Applied Surface Science Advances 7 (2022) 100206

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Applied Surface Science Advances

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Picosecond laser patterning for ultrathin spectrally selective solar

mini-modules with transparent metal-oxide multilayer electrodes
Norbert Osterthun *, Hosni Meddeb, Nils Neugebohrn, Oleg Sergeev, Kai Gehrke, Martin Vehse,
Carsten Agert
German Aerospace Center (DLR) Institute of Networked Energy Systems, Urban and Residential Technologies, Carl-von-Ossietzky-Str. 15, 26129, Oldenburg, Germany

A R T I C L E I N F O A B S T R A C T

Keywords: Semitransparent solar cells featuring spectrally selective light transmission have been developed for agrivoltaic
Picosecond laser patterning applications. One novel approach for this technology is the combination of a metal-oxide multilayer electrode
Monolithic integration with an ultrathin germanium solar cell. However, the combination of this electrode possessing multiple thin
Metal-oxide multilayers
silver layers with the ultrathin absorber imposes additional challenges for the laser scribing processes that are
Ultrathin solar cell
Spectral selectivity
used for the module integration. In this work, we report on a picosecond laser patterning approach for the
Agrivoltaic monolithic interconnection of a spectrally selective solar cell on mini-module level. We found, that a green (532
nm) and an infrared laser (1064 nm) are suitable for the scribing of the metal-oxide multilayer electrode and the
ultrathin absorber. Our approach is an important step towards large scale module fabrication for versatile
agrivoltaic applications.

1. Introduction
Transparent thin film solar cells offer the possibility to meet the
demand for sustainable energy with novel photovoltaic applications like
PV windows [1–3] or spectrally selective PV for agrivoltaic applications
like vertical gardening, greenhouse applications or photo-bioreactors for
algae growth [4–7]. Typically, organic or inorganic absorbers are
combined with transparent conductive oxides (TCO) or TCO\metal\TCO
(OMO) electrodes to achieve semi-transparent solar cells [5, 8-14].
Recently, a spectrally selective solar cell with an ultrathin amor­
phous germanium (a-Ge:H) absorber has been demonstrated [14, 15]. In
order to apply this technology in agrivoltaic applications, the fabrication
of modules is necessary. Therefore, an interconnection process of the
spectrally selective solar cells has to be developed since the ultrathin
a-Ge:H absorber and the spectral selectivity lead to additional chal­
lenges, which do not occur for other solar cell technologies.
The a-Ge:H solar cell technology uses optical and electrical
confinement of photons and electrons to achieve relatively high effi­
ciencies of up to 5.2% for opaque solar cells with absorber thicknesses
between 2 and 20 nm [15–18]. Other than amorphous silicon, a-Ge:H
allows for broadband optical confinement due to the much higher ab­
sorption coefficient above 500 nm and suitable optical constants [15].
Moreover, the use of ultrathin absorber layers allows to fabricate
semi-transparent cells when the silver reflector of the opaque solar cell is
replaced by a transparent material [17].
For agrivoltaic applications a metal\TCO\metal\TCO (MOMO)
electrode can be integrated, to render these solar cells spectrally selec­
tive. In this configuration the power conversion efficiency is still higher
than 2% [14, 15]. The MOMO electrode has the advantage that the ratio
of transmittance and photocurrent generation can be precisely adjusted.
This has been used to fabricate optical demonstrators, which have been
integrated in lab-scaled photo-bioreactors [7]. Significant algae growth
has been demonstrated for illumination through the spectrally selective
solar cells, proving the suitability of this technology for such applica­
tions. The fabrication processes of these spectrally selective solar cells
include the scalable and industry-compatible thin film deposition tech­
niques sputtering and plasma enhanced chemical vapor deposition
(PE-CVD). However, the large-scale realization of spectrally selective
modules for greenhouse applications requires the interconnection of
individual solar cells, which has not yet been established for this
technology.
Thin film solar modules are typically fabricated by the monolithic
series interconnection of individual cell stripes. The laser process is
already established for example for amorphous silicon [19, 20] and
organic [21–23] solar cells. Furthermore, the suitability of this process
for ablation of novel electrodes like silver nanowire [21, 22] and OMO

