We report on femtosecond (fs) laser experiments yielding the time constants τrel for the non-radiative relaxation from
optically excited high energy MNa** states to the fluorescent MNa* state in CaF2 samples. The values obtained with the
third and second harmonics of the fs laser amount to τrel (262 nm) = (3.0 ± 0.3) ps and to τrel (392 nm) = (1.0 ± 0.1) ps for
the two selected MNa** states at 4.7 eV (262 nm) and 3.2 eV (392 nm) excitation energy, respectively. These time
constants were derived from depletion processes of the fluorescence at 740 nm (MNa* state) using fs laser pulses of the
NIR fundamental wavelength (785 nm) at variable delay relative to the UV fs laser pulses. In addition, photobleaching of
the MNa centers upon UV fs laser irradiation is observed and simulated by assuming a constant fraction of MNa bleaching
per pulse for a given laser fluence. This fraction ranges from 0.14% per pulse at 392 nm and 0.28mJ/cm2 to about 1% per
pulse at about 6 mJ/cm2.
The influence of Na stabilized F and M centers on the DUV absorption behavior of CaF2 is comparatively studied for
nanosecond and femtosecond laser pulses by in-situ transmission and laser induced fluorescence measurements.
For 193 nm nanosecond pulses the steady state transmission of ArF laser pulses through CaF2 is measured in dependence
on the incident fluence H ≤ 10 mJ cm-2 pulse-1. The related absorption coefficients αst(H) are proportional to H and
rationalized by effective 1- and 2-photon absorption coefficients αeff and βeff, respectively. The αeff and βeff values
increase with the Na content of the CaF2 samples as identified by the fluorescence of Na related MNa centers at 740 nm.
This relation is simulated by a complex rate equation model describing the ArF laser induced MNa generation and
annealing. MNa generation starts with intrinsic 2-photon absorption in CaF2 yielding self-trapped excitons (STE). These
pairs of F and H centers can separate upon thermal activation and the F centers combine with FNa to form MNa centers.
MNa annealing occurs by its photo dissociation into a pair of F and FNa centers.
Comparative transmission measurements with DUV femtosecond pulses are done using the fourth harmonic of a Ti:Safs-
laser at 197 nm. The resulting βeff values virtually show no dependence on the MNa center concentration. Furthermore,
the absolute βeff values are lower by a factor of three compared to those obtained for nanosecond pulses. This is
explained by additional two-step absorption for nanosecond pulses after formation of self-trapped excitons (STE).
Thermal lens effects are one of the major problems in using optics for high power laser applications such as optical
lithography or material processing. The thermal lens results from the combination of the absorption in the bulk material
or the optical coatings, the thermal conductivity and the temperature change of the refractive index (dn/dT). We present
how the laser induced deflection (LID) technique allows the direct and absolute measurement of the bulk and surface or
coating absorption. The LID measurement signal, comprising of absorption, thermal conductivity and dn/dT, is directly
used to compare the tendency to built thermal lenses in different optical materials. Furthermore, it is shown how the LID
measurement signal in principle can be used to determine the thermo-optical material constants thermal conductivity and
dn/dT. Regarding direct absorption measurements, a new experimental strategy is introduced to separate bulk from
surface or coating absorption. Hereby, the closest attention is paid to measure directly the residual absorption of
transparent optical coatings, e.g. single layers or AR coatings, with negligible contribution from the substrate absorption.
In addition, numerical simulations of the thermal lens induced probe beam deflection are introduced, which allow to
design optimized strategies for particular measurement problems.
