Dip-Pen Nanolithography

Measurement of Mass Transfer during Dip-Pen

Nanolithography with Phospholipids
Soma Biswas, Michael Hirtz, and Harald Fuchs*

Dip-pen nanolithography (DPN) has been extensively used before for patterning
surfaces; however a complete understanding of the ink transport mechanisms is still
lacking. Moreover, quality control of the fabricated structures is a bottleneck in DPN
fabrication, and one aspect of this is the quantification of the ink mass transfer to the
substrate during the lithographic process. There is a demand for measuring the exact
amount of molecules deposited on a surface by lithographic methods, especially for
biological applications. This article demonstrates a quantitative method for measuring
the amount of ink transferred onto the substrate in DPN with phospholipids
by dynamic force spectroscopy. To achieve this, the harmonic oscillation of a
microcantilever in an atomic force microscope is used, obtaining picogram mass
sensitivity in the determination of mass deposition.

1. Introduction
The ability to tailor the chemical composition and structure of a surface at the nanometer length scale is essential for
fabricating novel nanomaterials, understanding underlying
nanoscience and engineering, developing integrated systems
for demanding applications and ultrahighly sensitive biosensors. Nanolithography is the art and science of etching, writing,
or printing at the nanoscopic level, in which the dimensions
of characters are in the order of nanometers. In particular,
scanning probe microscopy (SPM)-based approaches offer
both ultrahigh resolution and in situ imaging capabilities.
Dip-pen nanolithography (DPN), a method for directly
depositing molecules from an ink-coated atomic force microscope (AFM) tip onto a substrate of interest, is a powerful tool

Dr. S. Biswas,[+] Dr. M. Hirtz,[+] Prof. H. Fuchs

Institut fr Nanotechnologie (INT) and Karlsruhe Nano Micro Facility (KNMF)
Karlsruher Institut fr Technologie (KIT)
76344 Karlsruhe, Germany
E-mail: fuchsh@uni-muenster.de
Prof. H. Fuchs
Physikalisches Institut
Westflische Wilhelms-Universitt, and Center for Nanotechnology
(CeNTech)
48149 Mnster, Germany
[+] S.B. and M.H. contributed equally to this work.
DOI: 10.1002/smll.201100381
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for creating micro- and nanoscale patterns of small molecules,[13]

biological macromolecules,[46] conducting polymers,[4] and inorganic materials.[7,8] The technique also has been used to study
monolayer growth and exchange processes in-situ with kinetic
control over such processes.[9,10] Although DPN has emerged as
a useful tool for fabricating nanostructures, the mechanism of
ink transport is far from understood, and a consistent, quantitative analysis of the factors that influence it has not been carried out. Some researchers have proposed that the meniscus is
central to the transport process,[1,11,12] while others have concluded that in some cases water plays no role in the transport
process.[13,14] The patterning process in a DPN experiment can
be broken down into two elementary processes: the first step
is molecular transport from the tip to substrate, which in many
cases involves dissolution of ink into the meniscus that naturally
forms between the tip and sample at ambient conditions. The
second step is ink adsorption onto the surface and monolayer
formation. Both the transport and adsorption of ink molecules
generally depend on several physical parameters, including temperature, relative humidity (RH), the physicochemical properties of the ink and surface, writing speed and tipsubstrate
contact force. To develop and fully control DPN, it is essential to
increase our understanding of the relative importance of these
variables for a set of representative inks and substrates.
DOPC (1,2-dioleoyl-sn-glycero-3-phosphocholine) is
a versatile ink for DPN under humidity-controlled conditions and can be used as a carrier ink for the multiplexed
and/or massively parallel patterning of functional lipophilic

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S. Biswas et al.

materials.[15,16] For many applications (e.g., in arraying proteins or other bioactive substances), it is desired to know how
much of an ink was deposited in each lithographic feature.
One approach to quantify the amount of transferred ink is
by subsequent observation with fluorescence microscopy.[17]
The cantilever arrays typically used in DPN offer another
convenient way to address this problem in situ by using the
cantilever itself for mass detection:[1820] generally there are
two kinds of sensing methods utilizing microcantilevers as
a very sensitive chemical sensor or mass sensor; one is to
detect the static bending caused by surface stress due to analyte adsorption onto a flexible cantilever on which a chemically active layer is coated.[21,22] This method is believed to
be very sensitive; however, quantitative evaluation is difficult
because the stress induced by the adsorption is unpredictable.
Furthermore, the drifts of the signal caused by the optical
sensing system make long-time measurements difficult. The
other method is to use resonant frequency changes due to
mass loading;[2224] It seems particularly effective when mass
loading does not cause surface stress. Therefore, we decided
to take the approach of using the harmonic oscillation of a
microcantilever in an AFM to measure the amount of ink
transfer to the substrate in the case of DPN with phospholipids, obtaining a picogram mass sensitivity.