* Corresponding author.
E-mail address: norbert.osterthun@dlr.de (N. Osterthun).

https://doi.org/10.1016/j.apsadv.2021.100206
Received 3 August 2021; Received in revised form 21 December 2021; Accepted 27 December 2021
Available online 10 January 2022
2666-5239/© 2022 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
N. Osterthun et al.
electrodes on glass and polyethylene substrates has been demonstrated
[21, 23]. However, the interconnection process for a MOMO multilayer
electrode with two absorbing metal layers is not developed yet, although
the application of the MOMO might be interesting for other thin film
solar cell technologies as well.
The monolithic interconnection is a three-step pattering process (P1,
P2, P3) which is commonly performed by laser ablation [19-21, 24, 25].
In superstrate configuration the laser scribes are performed through the
glass substrate and layers are ablated via micro-explosions away from
the sample. Although using picosecond laser pulses cannot avoid ther­
mal damage completely [26] detrimental thermal effects within the
laser irradiation zone can be at least minimized in comparison to
nanosecond laser pulses [23]. Furthermore, the energy density threshold
can be significantly reduced for scribing of thin metal/oxide multilayers
in contrast to typical µm-thick AZO, since the silver layers in the met­
al/oxide electrode lead to steep temperature increase at glass interface,
enabling more efficient P1 scribing by a reduction of the fluence in a
single laser pulse [27].
Regarding the monolithic interconnection for a spectrally selective
mini-module a careful selection of suitable laser wavelengths for each
individual laser cut are required. The specifications of laser patterning in
our structure impose the absorption of the laser beam in the first silver
layer of the MOMO electrode at the P1 ablation, whereas transmission is
required in the P2 and P3 cuts for selective removal of the ultrathin
absorber. It is well-known that the effectiveness of laser ablation
strongly depends on the absorption of the material. Thus, the choice of
the laser wavelength can be approximately defined according to the
wavelength dependence of the material absorption coefficient [28],
neglecting that non-linear effects due to ultra-fast picosecond laser
pulses can have an influence on the energy absorption.
In this work, the laser ablation of the MOMO electrode and the
desired ablation of the absorber on top of the electrode is reported. The
developed laser cuts were used for the fabrication of the first spectrally
selective ultrathin mini-module based on an a-Ge:H nanoabsorber with
metal-oxide multilayers as transparent conductive electrodes. Different
sets of laser wavelengths and powers are studied for the suitable selec­
tion of each laser patterning step considering the requirements for the
ablation of the absorber and the MOMO. Laser structuring of and
through the MOMO is especially interesting for other PV and optoelec­
tronic technologies as well.
