Journal of Photopolymer Science and Technology

Volume 29, Number 6 (2016) 849－858 Ⓒ 2016SPST

Review

The Molded Mask Method:

The Origin of Nanoimprint Lithography

Susumu Fujimori

Faculty of Engineering Div. 2,

Tokyo University of Science,
6-3-1, Niijuku, Katsushika-ku, Tokyo, 125-8585, Japan
E-mail: fujimori@rs.tus.ac.jp

This paper describes the invention of the molded mask method in the 1970s, which is
considered to be the origin of current nanoimprint lithography. The molded mask method
was proposed and developed in order to fabricate fine patterns and three-dimensional
structures by combining molding technology and dry etching technology. The concept
was the same as the technology now called nanoimprint lithography. In the 1970s, we
had the idea that even very fine patterns (as small as ten nanometers across) could be
fabricated by the molded mask method based on the similarity of this approach with
specimen preparation for electron microscopy. How the molding mask method was born,
the results of demonstration experiments, and studies conducted in the 1970s to solve
technical problems are described in this paper. Recent progress in and applications of
current nanoimprint lithography are also discussed with reference to the molded mask
method.
Keywords: nanofabrication, nanoimprint, lithography, molding, dry etching

1. Introduction method were conducted about one decade before the

Nanoimprint lithography has been the object of
much research and development in the field of
nanofabrication technology. Many studies have
been conducted worldwide since the 1990s when S.
Y. Chou et al. reported that fine patterns on the order
of 100 nm can be fabricated by imprint technology
(thermal nanoimprint) and C. G. Willson and co-
workers reported that photoresist can be used as an
imprinted material (UV nanoimprint) [1,2]. These
studies are often referred to as the origin of current
nanoimprint lithography. Prior to this, a patent
application by L. S. Napoli and J. P. Russell filed in
1987 claimed an invention similar to nanoimprint
lithography [3].
However, a technology identical to nanoimprint
lithography was proposed and studied in the 1970s
in Japan. The technology was developed as a novel
method to replicate fine patterns and three-
dimensional structures, and was named the “molded
mask method” [4]. Studies on the molded mask
patent by L. S. Napoli was filed and about two
decades before publication of the reports by S. Y.
Chou and C. G. Willson. Therefore, the origin of
current nanoimprint lithography can be traced back
to the molded mask method.
This paper describes the concept behind and the
basic processes of the molded mask method and
compares these with current nanoimprint
lithography. The advantages and disadvantages of
nanoimprint lithography are also discussed with
reference to the molded mask method invented in
the 1970s.
2. Background of the Molded Mask Method
During the 1970s, many electronic device
manufacturers were competing to achieve
high-density integration of electronic
components and photolithography was a core
technology for fabricating fine patterns on Si
surfaces [5,6]. These manufacturers aimed to

