Analytical Letters

ISSN: 0003-2719 (Print) 1532-236X (Online) Journal homepage: https://www.tandfonline.com/loi/lanl20

Fabrication of Interdigitated Electrodes using

Molecular Beam Epitaxy and Optical Lithography

Alia Colniță, Daniel Marconi & Ioan Turcu

To cite this article: Alia Colniță, Daniel Marconi & Ioan Turcu (2016) Fabrication of Interdigitated
Electrodes using Molecular Beam Epitaxy and Optical Lithography, Analytical Letters, 49:3,
378-386, DOI: 10.1080/00032719.2015.1033719

To link to this article: https://doi.org/10.1080/00032719.2015.1033719

Published online: 15 Dec 2015.

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ANALYTICAL LETTERS
2016, VOL. 49, NO. 3, 378–386
http://dx.doi.org/10.1080/00032719.2015.1033719

SENSORS

Fabrication of Interdigitated Electrodes using Molecular Beam

Epitaxy and Optical Lithography
Alia Colniță, Daniel Marconi and Ioan Turcu
Department of Molecular and Biomolecular Physics, National Institute for Research and Development of
Isotopic and Molecular Technologies, Cluj-Napoca, Romania

ABSTRACT ARTICLE HISTORY

This study reports the fabrication of interdigitated electrodes using Received 29 August 2014
molecular beam epitaxy and photolithography techniques. Sandwich- Accepted 21 March 2015
based 10 nm silver and 50 nm gold films were deposited on glass KEYWORDS
substrates using magnetron sputtering and molecular beam epitaxy Interdigitated electrodes;
deposition. The thickness and roughness were determined by use of a molecular beam epitaxy;
suitable mathematical model and ellipsometric measurements. The photolithography
gold film (111) orientation was determined by X-ray diffraction. Optical
microscopy measurements were made for the lateral resolution
determination of the fabricated electrodes and the quality was similar
to that of the photomask. Atomic force microscopy measurements
offered information regarding the topography of the sample and the
possible application of the fabricated system for molecular detection.

Introduction
Integration and miniaturization are the most important characteristics of modern analytical
chemistry, where micro electro-mechanical systems have an important role in the
fabrication of miniaturized analytical devices (Shi, Rust, and Ahn 2006). Micro electro-
mechanical system processed microelectrode arrays (interdigitated arrays) have been used
in electrochemical biosensors, molecular electronics, and detectors for capillary electro-
phoresis or liquid chromatography because of the high sensitivity derived from the
precisely controlled pattern (Fang et al. 2012; Y. Wang, Ye, and Ying 2012; Lee et al.
2013; H. Wang et al. 2013; Liu, Kolesov, and Parkinson 2014). The detection of biomolecular
interactions using electrochemical impedance spectroscopy (EIS) has attracted a topical
interest in biosensor applications (Yang, Guiseppi-Wilson, and Guiseppi-Elie 2011; Lu
et al. 2014). Because the interdigitated microarray electrodes are more sensitive than con-
ventional gold electrodes and compatible with microarray construction of DNA sensors
through silicon technology, interdigitated arrays have been applied as impedimetric sensors.
Due to the broad spectrum of applications, interdigitated electrodes were optimized for
a wide range of applications, including sensors, biosensors, acoustic sensors, and chemical

CONTACT Alia Colniță alia.ungurean@itim-cj.ro Department of Molecular and Biomolecular Physics, National
Institute for Research and Development of Isotopic and Molecular Technologies, Donat 67-103, 400293 Cluj-Napoca,
Romania.
This paper is part of a special issue presented at the Third International Conference on Analytical and Nanoanalytical
Methods for Biomedical and Environmental Sciences, IC-ANMBES 2014, which was held from June 13-15, 2014, at Aula of
Transilvania University of Brasov, Brasov, Romania, organized by Dr. Monica Florescu.
Color versions of one or more of the figures in the article can be found online at www.tandfonline.com/lanl.
© 2016 Taylor & Francis
 ANALYTICAL LETTERS 379