2. Results and Discussion

2.1. General Experimental Setup
All DPN experiments presented here were done on
plasma-cleaned glass substrates with the phospholipid DOPC
mixed with 1 mol% of a fluorophore-labeled lipid (1,2dioleoyl- sn -glycero-3-phosphoethanolamine- N -(lissamine
rhodamine B sulfonyl) at two different RH values (i.e.,
(65 1)% and (50 1)%) keeping other parameters fixed.
After coating the tip with ink 40 dots were written on a plasmacleaned glass substrate. The amount of the ink transferred to
the substrate during the writing of each dot was determined by
measuring the change in resonance frequency of the cantilever
with which writing was done. The AFM was operated in noncontact mode for measuring the resonance frequency of the
cantilever before coating the tip with ink, after coating with ink,
and after writing of each dot, while the dots themselves were
written in contact mode. For calculating the mass transfer, the
resonance frequency of the cantilever measured experimentally after making each dot has been fitted with a Lorentzian
fit by in-house-developed software (see Experimental Section
for details). We have also measured the area of each dot from
fluorescence microscopy images of the patterned samples.

2.2. Mass Sensitivity in Harmonic Vibration

When an AFM cantilever is oscillating, the resonance frequency f of the cantilever is given by
f =

1
2B

k
,
M

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(1)

where k is the spring constant of the free cantilever and M is

the effective mass of the cantilever. When the resonance frequency shift f occurs due to a mass change, the mass change
m can be calculated by[25]
m = 2

M
f
f

(2)

From Equation 2, in order to enhance the sensitivity for

small m, it is necessary to use a cantilever with a preferably
small mass and a high resonance frequency and to detect a small
resonance frequency shift with high resolution. AFM cantilevers fulfilling these requirements are commercially available.
The detection is carried out using the noncontact AFM method
in our case. When a cantilever with a mass of 11.3 ng and a
resonance frequency of 306.7 kHz is used, a mass sensitivity
m/f = 0.07 pg/Hz is obtained. To determine the sensitivity of
our instrumental setup, we measured the resonance frequency
of a cantilever in air 10 times by recording the frequency curve
and fitting a Lorentzian function to it. The obtained resonance
frequencies showed a standard deviation of 0.001 kHz, which
corresponds to a theoretical sensitivity in the range of 0.07 pg.
2.3. Measuring the Change in Resonance Frequency
of the Vibrating Cantilever
Figure 1a shows the frequency spectra of the cantilever
before being coated with the DOPC ink, after being coated
with ink, and after making 50 dots on the plasma-cleaned
glass substrate. As can be seen from the figure, the resonance frequency of the cantilever was initially 306.7 kHz
and decreased to 273.3 kHz after being coated with ink. The
decrease in resonance frequency is evident from Equation 1
as the effective mass of the cantilever was increased in this
case. After making 50 dots, the resonance frequency was
increased to 273.6 kHz as the effective mass of the cantilever
decreased because of ink transfer to the substrate. Figure 1b
shows the enlarged version of the rectangular region marked
in Figure 1a. The optical micrograph image of the tip after
coating with the ink (marked with white circle) is shown in
Figure 2a, and a sample image of the fluorescent dots written
on the substrate is given in Figure 2b.
To ensure that the observed frequency shift is really due
to mass transfer from tip to sample, a negative control experiment was performed where the same writing procedure was
applied with a bare tip that was not inked with lipids (see
Supporting Information). In another control experiment the
resonance frequency of a bare and a lipid-loaded cantilever
was measured under different humidities. Condensation
of water was observed during these experiments (see Supporting Information), but no impact on the mass transfer is
expected due to this effect since all writing experiments were
carried out at a fixed humidity.
2.4. Ink Transfer with Varying Relative Humidity
In Figure 3a,b the resonance frequency of the cantilever
after generating each dot on the surface has been plotted