Received October 28, 2016

Accepted November 26, 2016
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realize large-scale integration (LSI) with Figure 1 shows the basic concept behind the
submicron patterns. Photolithography, which molded mask method and shows that it is
is based on light exposure through a essentially the same as present-day
photomask and subsequent photographic nanoimprint lithography [4,11-16].
development, was a standard technology for The molded mask method is based on the
mass-producing devices and components with direct contact of the mold to a plastic thin film
fine patterns. However, it was difficult to on a substrate such as a Si wafer. The three-
obtain submicron patterns using dimensional surface structure of the mold is
photolithography because the exposure light replicated to the plastic film by pressing the
cannot be focused to a size smaller than its mold onto the film. In contrast, in
wavelength because of the optical diffraction photolithography, a two-dimensional pattern is
limit [7]. Therefore, exposure to light with a printed on a photoresist film through a
shorter wavelength, such as X-rays or extreme photomask. The size of the pattern printed on
ultraviolet (EUV) light, was widely studied, as the photoresist is limited by the wavelength of
well as electron beam exposure [8,9]. These the exposed light because of optical diffraction,
technologies continue to be studied and whereas the accuracy of the patterns obtained
developed to the present day. in the plastic film in the molded mask method
We believed that EUV- or X-ray-based depends only on the surface shape of the mold,
technologies would be difficult to develop to a which enables the replication of patterns less
practical level because the production than 1 μm in size.
equipment was too expensive. We therefore The following basic processes were devised
sought a low-cost technology and had the idea for the molded mask method in the 1970s.
that the method used to prepare specimens for
electron microscope observation allows for the
replication of very fine structures at low cost.
In electron microscopy, the profile of the solid
surface is often replicated to a thin film of
another material to allow observation by the
electron microscope [10], and even fine
structures on the order of 10 nm can be
observed in specimens prepared by this replica
method. We believed that very fine structures
could be replicated by direct contact of the
original material to a plastic thin film, and that
this simple replication method would be
superior to conventional photolithography,
which is fundamentally limited by optical
diffraction. This was the basis for our molded
mask method.
We conducted feasibility studies in the
1970s on the molded mask method and
demonstrated its technical features and
applicability as a novel technology for
fabricating devices and components [4, 11-16]. Fig. 1. Concept of the molded mask method,
One decade after the invention of the molded reported in 1976 [4,11].
mask method, Napoli and Russell filed their
patent in the United States and another decade 3.1. Fabrication of Plastic Resin Mold
later the studies by S. Y. Chou and C. G. A high-quality master pattern with three-
Willson were reported. Therefore, we can trace dimensional fine structures is prepared in
the origin of nanoimprint lithography back to advance and used as the original mold. The
the molded mask method invented in the 1970s. quality of the master pattern is important in the
molded mask method because it is the primary
3. Concept behind the Molded Mask Method determinant of the quality of the replicated

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pattern.
A plastic resin mold is fabricated from the
master pattern, as shown in Fig. 1(a), and this
resin mold is regarded as the child mold
generated from the parent mold (the original
master pattern). We examined a variety of
plastic materials such as acetylcellulose,
epoxy resin, polyester resin, and
polypropylene as materials for the child mold.
A silicone resin, poly(dimethylsiloxane)
(PDMS), showed the best release
characteristics from the mold and therefore
PDMS was typically used as the material for
making the child mold.
The process of mold fabrication can be
repeated over multiple generations, from the
original parent mold to a child mold, from the
child mold to a grandchild mold, and so on. A
number of molds are prepared in this manner,
greatly decreasing the overall cost of fine
pattern fabrication. Excellent release
characteristics from the mold are necessary, so
that one mold can be used repeatedly.
3.2. Coating of the Mask Material and
Fabrication of the Molded Mask
To fabricate fine patterns on Si wafers,
which are widely used for integrated electronic
components, the Si surface is usually etched
along photoresist patterns by wet etching or
dry etching. The molded thin film on the Si
wafer was regarded as a mask for this etching
process and thus we named this technology the
“molded mask method”.
We usually employed a negative-type
photoresist as the mask material and a Si wafer
as the substrate. The photoresist is coated on
the Si wafer, pressed with the PDMS mold, and
hardened by exposure to UV light. Then, the
PDMS mold is released from the photoresist
film on which the fine patterns are replicated,
resulting in the formation of the molded mask
on the Si wafer substrate, as shown in Fig. 1(b).
The thickness of the concave portion of the
molded photoresist film, called the “residual
layer” in current nanoimprint technology,
should be very thin so that the patterns can be
engraved into the Si surface without losing the
intended pattern shape in the following etching
process.
3.3. Etching
Dry etching technology evolved
considerably in the 1970s [17] and was found
to be suitable for the etching process in the
molded mask method. We utilized plasma
etching or ion etching in most of our
experiments. The molded mask formed on the
Si wafer is etched first, and subsequently the
Si surface is etched in the region where the
concave portion, the residual layer of the mask,
is removed and the underlying Si surface is
directly exposed to an etchant gas. The
patterns in the molded mask are engraved and
replicated onto the Si wafer surface in this
manner. Dry etching techniques such as plasma
etching, ion etching, and reactive ion etching
played an important role in the development of
the molded mask method because they allowed
the directional and selective etching of the
molded mask and substrate, providing high
quality fine patterns on the substrate surface.
After the intended pattern is fabricated on
the Si surface, the residual molded mask is
removed from the Si surface, as shown in
Fig.1(c), by etching with the optimal etchant
for the mask material.
4. Experimental Examples of the Molded
Mask Method
We conducted various experiments in the
1970s to examine the feasibility of the molded
mask method [4,11-16].
4.1. Diffraction Grating
The smallest pattern we could obtain at the
time was a diffraction grating, and thus we first
attempted to replicate planar reflective
diffraction gratings with 300 lines/mm (3.3 μm
pitch), 1200 lines/mm (0.83 μm pitch), and
3600 lines/mm (0.28 μm pitch).
The molded mask method consisted of the
following steps: Fabrication of a mold from the
master pattern (original diffraction grating)
⇒ Coating of mask material on the substrate
⇒ Fabrication of the molded mask ⇒
Etching.
The silicone resin PDMS was used as the
material for the mold because, as described
above, the mold is released readily from the
master pattern. Liquid PDMS was poured onto
the master pattern and covered with a glass
plate. The PDMS was cured, solidified, and
demolded from the master pattern, providing
the PDMS resin mold supported by the glass
plate, as shown in Fig. 2.
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Fig. 2. Preparation of PDMS resin mold [16]. This

