In: Lithography: Principles, Processes and Materials ISBN: 978-1-61761-837-6

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Chapter 5

LASER INTERFERENCE LITHOGRAPHY

Henk van Wolferen and Leon Abelmann

MESA+ Research Institute for Nanotechnology,
University of Twente, Enschede, The Netherlands

ABSTRACT
In this chapter we explain how submicron gratings can be prepared by Laser
Interference Lithography (LIL). In this maskless lithography technique, the standing
wave pattern that exists at the intersection of two coherent laser beams is used to expose a
photosensitive layer. We show how to build the basic setup, with special attention for the
optical aspects. The pros and cons of different types of resist as well as the limitations
and errors of the setup are discussed. The bottleneck in Laser Interference Lithography is
the presence of internal reflection in the photo-resist layer. These reflections can be
reduced by the use of antireflection coatings. However the thicknesses of these coatings
depends on the angle of exposure and the material property or combination of materials
in thin films. We show with some examples how to deal with this issue. Finally we show
examples of more complex patterns that can be realized by multiple exposures.

1. INTRODUCTION
In 1801 Thomas Young established the wave theory of light by means of his famous
double slit experiment. This experiment showed the effect of the interference of light in
beautiful colors.
Humphrey Lloyd describes in 1843 the use of a mirror to show interference of light.
In 1891 Nobel Prize winner Gabriel Lippmann used interference of light to create the first
color photograph. For this he used a glass plate with a fine grain high-resolution
photosensitive layer (Lippmann-emulsion film) in contact with a high reflecting (mercury)
surface as a mirror.
Dennis Gabor published the first hologram in 1948 as “A New Microscopic Principle”
based on interference. In 1960 Theodore H. Maiman demonstrated the first functioning laser
134 Henk van Wolferen and Leon Abelmann

at Hughes Research Laboratories. This was the start of using interference as a useful tool to
measure distances, speed and accelerations but also to create holograms as shown by Emmett
Leith at the Optical Society’s 1964 Spring Conference. The laser found its way into more and
more applications.
In 1967 P.H. Langenbeck[4] used a laser as a source for the Lloyd’s interferometer for
flatness testing over a large surface. Around 1970 several researchers were experimenting
with photoresist to create holograms and diffraction gratings, and holographic or Laser
Interference Lithography was born. Ever since, the Lloyd’s Mirror Interferometer has been
used to either push the limits of lithography or to create a simple setup to create high-
resolution line patterns on almost any surface structure. The depth of focus is unique in the
world of lithography. Not just a few microns but millimeters or even meters are possible in
Laser Interference Lithography. There are also disadvantages like the difficulty in aligning it
to another structure.
In the last 40 years the Lloyds’ Mirror Interferometer has been used as a lithography tool
for many applications. It started as a flexible tool to use to make gratings for coupling into
optical waveguides. The double exposure at 90º and 60º found its application in magnetic
recording[6], micro sieves[8] and 2D-photonic crystals[9].

2. THEORY
When two laser beams from the same source coincide, an interference pattern is created
as illustrated in figure 1. Their intensity and phase relation result in a holographic pattern
consisting of dark and bright spots containing all information about the two interfering
beams.
The intensity I r of this spot can be described by

Ir = I1 + I2 + 2 I1I2 × cosϕ Equation 1.[1]

where φ is the phase difference between the two beams at that particular place. The phase
difference φ is due to the angle between the two coherent laser beams. The two laser beams
will only interfere over a distance where their phase-relation is constant. This distance is
called coherence length and depends on the bandwidth of the laser. If the wave-front of the
laser is free of any distortion, we obtain structures of lines with a well-defined spacing: a
diffraction- or Bragg-grating.
The period of this periodical structure Λ is

λ Equation 2.
Λ=
sin(θ1 ) + sin(θ 2 )

where λ is the wavelength of the laser and angle θ1 and angle θ2 are the angles between the
normal of the exposed surface and the beams 1 and 2, as is indicated in figure 1. The intensity
of the grating is sinusoidal and can be used for different applications. In the following we will
discuss the lithographic ability of this sinusoidal interference pattern by exposing it to a
photosensitive layer, either positive or negative.
 Laser Interference Lithography 135

Figure 1. Interference of two coherent laser beams

3. INSTRUMENTATION
The design of a laser interferometer for resist exposure is relatively simple, at least
compared to state of the art mask e-beam lithography systems. In this section, we discuss the
choice for the laser and optical path design.

