Subwavelength proximity nanolithography using a plasmonic lens

Sungkyu Seo,a兲 Hyun Chul Kim, Hyungduk Ko, and Mosong Cheng
Department of Electrical and Computer Engineering, Texas A&M University,
College Station, Texas 77843-3128
共Received 10 June 2007; accepted 8 October 2007; published 7 December 2007兲
This article presents a novel device, the plasmonic lens 共PL兲, consisting of equally spaced ring
apertures in a metal film deposited on a fused silica substrate. It was fabricated by electron-beam
lithography 共EBL兲 and reactive-ion etching 共RIE兲. When illuminated by a collimated laser, a
cylindrical surface plasmon 共SP兲 is excited in the PL, scattered by the structure, and propagates. As
a result, the PL focuses a subwavelength spot in the midfield, i.e., the focal length is several microns.
The authors experiment demonstrated that 90–300 nm spots 共up to ␭ / 4兲 with pitches of 400–500
nm, focal length of 1.7 ␮m, were printed by a PL using 405 nm laser. The authors
three-dimensional electromagnetic simulation predicted a full width at half maximum 共FWHM兲 of
210 nm, equivalent to an aberration-free lens having an unity numerical aperture 共NA= 1兲. The
experimental result agreed well with the simulation. A theoretical model is also presented. Given its
small footprint and subwavelength resolution, the PL holds great promise in direct-writing and
scanning microscopy. © 2007 American Vacuum Society. 关DOI: 10.1116/1.2804517兴

I. INTRODUCTION ported are similar to contact lithography except that they

Subwavelength imaging in a diffraction-limited system
can be achieved via a variety of means such as apodization,1
confocal microscopy, and liquid immersion microscopy
and/or lithography.2 Recent progress in nanofabrication tech-
niques provides alternatives to these techniques by creating
subwavelength apertures that can excite the optical near-field
with lateral dimensions much shorter than the wavelength.
However, the issues associated with the light emerging from
these subwavelength apertures, such as very low transmis-
sion and diffraction toward all directions, make them effec-
tive only within a fraction of a wavelength from the
apertures.3 This creates particular difficulties in lithography,
which needs to pattern a resist layer of a certain thickness in
the presence of topographical variation of the wafer. In other
words, an effective lithography technique must provide a sat-
isfactory working distance 共WD兲 and depth of field 共DOF兲. It
was proposed that the near field can be enhanced by a sur-
face plasmon 共SP兲 excited on a metal layer whose dielectric
constant is negative.4 Since then, subwavelength plasmonic
imaging techniques, which promise higher transmission and
confinement of the near-field, have been widely investigated.
A SP is an electromagnetic surface mode excited on the in-
terface between a metal and a dielectric material.5 The SP
decays exponentially in both the lateral and axial directions.
Meanwhile, the wavelength of the SP can be shorter than the
corresponding light. Thus, the imaging resolution using the
SP can be much higher than the diffraction limit. The SP, as
a result of collective oscillation of free electrons in metal, is
much stronger than the near-field directly created by a sub-
wavelength aperture.6 This means the plasmonic imaging has
much higher throughput than conventional near-field optics.
The plasmonic imaging techniques that have been re-
a兲
Electronic mail: seo_sungkyu@tamu.edu
insert a metal film, e.g., silver or aluminum, between a mask
and a resist layer7–9 or deposit a titanium 共Ti兲 shield on a
sample10 to improve the resolution. For example, a 60-nm
hole array was patterned with I-line illumination.11 Blaikie
et al. demonstrated that 250-nm resolution in proximity li-
thography with a mercury lamp when a silver film was in-
serted between the mask and the wafer.12 Zhang et al. re-
ported a novel superlens that images a nano object in near
field.13 Although SP structures have been used to create a
strong near-field as small as 25 nm, the distance between the
mask and resist 共the WD兲 is still within a fraction of the
wavelength due to the decay of the SP in the axial
direction.14,15 The small WD creates great difficulties in
overlay and alignment, mask contaminations, focusing, and
dose control, which severely limit the manufacturability.
The effects of the SP in far-field have also been studied.
Researchers demonstrated that SP resonant structures, e.g., a
periodic texture on the exit side of an aperture in a metal
film, can enhance the transmitted lightwave and confine it to
a small divergence angle.16–19 The propagation of the SP to
the far-field is attributed to it being scattered by surface
structures on the metal.20
In this article, we report on a proximity lithography tech-
nique that uses a plasmonic lens 共PL兲 to print sub-100 nm
features in the “midfield,” i.e., the PL focuses the incident
light to a spot narrower than the diffraction limit with a focal
length of several wavelengths. The PL consists of equally
spaced ring apertures in a Ti film on a fused-silica substrate.
Both simulation and experiment showed that the PL focused
a collimated violet laser beam 共␭ = 405 nm兲 to write sub-100
nm spots with 400–500 nm pitch located 1 − 5 ␮m away
from the PL. The device structure, model, fabrication pro-
cess, and direct-writing experiment are detailed later.