corresponds to the process described in Section 3.1
and illustrated in Fig.1(a).

A negative-type photoresist (OMR83, Tokyo

Ohka Kogyo) was used as the mask material
and coated on a Si wafer by spin-coating. The
photoresist film was pressed with the PDMS
mold, then the photoresist was polymerized
and hardened by exposure to UV light.
Demolding the PDMS mold provided the
molded mask on the Si wafer.
Next, the sample was placed in a plasma
etching apparatus and the surface was etched
using gas plasma. The molded mask was Fig. 4. Micro-sized test patterns fabricated by
etched first and after the concave portion of the molded mask method, reported in 1977 [4, 12].
mask was removed, the underlying Si surface
was exposed to an etchant gas plasma and
etched, engraving the grating pattern on the Si
wafer. Figure 3 shows the grating obtained
using this approach and demonstrates that fine
patterns can be replicated by the molded mask
method.

Fig. 5. Surface profiles of master pattern, molded

Fig. 3. Example of diffraction grating replicated on
mask, and Si wafer, reported in 1977 [4,12].
Si wafer (pitch: 3.3 μm), reported in 1976 [4,11].

4.2. Micro-sized Test Pattern

Following the diffraction grating
experiment, the replication of micro-sized test
patterns was also studied to clarify the features
of the molded mask method. The micro-sized
test patterns comprised lines and spaces of
varying width from 1 to 20 μm.
The patterns obtained in this experiment are
shown in Fig. 4 in the order of the process of
the molded mask method: (a) master pattern
(original micro-sized test pattern), (b) PDMS
Fig. 6. Etching rates of the molded mask
mold, (c) molded mask made of photoresist (photoresist) and substrate (Si wafer) [4,16].

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and (d) replicated pattern formed on a Si wafer compared with that obtained using xylene
after dry etching. (boiling point of 140 °C).
The surface profiles of the patterns for each
of the original test pattern, molded mask, and
Si wafer were measured using a stylus-based
profilometer, as shown in Fig. 5. It is notable
that the depths of the replicated patterns on the
Si wafer are larger than the depths of the
original test patterns, indicating that the aspect
ratio of the patterns can be increased by using
the molded mask method. In this experiment,
the etchant gas was CF 4 + O 2 , which can be
used for rapid plasma etching of Si because the Fig. 8. Surface profile of patterns replicated on
etching rate of the Si wafer is higher than that mask material film (molded mask), reported in
of the photoresist. Figure 6 shows the etching 1977 [4,12].
rates of the photoresist and Si wafer in the
plasma etching, resulting in the replicated Improvement in the shapes of patterns
patterns being deeper than the original patterns. replicated to the mask material film is shown
Another result to be noted in Fig. 5 is the in Fig. 9, in which the depth of the replicated
shape of the molded mask: the center of the pattern is plotted against the boiling point of
concave part tends to rise, while the center of the organic solvent.
the convex part tends to indent in the opposite
direction. This tendency becomes more
prominent in wide patterns. When the mask
material is pressed by the mold, it should move
along the pattern of the mold surface. However,
if the mask material is insufficiently fluid, the
pattern of the soft PDMS mold will deform,
leading to replication of deformed patterns on
the mask material film, as schematically
illustrated in Fig. 7. To avoid deformation of
the replicated patterns, the surface of the mold
should be hardened and/or the mask material
should be fluid.
F ig. 9. Depth of pattern replicated on mask
material film (molded mask) versus boiling point
of organic solvent of photoresist, reported in 1977
[4,12].