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Mass Transfer during Dip-Pen Nanolithography

Figure 1. Frequency spectra of the cantilever in air before being coated with ink (DOPC+Rhodamine) (black curve), after being coated with ink (red
curve), and after making 50 dots on the surface (green curve). b) The magnified version of the rectangular region marked in (a). The images show
that the resonance frequency of the cantilever increases with decrease of the effective mass of the cantilever and vice versa, as expected.

versus the number of dots. The data has been taken at RH =

(65 1)% (a) and RH = (50 1)% (b). The black curve shows
the experimental data whereas the red line and the green line
are two linear fits to the experimental data points. It is evident from the figure that there are two different regimes for
ink transfer to the substrate. The ink transfer in a written dot
is proportional to the frequency shift of the cantilever. Initially, for the first 56 dots the average ink transfer per dot
is increased (the slope of the red line is 0.0327 0.0031 kHz
for RH = 65% and 0.0254 0.0016 kHz for RH = 50%); then
the average ink transfer declines to a lower steady value for
the remaining dots made on the surface (the slope of the
green line is 0.0016 0.0003 kHz for RH = 65% and 0.0013
0.0004 kHz for RH = 50%). The average mass transfer corresponding to the two different ink transfer regimes has
been calculated according to Equation (2). The average mass
transfer corresponding to the red and green line fits to the
experimental data are 2.03 0.19 and 0.10 0.02 pg, respectively, in the case of RH = 65% and 1.59 0.10 and 0.08
0.02 pg, respectively, in the case of RH = 50%.
Figure 3c,d show the area of the written dots plotted
against the number of the dot for RH = 65% and RH =
50% respectively. The black curve shows the experimental
data and the red curve shows the second order exponential

decay fit to the experimental data points. The area of the dots
has been measured from a fluorescence microscopy image
of the dot patterned substrate using ImageJ.[26] The area of
dots decreases within the first few dots and then stabilizes in
a similar way like the average mass transfer stabilizes after
the first few dots. This is in agreement with the procedure
of bleeding the tips in DPN, where tips are freed from
excessive ink by writing some sacrificial structures before
performing the actual wanted lithographic structure. It is
interesting to note that the measured area is not directly correlated to the amount of transferred ink: although less ink
was transferred to each dot on average in the case of RH =
50% the area per dot is most of the times slightly higher than
in the case of RH = 65%. This reflects the factor that the dot
shape will vary with humidity due to changes in surface tension and contact angle and thus the projected dot area will
not directly translate into the dots mass.

2.5. Calculating the Average Number of Molecules Per Dot

Having obtained data on the average mass deposited in
each dot, we can easily extract information on the amount
of molecules in each dot. This information is of great interest

Figure 2. a) Optical micrograph image of the cantilever after being coated with the ink. The tip region is marked with a white circle. b) Fluorescently
labelled dots made on a plasma cleaned cover slip at RH = 50%. White scale bars correspond to 50 m.
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Figure 3. The resonance frequency of the cantilever after writing of each dot at a) RH = 65% and b) RH = 50%. There are two different regimes of
average ink transfer to the substrate marked with a red and green linear fit in the graphs. The average mass transfer per dot corresponding to the
red line is 2.03 0.19 pg for RH = 65% and 1.59 0.10 pg for RH = 50%. For the green lines, the mass transfer is 0.10 0.02 pg for RH = 65% and
0.08 0.02 pg for RH = 50%. The dot area for each dot as measured by fluorescence microscopy is shown for c) RH = 65% and d) RH = 50%.

when applying DPN for biological applications such as

immunoassays or general arraying of proteins and functional
biomolecules. In the case of DPN with lipids, DOPC is generally used as a carrier ink with relatively small admixing
of the desired functional molecule. In our experiment, the
fluorescence-labeled lipid acts as a model for a functional
admixing. If two kinds of molecules with molar masses M1
and M2 are mixed in molar fractions of X1 and X2, the number
of molecules n1 of the first kind in an amount of mixture with
the total mass m can be calculated by
n1 =

m A
X2
X1

M2 + M1

(3)

where A denotes Avogadros constant. Having calculated the

number of molecules n1 of the first compound, the number of
molecules of the second n2 is given by
n2 =

