Dual wavelength laser damage mechanisms in the ultra-short pulse

regime
Mark Gyamfi*a, Marion Costellaa, Thomas Willemsena, Peter Jürgensb, Mathias Mendec, Lars
Jensena, Detlev Ristaua
a
Laser Zentrum Hannover e.V., Laser Components Department, Characterization Group,
Hollerithallee 8, 30419 Hannover, Germany;
b
Max-Born-Institut f. Nichtlineare Optik u. Kurzzeitspektroskopie e.V., Max-Born-Str. 2 A, 12489
Berlin, Germany
c
Laseroptik GmbH, Horster Str. 20, 30826 Garbsen, Germany

ABSTRACT

New ultrashort pulse laser systems exhibit an ever increasing performance which includes shorter pulses and higher
pulse energies. Optical components used in these systems are facing increasing requirements regarding their durability,
and therefore understanding of the damage mechanism is crucial. In the ultra-short pulse regime electron ionization
processes control the damage mechanisms. For the single wavelength, single pulse regime the Keldysh [1] and the Drude
model [2] allow a quantitative description of these ionization processes. However, in this model, the electrical field is
restricted to a single wavelength, and therefore it cannot be applied in the case of irradiation with two pulses at different
wavelengths. As frequency conversion is becoming more common in ultra-short pulse applications, further research is
needed in this field to predict the damage resistance of optical components. We investigate the damage behavior of high
reflective mirrors made of different metal oxide materials under simultaneous exposure to ultra-short pulses at the
wavelengths 387.5 nm and 775 nm, respectively.
Keywords: fs-LIDT, dual wavelength, ultra-short pulse damage

1. INTRODUCTION
Since the introduction of commercial femtosecond chirped pulse amplification systems two decades ago, femtosecond
laser systems have found their way into many applications in industry, medicine and measurement technology.
Applications are ranging for example from laser-micromachining of a broad spectrum of materials [3] over grating
inscription in fibers [4] even to the removal of biological tissue [3, 5, 6]. Material ablation and spectroscopy are further
topics where in recent years employment of pulse pairs or even pulse trains allowed an enhancement or refinement of the
processes. Each of these applications has different specific requirements for the employed radiation, and to meet the
different demands for the optics used in the corresponding laser systems, advanced dielectric thin films coatings are
necessary. For a further optimization of the involved optical coatings, an understanding of the fundamental mechanisms
of laser-induced damage of coatings and bulk materials is necessary. In recent years, research in the field of laser-
induced damage was concentrated on single wavelength modeling and testing. However, more and more ultra-short pulse
applications are dependent on frequency conversion to higher harmonics [7, 8] demanding for a more detailed
understanding of laser damage mechanisms in the near UV spectral range and at multi-wavelengths. Compared to the
nanosecond regime, where damage is often defect initiated and thermally driven, damage in the femtosecond regime is
dominated by intrinsic electronic effects with relatively small thermal contributions. Theoretical models for femtosecond
laser damage are based on excitation dynamics of electrons in a solid dielectric under irradiation with intense laser
pulses. Most models consider a certain free electron density in the material as a criterion for the onset of catastrophic
damage of the dielectric material. In this paper we present dual wavelength laser damage studies on dielectric HR390 nm
/HR780 nm mirrors. A measurement routine for dual wavelength laser damage testing is described and damage tests
results are given. We investigate the influence of different delays between the two pulses and compare the measured
damage thresholds for different metal-oxide materials.
*m.gyamfi@lzh.de; phone +49 511 2788 283; fax +49 511 2788 100; lzh.de

Laser-Induced Damage in Optical Materials 2016, edited by Gregory J. Exarhos, Vitaly E. Gruzdev,
Joseph A. Menapace, Detlev Ristau, MJ Soileau, Proc. of SPIE Vol. 10014, 100141B
© 2016 SPIE · CCC code: 0277-786X/16/$18 · doi: 10.1117/12.2245156

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 2. EXPE
ERIMENTA
AL METHOD
DS
2.1 Laser-ind
duced damagge test bench
A commerciaal Clark CPA22110 Ti:Sa reegenerative am mplifier systemm operating at
a a wavelengtth of 775 nm with a repeti-
tion rate of 1 KHz is employed for the damage testss. The system m delivers pulsses with a pullse energy of up to 1 mJ ata
775 nm with a sech² pulse shape and a pulse
p durationn of 150 fs. A 50 % beam splitter
s separattes the beam into
i two beam
m
paths, where in one of them m a 1 mm thick BBO crysttal generates the t second haarmonic radiattion used in th he experimentt.
Afterwards, a dichroic HR R390 nm /HT7780 nm mirrorr recombines the t two pulsess. Both beamss are focused via v a lens withh
a focal lengthh f=500 mm, leading
l to a sppot diameter inn the sample plane
p of approoximately 1033±5 µm for the fundamentaal
pulse and 1009±5 µm for the t second haarmonic. Acccording to ISO O 21254, dam mage was deteected during irradiation byy
detection of scattered
s light with a photoddiode. A schem matic of the setup is depicteed in Figure 11a.