Next we attempted to harden the PDMS

mold by using a hard polyester resin supported
by soft PDMS as the mold, as shown in Fig. 10.

Fig. 7. Schematic of distortion of pattern shape in

the molded mask fabrication process [4,16].

Accordingly, we attempted to increase the

fluidity of the mask material by adding a high
boiling point solvent to the photoresist. Figure
Fig. 10. Schematic of the mold with polyester resin
8 shows the results of this experiment. The
on the surface supported by PDMS resin [4, 16].
shape of the patterns in the molded mask
obtained in the presence of dichlorobenzene The polyester resin was expected to be
(boiling point of 180 °C) was much improved sufficiently hard to prevent pattern

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deformation when the mold was pressed onto
the mask material film. However, we found
that polyester resin is stiff and not suitable for
pressing uniformly over the entire mask
material film on the Si wafer substrate, and
thus the soft silicone resin PDMS is still used
to support polyester resin with fine pattern on
the surface. This drastically reduces pattern
deformation, as indicated in Fig. 11. This
figure compares the surface profile of the
patterns obtained using the polyester resin to
that obtained using silicone resin (PDMS).
PDMS was also used as a mask material in this
experiment because liquid PDMS film coated
on a substrate is sufficiently fluid to smoothly
move along the pattern of the mold.
Fig. 11. Surface profiles of patterns replicated on
Si wafer substrate obtained from (a) the
combination of soft PDMS resin as a mold and
photoresist film as a mask material and (b) the
combination of hard polyester resin as a mold and
fluid PDMS film as a mask material [4,16].
Schematic of the surface profile for an original
master pattern of micro-sized test pattern is shown
in (c) for reference.
By hardening the mold surface and
fluidizing the mask material film, we
succeeded in greatly reducing pattern
distortion in the mold pressing on the mask
material film. However, we were concerned
that pattern distortion could nonetheless be a
significant drawback to the molded mask
method when both small and large patterns are
to be replicated at the same time. In this
application, a short distance of mask material
854
movement is sufficient for small pattern
replication while a longer distance is needed
for large pattern replication. As a result, the
optimum pressing conditions are different for
small and large patterns.
To avoid this problem, another mask
material coating method was attempted during
our studies in the 1970s [4,12,13]. The mask
material is usually coated on a Si wafer
substrate but in this alternative method it is
coated on the surface of a mold, as shown in
Fig. 12(a). The mask material flows along the
pattern on the mold surface and the concave
portion fills with the mask material while the
surface of the coated mask material film tends
to flatten due to surface tension. A substrate is
pressed and adhered to the flattened surface of
the mask material. After the mask material is
hardened, it is removed from the mold and the
molded mask is obtained on the substrate. The
pressing force in this method is reduced and
thus pattern deformation in the molded mask is
also reduced. An example of a molded mask
formed using this method is shown in Fig.
12(b).
Fig. 12. Molded mask fabrication by another
method in which the mask material is coated on the
surface of the mold, reported in 1977 [4,12]. (a)
Concept of another method: mask material
(photoresist) coated on a mold fills in the concave
part of the patterns, while the surface of the mask
material film tends to be flattened due to surface
tension. (b) An example of the molded mask
fabricated by this method.
We also attempted to use a releasing agent
to separate the molded mask from the mold
 J. Photopolym. Sci. Technol., Vol. 29, No. 6, 2016
more easily, but it was not used in most of our
experiments, because the intrinsic releasability
of the PDMS mold was sufficient to conduct
feasibility studies at that time.
4.3. LSI Photomask Pattern
Many engineers and researchers in the field
of semiconductor devices and components
made great efforts in the 1970s to realize LSIs
with submicron patterns. We attempted to
apply the molded mask method to the
fabrication of LSIs, and particularly to the
fabrication of photomasks used for the LSI
manufacturing process [4,13]. We employed
the LSI test pattern prepared by electron beam
writing as the master pattern (original mold)
and attempted to replicate the LSI pattern onto
a Cr-coated glass substrate widely used as a
photomask at the time. The patterns obtained
in this experiment are shown in Fig. 13 and
confirmed that 2 μm square windows, which
are important in LSI patterns, are formed on
the substrate surface.
Thus, the applicability of the molded mask
method to the LSI fabrication process was
demonstrated.
Fig. 13. LSI patterns fabricated on Cr-coated glass,
reported in 1977 [4,13].
4.4. Three-dimensional Pattern Micro-lenses
Pattern replication by molding technology is
intrinsically the replication of three-
dimensional shapes and thus the molded mask
method was considered suitable for the
fabrication of three-dimensional patterns. We
attempted to apply the method to the
replication of micro-lenses to check the
feasibility of the technology [4, 16]. The
master pattern (original micro-lens) was
prepared by focused ion beam machining.
Figure 14 shows the result of this experiment.
Fig. 14. Replication of micro-lens by the molded
mask method [4, 16]. (a) Second replicated mold
made of polyester resin. (b) Molded mask made of
PDMS resin. (c) Micro-lens pattern finally
obtained on Si wafer surface.
The micro-lens was formed on a Si wafer
surface but its shape was inferior to that of the
mold, as indicated by the difference in the
radius of curvature between the lens on the
molded mask and that on the Si wafer surface.
It was expected that this deterioration in the
shape of the micro-lens can be reduced by
optimizing the dry etching conditions.
Through the above experiments, the feasibility
of fabricating three-dimensional patterns by
the molded mask method was also
demonstrated.
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4.5. Pressing Machine enabling the efficient fabrication of multiple