X2
n1
X1

(4)

Executing these calculations with the experimental

values (X1 = 99 mol%, X2 = 1 mol%, M1 = 786.113 g/mol,
M2 = 1319.753 g/mol, and m50% = 0.10 pg, m65% = 0.08 pg
respectively), we end up with about 7.5 107 DOPC molecules admixed with 7.6 105 molecules of the functional

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compound in the case of RH = 65% and 6.0 107 DOPC

molecules admixed with 6.1 105 molecules of the functional
compound in the case of RH = 50%. These values translate
into a deposition of 1.26 amol of the functional compound
into one dot at RH = 65% or 1.01 amol at RH = 50%.

2.6. Estimating the Mass Transfer for Each Individual Dot

Finally, we have calculated the amount of ink transferred
to the substrate during the writing of each particular dot to
estimate the feasibility of mass quantification on a single dot
basis in our current setup. For calculating the mass transfer,
the resonance frequency of the cantilever measured experimentally after making each dot has been fed into a program
as an input parameter, and the mass transfer has been calculated using Equation 2 mentioned above. Figure 4 shows
the change in mass after writing each dot as a function of
number of the dot (for (a), RH = (65 1)% and for (b), RH =
(50 1)%). The black curve shows the experimental data. The
red line and the green line show the average mass transferred
to the surface corresponding to two different regions of the
data shown in Figure 3a,b.
It is obvious from the graphs that the instrument is
working at the edge of obtainable sensitivity for this setup,

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Mass Transfer during Dip-Pen Nanolithography

Figure 4. Amount of ink transfered to each specific dot for a) RH = 65% and b) RH = 50%. The average mass transferred to the surface corresponding
to the two different regions from Figure 3 has been indicated by the red and the green lines in the graph.

reflected by an overall large fluctuation in the detected mass

change for each dot leading to artifacts in the form of apparently negative masses for several dots. Principally such measurements could also mean that the tip acquired material from
the surface during writing, but this can be ruled out because
the inspection of the patterns by fluorescence microscopy
proves the dots were actually written onto the surface. Analyzing the frequency shift and calculated mass transfer on a
single dot feature, we conclude that the practical mass sensitivity in our setup is about 1 pg (in contrast to the theoretical value of 0.07 pg calculated above). Since this sensitivity
limit is in the range of mass that is deposited into a single
dot, single-dot analysis does not seem not feasible with our
current commercial available setup for routine production of
lithographic structures over wide areas.

3. Conclusion
We demonstrated a straight forward way of measuring the
mass transfer into single lithographic features during DPN
with phospholipid inks using the change in resonance frequency of a microcantilever and its changing mass. Although
the AFM combined with the commercial DPN setup that we
have used is not as sensitive with regard to frequency shifts
as dedicated AFM setups, we could still achieve sub-picogram
sensitivity by fitting resonance curves and averaging over
several lithographic features. The method has the potential
to be used as a standard method to determine the amount
of deposited material, e.g., during arraying of bioactive substances such as proteins or allergens for immunoassays. It
would be desirable for future DPN setups to enable readout
of the frequency shift for single pens of a pen array before
and after lithography, enabling a quantitative determination
of ink transfer onto the substrate for each individual tip as
well as trying to enhance the stability of the system, so that
the theoretically possible sensitivity limit (0.1 pg; that is,
still one order of magnitude better than the 1 pg obtained
for single-dot analysis) can be achieved. Nevertheless, useful
information on the average amount of active compound in
a single lithographic feature can still be obtained by determining the mass change over several features (e.g., such as the
40 to 50 dots as presented here), which is feasible for quality
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control of immuno- or other protein assays since these usually contain hundreds to thousands of single dot features.

