silica). The water vapor content of the ambient gas was found to control the change in the LIDT. The LIDT of bulk
fused silica surfaces did now show any dependence on the ambient gas pressure. Hydrocarbons (toluene) did not change
the multiple pulse LIDT for Hafnia films
In this work we use electron spin resonance (ESR) spectroscopy to investigate defects in dual ion beam sputtered HfO2
and SiO2 films. "As-grown" SiO2 films exhibit an ESR feature consistent with an E' center associated with an oxygen
vacancy previously reported. A similar feature with axial symmetry is seen in HfO2 films. The defect giving rise to the
HfO2 ESR feature is distributed throughout the film. In addition, post process annealing of HfO2 and SiO2 films greatly
reduces these defects.
We present a complete systematic study on the effect of assist beam energy on SiO2/HfO2 quarter wave stacks deposited
by dual ion beam sputter (DIBS) deposition. Increasing assist beam energy results in lower surface roughness and
reduced micro-crystallinity. The coatings also show reduced mechanical stress. The improvements in the structural
properties are accompanied by a reduction in the absorption loss and an increase in the laser resistance to damage at 1
μm.
Subpicosecond laser induced breakdown of dielectric films has gained a great deal of attention in laser nano- and
micromachining and in the development of optical coatings for the next generation of high-power ultrafast laser system.
The understanding of the fundamental processes affecting the breakdown behavior and how they depend on the material
properties and the film deposition is highly desirable for improving the coating performance. In the present work we
compare the single and multiple pulse damage behavior of as-grown and annealed HfO2 films. Annealing can reduce the
film absorption near the band edge but its impact on the single and multiple femtosecond pulse damage behavior
remained open. Damage measurements with pairs of pulses of variable subpicosecond delay in bulk fused silica revealed
a partial recovery toward single pulse behavior on a few hundred fs time scale. We investigate if such behavior also
occurs in hafnia films and identify the time scale for a full recovery. Our experimental results are compared with
existing theoretical models[1], which allows us to suggest microscopic changes that occur during the annealing process.
We investigate the variations that occur with changes in the number of layers and with the use of the assist beam
main and assist beam energy on the morphology of HfO2/SiO2 quarter wave stacks deposited by dual ion beam
sputtering. We show how the addition of sequential HfO2/SiO2 bilayers, up to eight, affects the surface roughness
and micro-crystallinity of the top HfO2 layer. We also show that use of the assist source significantly smooths the
surface while simultaneously reducing microcrystallinity. The HfO2/SiO2 structures are very robust and can
withstand fluences in excess of 3 J/cm2 generated by 1ps pulses from a chirped amplified Ti:Sapphire laser.
Hafnium oxide (HfO2) is undoubtedly one of the most desirable high-index optical coatings for high power
laser applications. One of the key goals in the fabrication of oxide films with high Laser Induced Damage
Threshold (LIDT) is to minimize the number of film imperfections, in particular stoichiometric defects. For
HfO2 films deposited by ion beam (reactive) sputtering (IBS) of a hafnium metal target, stoichiometry is
controlled by the injection of molecular oxygen, either close to the substrate or mixed with the sputtering
gas or some other combination. Good stoichiometry is important to reduce the density of unoxidized
particles buried in the coatings, which affect the LIDT. This work evaluates the potential advantages of
using pre-activation of oxygen in the IBS of HfO2, with special emphasis on its impact on LIDT and film
stress. For the experiments, oxygen was activated by an independent plasma source and then introduced
into a commercial IBS chamber. The optical properties of the films were characterized using
spectrophotometry and ellipsometry. Their structural quality and composition were determined from x-ray
diffraction and x-ray photoelectron emission spectroscopy. The stress was determined from interferometer
measurements. For optimized conditions, 2.5 J/cm2 LIDT was measured on HfO2 films at λ=800 nm with 1
ps and 25 mJ pulses from a chirped amplification Ti:Sapphire laser. In the range of oxygen variations under
consideration the effects on LIDT are shown to be minimal.
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