2271 J. Vac. Sci. Technol. B 25„6…, Nov/Dec 2007 1071-1023/2007/25„6…/2271/6/$23.00 ©2007 American Vacuum Society 2271
2272 Seo et al.: Subwavelength proximity nanolithography
II. DESIGN AND MODELING
For simplicity, consider a two-dimensional SP on the xz
plane. Denote the z axis as the optical axis and the x axis as
the lateral direction. Then the wave number of the SP in the
x direction is given by
ksp,x = k0冑␧m␧d/共␧m + ␧d兲, 共1兲
where k0 is the wave number in free space and ␧m and ␧d are
the relative permittivity of the metal and dielectrics, respec-
tively. In the spectra of interest, ␧m is a complex number
whose real part is negative. The wavelength of the SP in the
lateral direction is given by ␭sp,x = 2␲ / Re兵ksp,x其.
When the light frequency approaches the plasmon fre-
quency of the metal, Re兵ksp,x其 can be significantly higher
than k0; so ␭sp,x is much smaller than ␭0, the wavelength in
free space. That is to say, the SP can have higher lateral
resolution than the light due to its engineered larger wave
vector ksp,x共⬎k0兲 achieved by selecting the absolute value of
the negative dielectric constant of the metal matching the
positive dielectric constant of the dielectrics.11 Moreover,
Im兵ksp,x其 ⫽ 0, which means that the SP decays exponentially
in the lateral direction. This further reduces its spreading,
resulting in even higher resolution.
However, the SP is also localized in the axial direction. Its
wave number in the z direction in the dielectric material is
given by ksp,z = k0␧d / 冑␧m + ␧d. So the SP decays exponentially
in the z direction. For the most interesting plasmonic metals
such as Au and Ag, the SP practically vanishes within ␭0 / 2.
So the SP cannot be used directly in proximity lithography.
To this end, a propagating SP is needed, which can be ob-
tained by disturbing it with apertures or nanoparticles.20 We
further conjectured that if a SP had a cylindrical or spherical
symmetry, it should tend to converge or diverge. Thus, we
constructed a plasmonic structure, named a PL, which con-
sists of a set of concentric ring apertures in a metal film
deposited on a fused silica substrate. Being illuminated, the
rings excite a cylindrical SP. The SP is then disturbed by the
apertures and becomes a propagating wave that still has cy-
lindrical symmetry and converges in the midfield.
The design of a plasmonic lens is shown in Figs. 1共a兲 and
1共b兲. The width of the rings is a and the inner and outer radii
of the nth ring are given by Rn,inner = nr − a / 2 and Rn,outer
= nr + a / 2, respectively. We chose titanium as the metal be-
J. Vac. Sci. Technol. B, Vol. 25, No. 6, Nov/Dec 2007
2272
FIG. 1. 共a兲 Cross-section and 共b兲 top-down views of the
plasmonic lens design 共drawings are not to scale兲.
cause it has a smaller imaginary term of ksp,zd than Ag or Au
at ␭ = 405 nm. We simulated the optical field exiting a
simple PL that has only one ring, a = 150 nm, r = 3 ␮m, us-
ing TEMPEST, a finite-difference time-domain 共FDTD兲
Maxwell equation solver, using four Itanium-2 processors on
an SGI Altix 3700 supercomputer. To select the optimized a
and r in a Ti film, we performed a number of numerical
simulations by changing the width and the radius of ring, and
the thickness of the Ti film. Each node of the simulation
domain was set as 20 nm 共⬃␭0 / 20兲. The dielectric constants
of Ti and silica were chosen as ␧Ti
= −2.22+ j6.66 and ␧Silica = 2.16, respectively.21 The exit sur-
face of the PL was placed on the plane z = 0. Assuming a
circularly polarized coherent plane wave, ␭ = 405 nm, nor-
mally incident on the backside of the silica, the simulated
light field is graphed in Fig. 2共a兲. It shows that the wave
propagating along the optical axis has three axial maxima
within the simulation domain, located at z = 1.6, 2.2, and
3.2 ␮m. The full width at half maximum 共FWHM兲 of the
beam at these axial maxima is 210 nm, comparable to a. The
distance between an axial maximum and the exit surface of
the PL is defined as its focal length. As in other optical sys-
tems, the light-field distribution on the image plane can be
defined as its point-spread function 共PSF兲. The PSF of a
diffraction-limited system with a circular aperture pupil is
known as the Airy pattern and the diameter of the main lobe
is given by 1.22␭ / NA, where NA is the numerical aperture.22
The FWHM of the Airy pattern is 0.52␭ / NA. The normal-
ized PSF of the PL on the focal plane z = 1.6, 2.2, and
3.2 ␮m are compared in Fig. 2共c兲. The FWHM of this
simple PL at z = 3.2 ␮m is calculated as 210 nm, equivalent
to 0.52␭, indicating that the PL is equivalent to a lens with
NA= 1. But the side lobes are higher than the Airy pattern,
indicating energy leakage from the main lobe. This effect
also appears in the apodization.1
Figure 2共b兲 graphs the light field on the exit surface of the
PL. The light transmitting through the rings excites cylindri-
cal SP waves, and the interference of the SP waves with the
zero-order transmitted wave forms a circular standing-wave
pattern, shown as the many concentric rings in the graph. In
a cylindrical coordinate system 共r , ␪ , z兲, the SP has a mag-
netic field along the ␪ axis and an electric field along the r
and z axes. The components of the SP are given by23
2273 Seo et al.: Subwavelength proximity nanolithography 2273