sensors (Alexander, Price, and Bhansali 2010). The sensing ability of interdigitated electro-
des is strongly influenced by their geometrical properties. Min and Baeumner (2004) have
shown that the measured signal is greatly influenced by the electrode thickness as by the
gap size, while a smaller electrode finger width resulted in a better signal-to-noise ratio
than wider electrodes. Many electrode systems with various geometries were evaluated with
the goal to increase the sensitivity. An electrode that has attracted attention is the interdi-
gitated electrode (Shim, Rust, and Ahn 2013). This geometry offers several advantages in
addition to other possible configurations, such as steady-state signals, low ohmic drop of
the potential, increased signal-to-noise ratio, diffusion-controlled currents, small charging
currents, reduced solution resistance, and favorable signal-to-noise ratios (Couniot et al.
2013; Settu et al. 2013). These advantages have led to the use of these systems consisting
of two electrodes at the expense of conventional circuits based on three electrodes
(three-electrode potentiostatic circuits) (Xiao et al. 2011; Settu et al. 2013). The fabrication
of micro-interdigitated electrodes on glass surfaces reduces the parasitic capacitance of the
sensor, resulting in an increase in sensitivity during measurement (Settu et al. 2013). The
optimization process includes the number of fingers (N), electrode finger width (w), and
the distance between the finger (s) and the thickness of the fingers (h) (Settu et al. 2013;
Chou and Lee 2014; Rahman, Mukhopadhyay, and Yu 2014).
Starting from this basis, the novelty of this work consists in the fabrication of metallic
interdigitated microelectrodes with a good lateral resolution, a small roughness on large
atomically flat terraces, and a highly oriented crystallographic structure. A modern, ultra-
clean and highly directional deposition technique (molecular beam epitaxy) was used. High
quality electrodes with excellent uniformity were obtained by decreasing the number of
defects that developed during the deposition process.

Experimental
Instrumentation
Metallic deposition and characterization
A custom made radiofrequency magnetron sputtering system was used in order to deposit
10 nm of Ag, which served as an intermediate metallic layer between the substrate and the
Au electrodes. The role of Ag layer was to improve the Au adherence on glass, as suggested
by Ghorbanpour and Falamaki (2013). The room temperature deposition of 50 nm Au film
was made using an ultra-high vacuum molecular beam epitaxy system (Lab-10 MBE, Omi-
cron GmbH, Germany). The thickness of the metallic films determined was in situ by a
calibrated quartz monitor and a beam flux monitor, respectively. Ex situ thickness mea-
surements were made by using an ellipsometer (M2000 V J.A. Woollam). The Au film
was characterized by X-ray diffraction (XRD), atomic force microscopy (AFM), and optical
microscopy techniques. The X-ray diffractograms were obtained using a Bruker D8
Advance X-ray Diffractometer with Cu Kα radiation (λ ¼ 0.15406 nm). The AFM images
were acquired using a Dip-Pen Nanolithography system (Nanoink, USA) operating at
room temperature in noncontact mode. The obtained images were visualized using SPIP
software (Scanning Probe Image Processor (SPIP) version 6.0.10 Image Metrology ApS,
Lyngby, Denmark). The program was also used to evaluate roughness of deposited thin
films. The optical microscopic images were obtained on an inverse optical microscope
380 A. COLNIȚĂ ET AL.

(XDS-2, Optika, Italy) with a 5� objective and connected to the computer through a CCD
camera (Optikam Pro, Optika, Italy).
Photolithography
The photolithography process was made using a homemade photolithographic system
equipped with 395 nm light source. The chemical treatment of the glass substrates was
followed by plasma cleaning to increase the Ag adherence on glass. This was done using
a Femto low pressure plasma system from Diener Electronic GmbH, Germany.