4. Experimental Section
Materials: The DOPC (phase transition temperature, Tm =
16.5 C, molecular weight = 786.113 g/mol), and the fluorophore-labeled
phospholipid
(1,2-dioleoyl-sn-glycero-3phosphoethanolamine-N-(lissamine rhodamine B sulfonyl) (18:1
lissamine rhodamine/PE), molecular weight = 1319.753 g/mol)
were purchased from Avanti Polar Lipids, Alabaster, AL, USA.
Chloroform (high-performance liquid chromatography (HPLC)
grade) was purchased from Sigma. Ultrapure water with a resistivity of 18.2 Mcm was used. Glass coverslips (18 mm 18 mm)
were purchased from VWR Scientific. Tapping mode cantilevers
were purchased from Budget Sensors.
Experimental Methods: The experiments were carried out using
commercially available instrumentation. Tip coating, DPN writing,
and measuring of the resonance frequency of the cantilever
were carried out using a commercial DPN writer combined with
AFM (DPN 5000, NanoInk Inc., USA, software packages InkCAD
and SPM Cockpit) and the following accessories: Tapping mode
cantilever (from Budget Sensors, aluminum-coated rectangular
cantilever with resonance frequency 300 KHz and spring constant 40 N/m according to manufacturers value) and inkwells of
type IWL-0021-01 (custom-made from NanoInk Inc., USA). The ink
wells are microfluidic chips that allow for depositing the desired
ink dissolved in an appropriate solvent (chloroform) into an ink
reservoir. The ink reservoir is large enough for convenient handling with pipettes and is connected to the actual microwells for
dipping the tips via microchannels (typical width 6 m). The inkwells were filled with a chloroform solution of the phospholipid ink
(1 L, 10 mM, doped with 1 mol% of the dye-labeled lipid). The
solvent was allowed to evaporate for at least 1 h before coating
the tips. The cantilevers were plasma treated with oxygen
(10 sccm, 100 mTorr, 30 W, 5 min) prior to inking. Tips were inked
by placing them in contact with the inkwell and increasing the
humidity to (70 1)% for at least 45 min. Glass substrates were
plasma-treated with oxygen (20 sccm, 100 mTorr, 100 W, 30 s) to
render them hydrophilic. After preparation of the substrates and
coating of the tips with ink, the tip was brought into contact with
the surface for 10 s to write a dot and then retracted 20 m above

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the surface to check the resonance frequency after writing the dot.
This procedure was repeated 40 times to write 40 dots, and the
whole run of 40 dots was performed twice (with re-inking of tip in
between experiments) at two different RH values of (65 1)% and
(50 1)% with a controlled temperature of T = 22 1 C. After
changing the RH inside the glove box, the system was allowed to
equilibrate for approximately an hour to stabilize. The AFM was
operated in noncontact mode (approximately 20 m above the
sample surface) for measuring the resonance frequency of the cantilever before coating the tip with ink, after coating with ink, and
after writing of each particular dot.
Fitting of Resonance Curves: To determine the resonance frequency from the recorded resonance curves, a small in-housedeveloped visual basic program was used. The program reads
in the recorded resonance curves saved by the AFM software
and performs a least-squares fit to determine a Gaussian fit. The
parameters obtained from this first fit are then used as starting
parameters for a second least-squares fit with a Lorentzian function of which the peak frequency is regarded as the resonance
frequency of the cantilever. This two-step approach ensured a
better convergence than directly fitting a Lorentzian function to
the raw data.
Fluorescence Microscopy: This was carried out on an upright
Eclipse 80i fluorescence microscope (Nikon). Patterns were
aligned for imaging using alignment markers scratched onto the
glass surface. Bleaching of fluorophores was minimized (especially
for quantitative measurements) by first focusing on the alignment mark before exposing the patterned area to light, and the
lamp intensity was kept at a minimum. For quantitative measurements of each dot made on the surface as shown in Figure 3, the
fluorescence intensity and area of the dots were measured using
ImageJ.[26]

Supporting Information
Supporting Information is available from the Wiley Online Library
or from the author.

Acknowledgements
The authors want to thank S. Sekula-Neuner, T. Laue, and F.
Brinkmann for their support and useful discussions. S.B. thanks
the Helmholtz Association for nancial support. H.F. acknowledges
support from DFG (TRR 61) and the World Class University program
of the Korean Ministry of Education, Science, and Technology at
Gwangju Institute of Science and Technology. This work was partly

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carried out with the support of the Karlsruhe Nano Micro Facility
(KNMF, www.knmf.kit.edu), a Helmholtz Research Infrastructure at
Karlsruhe Institute of Technology (KIT, www.kit.edu).
This Full Paper is part of the Special Issue dedicated to Chad Mirkin
in celebration of 20 years of inuential research at Northwestern
University.
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2011 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Received: February 25, 2011

Revised: May 10, 2011
Published online: June 8, 2011

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