Fig. 1. a) Stack of the SSSC (substrate configuration). The red and blue arrows demonstrate the spectrally selective light transmission of the solar cell. b) SEM cross-
section of the SSSC. Colors indicate the different parts of the SSSC. c) Steps of the monolithic interconection for the SSSC.
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Applied Surface Science Advances 7 (2022) 100206
2. Experimental details
2.1. Device fabrication
Fig. 1a shows the stack of the SSSC. An active multilayer stack (AML)
with a thickness of approximately 38 nm is the separating the top from
the bottom electrode. The bottom electrode is composed of AZO/Ag
multilayers in MOMO configuration, while an AZO/Ag dual layer is used
as top electrode. The AML forming the n-i-p diode configuration consists
of doped and intrinsic hydrogenated amorphous silicon embedding the
germanium absorber (7 nm n-a-Si:H/ 7 nm i-a-Si:H/ 10 nm i-a-Ge:H/ 7
nm i-a-Si:H/ 7 nm p-a-Si:H). Fig 1b. shows a scanning electron micro­
scopy (SEM) image of a cross-section of the SSSC stack. The layer
thicknesses are confirmed and the top and the bottom electrode are
clearly separated from each other by a continuous AML.
The spectrally selective MOMO electrode was deposited with an in-
line vacuum system (Vistaris 600 Singulus Technologies) on a 30 × 30
cm2 glass substrate, which was cut into 10 × 10 cm2 pieces. Aluminum
doped zinc oxide (AZO) films were deposited via DC magnetron sput­
tering from a planar AZO target with an aluminum oxide (Al2O3) doping
of 2%. The silver layer was deposited via RF magnetron sputtering from
a planar silver target. We chose the techniques due to the higher sputter
rate of AZO for DC sputtering compared to RF sputtering. During the
process, the carrier performs multiple lateral passes in front of the ver­
tical target, until the aimed layer thickness is reached. The detailed
sputtering process parameters can be found in Table 1.
Functional silicon and germanium layers composing the n-i-p
structure with a total thickness of approximately 38 nm were deposited
via plasma enhanced vapor deposition in an in-line vacuum system
(Phoebus PECVD Lab C from Leybold). The detailed process is described
elsewhere [15]. The front contact of the minimodule was deposited via
dc magnetron sputtering in two chambers of a clustertool type CS400PS
(from von Ardenne). A silver target and an AZO target with 0.5 wt.%
Al2O3 doping was used. The detailed parameters can be found in table 2.
2.2. Laser structuring and characterization
A laser structuring tool with a neodymium-doped yttrium vanadate
(Nd∶YVO4) diode-pumped solid-state laser with a pulse frequency f of
100 kHz was used for the laser structing (from 3-D-Micromac Lumera
Super Rapid). A gaussian profiled picosecond laser beam with a wave­
length of 1064 nm (IR) with a maximum power of 14 W and 532 nm
(green) with a maximum power of 8 W was used. The green laser
wavelength was achieved by frequency doubling, resulting in the
N. Osterthun et al. Applied Surface Science Advances 7 (2022) 100206