We report on two approaches to strongly shorten life time testing of fused silica's absoption degradation upon 193 nm
laser irradiation. Both approaches are based on enhancing the two photon absorption (TPA) induced generation of E' and
NBOH defects centers in fused silica compared to common marathon test irradiation parameters. For the first approach
the irradiation fluence is increased from typical values H<1 mJ/cm2 to H=10 mJ/cm2, therefore increasing the peak laser
power for a more efficient TPA process. To avoid microchannel formation in the samples, being a common break-down
criterion in marathon tests based on transmission measurements, a small sample of 10 mm length is irradiated and the
absorption is measured directly by the laser induced deflection (LID) technique. For comparing the experimental results
with a real marathon test at H=1.3 mJ/cm2, an experimental grade sample with very low hydrogen content, i.e. fast
absorption changes due to reduced defect annealing, is choosen. During the fluence dependent absorption measurements
after the prolonged irradiation at H=10 mJ/cm2 it is found, that both experiments reveal very comparable absorption data
for H=1.3 mJ/cm2. For investigating standard material with high hydrogen content, i.e. slow absorption increase due to
effective defect annealing, a sample is cooled down to -180 °C in a special designed experimental setup and irradiated at
a laser fluence H=10 mJ/cm2. To control the increase of the defect density and to determine the end of the TPA induced
defect generation, the fluorescence at 650 nm of the generated NBOH centers is monitored. Before and after the low
temperature experiment, the absorption coefficient is measured directly by LID technique. By applying both, elevated
laser fluence and low temperature, the ArF laser induced generation of E' and NBOH centers in the investigated sample
is terminated after about 1.2*107 laser pulses. Therefore, a strong reduction of irradiation time is achieved in comparison
to about 1010 pulses required in common marathon test applications.
Residual absorption in optical thin films due to impurities or defects causes thermal lens formation upon high power
DUV laser irradiation. Furthermore, it may be one reason for functional degradation during prolonged laser irradiation.
Pulsed ArF laser induced fluorescence (LIF) and direct absorption measurements (LID technique) are applied to
investigate high reflecting coatings made from LaF3, MgF2 and AlF3 with respect to the influence of different raw
materials and deposition temperatures. LIF measurements reveal emission bands that are partially attributed to certain
impurities or defects which either origin from the raw material or the coating process. In addition, LIF measurements of
single MgF2 and LaF3 layers are performed to investigate different raw material qualities and coating processes. The
experimental results show the potential of both techniques for sensitive accompanying of coating process development.
At 193nm and 527 nm, the laser induced deflection (LID) technique is applied to measure directly and quantitatively
residual absorptions in high reflecting optical coatings. In addition, combined measurements of absorption, transmission,
reflectivity and scattering for HR mirrors at 193 nm reveal very good results for the energy balance.
Cavity ring down (CRD) spectroscopy is a sensitive technique to characterize highest mirror reflectivities by determine
the photon lifetime within a resonator. A CRD setup, designed for both, cw and pulsed lasers, serves for measurements.
First measurements at λ = 532 nm reveal ultra high reflectivities of r ≥ 99.99 %. Accompanying, residual absorption of
HR coatings (ppm range) is measured directly by LID technique to quantify the different loss mechanisms contributing
to the CRD result. Additionally, the CRD setup is applied to determine the total bulk loss of (58 ± 25) ppm/cm in fused
silica at λ = 675 nm by measuring a thickness series.
The absorption of ArF laser pulses in calcium fluoride, fused silica as well as in highly (HR) and partially (PR) reflecting
fluoridic coatings is directly measured using the laser induced deflection technique (LID).
For the calcium fluoride sample it is proved that the LID technique allows to separate surface and bulk absorption by
measuring only one sample with the size 20 x 20 x 10 mm3. At a laser pulse fluence Φ = 36 mJ/cm2 and a repetition rate
f = 1 kHz the bulk absorption coefficient and the surface absorption are determined to 0.0029 cm-1 and 0.00043 (two
surfaces), respectively. For the HR and PR coatings the ArF laser absorption is 0.0004 for Φ= 22 mJ/cm2 (f = 1 kHz)
and 0.0066 for Φ= 40 mJ/cm2 (f = 1 kHz), respectively. For the example of the PR coating the influence of high coating
scattering on the LID measurements is discussed and an appropriate measuring procedure is derived and applied to avoid
the scattering influence.
In addition to the established LID setup requiring rectangular substrate dimensions a modified setup is introduced
enabling the measurement of cylindrical optical elements. The principle of the new LID setup is explained and first
measurements at fused silica are presented.
Calcium fluoride and fused silica are low absorbing key optical bulk materials for pulsed DUV laser application. Due to their large band gap fluoride thin films play a key role for applications in the DUV spectral region. For their main use in laser microlithography, these materials are commonly characterized by in situ transmission measurements. A differentiation is not possible between absorption and scattering. Therefore, experimental techniques are highly attractive which selectively characterize the absorption process using small samples. A direct absorption measurement method using laser induced deflection of a probe beam (LID) was introduced and applied to bulk and thin film materials. Laser induced fluorescence (LIF) in bulk materials and coatings is investigated to correlate the absorption with microscopic properties like intrinsic and extrinsic defects.
