CHIN. PHYS. LETT. Vol. 28, No.

3 (2011) 038101

Fabrication of a Polymer Micro Needle Array by Mask-Dragging X-Ray

Lithography and Alignment X-Ray Lithography *
LI Yi-Gui(李以贵)1** , YANG Chun-Sheng(杨春生)1 , LIU Jing-Quan(刘景全)1 , SUGIYAMA Susumu(杉山进)2
1
Institute of Key Laboratory for Thin Film and Microfabrication Technology of Ministry of Education, Research
Institute of Micro/Nano Science and Technology, Shanghai Jiao Tong University, Shanghai 200240
2
Global Innovation Research Center, Ritsumeikan University, Kusatsu, Shiga 525-8577, Japan

(Received 13 October 2010)

Polymer materials such as transparent thermoplastic poly(methyl methacrylate) (PMMA) have been of great
interest in the research and development of integrated circuits and micro-electromechanical systems due to their
relatively low cost and easy process. We fabricated PMMA-based polymer hollow microneedle arrays by mask-
dragging and aligning x-ray lithography. Techniques for 3D micromachining by direct lithography using x-rays
are developed. These techniques are based on using image projection in which the x-ray is used to illuminate
an appropriate gold pattern on a polyimide film mask. The mask is imaged onto the PMMA sample. A pattern
with an area of up to 100 × 100 mm2 can be fabricated with sub-micron resolution and a highly accurate order
of a few microns by using a dragging mask. The fabrication technology has several advantages, such as forming
complex 3D micro structures, high throughput and low cost.

PACS: 81.16.Nd, 81.16.Rf, 81.07.Oj DOI: 10.1088/0256-307X/28/3/038101

Poly(methyl methacrylate) (PMMA) has a good
compatibility with human tissue and can be used to
replace intraocular lenses for eye treatments. PMMA
is also used in laser disc optical media. The PMMA-
based polymer complex micro fabrication for a de-
vice such as electrostatic combdrive actuator plays
an important role in microelectromechanical systems
(MEMS). Researchers have discovered its application
in precision equipment such as microconveyer systems
and micro motors, etc. The multi-layer polymer mi-
cro fabrication can be applied for a large displacement
actuator and precision sensors[1−6] However it should
be noted that a majority of these combdrive actuators
were fabricated using silicon-based materials or met-
als, and the aspect ratio of these actuators is relatively
low. Some results from the fabrication of a polymer
combdrive actuator have been published by Zhao and
Cui[7] with an aspect ratio of 12:1 using hot emboss-
ing technique. The precise depth of x-ray lithography
can be easily controlled by the exposure dose to en-
able microstructures to be realized. When combined
with the moving mask exposure method, which can
control the exposure energy distribution (i.e. control
or change the total exposure dose for a work piece) full
3D structures can be rapidly formed. In this Letter,
we present a PMMA-based micro needle array fab-
rication process in which a micro needle array with a
throughhole was fabricated using an x-ray lithography
technique with mask dragging and alignment technol-
ogy.
Mask dragging is a powerful technique for structur-
ing surfaces in the fabrication of micro needle arrays,
concave and convex cylindrical profiles, pyramids and
many other surface relief features. Figure 1 shows the
mask dragging technique. Figure 1(a) shows that the
PMMA resist beneath an x-ray mask is dragged dur-
ing the x-ray irradiation. When the mask is triangu-
lar in shape, the irradiated PMMA resist is developed
as a wedge-shape grating (Fig. 1(b)). If the resist is
further dragged perpendicular to the previous direc-
tion (Fig. 1(c)), it can be developed into micro needles
(Fig. 1(d)). If the resist is irradiated by an alignment
x-ray mask with holes (Fig. 1(e)), the resist can be de-
veloped as micro needles with through-hole (Fig. 1(f)).
This idea creates complicated micro structures with a
simple mask.
An x-ray mask with a group of triangle patterns
was used. A PMMA resist as a work piece was set
up at a narrow gap against the x-ray mask. In the
case of mask dragging, when the PMMA is exposed,
the two-dimensional configuration of the mask pat-
tern was transferred to the three-dimensional struc-
ture whose cross-section shape is similar to that of the
mask pattern. The PMMA microneedles with sharp
tips and sloped sidewalls were fabricated by exposing
it again through rotating the resist by 90∘ after the
first exposure.
Alignment exposure is the key process in our fab-
rication method. Due to the transparent polyimide of
x-ray mask, the alignment can be realized by a dig-
ital microscope. In the alignment process, a simple
but low-cost alignment tool made of aluminum was

* Supported by the Shanghai Pujiang Talent Plan Sponsorship (No 09PJ1406200), the International Cooperation Project from the

Ministry of Science and Technology of China (2009DFB10330), Aviation Key Laboratory Foundation of China (No 20080857002),
and National Natural Science Foundation of China under Grant Nos 60777016, 50775149 and 60976081.
** Email: ygli@sjtu.edu.cn