Table 1
Sputtering process parameters of the MOMO bottom electrode.
3
Material Thickness (nm) Mode Power (W) Power density (W/cm2) Gas flow Ar/O2 (sccm) Pressure (10− mbar) Passes Speed (m/min)

AZO 270/95 DC 3000 5 290/29 4.5 14/6 1.78/2.16

Ag 15/15 RF 700 1.17 800/- 8 2 2.25

completely from the glass substrate. Therefore, the laser has to be

Table 2
Sputter parameters of the metal-oxide top electrode.
Material Thickness Power Power Gas flow
(nm) (W) density (W/ Ar/O2
cm2) (sccm)
AZO 15 1000 2.04 100/10
Ag 72 200 0.41 60/-
reduced maximum laser power. A precise adjustment of the laser power
can be achieved with a motorized laser power attenuator. The corre­
sponding fluence F can be calculated with F = P / (f * A), where A de­
scribes the effective focal spot area. The beam diameter estimated from
the 90/10 knife edge method for the infrared laser is approximately 973
µm, whereas it is 757 µm for the green laser. A galvo-head scanner with a
scanning field of 5 × 5 cm2 and an objective of 163 mm was used for all
scribes. The solar cells substrate is fixed on a balanced holder, ensuing a
perpendicular incoming laser beam. The laser scribes for the selection of
the laser wavelengths and laser power were performed with a scribing
speed of 1000 mm/s. The P1 scribe for the fabrication of the minimodule
was performed at 1000 mm/s and 2.7 W, whereas a scribing speed of
1800 mm/s and a power of 0.3 W was used for the P2 and P3 scribe.
After the P1 scribe with the MOMO electrode was cleaned in an indus­
trial dishwasher at 60 ◦ C with DI water. Subsequent to the P2 and P3
scribes with the green laser, the scribes were cleaned with a nitrogen gun
to avoid damage to the very thin AML. After the final P3 laser cut the
modules were annealed for 2 h at 130 ◦ C.
The laser scribes were characterized via microscopy and profilom­
etry. Additional optical characterization was performed using an Agilent
Cary 5000 spectrophotometer using an integrating sphere. The software
CODE was used to optically simulate the measured UV–VIS spectra of
the MOMO electrode and calculate the absorption contribution of the
individual layers in the MOMO [14]. The current-voltage-curves were
recorded with probe pads in a WACOM dual lamp solar simulator ac­
cording to standard test conditions (AM1.5 G spectrum, 1000 W/m2,
25 ◦ C).
3. Results and discussions
The fabrication of a mini-module can be achieved by the serial
interconnection of single SSSCs via the monolithic approach as shown in
Fig. 1c. With the P1 scribe, the MOMO electrode has to be removed
absorbed in the first metal layer directly adjacent to the glass substrate.
After the P1 scribe and the following deposition of the AML, the latter
Pressure has to be removed with the P2 laser scribe to allow serial interconnec­
(10− 3 mbar)
tion of the top contact with the back contact of the neighbor cell. Finally,
after the deposition of the top electrode the P3 laser scribe is executed to
8
separate the front electrode of the adjacent solar cells by ablation of the
6
AML and top electrode.
In order to choose suitable laser wavelengths for the different scribes,
the optical properties of the MOMO electrode have to be considered.
Fig. 2a shows the measured transmission and reflection of the complete
MOMO as well as the individual absorption of the layers, which were
calculated with the software CODE as described in [14]. It can be seen,
that the MOMO features two transmission maxima at 470 nm and 680
nm, while other wavelengths are mainly reflected. Furthermore, the
calculation of the layer absorption shows, that the transmission maxima
are limited due to absorption of the silver layers. However, the high
absorption coefficient of the silver leads also to a broad spectral band,
which makes several laser wavelengths suitable for ablation of the
MOMO electrode (see Fig. 2a). Therefore, the green (532 nm) as well as
the IR laser (1064 nm) can be used for the P1 laser scribe.
For the P2 and P3 laser scribe a transmission of the laser beam
through the MOMO and an absorption in the AML is necessary. At the
laser wavelengths of 532 nm the transmission of the MOMO electrode is
21% (Fig. 2a) and silicon as well as germanium have a high absorption
coefficient (Fig. 2b). Therefore, we assume, that the green laser can be
absorbed in the AML and ablate it, although non-linear effects might
lead to a different result. In contrast, the transmission of the MOMO at
1064 nm is only 2% and silicon and germanium show only a rather small
absorption coefficient. Therefore, to ensure the ablation of the full AML,
the green laser is chosen for the P2 and P3 laser scribes.
To validate the assumption for the choice of the laser wavelength,
different laser conditions with the green and IR laser were tested on a
MOMO electrode adjacent to glass substrate. Fig. 3 shows optical mi­
croscopy pictures of individual cuts with the IR and green laser. The
laser power for the IR laser is varied between 0.58 W and 4.78 W to
achieve a complete MOMO ablation. As demonstrated in Fig. 3a, all laser
cuts with the infrared laser lead to a complete ablation of the MOMO
electrode indicating a large process window for the P1 laser cut. The
laser power the green laser was varied between 0.06 W and 2.68 W. A
laser power of above 0.11 W leads to complete ablation of the MOMO
electrode. Therefore, the green laser would also be suitable for the P1

Fig. 2. a) Stacked area plot for calculated layer absorptions in the MOMO electrode as well as measured reflection and transmission. The green and red line indicate
the laser wavelengths. b) Absorption coefficient of the silicon and germanium thin films used in the SSSC.