The molded mask method requires sets of patterns.
fabrication of a molded mask by pressing a
mold onto a mask material film. We therefore
designed and prototyped a pressing machine in
the 1970s based on the configuration of a
conventional mask aligner [4,14,16]. A
schematic of the prototyped pressing machine
is shown in Fig. 15. A mold is fixed at the
upper end and a substrate coated with mask
material film is placed at the lower end of the
press. The substrate is aligned and contacted
with the mold using X-, Y- and Z- axis fine
manipulators. A semispherical movable stage
is used to hold the substrate in order to provide
uniform contact. Then, the substrate is pressed
up to the mold by a piston driven by high-
pressure gas. The gas pressure was typically
changed from 0.5 to 5 kg/cm 2 . The machine
was also equipped with an optical microscope
for sample observation and a UV light
exposure device to harden the photoresist film
as the mask material.
This pressing machine was mainly used to Fig. 16. Step-and-repeat method in molding and
study the relation between the pressing force UV exposure in molded mask fabrication process,
and the pattern-replicated area on the mask described in the patent filed in 1975 [4,14]. The
material film (molded mask). The basic processes of (c) alignment of the substrate with the
concept behind this machine remains mold and (d) UV exposure to harden the mask
applicable to current nanoimprint lithography. material film pressed by the mold are done in the
step-and-repeat manner. Multiple sets of patterns
are obtained on the substrate after the etching
process, as shown in (e).

5. Current Nanoimprint Lithography

Fig. 15. Schematic of the pressing machine for the
molded mask fabrication process [16].
This pressing machine was improved with
the intent of mass production by introducing a
step-and-repeat method into the process of
molding and hardening mask material film,
which was proposed and patented in the 1970s
[4,14]. The processes of aligning the substrate
with the mold, pressing the mold onto the mask
material (photoresist) film, and hardening the
photoresist by UV exposure are done in a step-
and-repeat manner, as illustrated in Fig. 16,
Viewed from the Perspective of the
Molded Mask Method
As described in Sections 3 and 4, the
technology currently known as nanoimprint
lithography is the same as the molded mask
method. The features and problems of
nanoimprint technology were already clear
from our studies on the molded mask method
in the 1970s.
The advantages of the molded mask method
are as follows.
(1) The size of the patterns replicated is not
limited by a physical phenomenon such as
optical diffraction. It may be possible to
replicate patterns as small as 10 nm.
(2) Three-dimensional structures can be
replicated because this method is based on
three-dimensional mold pressing. The
shape obtained after an etching process can
be controlled by the etching condition. It is