Precise absorption measurements of bulk materials and coatings upon pulsed ArF laser irradiation are presented using a compact experimental setup based on the laser induced deflection technique (LID). For absorption measurements of bulk materials the influence of pure bulk and pure surface absorption on the temperature and refractive index profile and thus for the probe beam deflection is analyzed in detail. The separation of bulk and surface absorption via the commonly used variation of the sample thickness is carried out for fused silica and calcium fluoride. The experimental results show that for the given surface polishing quality the bulk absorption
coefficient of fused silica can be obtained by investigating only one sample. To avoid the drawback of different bulk and surface properties amongst a thickness series, we propose a strategy based
on the LID technique to generally obtain surface and bulk absorption separately by investigating only one sample. Apart from measuring bulk absorption coefficients the LID technique is applied to determine the absorption of highly reflecting (HR) coatings on CaF2 substrates. Beside the measuring strategy the experimental results of a AlF3/LaF3
based HR coating are presented. In order to investigate a larger variety of coatings, including high transmitting coatings,
a general measuring strategy based on the LID technique is proposed.
The performance of optical coatings for high power DUV/VUV laser applications depends amongst others on residual absorption in the thin film layers due to impurities or defects. Using pulsed F2 laser induced fluorescence measurements (LIF), characteristic non-intrinsic emissions of praseodymium, cerium and hydrocarbons are identified for several high reflecting AlF3/LaF3 based mirrors on CaF2 substrates. The separate investigations of single AlF3 and LaF3 layers on silicon wafers indicate that these emissions result from the LaF3 material. The amount of the impurities, however, varies strongly between different LaF3 material grades. The influence of different LaF3 material grades on the absorption properties of high reflecting mirrors is measured for the first time upon ArF laser irradiation using the laser induced deflection technique (LID). Low absorption values of less than 1*10-3 are obtained for all samples. The absorption, however, varies by more than a factor of 2 which is correlated to the appearance of the praseodymium and cerium emissions in the LIF spectra.
Combined measurements of transmission T, absorption A and total scattering TS revealed the high accuracy of all applied measurement techniques by obtaining a sum T+A+TS+R = (100±0.3)% (R denotes the Fresnel reflection). In order to investigate CaF2 at high fluences, a variety of samples from high purity excimer grade to research grade was irradiated (80 ... 150 mJ/cm2, 2*106...7*106 pulses) and characterized before and after irradiation by total scattering, laser induced fluorescence (LIF) and transmission measurements. Total scattering mappings showed negligible and
measurable scattering in excimer grade and some research samples of minor purity, respectively. For the first time to our knowledge, laser induced fluorescence measurements revealed increasing (580nm, 740 nm) as well as decreasing (313 nm, 333 nm) emissions. The small increases of the linear absorption, obtained in all samples by transmission measurements, were used to distinguish high from minor quality material. For high quality samples the linear absorption change scales with NH3 (N: number of pulses), whereas for minor quality research samples a NH2-scaling was found.
Concentration distributions of formaldehyde were measured in a technical fuel mixing system by Planar Laser Induced Fluorescence (PLIF) using a novel all solid state disk laser system. This compact and efficient laser generates tunable, narrow bandwidth pulses with kHz repetition rate and energies of up to 25 mJ around 1030 nm. After frequency conversion to the UV spectral region, laser pulses with energies of up to 4 mJ excite different combustion relevant species inside of a semi-technical reactor. This reactor generates a homogeneous fuel vapor/air-mixture using the so-called cool flame. Since the mixture of fuel and air is a key factor concerning efficiency of combustion, the fast fuel injection and mixing processes were investigated with this laser system. Directing a light sheet into the reactor and collecting the fluorescence with an intensified CCD camera, we recorded PLIF images of formaldehyde concentration distributions using an excitation wavelength of 343 nm. In this way we characterized the turbulence of the injection process close to the fuel injection nozzle with 1 kHz repetition rate, and proved the excellent homogeneity of the fuel-air mixture close to the end of the reactor, where fuel-air mixture was burned in a hot flame. By means of scattered light from fuel droplets the mean flow velocity could be estimated. In the hot flame above the reactor spectrally resolved LIF of OH radicals could be recorded.