3
N. Osterthun et al.
Fig. 3. Laser structuring of the MOMO with different laser powers for IR (a) and green (b) wavelengths. c) Influence of laser power on scribe width.
scribe. Both lasers were tested at the laser powers of 0.58 W and 2.7 W.
No difference can be observed, indicating that both laser wavelengths
are equivalent suitable for the P1 laser scribe. Furthermore, wider
stripes are obtained with increasing the laser power as shown in Fig. 3c.
The small standard deviation indicates high line width accuracy. Hence,
a precise control of the P1 patterned line width is achieved by varying
the laser power.
For the P2 and P3 scribe the green laser has to ablate the AML
without damaging the silver layers in the MOMO. Minor damage of the
AZO layers is acceptable, as long as the conductivity of the silver layers
in MOMO is not impaired. In Fig. 3b, it is shown that a power of 0.11 W
for the green laser does not lead to ablation of the MOMO electrode
completely, but, damages the MOMO. At 0.06 W no ablation can be
observed, indicating that the laser power is not high enough for material
ablation. Since the preservation of the silver layers in the MOMO elec­
trode is desired during the P2 and P3 steps, a green laser power between
0.06 W and 0.16 W might be appropriate for the P2 laser cut.
To further investigate the suitability of the green laser for the P2 and
P3 scribe, an AML stack was deposited on top of a MOMO. On these
samples, laser cuts using the corresponding green wavelength with
varied powers between 0.14 W and 0.06 W were performed. We choose
to cut 5 × 5 mm2 boxes in the AML to allow optical inspection. This
allows to confirm, that the MOMO stays unaffected by the laser
patterning process, since a high reflectivity of green light can only be
achieved with an intact silver layer. However, negative effects like
heating of the AML are not considered in this study.
Fig. 4a depicts an image of the laser cuts taken with a camera. Violet
reflection indicates areas with the MOMO electrodes and the AML,
whereas green reflection occurs from areas with the MOMO electrode
only. Between 0.14 W and 0.12 W, clear green reflections of the MOMO
electrode can be seen. The green reflection becomes less intense with
decreasing laser power. The two fields corresponding to a power close to
0.06 W show negligible visible contrast to the parts of the sample with
no laser scribing. Therefore, the laser power is not high enough to
achieve any ablation. The optical impression is confirmed by reflection
Fig. 4. a) Camera picture of the P2 laser test cuts of a sample with MOMO electrode and AML. b) Reflection measurement of the P2 laser scribes. c) Dektak pro­
filometer measurements of the P2 laser test cuts.
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Applied Surface Science Advances 7 (2022) 100206
measurements shown in Fig. 4b, which are consistent with the reflection
spectrum measured prior to the deposition of the AML. A reflection of
almost 80% at 550 nm is achieved for laser powers of 0.12 W and 0.14
W. A drastic and progressive decrease of the reflection in the wavelength
between 500 and 600 nm is obtained when the laser power is reduced
from 0.11 W down to 0.07 W. The decrease of the reflection indicates
that the AML layers are not completely ablated resulting in additional
absorption in this wavelength range.
This is confirmed by profilometry measurements shown in Fig. 4c.
For laser powers between 0.14 W and 0.12 W the ablated thicknesses are
around 45 nm. This indicates a complete ablation of the AML plus some
nanometer AZO. The ablation of some AZO is not critical, as long as the
silver layers remain. Between 0.08 W and 0.11 W, the ablated layer
thickness decreases. This indicates only partial removal of the AML
stack. For laser powers above 0.08 W less than 1 nm is ablated and,
therefore, the AML mostly remains. From the measured thicknesses and
optical results, it can be concluded that a laser scribe with 532 nm and a
power above 0.13 W appears suitable for P2 and P3 scribing. For the P1
scribe good results were achieved with a laser power of 2.7 W for both
laser wavelengths. We choose to continue with the infrared laser, since
