Optics and Lasers in Engineering 49 (2011) 605–608

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Optics and Lasers in Engineering

journal homepage: www.elsevier.com/locate/optlaseng

Darkening enhancement in SK3 glass with quartz under irradiation of

femtosecond laser pulses
Kazem Jamshidi-Ghaleh a,n, Erik S. Lotfi b, Hossein Masalehdan c
a
Department of Physics, Azarbayjan University of Tarbiat Moallem, Tabriz, Iran
b
Bonab Engineering and Technology Complex, Bonab, Iran
c
Optics and Laser Engineering Group, Faculty of Physics Engineering and Young Research Club, Islamic Azad University, Bonab Branch, Bonab, Iran

a r t i c l e i n f o abstract

Article history: In this paper, the femtosecond laser-induced darkening in SK3 glass is investigated. A sample with
Received 24 September 2010 3-mm thickness is irradiated with 200 fs laser pulses (FLP) at 800 nm wavelength and 1 kHz repetition
Received in revised form rate. When a piece of quartz or sapphire, which does not show darkening effect under IR irradiations, is
3 January 2011
placed in front of the sample, the laser-induced darkening is enhanced. The directly darkened region in
Accepted 21 January 2011
the sample gets darker on placing a piece of quartz or sapphire in front of the sample. When a piece of
ULE glass that shows darkening effect by IR-FLP irradiations is placed in front of the sample, SK3 sample
Keywords: does not get that dark. We believe the enhancement of the darkening in SK3 glass sample by the quartz
Optical properties modification or sapphire is related to the absorption of the short wavelength component of the white light, which is
Darkening effect
generated and not absorbed in the quartz or sapphire.
Darkening enhancement
& 2011 Elsevier Ltd. All rights reserved.
SK3 glass
Femtosecond pulses

1. Introduction sub-wavelength ripples and micro-voids) that cause the perma-

Focused femtosecond laser radiation can induce highly loca-
lized permanent changes in the chemical and physical properties
of transparent dielectrics allowing femtosecond laser dielectric
modification to be used in fabrication of photonic, and micro-
fluidic components, optical storage, and nanostructures [1–10].
Studies of femtosecond laser modified regions inside various
glasses have identified different regimes as the light intensity at
the focus is increased, viz. the production of: (i) smooth refractive
index changes, (ii) birefringence zones, and (iii) micro-voids
disruptions [1]. The birefringence induced by focused fs radiation
is ascribed either to laser-induced stress, or to the formation of
self-ordered nano-gratings of sub-wavelength periodicity orien-
tated perpendicular to the laser light polarization leading to
anisotropic reflection. This method relies on the use of the
nonlinear multi-photon absorption for coupling the laser energy
into a glass material and allows the photo-writing of three-
dimensional microstructures inside the bulk of the glass. The
darkening effect or formation of color centers, investigated in this
paper, should go to the first regime. But investigation of the
second and third regimes (i.e., formation of nanograting or
n
Corresponding authors.
E-mail addresses: k-jamshidi@azaruniv.edu (K. Jamshidi-Ghaleh),
H.Masalehdan@gmail.com (H. Masalehdan).
nent change has attracted much attention [1–3]. Also, the non-
linear propagation (filamentation) of femtosecond laser pulses in
transparent materials has been investigated [11–13]. This knowl-
edge is highly correlated to the self-focusing and supercontinuum
generation discussed in this paper.
The permanent change needs laser intensities higher than the
glass breakdown threshold [14] but the color centers occur at
intensities well below the glass damage threshold [15–18]. Color
centers appear due to the trapping of the free electrons or holes in
the glass defects and formation of the new energy levels in
forbidden bands of the glasses. The trapped particles exhibit
localized energy levels that typically have absorption bands in
the infrared, visible, and ultraviolet regions, which make the
glass colorful. Color centers are easily distinguishable from persis-
tent laser-induced damage, because thermal annealing of the
darkened sample about 150 1C bleaches the darkened regions [16],
i.e. it erases the induced absorption bands and returns the glass to
its original transparent state without any cracking. The physical
mechanism responsible for the darkening effect in the glasses
under irradiation of IR-laser lights is not exactly clear and there are
two schools of thoughts. Efimov et al. have related the darkening
effect to the direct absorption of IR- multi-photons from femtose-
cond laser light to generating free-carriers in the conduction
band [15]. But Dicenson et al. believe that short wavelength
component absorption of the generated supercontinuum light is
dominant [18]. Also, darkening effect by irradiation of the FLP is