The laser induced deflection technique (LID) is introduced for measuring small absorption coefficients of highly transparent DUV/VUV optical materials with high sensitivity and accuracy. The measuring principle, the calibration and the developed experimental realization are explained. At 193 nm in situ absorption and fluorescence measurements of fused silica give evidence that a commonly observed absorption decrease at the onset of laser irradiation is a bulk effect and due to a diminution of oxygen deficient centers ODC II. This decline is caused by a single photon absorption process and terminates after a dose of 4-5 kJ/cm2. Fluence dependent bulk absorption measurements of fused silica are presented which indicate the presence of a nonlinear dependence between the absorption coefficient α and the fluence H. For calcium fluoride a very good agreement between direct absorption and conventional transmission measurements is obtained. At 157 nm, a modified compact experimental setup is introduced which exhibits a significantly higher sensitivity than that applied for 193 nm experiments. First measurements of high quality calcium fluoride show that the obtained absorption is independent on the laser repetition rate. The investigation of equivalent CaF2 samples of different thickness (10 mm and 20 mm) indicates that the measured absorption coefficient is virtually free of contributions from the irradiated surfaces. Finally, a very good agreement is obtained by comparing LID data with transmission measurements of 100 mm long samples.
An all solid state disk laser system-named "Advanced Disk Laser (ADL)" -particularly tailored for laser induced fluorescence (LIF) in combustion processes is presented. The system currently under development comprises an Yb:YAG-seedlaser and a regenerative amplifier. Both are based on the disk laser concept as a new laser architecture. This allows a tunable, compact, efficient diode pumped solid state laser (DPSSL) system with repetition rates in the kHz region. After frequency conversion to the UV-spectral region via third and fourth harmonics generation, this laser-due to its unique properties such as single-frequency operation, wavelength tuneability and excellent beam profile-is well suited for excitation of small molecules such as formaldehyde, OH, NO or O2, which are characteristic for combustion processes.
Using the method of planar laser induced fluorescence (PLIF) we observed concentration distributions of formaldehyde in cool and hot flames of a specially designed diethyl-ether burner. The images recorded with 1 kHz repetition rate allow visualizing the distribution of formaldehyde on a 1 ms time scale. This demonstrates for the first time the usability of this novel laser for LIF measurements and is the first step towards integration of the ADL into capsules for drop towers and the international space station.
Carbon monoxide distributions around igniting n-heptane droplets were determined using absorption measurements. The emission of a quantum cascade laser at 4.6 μm was shaped to a parallel laser beam using a lens. For detection, a plane through the droplet, perpendicular to the laser beam was imaged onto the focal plane array of a mid-infrared camera. For background suppression a long-pass filter was mounted in the detection ray path. To estimate the detection sensitivity of the set-up, CO absorption in a reference cell was measured. In addition, CO transmission spectra were calculated for
different temperatures based on HITRAN 2000 catalogue.
Concentration profiles of OH, O2 and NO as well as temperature fields in diffusion flames of a length of approx. 300 mm and 40 mm in diameter used for gas-phase synthesis of fused silica have been determined by Planar Laser Induced Fluorescence (PLIF). The measurements have been carried out using a tunable spectrally narrowed KrF laser, whose wavelengths could be switched pulse-to-pulse. The laser beam was shaped as a light sheet into the flame at a fixed position. The flame area under investigation was monitored by moving the burner mounted on a stepper motor. By adapted synchronization the laser induced fluorescence was continuously recorded over the height of the flame perpendicular to the laser light sheet with an intensified CCD camera (10 fps, 8 bit dynamic range, 768 x 576 pixels). By image processing the spatial offset between images was corrected and superposed images were averaged and analyzed. This method allows to investigate the flame by recording 2D-fluorescence images including an automatic correction of intensity inhomogeneities of the laser light sheet. Based on the excited radical or molecule the fluorescence images were used to determine concentration and temperature distributions to build up a 2D-map of the flame. The PLIF experiment was calibrated with precise determination of the temperature at one coordinate of the flame by Spontaneous Vibrational Raman Scattering (VRS) of N2. As a result temperatures up to 3200 K could be determined with an accuracy better than 3% and a spatial resolution better than 1 mm. Temperature variations in the flame at different gas flows of fuel and oxidizer could be monitored sensitively. Also, the influence of different carrier gases like N2, Ar and He on the temperature distribution was investigated. Fluctuations in gas flow caused by turbulence could be monitored as well.