3.1. Choice of Laser

A holographic setup to create 1, 2 and 3 dimensional gratings consists of respectively 2 or

3 or 4 beams from the same laser source coinciding at the same place under a given angle.
The application and the spectral sensitivity of the substrate will be decisive for what type of
laser will be suitable. The wavelength of the laser should match the sensitivity and absorption
of the substrate. At the same time, the coherence-length should be long enough to overcome
the optical path length difference. Pulse lasers have a short coherence length in the range of
their pulse length, whereas Continuous Wave (CW) lasers have a very long coherence-length.
CW- laser have the additional advantage in that it is easy to control the exposure dose by
changing only the exposure-time. Light will only interfere with their polarization vector in the
same direction; therefore a polarized laser will give the best result.
Basically two instrumentation architectures are found for Laser Interference Lithography:
the Lloyd’s Mirror Interferometer, which is used for high resolution, and the Dual Beam
Interferometer, which is used for large areas.
136 Henk van Wolferen and Leon Abelmann

Figure 2. Lloyd’s Mirror Interferometer

3.2. Lloyd’s Mirror Interferometer

The simplest interference pattern to realize is a Bragg grating. This can be made with a
so-called Lloyd’s Mirror Interferometer that is composed of a laser with a long coherent
Gaussian beam, a lens, a pinhole and a mirror. The mirror is placed perpendicular to the
exposed surface (substrate) to create the second beam (see figure 2). If the substrate and
mirror are placed on a rotating table the period of the Bragg grating can be easily and
accurately changed. The lens and the pinhole are placed into the beam path to create a
diverging beam. The laser beam should be s-polarized: the reflected and direct beams must
have their polarization vector in the same direction to have optimal interference.
The beam centre is aligned at the intersection of the mirror and the substrate. The
Gaussian beam should be symmetrically aligned over the substrate and mirror to have
intensity I1 equal to intensity I2.
At the intersection of mirror and substrate the angle θ1 and angle θ2 are equal. Away from
the mirror the period will have an error because angle θ1 and angle θ2 are not equal. The angle
θ1 and angle θ2 will change in relation to the diverging beam angle α.

α = θ1 − θ 2 Equation 3.

We can calculate this error by using a sine-rule and rewriting equation 2 to:

λ
Λ= Equation 4.
⎛θ + θ ⎞ ⎛θ − θ ⎞
2⋅ sin⎜ 1 2 ⎟⋅ cos⎜ 1 2 ⎟
⎝ 2 ⎠ ⎝ 2 ⎠

The period Λ will be:

λ
Λ= Equation 4.
2⋅ sin(θ )

where θ is the angle at the intersection of mirror and substrate and the error is
 Laser Interrference Lithoggraphy 137

1
Error = 100⋅ (1 − )% E
Equation 5.
cos( α 2)

This error can

c be broughht to zero by ussing a hyperboolic concave mirror
m to creatte a parallel
beeam where α = 0º.
The Lloyd’’s Mirror Interrferometer is considered
c to be
b a “one beam m interferomeeter”. Since
thhe mirror close to the subbstrate createss the second beam, only optical path differences
beetween the miirror and substtrate give rise to a disturbedd interference pattern.
p

Fiigure 3. The Llo

oyd’s Mirror innterferometer onn a vibration conntrolled table with
w air shield inn the authors
laaboratory

To avoid optical path differences, airflowa over the mirror and

a substrate should be
minimized. Ad
m dditional distuurbance of thhe interferencce pattern duue to vibratioons can be
reeduced by plaacing the compplete setup onn a vibration-iisolated table or on a very solid floor
(FFigure 3). Of course,
c the rottation table shoould be drift free
f during expposure.
The exposure area EA of the Lloyd’s Mirror Inteerferometer iss limited by size s of the
m
mirror Mx , Myy and the rotatiion angle θ:

M My⋅ tan((θ ) .
EA = Mx⋅ E
Equation 6.