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also possible to fabricate patterns deeper
than those of the original mold.
(3) The cost to mass-produce devices and
components with fine patterns is lower
than that of other methods such as EUV and
X-ray lithography because the
configuration of the manufacturing
equipment is less complicated.
(4) This approach is particularly suitable for
fabricating structures composed of simple
repeats of small patterns.
The disadvantages of the molded mask
method are as follows.
(1) Direct contact and pressing by a mold on a
mask material may generate defects in the
molded mask. Defects is a serious problem
even in other methods such as photo-, EUV
and X-ray lithography, and they should be
considered more carefully in the molded
mask method.
(2) The replication of complicated patterns
comprising small and large features may
require some ingenuity. This problem was
basically solved by employing a stiff mold
and a fluid mask material. However,
precise replication of complicated patterns
over a wide area is not easy.
Current nanoimprint lithography has
recently progressed significantly [18-27]. Very
small patterns can be replicated and practical
applications in the manufacture of devices and
components is widespread. The idea of a drop-
on-demand micro dispensing method for the
mask material coating [22], is considered
important because it may solve the problems
encountered in the replication of complicated
patterns.
However, it is necessary to first have a high
quality master pattern as an original mold in
order to make high quality replication by
nanoimprint lithography. It was difficult to
obtain an original mold with very fine patterns
in the 1970s. Now, however, there are various
original molds with fine patterns available for
the development of nanoimprint lithography
owing to progress in nanofabrication
technology, as shown in Fig. 17. These
favorable circumstances will contribute to
further advancement of the technology.
The problem of defects in the molded mask
has been significantly lessened by recent
developments. In the 1970s, most of our
experiments were conducted in ordinary
laboratories and not in a clean room
env iro n men t. Th e defect d en sity will b e
Fig. 17. Examples of original molds for
nanoimprint lithography currently available,
courtesy of NTT Advanced Technology
Corporation.
reduced to an acceptable level by conducting
the processes in current advanced clean room
environments.
Promising applications of nanoimprint
lithography include optical components and
biochips, which have already been
manufactured utilizing this technology. These
include micro-lenses and a moth eye structure
as an anti-reflective surface on displays.
Application to integrated electronic devices
such as NAND flash memory devices is
currently being actively advanced in the LSI
manufacturing industry [18]. It is expected that
further development to reduce defect density
will make this important application
achievable.
6. Summary
The molded mask method invented in the
1970s is an innovative technology that enables
fine pattern fabrication and is unaffected by
the optical resolution limit of photolithography.
The method combines molding technology and
dry etching technology in a creative way. Very
small patterns can be replicated onto a resin
film using molding technology and the
replicated patterns can be engraved into a hard
and brittle substrate such as a Si wafer using
dry etching technology.
This molding technology is suitable for
replicating three-dimensional structures. It
was suggested in the 1970s that small patterns
on the order of ten nanometers can be
replicated based on the resolution of the
replica method used to prepare specimens for
electron microscopy.
Dry etching techniques such as plasma
etching, ion etching, and reactive ion etching
began to be developed in the 1970s, making
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possible directional and selective etching.
These techniques were indispensable in
developing the molded mask method, because
the etching of the molded mask and substrate
is needed to engrave fine patterns onto the
substrate surface.
The utility of the molded mask method was
clearly demonstrated in the 1970s in
experiments using gratings, micro-sized test
patterns, LSI patterns, and micro-lenses.
The advantages and disadvantages of the
molded mask method had been examined in
detail and most of the technical features of this
approach had been clearly demonstrated in the
studies conducted in the 1970s. As seen in this
review, current nanoimprint lithography
originated from the molded mask method
invented in the 1970s.
Recent progress in nanoimprint lithography
is enabling many practical applications, such
as the fabrication of optical components and
LSI memory devices. The utility of the molded
mask method has now been unambiguously
demonstrated through technological
improvements in current nanoimprint
lithography.
Acknowledgements
The author expresses his sincere
appreciation to Mamoru Kondo, Kazutoshi
Nagai, Hiroshi Yasuda, Ken-ichi Kubodera and
everyone involved in the development of the
molded mask method at NTT Laboratories in
the 1970s. The author also expresses
appreciation for the opportunity to publish this
paper.
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