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September 15, 1999 / Vol. 24, No.

18 / OPTICS LETTERS

1311

Infrared photosensitivity in silica glasses exposed to


femtosecond laser pulses
D. Homoelle, S. Wielandy, and Alexander L. Gaeta
School of Applied and Engineering Physics, Cornell University, Ithaca, New York 14853

N. F. Borrelli and Charlene Smith


Glass and Glass-Ceramics Research, SP-FR-3, Corning, Incorporated, Corning, New York 14831
Received May 7, 1999
We investigate the use of infrared femtosecond laser pulses to induce highly localized refractive-index changes
in fused-silica glasses. We characterize the magnitude of the change as a function of exposure and measure
index changes as large as 3 3 1023 and 5 3 1023 in pure fused silica and boron-doped silica, respectively. The
potential of this technique for writing three-dimensional photonic structures in bulk glasses is demonstrated by
the fabrication of a Y coupler within a sample of pure fused silica. 1999 Optical Society of America
OCIS codes: 320.7130, 190.4180, 230.4000, 230.7370, 160.2750.

Exposing a material to light can induce permanent


changes in its properties. An important technological example of this effect is UV irradiation of glasses,
which produces changes in the refractive index as a
result of densif ication or of the formation of defect
centers in the exposed region. The magnitude of the
index change is found to depend on the exposure
conditions and on several properties of the glass,
including dopants and preparation.1 Such photosensitivity is responsible for revolutionizing fiber communications systems, since it allows for the fabrication
of Bragg gratings and other photonic devices within
fibers.2 Nevertheless, fabrication techniques involving UV photosensitivity are, for the most part, limited to the production of one- and two-dimensional
structures.
Recent experiments indicate that structural modifications of wide-gap dielectrics exposed to intense IR
femtosecond pulses can be confined to submicrometersized regions.3,4
A critical advantage of using ultrashort pulses relative to longer pulses is based on
the fact that the electrons can acquire significant energy from the pulse before transferring the energy to
the surrounding lattice, which can result in highly localized laser-induced breakdown. Recent experiments
indicated that glasses exposed to such pulses can exhibit photosensitivity similar to that achieved with
UV light.5 Although the physical mechanisms responsible for IR photosensitivity are still under investigation, the process is initiated by a multiphoton
absorption process and therefore exhibits a highly nonlinear dependence on the intensity of the illuminating beam.4,6 This nonlinear dependence on intensity
allows for the fabrication of three-dimensional photonic structures by translation of the sample with respect to the focal point. This idea has been applied to
the formation of waveguides in a variety of glasses7
and to three-dimensional optical storage.8,9 Similar
multiphoton excitation techniques using femtosecond
lasers have also been applied to various photopolymers
as a means of implementing data storage,10 creating
0146-9592/99/181311-03$15.00/0

polymer microstructures,11,12 or fabricating photonic


devices.13
In this Letter we characterize the photosensitive
response of pure and boron-doped fused-silica glasses
as a function of exposure. The refractive-index change
in the glass is determined for various exposure conditions by fabrication of waveguides in the glass and
measurement of the numerical aperture (NA) of the
waveguides. We find under a restricted range of conditions that index changes as large as 3 3 1023 can be
obtained in undoped fused silica and 5 3 1023 in borondoped fused silica. Such a study is important for
determining the optimal conditions for producing
the requisite refractive-index changes for fabricating
photonic devices. An example of the potential of this
technique for creating three-dimensional photonic
structures is demonstrated by the fabrication of a
Y coupler within a sample of undoped fused silica.
A schematic of the experimental apparatus is shown
in Fig. 1. Femtosecond IR laser pulses of 60-fs duration are generated from a multipass Ti:sapphire
amplif ier at a wavelength of 820 nm and a 1-kHz repetition rate. The laser beam is focused into the sample
by a 103 (0.16-NA) single-aspheric-lens microscope objective, resulting in a beam-waist diameter of 5 mm,
and photonic structures are written by translation of
the sample with respect to the focal region by use of
a computer-controlled three-dimensional stage that
has a resolution of 200 nm. The use of this relatively
long-working-distance objective allows us to write
waveguides as long as 2 cm parallel to the beam. A
photograph of the near-field intensity prof ile of the
mode as it exits the waveguide is shown in Fig. 2.