Since opticcally flat, big mirrors

m are exxpensive and difficult
d to hanndle, the expossure area is
ussually limitedd to a few squuare cm. Moreeover, dust paarticles on thee mirror will disturb the
innterference patttern. The mirrror should havve a perfect sm mooth surface with no tiny holes
h in the
reeflecting surfaace, so dielectrric mirrors aree to be preferreed.
138 Henk van Wolferen and Leon Abelmann

3.3. Dual Beam Interferometer

If a larger area is to be exposed a Dual Beam Interferometer setup is required. In a dual

beam setup the laser beam is split into two beams. See figure 4. The two beams are expanded
and filtered by a pinhole and both have to be aligned to the substrate. Their intensity and
Gaussian profile should be the same and overlap at the substrate and their optical path length
difference should be within the coherence length of the laser.

Figure 4. Dual Beam interferometer with beam-splitter BS and mirrors M1 and M2

The two beams in the Dual Beam interferometer have different optical paths. This
difference makes the dual beam setup more sensitive to airflow. This airflow will give a phase
difference between the two beams and the interference pattern will fluctuate. A phase-
correction system is needed to compensate any change in phase due to this airflow. The phase
difference should be measured close to the substrate. The airflow will also change the wave
front. The wave front cannot be corrected and therefore it is recommended to use a cover
shield to minimize any possible airflow (as in figure 3). Despite the cover shield, still very
slow and small airflows will remain so a phase-correction system cannot be omitted. The dual
beam interferometer needs more time to build and maintain. If you want to change the grating
period Λ the setup has to be rebuilt and re-aligned. For 2D structures the substrate has to be
placed on a rotating table itself and for 3D structures a more complex setup with more laser
beams has to be made.

3.4. Requirements on Beam Size and Shape

The laser beam has a Gaussian intensity, which will give rise to a variation in exposure
dose over the substrate. By expanding the laser beam to a size of 5 times the exposed area this
variation will be reduced to 10%. The radius of a diverging Gaussian beam W(z) at a large
distance z can be calculated with:

λ⋅ z
W ( z) = Equation 7.
π ⋅ W0
 Laser Interrference Lithoggraphy 139

where W0 is thee radius of the beam at focus point and λ is

w i the wavelenngth of the laseer.
To steer thhe beam fromm the laser to thet substrate at the right position highlyy reflecting
m
mirrors are useed. Due to imppurities in thee optical path, like dust on the steering-mmirrors and
laaser-output, th
he wave front of the Gaussiian beam will be disturbed.. This wave frront can be
coorrected by ussing an opticaal filter consissting of a lenns and a pinhoole. The diam meter of the
piinhole Dp is giiven by

4⋅ λ ⋅ f
Dp = E
Equation 8.
π ⋅ wb

Fiigure 5. Focus in
i pin hole

where wb is thee radius of thhe laser beam and f is the focal

w f length of
o the focusingg lens. The
ennergy of the laser
l beam is very high at focus. Standard pinholes will w melt or at a least get
daamaged by thiis high energyy. Commerciall available pinnholes for highh-energy appllication can
reesist energies up to 70MW Watt/cm2. Whhen focusing a laser how wever, the cenntre of the
G
Gaussian beamm is overriding this value eassily. The alignnment of the pinhole
p shouldd always be
doone with low energy, but mostm lasers willl change theirr beam path when w set to low
wer energy,
w
which severely complicates thet alignment procedure.
Another prroblem is that these pinholess are more like a pipe insteaad of just a hoole. (A 5um
hiigh-energy pin nhole has for instance
i a thicckness of 15umm.) At the focal point, the laaser should
fit into this pin--pipe instead of
o just a pin-hhole (see figuree 5). The widtth of the focussed beam at
thhe entrance of the pipe can beb calculated from:
f