© 2011 Chinese Physical Society and IOP Publishing Ltd

038101-1
 CHIN. PHYS. LETT. Vol. 28, No. 3 (2011) 038101
used as an adjustable PMMA stage, which consists
of a manual 𝑋–𝑌 –𝑍 stage for positioning. Figure 2
shows the exposure chamber with the alignment tool.
The exposure chamber is 0.6 × 0.6 × 0.6 m3 and can
offer two kinds of exposure environment: vacuum (be-
low 1×10−4 Pa) and helium atmosphere (up to 1 atm).
A 0.2-mm-thick beryllium (Be) window, which has a
rectangle aperture of 5×30 mm2 , was used to separate
the ultra-high vacuum section from the low vacuum
section. After passing through the Be window, the
photon energy range was 2–10 keV. The x-ray has a
0.15–0.95 nm wavelength. The x-ray mask was formed
using a 200-µm-thick polyimide as a supporting mem-
brane, a 3.5-µm-thick Au as an x-ray absorber and a
5-inch aluminum square frame with a 4-inch-diameter
circular hole. The total occupied area of Au absorber
on the x-ray mask should not exceed 7.5 × 7.5 cm2 .
The mask is recommended for fabrication of a PMMA
with a depth up to 500 µm.
x-ray
First mask
dragging direction
(a) (b)
Second mask
dragging
direction
(d)
(c)
(e) (f)
Fig. 1. Mask dragging technique. (a) PMMA resist be-
neath an x-ray mask is dragged during the x-ray irradia-
tion. When the mask has a triangle shape, the irradiated
PMMA resist is developed as a wedge-shaped grating (b).
If the resist is further dragged perpendicular to the pre-
vious direction (c), it can be developed into microneedles
(d). If the resist is irradiated by an alignment x-ray mask
with holes (e), the resist can be developed into micronee-
dles with through-hole (f).
Alignment stage
x-ray
Fig. 2. The exposure chamber with the alignment tool.
A schematic view of this alignment is shown in
Fig. 3. A digital microscope (KEYENCE VH8000)
was used to observe the first layer structures through
polyimide layer on the display. The patterns of the
propping pad have a smaller area than patterns on the
mask. Once the patterns on the substrate were hidden
038101-2
under the mask, the alignment was finished and the
stage was locked and fixed. An example for the fab-
rication of microneedle array is shown in Fig. 4. Fig-
ure 4(a) shows the hole mask. Figure 4(b) shows the
fabricated microneedles and Fig 4(c) shows the align-
ment for throughhole microneedle fabrication. The
alignment stage has an alignment deviation of ±3 µm,
which is small compared to the dimensions of the mi-
crostructures. This ±3 µm deviation was caused by a
shift of the stage after a manual lock. The exposed
depth in PMMA depends on x-ray dosage and the
absorption coefficient of the PMMA sheet. Depth of
the structures after developing can be predicted using
deposited x-ray doses. The superconductor compact
storage ring AURORA made in Ritsumeikan Univer-
sity was employed for the exposure. After the align-
ment, the portable stage was set up inside the expo-
sure chamber and dragging x-ray exposure was em-
ployed to avoid the curving surface due to the x-ray
Gaussian intensity distribution of x-ray source.[8]
Digital
microscope
x-ray
mask
100.00 mm
Polymer
Fig. 3. A schematic view of the alignment method.
(a) (b) (c)
Fig. 4. An example for micro needle fabrication: (a) the
hole mask, (b) the fabricated micro needles, (c) alignment
for through-hole micro needle fabrication.
Figure 5 shows the correlation between exposure
dose and the depth of the PMMA microstructure.
Data were collected in experiments with a develop-
ing time of 180 min and a developing temperature of
37 ∘C. The exposed depth in PMMA depends on x-ray
dosage and the absorption coefficient of the PMMA
sheet. The depth of the structures after developing
can be predicted by the deposited x-ray doses. In this
work, the selected dosage was 0.03 A·h, which is close
to the theoretical value. The PMMA sheet was care-
fully left in the developer for 3 h, then in the stopper
again for 15 min and rinsed by purified water for an-
other 15 min. The solution was stirred at a speed of
200 rpm under a constant temperature of 37 ∘C. A fast
 CHIN. PHYS. LETT. Vol. 28, No. 3 (2011) 038101
stirrer speed can destroy the structure and a higher or
lower temperature can cause a higher internal stress
in the PMMA structure. The rationale behind devel-
oping the PMMA at 37 ∘C is that in the future we will
use the PMMA as a template structure for making
a mold by nickel electroplating. The ideal tempera-
ture of a nickel-sulfamate bath is 37 ∘C at a pH of 4–5
and a low current density. A higher or lower temper-
ature can cause a higher internal stress in the PMMA
structure. A long developing time (about 8 h) will be
required to form the hole.
400 Development time 180 min
300
Depth (mm)
200
100
0 3 µm were achieved with the assistance of microscope
0.00 0.02 0.04 0.06
Dose (ASh)
Fig. 5. Correlation between exposure dose and the depth
of the PMMA micro structure.
(a) (b)
Through-hole
500 mm
Fig. 6. Correlation between exposure dose and the depth
of the PMMA micro structure.
Figure 6 shows the fabricated microneedle array
with throughhole. Figure 6(a) shows the microneedle
array from top view. In Fig. 6(b) the rear side image
shows that through-holes were fabricated. Since the
correclation between the x-ray dosage and the process-
ing depth was not linear, the fabricated structure de-
creased the height when compared with the designed
height and a little deform occurred in the the devel-
oping process. Considering the influence of the x-ray
diffraction due to a 30µm-gap between LIGA mask
and the PMMA resist plate, the structures became
sticky when the fabrication pattern was less than 3 µm
in width. Moreover, the simulation of the intensity
distribution shows that the rough structure in the bot-
tom can also be affected by the diffraction.
A hollow microneedle array was fabricated on a
PMMA plate using the dragging x-ray lithography
technique and the alignment x-ray lithography. The
advantages of this method are that most of the pro-
cesses can be performed at room temperature and the
PMMA structure has less stress and higher flexibil-
ity when compared with other 3D micro structure on
silicon or polysilicon. The production of hollow mi-
croneedle arrays with a pore size of 30 µm was con-
firmed. PMMA etching thickness was varied with ex-
posure dose, developing time and temperature. Drag-
ging mask x-ray lithography resolutions of around
0.08 0.10 and custom-made alignment tool. Mask dragging is
the unique method for parallel patterning 3D struc-
tures into surfaces and creating an almost unlimited
variety of different features and shapes.
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