Fig. 1. Schematic of the experimental setup.


1999 Optical Society of America

1312

OPTICS LETTERS / Vol. 24, No. 18 / September 15, 1999

Fig. 2. Intensity profile of the light as it exits the waveguide in the pure fused-silica sample. The inset is the
two-dimensional image of the prof ile. For this case the
waveguide was formed with 1-mJ laser pulses and by scanning of the sample at 20 mms.

For measurements of the index change it would be


convenient to expose a relatively large cross-sectional
area uniformly and perform interferometric measurements. However, attempts to increase the size of the
beam by operating at a smaller NA lead to strong nonlinear self-focusing effects that result in supercontinuum generation14 and inability to control the beam
focus. Thus, to characterize the photosensitive response to IR irradiation, we wrote circular waveguides
similar to those demonstrated in Ref. 7 by translating each sample along the direction of the laser beams
propagation so that the focal spot traversed the entire
length of the piece. Such longitudinal translation of
the sample with a velocity vs causes the focal region
to move through the glass with a velocity veff nvs ,
where n is the refractive index of the glass. Estimates
of the resulting refractive-index changes were made by
subsequent coupling of light from a He Ne laser into
the waveguides and measurement of the NA of the
cone of light that emerged. The NA of a step-index
waveguidep is related to the induced index change Dn
by NA 2nDn for small Dn. Since in our setup the
length of the waveguide was typically 1 cm, unguided
light from the focused He Ne beam interfered with the
light coupled out of the waveguide, which resulted in
an interference pattern of concentric rings in the far
field. The radius at which the fringes fade depends
on the NAs of the coupling lens and the waveguide;
by measuring this radius we could estimate the NA of
the waveguide. We estimate that the error in our measurements of the NA is approximately 30%.
Using this measurement technique, we characterized the induced refractive-index change in two silica
glasses as a function of pulse energy and translation speed of the sample. The results of measurements performed on pure and boron-doped 9%B2 O3
91%SiO2 samples are summarized in Table 1. We determined the waveguide diameter through inspection
transverse to the waveguide under an optical microscope, and in all cases the diameter of the waveguides
was approximately 3 mm and appeared to have a minimal dependence on incident pulse energy and translation speed. Under optimal conditions, the largest
index changes achieved 1023 are comparable with
the largest changes produced by use of UV-exposure
techniques. We estimated the total IR exposure required for producing the index changes by assuming

a diffraction-limited input beam, in which case the


single-pulse f luence F for a 1-mJ pulse is 4.7 Jcm2 ,
and each point of the waveguide was exposed to a
total f luence of Ftot fbF veff 3.6 kJcm2 for a
pulse repetition rate f 1 kHz, a confocal parameter
b 77 mm, and a translation speed vs 100 mms.
The largest measured index changes were comparable
with those measured previously,7 but the changes reported here were observed with a substantially lower
repetition rate and a correspondingly smaller total
f luence.
For the boron-doped sample the exposure required
for producing the same degree of index change was
signif icantly less than for the pure fused silica. This
point is illustrated by comparison of the exposure
required for producing the characteristic double-lobed
far-f ield pattern, which corresponds to the excitation of
higher-order guided mode. (In Table 1, this condition
is denoted by a dagger.) For a simple step-index
waveguide the threshold condition for the appearance
of the second mode is given by 2prNAl 2.4. We
measured the NA at the onset of the double-lobed
pattern to be 0.08, and at the wavelength of 633 nm
this value would correspond to a wavelength radius of
3 mm, which is within a factor of 2 of the observed
size. In both glasses the response of the material
saturated, and attempts to produce index changes
larger than the saturation value either by an increase
of the pulse energy or by a reduction of the translation
speed resulted in damaged waveguides that did not
eff iciently guide light. When it was viewed under
a microscope, this damage appeared similar to that
described by Glezer et al.8
A comparison can also be made of the relative
sensitivity of the two samples at an exposure energy of
2 mJ. The double-lobed pattern was initially observed
in the boron-doped sample when the translation speed
was 100 mms, whereas it did not appear in the pure
sample until the speed was slowed to 10 mms. An
alternative comparison is to look at the induced index
change for the same exposure. At an exposure of 2 mJ
and a translation speed of 100 mms, the induced index
change was 100 times larger.
For an explanation of this difference one would
need to understand the exact mechanism by which the
Index Changes Dn3103 in Boron-Doped
(Left) and Pure (Right) Fused
Silica for Various Energies and Scan Speedsa