The combination of in situ transmission and laser induced fluorescence (LIF) measurements of CaF2 at 193 nm and 157 nm laser irradiation reveals a correlation between selected fluorescence bands and the laser transmission. At 193 nm irradiation, the fluence dependent transmission |dT/dH| of calcium fluoride shows a significant dependence on the temporal pulse shape of the laser source. Furthermore, a quantitative correlation between transmission properties and fluorescence intensity of calcium fluoride is reported for the first time in case of a LIF band at around 740 nm. Newly defined LIF detection conditions yield a remarkable increase of the sensitivity for bands with short lifetimes. Furthermore, different excitation mechanisms for the investigated fluorescence bands are found from both, fluence and pulse number dependent LIF measurements. At 157 nm irradiation, a fluence dependence of the transmission (|dT/dH|,T0) is obtained which is comparable to that of 193 nm excitation. LIF investigations at 157 nm excitation reveal an increase in complexity of the spectra compared to those of 193 nm excitation. It is found that the LIF spectra at 157 nm excitation mostly consist of the same bands as for 193 nm irradiation. Some samples, however, show a LIF band vanishing relative to its intensity at 193 nm excitation or the appearance of new bands characteristic only for 157 nm excitation. From comparing two calcium fluoride samples at 193 nm and 157 nm irradiation it is assumed that the presence of a characteristic 157 nm excited LIF band at around 225 nm is responsible for a drop in transmission at 157 nm.
Under 193 nm excimer laser irradiation the laser induced deflection technique (LID) is applied to investigate directly the bulk absorption α of high quality fused silica and calcium fluoride. Fused silica samples are characterized by their fluence H dependent absorption α(H). Their small signal absorption coefficients α 0 are extrapolated by an appropriate fitting model. All investigated standard samples with high H2 content fulfill the requirement for optical lithography which is determined by an α0 of less than (formula available in paper). Prolonged direct absorption measurements at relatively high fluences of 10 and 20 mJ/cm2 by the LID technique are compared to state of the art marathon durability tests for H2 poor fused silica at a H = 1.3 mJ/cm2. The very good agreement of the results demonstrates that the measurement time for durability tests of fused silica can be reduced considerably by increasing the applied fluencs H. Calcium fluoride is investigated by both, direct bulk absorption (LID) and conventional transmission measurements. A very good agreement is found by comparing the results of both experiments. For investigations at 157 nm laser irradiation a new compact LID measurement device is introduced. Calibration measurements show that the sensitivity is significantly increased compared to the previous setup. The detection limit of the new setup is estimated to α values of (formula available in paper) for calcium fluoride and fused silica, respectively.
An experimental setup was established for in situ transmission and laser induced fluorescence (LIF) measurements of CaF2 at 193 nm laser irradiation. The known rapid damage process in CaF2 upon ArF laser irradiation is shown to terminate for all tested samples within 3×104 laser pulses for the applied fluences. Furthermore, it is demonstrated that for typical application values the fluence dependent transmission (FDT) at the end of the rapid damage process is independent of the irradiation history and determined by the specific crystal quality.
From the lifetimes and signal strengths of different present fluorescence bands the excitation and recording conditions for LIF investigations are derived. The results of laser induced fluorescence measurements at 193 nm excitation make evident that certain impurities or defects are responsible for the different transmission properties even of high purity CaF2 crystals. Comparing transmission and LIF data a quantitative correlation was found between selected emission bands and ArF laser stability of CaF2 material.
Luminescence measurements have been set up in order to study the interaction of UV-laser radiation with dielectric thin films. The pulsed laser excitation was carried out at 193-nm (6.4eV), the coating materials comprised wide-band-gap oxides and fluorides. Experiments show the significant optical response of single- and multilayer coatings on the low fluence excitation at sub-band-gap energy. Time- and spectrally-resolved measurements indicate characteristic emission bands of color centers in the deep-UV and vacuum-UV coating materials. An assignment of these optical transitions can be derived from the comparison with known bulk-material studies.