1
⎡ ⎛ λ⋅ z ⎞2 ⎤ 2

w(z) = w 0 ⎢1+ ⎜ 2⎟
⎥ E
Equation 9.
⎢⎣ ⎝ π ⋅ w 0 ⎠ ⎥⎦

Lens aberration will deffocus the spot and filtering might becomee impossible, therefore a
well-corrected microscope
w m leens should be used.
u
The above considerationn can be illusttrated by the design calcullations for ourr setup. To
exxpose a 10 cmc substrate with
w a Lloydd’s Mirror Intterferometer we
w use a 2666 nm laser
coombined withh a UV corrected microscoppe lens with a focus f=11.553 mm. The high-energy
h
piinhole has a diameter
d Dp of
o 5 um and a thickness off 15 um. To get the beam through
t the
140 Henk van Wolferen and Leon Abelmann

pinhole with maximum energy and optimum beam shape we need to expand the beam to a
radius wd of 1.5 mm to achieve a w0 of 0.55 um. The beam diameter at the entrance of the pin-
pipe will be 4.5 um. To achieve a maximum intensity variation of 10% over a 10 cm wide
substrate and mirror at θ=45o the laser beam should be expanded to a size of 5 x 10 cm x √2 =
71 cm. This means that the substrate has to be placed at z=460 cm away from the pinhole. At
z=460 cm the effective diverging beam angle α is atan(14/460) = 1.75º. The maximum error
in period Λ at θ=45o will be not more than 0.01%

4. PHOTO-RESIST EXPOSURE
The intensity pattern in the diffraction grating is transferred to a photoresist layer. Since
the angle of incidence of the light, as well as the wavelength, deviate from main-stream
lithography, selecting the type of photoresist and the correct thickness is far from trivial. By
using multiple exposures, more complex patterns than gratings can be realized.

4.1. Reflections and Standing Waves

The interference pattern created by the direct beam and the beam reflected from the
mirror in the Lloyd setup is shown in figure 6a. A second interference pattern, caused by
surface reflection is shown in figure 6b, and causes undesired standing waves in the vertical
direction. This is especially a problem for highly reflecting layers such as silicon or metals.

Figure 6. Reflection at surface

Figure 7. Modulation depth by interference between reflected and direct beam

 Laser Interference Lithography 141

The period of this vertical standing wave pattern is Λ = λ (n ⋅ 2 cos(a sin(sin θ n)))
where n is the refractive index of the material. The reflectivity of the substrate is depending
on the material property n and k and the angle θ and can be calculated with ellipsometry
software.
The intensity profile or modulation of standing waves can be calculated from eq.1, where
I1 and I2 are not equal. The modulation depth M is:

4⋅ I1 ⋅ I2
M = ⋅ 100% Equation 10.
I1 + I2 + 2⋅ I1 ⋅ I2

where I1 is the intensity of direct beam and I2 is the intensity of the beam reflected by the
substrates. See figure 7.
A standing wave like this exists of knots and bellies. The knot is always at or close to the
high reflecting surface, so there is no or little light close to the reflecting surface.
A high modulation depth might lace up the photoresist too much at the reflecting
interface and the resist pattern will fall over. Silicon substrates reflect over 60% at an angle θ
= 0º and even more at larger angles. To reduce these reflections we can add an extra layer
between the photoresist and the high reflective substrate: a so-called Bottom Anti Reflection
Coating (BARC). To prevent the light from bouncing inside the photoresist layer a second
anti reflection layer can be added on top of the photoresist. This Top Anti Reflection Coating
(TARC) acts on the same principle as the BARC.
For optimal control of the standing waves both anti-reflection-coatings should be applied.
How the antireflection layer works is explained in the next paragraph.