LIDT- Sample

Photodiodfe

-
I
Delay-

2-1 T=390nrt
Len

HR390nm /HTl
I` 1

I G4-
Mirror H
1

BRO
Attenuai

.= 780nm _¢nn _yen _inn n nn vr ¢en

- 150r
Delay [fa]
Shutter 5C0/50 Bcamspliner

Figure 1a (lefft): Schematic of

o the experimenntal setup. An additional
a arm extends
e the fundamental LIDTT measurement consisting of a
variable attennuator and a phhotodiode for onnline damage deetection: tempo oral overlap betw
ween the two puulses is measurred by a cross-
correlation between the fuundamental andd second harmonnic pulse via su um-frequency generation of thee third harmonic. Figure 1b
(right): Cross-ccorrelation tracee generated by overlapping thee fundamental and
a second harm monic radiationn.

The temporall overlap betwween the pulsees was monitoored with an additional
a BBBO crystal. Thhis crystal is installed at thee
sample positiion to generate a cross-corrrelation signall between the fundamental and second haarmonic pulsee, ensuring thee
temporal overrlap between the
t two pulsess. A signal traace of this crosss-correlation is shown in F
Figure 1b.

2.2 Measurem
ment and evaaluation routine
Departing froom the standarrd evaluation routine propoosed in the ISO O 21254 [9], several
s modiffications were applied to thee
evaluation algorithm. The assumption, that the dam mage mechanissms in the fem mtosecond puulse regime are
a intrinsic inn
nature impliees that any varriation in the site-specific
s d
damage fluencce is caused eiither by local inhomogeneity of the coat-
ing or fluctuuations of thee radiation soource, which are not mon nitored (e.g. pulse-to-pulse
p e fluctuations of the beam m
diameter). Duue to the indeppendent randoom nature of these
t parameters, a normal distribution w was used as th
he basis for thee
damage ensem mble. This is in accordance to the centrral limit theorem, which staates that the ssum of indepeendent random m
variables is best described by a normal distribution.
d
1 ( )
( )= (1)
√
√2 π

Where is the standard deviation

d andd is the meaan value of thee ensemble. Due
D to the intrrinsic nature ofo the damagee
mechanisms we
w assume, thhat damages thhat occur at loower fluencies would also occur
o at higheer fluencies an
nd undamagedd

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 sites would survive also lower fluencies. This cumulative approach drastically increases the number of sites in each
fluence bin, reducing the statistical error 1 , where N denotes the number of tested sites in the bin, for each fluence bin.
This cumulative algorithm for the calculation of the damage probabilities of the individual fluencies is described in detail
by Schrameyer et. al. [10]. Integration of the defect distribution delivers the fit function in Equation 2 used to calculate
the 50 % damage probabilities.
1 −
( )= 1+ (2)
2 √2

The measurement procedure followed the ISO 21254 with the addition of a second pulse at different fixed fluencies.
First, damage thresholds for the fundamental and second harmonic were measured. Afterwards, LIDT tests for the funda-
mental were then conducted, with the second harmonic pulse set to different fixed fluence levels between zero and the
damage threshold. During these tests, the delay between the fundamental and second harmonic pulse was kept constant.
After finishing a set of measurement at different second harmonic fluencies and constant delay, the delay was then varied
and the tests were repeated for different pulse delays.

2.3 Samples
The samples used for the experiments consisted of double high reflective mirrors deposited on fused silica substrates. As
high refractive index materials Nb2O5, Al2O3, HfO2 and Ta2O5 in combination SiO2 as low refractive index material were
used for all samples. The samples were prepared with an ion beam sputtering deposition process. The major design goal
for the mirrors was to ensure a high reflectivity at 390 nm and 780 nm, as can be seen in the transmission spectra plotted
in Figure 2.
ó
0

----
,______----
0
CO

-
Transmission [ %]

c
0
CD

,
O
-I,

20
H1203
HfO2
Ta2O5

0
400 600
'RoJil
Wavelength [nm]

Figure 2: 0° Transmission spectra of the four HR390 nm/HR780 nm mirrors.