Materials and methods

Metallic deposition and characterization
Glass slides (Carl Roth) of 13 � 15 mm dimensions served as substrates. The microelectrodes
were Au of 99.9995% purity (Premion, Alfa, Germany). To acquire AFM images, noncontact
silicon cantilevers (NT-MDT, Russia) with a resonance frequency of 320 � 80 kHz, a curva-
ture radius less than 10 nm, and a relative spring constant of 320 kHz were used.

Photolithography
The photomask used in this study was designed using specialized software and imprinted
on a polymer absorbing material. The steps involved in a photolithographic process are
shown in Figure 1. Prior the Ag film deposition, the glass substrates were ultrasonicated
for 8 min, in double-distilled water, acetone (Valmin Trading SRL, 99% purity), and
ethanol (Valmin Trading SRL, 99.3% purity). After the glass substrates dried, they were
treated in a low pressure O2 plasma for 2 min at a plasma power of 120 W. The Ag and

Figure 1. The photolithographic process.

 ANALYTICAL LETTERS 381

Au film depositions were followed by a thermal treatment at 200°C for 3 h. The treatment
was made not only to increase the Au attachment on Ag, but also to increase the structural
quality of the obtained films. A positive photoresist (Positiv 20), commercially available in
spray form, was used in this lithographic process. The metallic surface was covered with
photoresist and baked at 70°C for 30 min. The next step involved the ultraviolet irradiation
at 395 nm for 10 min. The untreated photoresist was developed in 0.7% NaOH, whereas
the free photoresist Au layer and the underneath Ag film were etched in aqua regia and
concentrated HCl, respectively. The final step was the photoresist removal performed in
acetone.

Results and discussion

Ellipsometric characterization of the metallic films
Ellipsometry is an optical technique that measures the change in polarization of the inci-
dent radiation that interacts with a sample (reflected or transmitted) (Azzam and Bashra
1977). The change in polarization is measured by the amplitude ratio (Ψ) and the phase
difference (Δ) between the light radiations, also known as the parallel component with
the incidence plane (p) and the perpendicular (e) component on this plane. In the ellipso-
metric spectroscopy, these two components are measured by a continuous change of the
wavelength using a scanning monochromator. The available spectral rage is 375–1000 nm,
while the incident angle of light on the surface may be set at 0° for transmission measure-
ments, or to 75° in case of reflection measurements. In order to obtain the material proper-
ties, a suitable mathematical model to describe optical measured data was applied. The
optical constants of the substrate (in this case, the microscope glass slide) such as the
refractive index (n), the extinction coefficient (k), and the film thickness were obtained
by fitting. The mathematical model can also be extended to characterize the roughness
of the surface.
Ellipsometric measurements were performed for the Ag/glass system and for Au/Ag/glass
sandwich for thickness evaluation of the metallic layers. Based on the experimental (Ψ, Δ)
spectra, the wavelength-dependent optical constants of the two layered structures n(λ) and
k(λ) were measured. The ellipsometric spectra were fitted using the Cauchy model (Fujiwara
2007) minimizing the mean squared error (MSE). The MSE was used as a risk function and
quantify the suitability of the fitting procedure. The obtained values were 0.718 for Ag/glass
and 8.336 for Au/Ag/glass system, respectively. The wavelength-dependence of the refractive
index and the extinction coefficients are shown in Figures 2 and 3 and the calculated para-
meters are listed in Table 1. The thicknesses are 12.4 nm for the Ag film and 49.2 nm for Au
film, in good agreement with the values preset for the film deposition.

X-ray diffraction characterization of the micro-interdigitated electrodes

The orientation of the Au thin film was studied using XRD in the Bragg-Brentano
geometry (θ–2θ). The scanning step was 0.02°C with 0.8 s/step and θ 2θ range was
between 10 and 90°C. Figure 4 shows the XRD pattern of the Au thin film deposited on
Ag/glass system. The diffractogram shows only one major peak corresponding to the crys-
tallographic plane with Miller indices (111). All other peaks of the Au film are much
382 A. COLNIȚĂ ET AL.

