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Sub-10-nm nanolithography with a scanning helium beam

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In this article, a pattern definition technique for dense sub-10-nm structures is presented, in terms of high resolution, high sensitivity, and a low proximity effect in a hydrogen silsesquioxane resist.
Abstract
Scanning helium ion beam lithography is presented as a promising pattern definition technique for dense sub-10-nm structures. The powerful performance in terms of high resolution, high sensitivity, and a low proximity effect is demonstrated in a hydrogen silsesquioxane resist.

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Sub-10-nm nanolithography with a scanning helium beam
Vadim Sidorkin
a
Kavli Institute of Nanoscience, Delft University of Technology, Lorentzweg 1, Delft 2628 CJ,
The Netherlands
Emile van Veldhoven
TNO Science and Industry, Stieltjesweg 1, Delft 2628 CK, The Netherlands
Emile van der Drift, Paul Alkemade, and Huub Salemink
Kavli Institute of Nanoscience, Delft University of Technology, Lorentzweg 1, Delft 2628 CJ,
The Netherlands
Diederik Maas
TNO Science and Industry, Stieltjesweg 1, Delft 2628 CK, The Netherlands
Received 13 April 2009; accepted 23 June 2009; published 24 July 2009
Scanning helium ion beam lithography is presented as a promising pattern definition technique for
dense sub-10-nm structures. The powerful performance in terms of high resolution, high sensitivity,
and a low proximity effect is demonstrated in a hydrogen silsesquioxane resist. © 2009 American
Vacuum Society. DOI: 10.1116/1.3182742
I. INTRODUCTION
With the ongoing trend toward miniaturization and ever
higher device performance, the need for controlled realiza-
tion of sub-10-nm dimensions is becoming increasingly im-
portant. For several decades, the mainstream lithography of
choice for defining nanostructures has been electron beam
lithography. In a long sequence of developments e.g., the
field emission gun, 100 kV acceleration voltage, / 4096 la-
ser interferometry, and 16-bit or higher digital-to-analog con-
verter technology, the electron beam technique has reached
the nanometer precision needed for sub-10-nm performance
in resist. Rather than the control and accuracy of the beam
writing process, the limiting factors are turning out to be the
electron-resist interactions in conjunction with the resist de-
velopment. We propose that scanning helium ion beam li-
thography SHIBL is the next step. In particular, low prox-
imity effects, in combination with the demonstrated high
sensitivity and resolution, make SHIBL a promising technol-
ogy for nanopatterning in the sub-10-nm regime, although
He ion impact on semiconductor nanodevice structures may
not always be harmless.
1
In the past, focused ion beam lithography FIBL has been
a somewhat less important player in the field of nanolithog-
raphy. Most work in the field of FIBL has been performed
using either a scanning beam or an ion projection approach,
which is based on Ga
+
ion sources. Even fewer beam studies
deal with light ions such as Be
+
,H
+
,H
2
+
, and He
+
.
24
An
early overview was given by Melngailis.
5
Besides the advan-
tages of higher sensitivity and lower proximity effects
6
com-
pared to the electron beam approach, major disadvantages of
the earlier FIBL work are a lower resolution due to a larger
beam diameter and certainly with respect to Ga+ion expo-
sure potential damage or contamination from the ion impact
Ga implantation
7
. High-resolution FIB tools have been
available for about 2 decades. Features including a 12–15 nm
linewidth in polymethyl methacrylate兲共PMMA resist
8
and
a 30 nm dot size in polyphenylsilsesquioxane resist
9
have
been reported. Today, the smallest probe size of Ga
+
ion
beams is typically around 5 nm, and direct engraving in a 20
nm thick membrane material yields nanopores as small as 3
nm in diameter.
10
Recently, scanning helium ion microscopy
11
with a he-
lium probe size of 0.75 nm in diameter was launched in the
market. In the work described here, we used the scanning
He
+
ion beam setup as a beam writing tool for nanolithogra-
phy and compare its performance with electron beam expo-
sure behavior. The expected advantages of SHIBL over elec-
tron beam lithography EBL comprise of reduced proximity
effects and the ability to write smaller features given the
subnanometer probe size. The former is due to a more direc-
tional scattering profile of He
+
ions and the different second-
ary electron SE generation mechanisms with ions in resist,
which causes a high yield of slow SEs.
1114
Altogether, these
characteristics greatly suppress the blurring background that
arises when writing dense patterns with EBL.
II. EXPERIMENT
A Carl Zeiss Orion™ Plus scanning helium ion micro-
scope and an FEI Strata DB 235 scanning electron micro-
scope SEM, both operating at 30 kV, were used for helium
ion beam and electron beam exposures, respectively. The FEI
setup and a Hitachi S4800 SEM were used for the inspection
of the developed structures. Especially, the latter imaging
setup is superior in contrast and resolution due to its sophis-
ticated system to handle the secondary and backscattered
electrons. A concise discussion of high-resolution scanning
electron and helium ion microscopy was published
recently.
15
Dose variations were achieved by means of the
beam current and by controlling the dwell time per pixel,
which varied from 20 to 2000
s.
a
Electronic addresses: v.a.sidorkin@tudelft.nl and sidorkin_vadim@mail.ru
L18 L18J. Vac. Sci. Technol. B 274, Jul/Aug 2009 1071-1023/2009/274/L18/3/$25.00 ©2009 American Vacuum Society
Downloaded 14 May 2013 to 131.180.131.253. Redistribution subject to AVS license or copyright; see http://avspublications.org/jvstb/about/rights_and_permissions