FIG. 2. Simulations of the 共a兲 optical field exiting a plasmonic lens and 共b兲 light field on the exit plane of this PL. The PL has one ring, a = 150 nm, r
= 3 ␮m. 共c兲 Comparison of the PSF at different planes, z = 1.6 ␮m 共dashed line兲, 2.2 ␮m 共dotted line兲, and 3.2 ␮m 共solid line兲.

Hsp,␪ = 关C1H共1兲 共2兲

1 共ksp,r兲 + C2H1 共ksp,r兲兴exp共jksp,zz兲,
III. PROXIMITY NANOLITHOGRAPHY

ksp,z To fabricate the PL structure, first a 100-nm-thick Ti film

Esp,r = Hsp,␪ , was deposited on a fused-silica substrate via dc sputtering
␻␧
with 3200 V / 40 ␮A under a pressure of 2 ⫻ 10−6 Torr.

Esp,z =
␻␧ r
冉
j Hsp,␪ ⳵ Hsp,␪
+
⳵r
, 冊
where ksp,r and ksp,z are the SP wave numbers in the r and z
directions, respectively; ksp,r = k0冑␧m␧d / 共␧m + ␧d兲, and ksp,z in
the dielectric is given by ksp,zd = k0␧d / 冑␧m + ␧d. H共1兲
1 and H1
共2兲
are the Hankel functions of the first and second kind, corre-
sponding to outward and inward traveling cylindrical waves,
respectively. C1 and C2 are the amplitudes. Due to the film
thickness and apertures, there also exist a zero-order trans-
mitted wave and wavelets directly transmitted through the
apertures. The resulting field in air, shown in Fig. 2共a兲, is the
summation of the fields diffracted by the apertures and the
disturbed propagating SP.
共2兲
Then an UV5 resist 共Shipley兲 was spun on the Ti. The spin-
ning took 60 s at 5000 rpm, followed by soft baking for 60 s
on a 135 ° C hotplate, which resulted in a 120-nm-thick re-
sist layer. Next, electron-beam lithography 共EBL兲 共JEOL
T330, adapted for EBL兲 was performed with a 0.04 ␮C / cm
line dose to write the apertures in the resist. The substrate
was then postexposure baked for 90 s at 135 ° C on the hot-
plate and developed in the mixture of MF312:H2O 共1:1.2兲
for 30 s. A 10-min hard baking in the 130 ° C convection
oven was done for better etching selectivity. Then, the un-
protected Ti was etched by reactive-ion etching at 1.2
⫻ 10−5 Torr with Ar 共3 sccm兲/CHF3 共30 sccm兲/He 共7.5
sccm兲 gases for 6.5 min at 350 W power. Finally, the resist
layer was stripped by AZ300T at 95 ° C for 15 min.