For both wavelengths, the highest field intensity is located near the interface between the first high and low refractive
index layers. Plots of these field intensities are shown in Figure 3.

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 HfO2 Al2O3

4001 775 nm
Air
400
- 775 nm Air
388 nm
388 nm A i I I

300 - 300 -

l'.
- 200

anon çnnn Ann() lnnnn 19nnn lannn

Opt. Thickness [nm] Opt. Thickness [nm]

Ta2O5 Nb2O5
Air Air
400 775 nm 400
388 nm
400 775 nm
1RR nm

300 j 300 300 -

r
= 200
1°7-'1

200

100-
A 1001

mu"m U
x
\ ÁI V
=" ^= coon =l o 01
arm AnnO 7000

Opt. Thickness [nm] Opt. Thickness [nm]

Figure 3: Field intensities for the different HR390 nm/HR780 nm mirrors. The intensities were calculated with the commercial
software Optilayer and are normalized to the incoming field.

3. DAMAGE STUDIES

1000on1 LIDT tests according to ISO 21254 were performed at 775 nm. In previous work [11], we presented results of
two-pulse LIDT testing on a Ta2O5 high reflective mirror. For the testing routine, the LIDT at the fundamental was
measured without second harmonic radiation. Afterwards the sample was exposed to second harmonic radiation and the
individual LIDT tests were repeated for different fluence levels at harmonic wavelength. The dual wavelength LIDT
behavior of this sample is shown in Figure 4.

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 1,0
I
1 80 fs
1
0.8

1
E0
C

©04
H
a I

-o
0 Ta2O5
nn n9 i
na nF
Fluence SHG [a.u.]
I
nR 1 n

Figure 4: Dual wavelength LIDT (0%, 20.000on1) behavior of a HR390 nm/HR780 nm mirror consisting of Ta2O5 as high refractive
index material and SiO2 as low refractive index material.

A clear decrease of the LIDT with increasing fluence of the second harmonic pulse was observable in these measure-
ments. In contrast to the nanosecond regime where a drastic decrease of the LIDT under exposure to harmonic radiation
at multiple wavelengths was reported in [12], no sudden drop of the LIDT was observed under simultaneous fundamental
and second harmonic exposure. Due to the experimental setup for this experiment, the second harmonic pulse was trail-
ing the infrared pulse at a fixed delay of 80 fs.
Table 1: Refractive index, bandgap and conduction band electron relaxation time for different materials.

Material Refractive Index @ 780 nm Bandgap [eV] Relaxation Time [fs] [13]

Nb2O5 2,25 3,5 n.a.

Ta2O5 2,17 3,8 550
HfO2 2,09 5,1 1100
Al2O3 1,65 6,5 410
SiO2 1,50 8,3 220

The damage tests of HfO2, Nb2O5 and Al2O3 presented in this work were also tested according to this routine but in
addition, the tests were repeated for different delays between the fundamental and second harmonic pulse. The results of
these measurements are shown in Figure 5. For the HfO2 mirror the delay between the pulses was set to 0 fs, -100 fs,
100 fs, -1000 fs and 1000 fs. Negative numbers denote a trailing second harmonic pulse and positive numbers a trailing
fundamental pulse. Similar to the Ta2O5 mirror, the HfO2 mirrors show a drop in the measured damage threshold due to
the second harmonic pulse. This drop of the damage threshold is most significant in the 0 fs delay case. In the case of a
delay of 100 fs, which is still an order of magnitude lower than the conduction band electron relaxation time in HfO2, no
significant difference could be observed between the two delay cases. In both instances, the measured LIDT values for
775 nm were higher than for a delay of 0 fs. Only at ±1000 fs, a significant dependence on the pulse sequence could be
observed. Here a trailing second harmonic pulse results in a higher damage threshold for all fluencies. At 60 % to 80 %
of the single wavelength threshold, this effect is most pronounced. For theses fluencies the damage threshold in the case
of a trailing blue pulse is almost 50 % higher than in the inverse case. Nb2O5 shows a very similar behavior to HfO2. For
this material, the lowest damage thresholds are also observed when the pulse overlap is highest. At a delay of ±100 fs,
there is already an observable dependency of the damage threshold on the pulse sequence. As for the HfO2, for a trailing
blue pulse the material exhibits a higher damage threshold than in the inverse case. For a delay of ±200 fs, this pulse
sequence dependency of the damage threshold has almost vanished and the influence between the two pulses is only