0143-8166/$ - see front matter & 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.optlaseng.2011.01.018
606 K. Jamshidi-Ghaleh et al. / Optics and Lasers in Engineering 49 (2011) 605–608
reported in some silicate glasses [16–19]. However, many aspects
of this effect, is not investigated until now.
In this paper, 200-FLP and 800 nm wavelength at 1 kHz
repetition rate is used to investigate the darkening effect and in
the SK3 glass sample. We have shown that by putting a piece
of quartz or sapphire, which does not get dark itself under
IR-femtosecond irradiations, in front of the sample, darkening
effect enhances. But other glasses that get dark under irradiation
of the FLP weaken the darkening effect in the sample.
2. Experimental setup
Fig. 1 shows the experimental setup used to investigate the
darkening effect and its enhancement in SK3 glass sample.
Irradiation was produced by a Ti:Sapphire CPA laser system
(Spectra Physics) that generates laser pulses with central wave-
length of l ¼ 800 nm and pulse duration of t ¼ 200 ð 7 10Þ fs,
running at a repetition rate of R¼1 kHz with the maximum
available single pulse energy of 450 mJ. A shutter (S) and an
attenuator (A) are used to control the number of incident laser
shots and single pulse energy. Two energy monitor devices (LTB),
one located in front and the other one behind the sample,
measure the input and output pulse energies.
The output of femtosecond laser source is focused with a 0.5 m
focal length lens (L) to form a 260 mm diameter spot, which is
measured by the edge scan method on the sample. With this
optical arrangement, the maximum peak irradiance on the sample
was measured in order of 1012 W cm  2, which is two orders of
magnitude lower than the glass breakdown threshold [14].
A 3 mm SK3 glass sample was placed in a 3D-stage and controlled
with a computer for translation. The sample was processed by
scanning it at the focal point of the lens. To analyze the
Fig. 1. Experimental setup to investigate the darkening enhancement in SK3 glass
sample by a piece of quartz in front of the sample. S: Shutter, A: Attenuator,
L: Lens, BS: Beam Splitter and EM: Energy Meter.
Fig. 2. Optical microscope image of laser-induced darkening in SK3 glass sample with 3-mm thickness at different number of laser shots and pulse energies; created
directly (left) and with 5 mm quartz in front of the sample (right).
experimental results, an optical microscope with 2 mm power
resolution was employed.
3. Results and discussion
Fig. 2 shows the optical microscope images of the visible
darkened sites that are generated in 3 mm SK3 glass sample,
directly (left) and with a 5 mm quartz in front of the sample
(right) at different incident pulse energies and shot numbers. In
each image, rows show different number of incident shots and
columns indicate the incident single pulse energies. It is clearly
seen that for each incident pulse energy and shot number, the
induced darkening is enhanced by the quartz. The area sizes of the
samples that are darkened directly and with quartz increase with
number of shots and pulse energy with a trend that can predict
the pulse energy accumulation model [19].
Even the directly darkened region in the SK3 glass sample gets
darker when a piece of the quartz is put in front of the sample. To
illustrate this, a 3-mm-thick SK3 glass is scanned at area of
5  5 mm2 with 200-FLP at pulse energy of 290 mJ, which is
higher than the darkening threshold. Then, a 5-mm-thick quartz
sample is placed in front of the SK3 sample, exactly over the
directly darkened area, and then a 1  1 mm2 area is scanned
under irradiation of the same incident pulse energy. The scanning
is conducted by zig-zag movement of the sample with a grating
distance of 25 mm, which is more than 12 times smaller than the
beam diameter at the sample (320 mm). The translation velocity is
set to 5 mm/s. As it is seen in Fig. 3, the 1  1 mm2 irradiated area
through the quartz has gotten darker using quartz.
SK3, un-irradiated
SK3, directly irradiated
SK3, irradiated with 5-
mm Quartz in front
Fig. 3. Shows a 1  1 mm2 enhanced darkened area by putting a 5-mm-thick
quartz in front of the 5  5 mm2 directly induced darkening in 3-mm SK3 glass
sample under irradiation of 200 fs laser pulses. The incident pulse energy in both
cases was 330 mJ (500 mJ cm  2).
 K. Jamshidi-Ghaleh et al. / Optics and Lasers in Engineering 49 (2011) 605–608 607