Table 1.

Energy mJ
Speed mms
5
10
20
50
100
200
400

0.5

1.0

2.0

4.0

, 0.5
,
2y ,
0.8,
0.1,
,
,

, 3y
3y , 1
4y , 0.07
3y ,
1,
1,
,

,
5y , 3y
3y , 2y
4y , 0.3
3, 0.03
1,
1,

,
,
, 3y
,
4y , 0.8
2,
1,

a
These values are calculated from the measured NAs of the
waveguides. , damaged tracks; , Dn too small to measure;
double-lobed pattern at 633 nm.

September 15, 1999 / Vol. 24, No. 18 / OPTICS LETTERS

Fig. 3. Y coupler drawn in a bulk sample of pure fused


silica guiding 514.5-nm light from an argon-ion laser.
The scattered radiation from the coupled argon-ion light
is observed in the photograph. The vertical direction
is magnified with respect to the horizontal direction for
clarity. The structure was drawn at a pulse energy of 1 mJ
and a scan speed of 30 mms.

index change is produced. Toward this end, we investigated the possible role of laser-induced densification
as a source of the refractive-index change.15 As a
result of the induced volume change, stresses develop that are manifested as birefringence. If one
assumes that the densification is uniform within
the cylindrical volume, one can calculate the relative
magnitude of the induced density change, drr, from
the observed birefringence. For light propagating
in the axial direction the birefringence is given by
dn 2Bs, where B is the stress-optic coefficient
and s is the induced stress. For this simple geometry one can relate the stress to the densification by
the expression s E61 2 ndrr, where E is
Youngs modulus and n is the Poisson ratio. The
refractive-index change that would accompany this
computed density change15 in fused silica amounts to
only 10% of the value obtained from the waveguiding estimate mentioned above. On the other hand,
independent measurement of the 193-nm excimerlaser-induced densification rate of the boron-doped
sample showed a 20-fold increase in refractive index
relative to that of a pure fused-silica sample,16 which
follows the same trend as that reported here. Another
similarity with UV densification is that the induced
index change can be annealed out at 800 C. One
possible explanation for the low value inferred from the
birefringence measurement is that the densification
pattern is not a pure cylinder, which could result in a
smaller measured birefringence.
The waveguides demonstrated here can serve as the
constituent building blocks for more-complex optical
circuits. To illustrate the possibilities of this technique we produced a waveguide Y coupler in a bulk
sample of pure fused silica. This structure is shown
in Fig. 3 guiding 514.5-nm light from an argon laser.
The relative coupling into the two branches depends
strongly on their splitting angle, and in this case the
splitting angle of 0.5 results in approximately equal
amounts of light into the two branches.
In summary, we have characterized the refractiveindex changes induced in pure and boron-doped fused

1313

silica by exposure to femtosecond IR laser pulses.


We found that although the boron-doped sample is
more sensitive to exposure, the maximal induced index
change is comparable with that of the undoped glass
and similar to what has been reported for UV exposure.
Our fabrication of a Y coupler in a bulk sample of
pure fused silica is indicative of the potential for using
femtosecond laser pulses to fabricate more-complex
photonic devices.
D. Homoelle, S. Wielandy, and A. L. Gaeta acknowledge support from the National Science Foundation through Cornell Center for Materials Research
grant DMR-9632275 and through grant PHY-9722575.
A. L. Gaetas e-mail address is a.gaeta@cornell.edu.
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