JVST B - Microelectronics and Nanometer Structures

2274 Seo et al.: Subwavelength proximity nanolithography
FIG. 3. SEM image of the PL used for the exposure experiment, consisting
of four rings in a 100-nm-thick Ti film, the ring width a = 150 nm, and the
inner radius of the first ring r = 3 ␮m.
Figure 3 shows a scanning electron micrograph 共SEM兲 of
the fabricated PL, which has four rings in a 100-nm-thick Ti
film with the parameters of a = 150 nm and r = 3 ␮m. A
proximity nanolithography system, depicted in Fig. 4, was
built to evaluate PL. A silicon wafer spin-coated with propy-
FIG. 5. 共a兲 AFM and 共b兲 section analysis of the developed spots in the resist, FWHM= 92 nm, with 0.13 mJ/ cm2 dose. 共c兲 AFM and 共d兲 section analysis of
spots exposed with 0.17 mJ/ cm2 dose, FWHM= 119 nm. The pitch was 500 nm.
J. Vac. Sci. Technol. B, Vol. 25, No. 6, Nov/Dec 2007
2274
FIG. 4. Experiment apparatus to record the optical field emanating from a
plasmonic lens. A gap of several micrometers is maintained between the PL
and resist.
lene glycol methyl ether acetate 共PGMEA兲-diluted S1805
共S1805:PGMEA= 2:1兲 positive resist 共at 7500 rpm for 40 s兲
was mounted on a Melles Griot six-axis nanopositioning
stage. A PL was mounted above the wafer. A 5-mW violet
laser 共␭ = 405 nm兲 was used to expose the resist through the
2275 Seo et al.: Subwavelength proximity nanolithography
FIG. 6. SEM of the developed spots, diameter 300 nm, and pitch 400 nm.
PL and a red light-emitting diode 共LED兲 共peak wavelength of
650 nm兲 was used with a charge coupled device 共CCD兲 cam-
era to observe and align the wafer/PL. Before exposure, the
gap between the PL and wafer was calibrated using the red
LED. The PL-wafer-beam splitter-CCD setup can be consid-
ered a Michelson interferometer using quasimonochromatic
illumination.22–24 We first made the PL and wafer in firm
contact by tuning the z axis, ␪x,ROLL, and ␪y,PITCH, and ob-
serving the fringe patterns until the pattern became uniform.
Then, the gap was adjusted to the desired value by tuning the
z axis. A step-and-expose process was conducted to print the
desired pixels. After developing the resist in the diluted
MF312 共MF312:H2O = 1:1.2兲 for about 10− 15 s, the spot
patterns provided “snapshots” of the PSF on the image plane.
Figure 5 shows the atomic force micrographs 共AFMs兲 of
an array of spots written by the PL shown in Fig. 3. Each
spot was exposed with 0.13 mJ/ cm2 dosage and the center-
to-center spacing was 500 nm. The gap between the PL and
resist, i.e., the WD, was 1.7 ␮m. Note that this WD was also
the focal length. Figure 5共b兲 shows the section analysis of the
spots. The spot size 共FWHM兲 was measured and averaged as
92 nm over 100 exposures. Figures 5共c兲 and 5共d兲 show the
spots that resulted from higher exposed energy
共0.17 mJ/ cm2兲, FWHM of 119 nm, and pitch of 500 nm.
Figure 6 shows the SEM of spots printed with a dose of
0.25 mJ/ cm2 and pitch of 400 nm. The spot size was 300
nm. Our simulation showed a FWHM of 210 nm, so the
spots in Fig. 5 may be underexposed, whereas in Fig. 6 they
may be overexposed. The resolved pitch, 400–500 nm under
the condition of coherent illumination, was only achievable
with a lens whose NA is close to unity. So, the printed spot
size and pitch clearly showed that the PL achieved an imag-
ing resolution equivalent to NA= 1.
IV. CONCLUSIONS
Here, we reported that a plasmonic lens that can focus a
subwavelength spot with a working distance 共also the focal
length兲 of 1 to several microns 共␮m兲. Several PLs were fab-
JVST B - Microelectronics and Nanometer Structures
2275
ricated by electron-beam lithography followed by reactive-
ion etching. The PL was used to focus a collimated 405-nm
laser to directly write an array of spots. The developed spot
sizes ranged from 90 to 250 nm when the dose varied from
0.13 to 0.25 mJ/ cm2. The pitches of the spots ranged from
400 to 500 nm. The highest imaging resolution 共90-nm spots兲
is more than a 100% improvement of the diffraction limit
共FWHM= 210 nm兲. A model and three-dimensional electro-
magnetic simulation results were also discussed. The PSF is
attributed to the cylindrical SP wave excited at the Ti/air
interface that is scattered by the apertures and becomes a
propagating wave converging in the midfield. The simulation
predicts a FWHM of 210 nm. So, the 90-nm spots observed
experimentally could be the result of underexposure. Never-
theless, the demonstrated 400-nm pitch with good imaging
quality indicates that the simulated FWHM, which is equiva-
lent to a perfect lens with NA= 1, is reasonable.
The PL, equivalent to NA= 1, has a much smaller foot-
print 共6 − 24 ␮m兲 than a lens or Fresnel zone plate. Thus,
thousands of PL can be integrated on a plate to build a direct-
writing system similar to zone plate array lithography.24 With
coherent illumination, the ultimate half-pitch limit is
FWHM/2, i.e., about 100 nm at ␭ = 405 nm. Partial coherent
illumination can further improve the resolution. The WD of
PL, 1.7 ␮m in our experiment, is much higher than other
plasmonic imaging techniques, allowing for much faster
scanning and alignment, much less danger of physical con-
tact, and thus can provide much higher manufacturability.
ACKNOWLEDGMENT
This work was supported by U.S. Navy-Office of Naval
Research under Contract No. N00014-06-1-0092.
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