A new setup was established to simultaneously record the bulk absorption of fused silica at 193 nm and its laser induced fluorescence (LIF). Bulk absorption coefficients in the 10-3/cm range are measured in a compact setup with small samples of 20 x 20 x 10 mm3 using an ArF pump laser and recording the ArF laser induced deflection (LID) of a diode probe laser beam. LIF is measured through an optical fiber coupled to an intensified gated CCD camera.
Within the first few pulses of ArF laser irradiation the bulk absorption coefficient and LIF emission around 300 nm and 400 nm (oxygen deficient centers, ODC) decrease considerably, sometimes to a fraction of their initial values. In smoe fused silica samples additional fluorescence in teh green-yellow wavelength region is found. This fluorescence increases in a strongly nonlinear way with the fluence. Assuming fluorescence excitation by single photon absorption the observed behavior can be explained by saturation of the absorption transition which put limitations on the fluence applicable in the experiments. Summarizing the obtained results a measurement instruction for precise absorption measurements of fused silica at 193 nm laser irradiation is suggested and fused silica samples have been investigated concerning their dependence of the absorption coefficient on the fluence. The results, in combination with transmission measurements of 300 mm long fused silica samples, confirm the nonlinear increase of the absorption with increasing fluence.
A compact experimental setup, based on the laser induced deflection technique (LID), measures small absorption coefficients in fused silica upon 193-nm irradiation with high sensitivity and accuracy. For that, two probe laser beams are passed numerous times through a sample and are deflected by a refractive index gradient which is generated by the power absorbed within the material. The absorption coefficient of the sample is determined by applying a comfortable and precise electrical calibration procedure. The investigation of two equivalent fused silica samples of different thickness confirmed that the setup allows to exclusively measure the bulk absorption of the material without contributions from the irradiated surfaces. Furthermore, influences of irradiation parameters like repetition rate and pulse width on the absorption coefficient of fused silica at a fixed applied energy density have been investigated. The results confirm the complexity of the absorption mechanism present in fused silica upon laser irradiation. In order to separate linear and nonlinear absorption two fused silica samples have been irradiated with different energy densities keeping the repetition rate and the pulse width constant. The results show a nonlinear dependence of the absorption coefficient on the energy density which can qualitatively be explained by the two-step absorption mechanism in fused silica.
A diagnostic system using a kHz solid state laser is under development. The system combines a high power diode pumped solid sate laser system as excitation source with an intensified fast scan camera system. The Yb:YAG disk laser oscillator and a regenerative amplifier generate tunable radiation, spectrally narrowed to $DELTA(lambda) < 5 pm, which will be converted by nonlinear crystal into the VIS and the UV spectral ranges. The excitation of the planar laser induced fluorescence of selected molecules and radicals at wavelengths inside the discussed spectral ranges is demonstrated in preparatory experiments. Examples are the OH radical, NO and formaldehyde molecules excited by a frequency doubled dye laser. From these experiments the needed pulse energies of the solid state laser system for light sheet shaping are derived. The system is under development for investigations of combustion processes under reduced gravity at drop tower Bremen, during parabolic flights and at the ISS.
The 157 nm lithography technology is supposed to become the system setup for the 100 nm respectively the 70 nm node. The first 157 nm Full-Field Scanner system is expected in 2002. Every currently evaluated optical design of such lithography systems makes a very intensive use of Calcium Fluoride as one of the few optical materials having the required transmittance at the F2 laser wavelength solely. Additionally the required further industrial production processes e.g. polishing and development of coatings are known from the 193 nm lithography where CaF2 is already in use. In this paper we report about R&D activities of the material development used for the high quality CaF2. Thus the main aspects on quality are discussed in detail.
The 157 nm lithography technology is supposed to become the system setup for the 100 nm respectively the 70 nm node. The first 157 nm Full-Field Scanner system is expected in 2002. Every currently evaluated optical design of such lithography systems makes a very intensive use of Calcium Fluoride as one of the few optical materials having the required transmittance at the F2 laser wavelength solely. Additionally the required further industrial production processes e.g. polishing and development of coatings are known from the 193 nm lithography where CaF2 is already in use. In this paper we report about R and D activities of the material development used for the high quality CaF2. Thus the main aspects on quality are discussed in detail.