Figure 2. (a) Refractive index and (b) extinction coefficient dependencies on the wavelength of the
incident light for the Ag/glass system. The dashed line represents the model used to fit the experimental
data.

Figure 3. (a) Refractive index and (b) extinction coefficients dependencies on the wavelength of
the incident light for the Au/Ag/glass systems. The dashed line represents the model used to fit the
experimental data.

Table 1. Calculated thickness and relative roughness coefficient of the metallic films.
Sample Thickness (nm) Roughness (nm)
Ag/glass 12.41 0.2
Au/Ag/glass 49.2 0.37
 ANALYTICAL LETTERS 383

Figure 4. X-ray diffraction pattern of the Au thin film.

smaller or not distinguishable, suggesting the preferential orientation of the crystallites

with (111) planes parallel to the substrate.

Optical microscopy characterization of the micro-interdigitated electrodes

Optical microscopy was used for lateral resolution evaluation of the photomask and elec-
trodes. The optical images were also a good indicator for the dimensions of the fabricated
electrodes and offered information on the electrode quality in comparison with the quality
of the mask. Figure 5 shows the mask geometry designed in the layout editor. The next step
involved the optical characterization of the electrodes. Figure 6 and Figure 7 show optical
microscopy images of two fingers of the fabricated electrodes. By comparing the geometri-
cal features of the mask and the fingers of the deposited electrodes, the lateral resolution of

Figure 5. Design of the mask.

384 A. COLNIȚĂ ET AL.

Figure 6. Lateral resolution of the electrode fingers by optical microscopy.

Figure 7. 1 � 1 µm AFM image of the Au electrodes.

the electrodes, the distance between two electrodes (301 µm), and the width of one
electrode (∼300 µm) were comparable with the preset values of the photomask.

Atomic force microscopy characterization of micro-interdigitated electrodes

AFM is a specialized technique for topological and morphological characterization of sur-
faces. Figure 7 shows an AFM image performed on the Au/Ag/glass layered structure,
where the gold film thickness was preset at 50 nm. In order to ensure large atomically flat
terraces at the surfaces of the fabricated electrodes, a necessary condition is that the root
mean square value was smaller than 1 nm. For the Au/Ag/glass system with a 50 nm gold
 ANALYTICAL LETTERS 385

thickness, the root mean square calculated value on a 1 µm � 1 µm AFM image was
0.33 nm. This result indicates that the electrodes obtained by this protocol were appropriate
for the fabrication of microstructured devices suitable in the field of biosensors and
molecular electronics.

Conclusions
The fabrication of metallic interdigitated pattern further used as microelectrodes was per-
formed by deposition of Au by using a molecular beam epitaxy ultra-high-vacuum facility
and faithfully replicating surface patterns using photolithography. The electrodes were
characterized using X-ray diffraction, ellipsometry, optical microscopy, and atomic force
microscopy to assess the surface topography. Characterization of structural properties of
Au electrodes was performed by XRD. The measured diffractogram shows only one major
diffraction maximum corresponding to the (111) crystallographic plane. This preferential
orientation of the Au thin film makes microstructured electrodes suitable for the fabri-
cation of devices with applications in biosensors and molecular electronics. The thickness
and roughness of the layered electrodes were assessed by spectroscopic ellipsometry mea-
surements. The wavelength-dependent optical constants of the samples were obtained
using the Cauchy theoretical model to fit the same spectroscopic ellipsometry data. The
interdigitated electrodes fabricated by molecular beam epitaxy and photolithography had
a good lateral resolution, a small roughness on large atomically flat terraces, and a highly
oriented crystallographic structure.

Funding
This work was financially supported by UEFISCDI, projects PN-II-ID-PCCE-2011-2-0027 and
PN-II-PT-PCCA-2011-3.1-0595.

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