ULE

SK3
Fig. 4. Upper line shows the darkened areas in 5 mm ULE glass in front of the SK3 and lower line are in SK3 sample at different shot numbers (right to left; 2000, 1000, 500,
300, 100, 50, 10, 5, 2, 1). Weakening of the darkening effect in SK3 sample is obviously seen.

100

Fluence Threshold (mJcm-2)

85

70

55

40

25
2.3 2.6 2.9 3.2 3.5 3.8 4.1 4.4 4.7 5
Thickness mm

Fig. 5. Exit spectrum from the quartz and SK3 samples in the UV–vis region at the Fig. 6. Incident laser fluence threshold at different thicknesses for white light
applied laser pulse energy of 250 mJ. generation in SK3 that causes darkening.

We did the same experiment, as the results of Fig. 2, but with a
5 mm ultra low expansion (ULE) glass that shows darkening effect
under irradiation of the FLP in front of the SK3 sample. Fig. 4
shows the results of this experiment at different shot numbers
and 290 mJ incident pulse energy. First line (upper) shows the
darkened sites in ULE and second line (down) in SK3. It is clearly
seen that the darkening effect in SK3 is weakened when ULE is
used in front of the sample.
From results of the above experiments, it seems that putting a
piece of quartz or sapphire (which does not show the darkening
effect under irradiation of FLP) in front of the SK3 sample,
increases the interaction length and causes self-focusing and
supercontinuum generation. It seems that, the short wavelength
components of the generated supercontinuum spectrum, which
cannot be absorbed in quartz (or sapphire) because of the wide
band gap energy, is absorbed in SK3 glass sample by a single or
two photon process. But in the case of ULE, in front of the SK3
sample, the short wavelength components of the supercontinuum
light is absorbed in the ULE and make it dark. Fig. 5 shows the UV
section of the supercontinuum spectrum exited from quartz and
SK3. In the SK3 these components have low intensities (3 times)
when compared to quartz.
Our experimental results show that, when the quartz (or
sapphire) is used in front of the sample for all incident pulse
energies, the darkening begins near the sample surface but in
direct irradiation for lower pulse energies, darkening starts from a
distance inside the sample surface. To check the darkening
dependency on the sample thickness, a sample with an edge
shape (see inset of Fig. 6) is irradiated at different thicknesses
with 200 fs laser pulses, and the threshold fluence that causes
darkening of various thicknesses of the sample is found. Fig. 6,
shows the behavior of the darkening-induced laser fluence
threshold versus the sample thickness. Threshold is defined as
the laser pulse energies that generate supercontinuum and cause
darkening inside the sample. An exponential trend predicts the
threshold.
4. Conclusion
The enhancement of laser-induced darkening in SK3 glass sample
by putting a piece of quartz is investigated. A 3-mm-thick SK3 glass is
irradiated with 200 fs laser pulses at 800 nm wavelength. When a
5 mm quartz that does not show darkening effect under irradiation of
the FLPs is put in front of the sample, the induced darkening is
enhanced. The results show that even directly darkened region gets
darker when a piece of quartz is put in front of the sample. Putting a
piece of other glasses that get dark themselves under FLP, decreases
the darkening in the sample. It seems that a piece of quartz or
sapphire in front of the sample increases the FLP interaction length
and causes self-focusing and supercontinuum or white light genera-
tion. The spectrum of the exit supercontinuum from quartz have
intensive UV component in comparison of the SK3. Short wavelength
components of the white light cannot be absorbed in the quartz or
sapphire (high band gaps materials) but get absorbed in the SK3 glass
sample.
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