This work deals with exposures in hydrogen silsesquiox-
ane HSQ resist from Dow Corning FOx-12 product on
silicon substrates. Resist thickness was achieved by tuning
the spin speed Karl Suss RC 5/8 and by appropriate dilu-
tion of HSQ with methyl isobutyl ketone. Typically, 1:10 and
1:1 dilutions are used for thicknesses of 5 and 55–70 nm,
respectively. All resist films were dried for 30 min in vacuum
at room temperature in order to minimize film roughness.
16
Two types of experiments were conducted. In the first
type, the exposure sensitivity is measured for both EBL and
SHIBL in HSQ films of 70 nm thick using a defocused
beam in a dose range from 0.1
C/ cm
2
to 1 mC/ cm
2
. Pat-
terns used for that purpose were 50 50
m
2
squares. After
development in MF 322 developer Rohm & Haas for 1
min, the height of the structures was measured by means of
profilometry Tencor. Sensitivity values were obtained as
the dose D
s
necessary to achieve 50% of its original thick-
ness after development. Contrast values were determined ac-
cording to the procedure of Thompson.
17
In the second type of experiments, high-resolution He
+
beam spot exposures were performed in 5 and 55 nm thick
layers of HSQ. Exposures were performed with a fine probe
size,a1pAbeam current, and a dwell time of 100
sat
20
m aperture and 7 mm working distance. A single imag-
ing raster scan was used, resulting in the formation of arrays
of dots with a variable pitch. The field of view FOV was
2525
m
2
and the numbers of pixels were 256 256,
512512, and 1024 1024, resulting in pitches of 98, 47,
and 24 nm, respectively. In one exposure, the FOV was 15
15
m
2
with 10241024 pixels, resulting in a pitch of
14 nm. A droplet of Au nanoparticles 共⬃20 nm in diameter
was placed directly on the resist surface, which allowed the
ion beam to be focused accurately in situ prior to the actual
writing in resist. After development for 5 min MF351 from
Rohm & Haas and immersion in a “stopper” solution
MF351: H
2
O=1:9, samples were rinsed with de-ionized
water and blown dry in nitrogen.
III. RESULTS AND DISCUSSION
A. Contrast and sensitivity
Residual HSQ film thickness dependencies after develop-
ment on helium ion beam and e-beam exposure dose are
shown in Fig. 1. The results demonstrate that HSQ resist is
4.4 times more sensitive for helium ions D
s
=313
C/ cm
2
than for electrons D
s
=1375
C/ cm
2
, whereas the contrast values are practi-
cally the same
=2.10.1 for both types of exposure. The
difference in sensitivity between SHIBL and EBL can be
partly due to the higher yield of SE for helium ions com-
pared to electrons of the same energy.
11
Additionally, the
resist sensitivity is further enhanced because in He
+
ion ex-
posure the fraction of low-energy SE is higher. The same
contrast for both EBL and SHIBL indicates similar molecular
weight distributions of cross-linked resist monomers. It is
solely the yield and energy distribution of the SE that differ.
The higher sensitivity of HSQ for He
+
than for electron ex-
posure is relatively moderate compared to the sensitivity en-
hancement by factors of 100–300 in PMMA under Ga
+
,He
+
,
H
+
, and Ar
+
exposure
18
and 16–50-fold enhancement in a
range of other resist products under He
+
ion projection
lithography.
19
Recent work on H
+
beam writing of HSQ at
MeV ion energy exposure shows a sensitivity of
3.2
C/ cm
2
,
20
which drops to about 20
C/ cm
2
sensitivity
upon HSQ resist aging. The difference between the values
from these studies and those obtained in our experiment with
helium ions could be due in part to differences in experimen-
tal conditions. Beam type and energy, initial thickness,
21
de-
velopment time, developer type, concentration, and
temperature
22
have been known to have a substantial impact
on the sensitivity of the resist. However, additional impact
from a different exposure mechanism cannot be ruled out.
B. Minimal feature size and proximity effect
SEM images of an array of isolated dots at a pitch of 98
nm in 5 and 55 nm thick HSQ films are shown in Figs. 2a
and 2b, respectively. The average dot diameters are 6 1
and 141 nm, respectively. These results prove the He
+
ion
beam capability for nanostructuring in ultrahigh resolution
mode. In both cases the exposure dose 100
s dwell time
per pixel and the development time 5 min were the same.
FIG. 1. Normalized thickness of HSQ resist film as a function of dose for
helium ion beam and electron beam exposures at 30 keV. The thickness was
normalized prior to the development. The sensitivity D
s
and contrast values
s
are shown in the inset.