Excimer laser pulses ((lambda) equals 193 nm, (lambda) equals 248 nm) induce transient and permanent defects in highly UV transparent optical glass for microlithography. Usually laser damage of fused silica is evaluated by time consuming and expensive marathon tests characterized by about 109 pulses at repetition rates of 400-1000 Hz and fluences of 0.5-10 mJ/cm2. Alternatively, short time tests using high laser energy densities have been developed to quickly evaluate influences of changes in the production technology. The following evaluation methods are used: Laser induced absorption at 193 nm measured by laser induced deflection (LID), Laser induced fluorescence at 650 nm (LIF) excited by 193 nm or 248 nm laser irradiation, H2 content measurement by means of a pulsed Raman spectroscopy at 248 nm laser excitation. Both, the LIF signal and the H2 concentration are measured locally resolved in a non-destructive way. The applied energy densities of the above methods vary from 1 mJ/cm2 to 600 mJ/cm2. The front face technique for investigating large diameter samples, e.g. mask blanks (6 inches and 9 inches), have been established.
The laser induced absorption of CaF2 caused by ArF excimer laser light has been observed at energy densities of F equals 2-30 mJ/cm2 per pulse and a repetition rate of R equals 50 Hz. The experiments show that the transmission of CaF2 samples depends on the pulse energy density. The change of the absorption coefficient with the time of irradiation can be described by an exponential model. Different experiments were performed where the energy density was increased and decreased stepwise. They prove that color centers not only are formed but also are annihilated by irradiation. Laser induced decrease of absorption was observed in all samples as soon as the energy density was decreased. Coloring and bleaching of the samples are completely reversible processes. The level of transmission depends on the energy density of the laser light and the quality of the material but not on the history of irradiation. The damage resistance of the material can be adjusted by the appropriate choice of the raw material and the process parameters. The reversibility of the laser induced absorption can be explained by a reaction equilibrium. This leads to a model where the concentration of absorbing defects depends on the current irradiation conditions. Using these equations the reversibility and the observed exponential dependence of the change of transmission with time can be explained. Assuming different dependencies of the reaction constants of coloring and bleaching on the energy density, the change of the absorption coefficient with pulse energy density can be calculated.
Large area photomask substrates of fused silica and a size of up to 9 inches by 9 inches are locally evaluated by laser induced fluorescence and H2 measurements. Using a narrow-bandwidth KrF excimer laser, pulsed UV Raman spectroscopy is applied to measure the content of molecular hydrogen as an indicator of laser durability. Due to expeditious H2 measurements, this technique allows to determine the local H2 concentrations across an entire 6 inch by 6 inch photomask substrate within one hour. ArF excimer laser induced fluorescence (LIF) measurements are applied to correlate the H2 concentration and the laser induced defect formation in fused silica. In most cases the NBOH defect density, determine by the intensity of the peak at (lambda) equals 650 nm in the LIF spectrum, shows a symmetric curve across the substrate diagonals with its lowest values in the center. The associated H2 concentrations are found to show a maximum in the center. Furthermore, pulsed UV Raman spectroscopy is used to monitor the H2 concentration during irradiation with several 105 pulses of high KrF laser fluence. At first a rise in the H2 concentration is observed. After a maximum value further irradiation leads to a drop of molecular hydrogen within the illuminated volume.
This paper describes a UV laser diagnostic system by means of which laser spectroscopic experiments were performed under microgravity conditions in a ground-based drop tower for the first time. A tunable, narrow bandwidth excimer laser is positioned at the top of the drop tower. The laser beam enters a falling drop capsule containing a specially adapted burner or combustion chamber. By the use of laser induced fluorescence spectroscopy measurements of 2D concentration and temperature profiles can be performed. Solutions of selected experimental problems such as laser beam collimation over a distance of more than 120 m, compensation of capsule drift, signal detection, and data acquisition (250 frames/s, 4.7 s measuring period), are discussed in detail. First measurements of laser induced predissociation fluorescence of OH radicals in a methanol flame under microgravity conditions are presented.
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