4.2. Anti Reflection Coating

To prevent reflection an extra layer can be added between the substrate and the photo-
resist. This layer should absorb the light and/or reflect it with a phase-shift π. At any
transition of materials with different refractive index n light will reflect in relation to
Fresnel’s Law:

⎛ n1 − n2 ⎞2
r =⎜ ⎟ Equation 11.
⎝ n1 + n2 ⎠

Figure 8 shows the antireflection layer with refractive index n2 on a substrate with
refractive index n3 in an environment with refractive index n1.
142 Henk van Wolferen and Leon Abelmann

Figure 8. Reflection at an antireflection layer

The optical path length in the antireflection layer will give a phase shift Ԅ. The phase
shift Ԅ is depending on the angle of incident θ, the refractive index difference between n1 and
n2, the thickness of the antireflection layer h and the laser-wavelength λ:

2⋅ h⋅ n2
φ=
⎡ ⎛n ⎞⎤ Equation 12.
λ ⋅ cos⎢a sin⎜ 1 ⋅ sin θ ⎟ ⎥
⎣ ⎝ n2 ⎠⎦

If the intensity of the reflection from transition n1-n2 is equal to the intensity of the
reflection from transition n2-n3 and the phase difference Ԅ is an odd number of π: the total
reflection is canceled out.
Commercially available BARC’s uses a combination of absorption and phase-shift. This
combination makes these BARC’s less critical to the substrate surface parameters n and k.
BARC in UV-Lithography is made for 3 wavelengths: the 365 nm wavelength (i-line), 248
nm (KrF) and 193 nm (ArF). These BARC’s are made for direct use on silicon or metal
surfaces. If the laser has another wavelength, the BARC might not work properly. For
example, the Brewer Science DUV52D is optimized for 248 nm and has a minimum
reflection around 60 nm thickness. The setup in the authors’ lab operates at 266 nm, where
the minimum reflection is at 170 nm. See figure 9. The reason for this is that the refractive
parameters of DUV52D at 248 nm are n = 1.9 and k = 0.43. The refractive parameters at 266
nm however are n = 2.07 and k = 0.23. The imaginary refractive index k is much lower at 266
nm and therefore the absorption is less and the BARC-layer is less efficient.
Figure 10 shows the effect of BARC-layer thickness from 5, 10, 20, 30, 40 and 50nm in
positive photoresist on a high-reflective silicon substrate with the same exposure dose. From a
series of experiments like this, the optimum BARC layer thickness can be selected. In
positive-resist the exposed resist is resolved in the developer. When the BARC-layer
thickness increases the reflection becomes less and the structures become thicker at the
bottom waist. From calculations we expected that 40nm of BARC-layer thickness should give
the optimum effect. The effective phase shift would be π. Unfortunately there is a knot at the
 Laser Interrference Lithoggraphy 143

innterface betweeen photoresisst and the BAR

RC-layer and due to the thrreshold there is
i a residue
off photoresist, as can be seeen in figure 10. The BAR RC Layer is hard
h to remove without
daamaging the structure. Therrefore a lower thickness of BARC-Layer
B s
should be appplied.

Fiigure 9. Reflecttion at the BAR

RC Layer at 248 nm and 266 nm
m

Fiigure 10. Positiv

ve photoresist with
w BARC layeer thickness varriation from 5 too 50nm
144 Henk van Wolferen and Leon Abelmann

Figure 11a. 30nm BARC at different layers

Figure11b. 100nm BARC at different layers

When using optically transparent (thin) layers the results of the calculations change, as
well as using different incidence angles, as is shown in figures 11a and b. In experimental
environments the parameters of the layers are not exactly known or even reproducible.
Optical calculations are therefore a good starting point, but the BARC-layer thickness often
needs to be optimized by experiment.
 Laser Interference Lithography 145

4.3. Selection of Photoresist

For a line pattern like the Bragg grating it is not important whether a negative or a
positive resist is used. Photosensitive layers in general are defined by their spectral
sensitivity, photosensitivity, contrast and threshold. The minimum intensity to activate the
photoresist is called the threshold. The spectral sensitivity should match the laser wavelength.
Photosensitivity is important in industrial environments to keep the processing time low.
Contrast and threshold are effective on the modulation depth of the resist shape. High-contrast
photoresist will amplify the modulation depth of the resist shape. The threshold will amplify
the modulation depth only in negative resist and reduces the modulation depth in positive
resist. However due to the intensity-knot at the surface there will be some residues of
unresolved positive photoresist (see figure 10b, 11d and 11e). Negative photoresist will have
no residues of unresolved resist left at the surface but might not have enough adhesion to the
substrate (see figure 10a).
If the BARC-Layer is tuned to the correct thickness like in figure 13a the shape of the
structure will always have some imperfections due to roughness, particles in the photoresist or
side effects like bridging in figure 13b.