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 observable at high fluencies. Increasing the delay further to ±500 fs shows no impact of the second harmonic pulse on
the damage threshold, even at fluencies close to the threshold of the second harmonic radiation. Observing no influence
at high fluencies near the damage threshold, no further tests for these delays were conducted. The high reflective mirror
consisting of Al2O3 and SiO2 showed no clear dependency of the damage threshold on the pulse sequence. While the
measurements at a delay of 0 fs indicate a consistent decrease of the LIDT with increasing fluence of the second har-
monic pulse, for delays of ±200 fs, ±500 fs and ±1000 fs no clear tendency was observable. A possible explanation for
this might be that for Al2O3 the damage detection scheme did not work very accurate. A later ex situ inspection of the
Al2O3 with a Nomarski microscope revealed some non-reversible material changes in the Al2O3 which did not cause a
significant increase in the scatter diode signal. However these changes were faintly visible even under Nomarski micros-
copy, due to mirror having a high reflectivity for parts of the visible spectrum. A phase sensitive online detection
scheme, perhaps an interferometric setup, might be a more accurate detection channel for these kinds of damages.

io]

11-1
ig 0,6 c 0,6 41-1'

O fs
r
2 I nrR
S '

rz0,41 100 fs
100 fs 200fs
6opin 1000 fs 1 o 500 fR
-100 fs -100 fs

02 1
-1000 fs
HfO2
-200 fs
-5no fR
Nb2O5
001 '-'1*--11
fin (1'2 nld nlfi n'a 1 'n (1 fl fl 11 d (1 F !1 R 1 (1

Fluence SHG [a. u.] Fluence SHG [a.u.]

c 0,6
Lo
N 0 fs
© 0, 200 fs
500 fs
1 000 fs
-200 fs
-500 fs
Al2O3
.1
1 1

: .

nn n7 na na n'A i'n
Fluence SHG [a.u.]

Figure 5: 1000on1 50 % LIDT values for the HfO2, Nb2O5 and Al2O3 double reflective mirrors. 1000on1 LIDT tests were conducted
for different fluencies and delays between the two pulses. The top left figure shows the results for the HfO2 mirror, top right for the
Nb2O5, and at the bottom the results for the Al2O3 mirrors are depicted. In the insets the respective delays between the two pulses are
denoted. A positive number marks a trailing fundamental pulse, a negative number a trailing second harmonic pulse. Fluencies shown
are normalized to the respective single wavelength damage threshold.

4. CONCLUSION
In this paper, the damage behavior of dielectric high reflective coatings under irradiation with two laser pulses of differ-
ent wavelengths was investigated. Measurements at delays longer than the pulse duration showed a strong dependency of
the LIDT on the pulse sequence. In this case, especially for HfO2 with a conduction band electron relaxation time of
1100 fs, a high population of conduction band electrons is still present when the second pulse arrives. This high density
of conduction band electrons leads to a decreased LIDT. In the case of a trailing fundamental pulse the decrease of the
LIDT is higher than in the inverse case of a trailing second harmonic pulse. Experimental results for the Nb2O5 mirror

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 show a similar behavior, although at shorter delays. For this material, the LIDT is also lower in the case of a trailing
fundamental pulse. Furthermore, for Nb2O5 at delays of 500 fs no interaction between the two pulses was observed. This
indicates, that over this time span a high percentage of electrons already relaxed into lower states. Conduction band
electron lifetime for Nb2O5 should therefore be much less than 500 fs. Experimental results for Al2O3 deviated from the
observed behavior of HfO2 and Ta2O5. Only for delays of 0 fs a clear drop in the LIDT for increasing fluence of the
second harmonic pulse was observed. Other delays showed no clear correlation between the second harmonic fluence
and the LIDT. However, the material exhibited non-reversible changes in the material, which were not observable in the
scatter signal we used for damage detection.

5. ACKNOWLEDGEMENTS
The authors thank the Federal Ministry of Education and Research (BMBF) for the financial support within the research
project Ultra-LIFE under grant 13N11558. This work was also supported by the Volkswagen Stiftung within the research
project “Hymnos” (contract no. ZN3061).

6. BIBLIOGRAPHY

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