FIG. 2. SEM images of arrays of dots written in a 5 nm and b 55 nm
thick HSQ layers at 98 nm pitch using scanning helium ion beam lithogra-
phy. Field of view is 900 nm in SE mode at 20 kV. Average dot diameters:
a 6 1 nm and b 14 1nm.
L19 Sidorkin et al.: Sub-10-nm nanolithography with a scanning helium beam L19
JVSTB-MicroelectronicsandNanometer Structures
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Nevertheless, the dot size for the thicker layer is about twice
as large as the thinner one. This observation corresponds
with previous results for electron beam exposure of HSQ
films of different thicknesses. Lines 2 pixels wide written
with an e-beam in 5 and 55 nm thick HSQ have linewidths of
11 and 24.5 nm, respectively,
21
when processed under iden-
tical exposure and development conditions but different
from the current He ion experiments. To our knowledge, the
best results in e-beam exposure of HSQ are currently 6 nm
lines on a pitch of 20 nm written at 100 keV.
23
The dot size as a function of pitch is shown in Fig. 3.
Remarkably, an identical dot size of 6 1 nm was achieved
down to a pitch of 14 nm see Fig. 3d. This observation
indicates an undetectably small proximity effect for helium
ion beam exposure. Several factors may be involved in this
low proximity effect. First, the scattering profile of helium
ions is known to be confined within a narrow cone penetrat-
ing relatively deep into the material with very low
backscattering.
11
Second, helium ions produce mostly low-
energy SE 20 eV, when derived from H
+
data on CO
2
,
scaled to the same velocity
14
, which do not travel far in the
resist.
Finally we need to address two other aspects in this work.
First, the exposure dose of 1 pA for 100
s corresponds to
about 600 ions/dot. The inherent shot noise implies a dose
uncertainty of 4%/dot. Although the insets in Figs. 3a3c
show dot-to-dot size irregularities, a possible relation to shot
noise is not likely, given the contrast curve in Fig. 1. The
observed nanometer scale irregularities touch on the second
aspect related to the minimum achievable feature size in
HSQ resist, where several factors play a role. Irrespective of
the writing probe size, HSQ studies in literature
23
and this
work indicate absolute lower limits of about 5–6 nm for
HSQ structures. Adhesion to the substrate becomes too low
with decreasing feature size in order to withstand the force
interactions during the wet development step. In addition, the
number of cross-linked resist monomers decreases with
shrinking feature size. Consequently, at some minimum fea-
ture size the contrast in the exposed area is too low to “sur-
vive” the development. Future work to test this size limit
hypothesis could deploy special patterns, wherein the ul-
trafine features are attached to larger scale structures that will
provide sufficient mechanical stability. With its negligible
proximity effect, SHIBL seems to be the best exposure tech-
nology by far to realize the ultimate limit in this matter.
IV. CONCLUSION
Scanning He
+
ion beam lithography on HSQ is demon-
strated to have very a high resolution and a superior low
proximity effect. Furthermore, He
+
ion exposure is several
times more effective than electron beam exposure at the
same acceleration voltage, whereas the contrast is equal.
Overall, He
+
ion beam lithography is a very promising tech-
nique for the formation of ultrahigh resolution structures of a
high density and having feature sizes in the sub-10-nm
range.
ACKNOWLEDGMENTS
This research is part of NanoNed, a national research pro-
gram on nanotechnology funded by the Ministry of Eco-
nomic Affairs in The Netherlands. Ping Cheng, Kees Hagen,
and Pieter Kruit are acknowledged for their contributions to
this work.
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FIG. 3. SEM images of arrays of dots written ina5nmthick HSQ layer
using SHIBL at pitches of a 48 nm, b 24 nm, and c 14 nm, and d the
average dot size vs pitch. The insets are SEM images at a higher magnifi-
cation. The average dot size for all pitches is 6 1nm.
L20 Sidorkin et al.: Sub-10-nm nanolithography with a scanning helium beam L20
J. Vac. Sci. Technol. B, Vol. 27, No. 4, Jul/Aug 2009
Downloaded 14 May 2013 to 131.180.131.253. Redistribution subject to AVS license or copyright; see http://avspublications.org/jvstb/about/rights_and_permissions
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References
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Using high-contrast salty development of hydrogen silsesquioxane for sub-10‐nm half-pitch lithography