Figure 12a. Negative resist pattern with reflection (b). Positive resist pattern with reflection

Figure 13a. Good BARC-Layer Thickness (b). Bridging effect in negative photoresist
146 Henk van Wolferen and Leon Abelmann

4.4. Multi Exposure

In a more complex pattern more than one exposure is needed. The desired structure
defines the choice between negative or positive resist. Expanding the Lloyd’s Mirror
Interferometer with a rotating substrate holder opens a whole new world of patterns. Rotating
the substrate over an angle β and expose the substrate a second time creates new patterns like
isolated lines, cubic and hexagonal structures of pillars and holes.
The substrate can be exposed many times. Changing the angle β between 2 exposures is
shown in figure 14b.
Rotating the sample 90 degrees between two exposures with the same period are shown
in figure 15. The pillars are made on a cobalt layer and the holes are made on a SiO2 layer.
The BARC-Layer is optimized to have a clean substrate, not a minimum reflection.
Rotating the substrate 60º results in hexagonal structures. Unfortunately the shape of the
holes of pillars will become elliptical. To make circular holes or pillars in a hexagonal
structure the Lloyd’s Mirror Interferometer should have two mirrors at 120º to each other[5].
All combinations of rotation angle and changing the period are possible until all the
photoresist is exposed. See Figure 16.

Figure 14a. Single exposure (b). Double exposure with 1o rotation

Figure 15. Double exposure with 90º rotation with positive and negative resist
 Laser Interference Lithography 147

Figure 16. Quadruple exposures of two superimposed periods at 60º and 90º rotation in positive resist.

Figure 17. Face centered orthorhombic lattice

It is easy to make a crystal-like structure with different lattices at angles other than 60º or
90º on a Lloyd’s Mirror Interferometer with a rotating substrate holder placed on a rotation
table. Expose the substrate at an angle θ1 for period Λ1, rotate the in a substrate holder over a
defined angle and expose the substrate again at an angle θ2 for period Λ2. To create a face
centered orthorhombic lattice where b = √2a for example, we need a double exposure with
period Λ2 = 1.15 x Λ1 and β = 54.7º. To make such a pattern on another kind of
interferometer will take much more time.

CONCLUSION
Laser Interference Lithography is a flexible tool for lithography to create periodic
patterns in photoresist. The setup is relatively simple, and by using the Lloyd’s Mirror
configuration, periodicities and pattern directions can be easily changed. It is advisable to use
continuing wave lasers. Due to the high intensities used, special care must be taken when
selecting pinholes for optical filtering. Since the angle of incidence and wavelength of the
148 Henk van Wolferen and Leon Abelmann

laser are different from mainstream lithography lines, extra effort has to be put into
optimizing anti-reflection coatings. By using multiple exposures, under varying angles, a
wealth of periodic patterns can be realized which can find their way into many different
applications.

REFERENCES
[1] Optics, Hecht, Zajac, 1984.
[2] Fundamentals of Photonics, B.E.A. Saleh, M.C. Teich, 1991.
[3] The CVI Melles Griot Technical Guide, 2009.
[4] Langenbeck, PH. Applied Optics, 1967, Vol.6, No 10.
[5] Johannus de Boor, Optics Letters, 2009, Vol34, No 12
[6] Haast, MAM. Journal of Magnetism and Magnetic materials, 1999, Vol 193, 1-3.
[7] Van Rijn, Journal of micromechanics and microengineering, 1999, Vol 9, No 2.
[8] Vogelaar, L. Advantage Materials, 2001, Vol 13, 20.