TL;DR: In this article, the authors used a mixture of salt and alkali to significantly increase the contrast of hydrogen silsesquioxane (HSQ) for negative-tone electron-beam resist.
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A model of secondary electron imaging in the helium ion scanning microscope

TL;DR: A combination of the 'semi-empirical' model for secondary electron production and the TRIM routines, has been used to construct a Monte Carlo simulation that can quantitatively interpret the generation of secondary electrons from materials by fast helium ions.
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Sub-5nm FIB direct patterning of nanodevices

TL;DR: In this article, the authors detail the advanced methodology for sub-10nm nanodevices fabrication using a high-performance FIB instrument. But they do not discuss the application of the FIB system to nanoengraving of membranes.
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A low magnification focused ion beam system with 8 nm spot size

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TL;DR: The use of focused ion beams for fine pattern writing was examined in this paper, where it was shown that the ability to write original patterns at 0.1 µm and below is a serious candidate for future fine pattern rewriting.
Related Papers (5)
Frequently Asked Questions (11)
Q1. What are the contributions mentioned in the paper "Sub-10-nm nanolithography with a scanning helium beam" ?

The authors propose that scanning helium ion beam lithography SHIBL is the next step. Most work in the field of FIBL has been performed using either a scanning beam or an ion projection approach, which is based on Ga+ ion sources. In particular, low proximity effects, in combination with the demonstrated high sensitivity and resolution, make SHIBL a promising technology for nanopatterning in the sub-10-nm regime, although He ion impact on semiconductor nanodevice structures may not always be harmless. Besides the advantages of higher sensitivity and lower proximity effects compared to the electron beam approach, major disadvantages of the earlier FIBL work are a lower resolution due to a larger beam diameter and certainly with respect to Ga+ion exposure potential damage or contamination from the ion impact Ga implantation. 

Plus scanning helium ion microscope and an FEI Strata DB 235 scanning electron microscope SEM , both operating at 30 kV, were used for helium ion beam and electron beam exposures, respectively. 

Adhesion to the substrate becomes too low with decreasing feature size in order to withstand the force interactions during the wet development step. 

19 Recent work on H+ beam writing of HSQ at MeV ion energy exposure shows a sensitivity of 3.2 C /cm2,20 which drops to about 20 C /cm2 sensitivity upon HSQ resist aging. 

the scattering profile of helium ions is known to be confined within a narrow cone penetrating relatively deep into the material with very low backscattering. 

Beam type and energy, initial thickness,21 development time, developer type, concentration, and temperature22 have been known to have a substantial impact on the sensitivity of the resist. 

The field of view FOV was 25 25 m2 and the numbers of pixels were 256 256, 512 512, and 1024 1024, resulting in pitches of 98, 47, and 24 nm, respectively. 

He+ ion beam lithography is a very promising technique for the formation of ultrahigh resolution structures of a high density and having feature sizes in the sub-10-nm range. 

With its negligible proximity effect, SHIBL seems to be the best exposure technology by far to realize the ultimate limit in this matter. 

The difference in sensitivity between SHIBL and EBL can be partly due to the higher yield of SE for helium ions compared to electrons of the same energy. 

In the first type, the exposure sensitivity is measured for both EBL and SHIBL in HSQ films of 70 nm thick using a defocused beam in a dose range from 0.1 C /cm2 to 1 mC /cm2.