this laser wavelength is usually used for the P1 scribe [19, 25, 29, 30].
After the development of optimized ablation processes for the
selected layers, the P1, P2, and P3 scribes can be combined to mono­
lithically interconnect the cell stripes for mini-modules preparation as
described in Section 2.2. Fig. 5 shows optical microscopy images and
SEM pictures as well as depth profile of the final laser scribes of the
fabricated module. In Fig. 5a and d it can be seen, that the P1 scribe
shows a high overlap of the laser spots to ensure complete ablation of the
MOMO electrode. This is confirmed by the height profile of the scribe,
since the depth of the cut is approximately 420 nm, which is in good
agreement with the layer thickness shown in Fig. 1b. From SEM cross-
section shown in the supplement (S1) it can be seen that the side wall
of the P1 scribe is completely covered by both the AML and the front
contact, as it is required for electrical separation. The scribe width of 57
µm (see Fig. 5g) ensures complete electric separation of two adjacent
N. Osterthun et al.
Fig. 5. a-c) SEM pictures of the P1, P2 and P3 scribe. d-f) microscopy pictures of the P1, P2 and P3 scribe. g-i) Height profile of the laser scribes from profilometer
measurements. The laser cut in Fig. 5g has a total depth of 420 nm.
cells. The P2 scribe has a depth of approximately 30 nm (see Fig. 5h),
which is slightly below the expected AML layer thickness of 38 nm. This
small offset might be induced by the following deposition of the top
electrode since the amount of deposited material might differ in the
scribe compared to the deposition on top of the AML. Furthermore, it
can be seen in Fig. 5h, that on both sides of the P2 scribe burr formation
occur. However, the top electrode is only slightly stretched at the incline
as the burr has width of 7–10 µm with a height of 50 to 100 nm.
Therefore, the burr formation should not hinder a sufficient contact. The
width of the P2 scribe is 20 µm, ensuring enough area for the connection
of the top electrode with the bottom electrode of the following cell. In
the microscopy and SEM picture (Fig. 5b and 5e), a well-defined laser
cut with a small amount of residual is visible. The laser spots have only a
small overlap, to ensure, that the MOMO is not damaged. The P3 scribe
has a depth of approximately 120 nm (Fig. 5i). Therefore, the approxi­
mately 90 nm-thick front contact was successfully removed. The burr
formation should not influence the minimodule performance, as no
further layer is deposited on top. In the SEM picture some residuals can
Fig. 6. a) Picture of the SSSC minimodule. b) Optical properties of the minimodule. c) Current-voltage curve of the minimodule.
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Applied Surface Science Advances 7 (2022) 100206
be seen, which could not be avoided at the current state of the devel­
opment. The achieved width of the different laser scribes is in good
agreement with values from literature, which are in the range between
30 µm and 120 µm [20, 24, 25]. Furthermore, burr formation is also
observed for other electrodes [21], however, it is already reduced for
pico-second laser scribing compared to mechanical scribing [24].
Therefore, the developed laser scribes should be suitable for
mini-module fabrication of a SSSC.
Finally, we show, that the newly developed laser scribing processes
are suitable for the fabrication of a SSSC mini-module fabrication. Fig 6a
shows a fully functional spectrally selective minimodule based on the
ultrathin germanium cell. The two transmission peaks of the MOMO can
be seen at 430 nm and 660 nm (Fig 6b). The additional transmission
peak at 530 nm occurs due to the following depositions on top of the
MOMO and can be avoided with a TCO front contact. The module
consists of 11 monolithically interconnected cells and has a total area of
7 × 7 cm2 isolated from the remaining area by a laser scribe. The
measured J-V characteristic of the device is plotted in Fig. 6c. An open
N. Osterthun et al.
circuit voltage (Voc) of 2.4 V was measured and the mini-module has a
power-conversion efficiency of 0.2%, a fill factor (FF) of 33.5% and a
short circuit current of 14.5 mA. This shows, that the monolithic inter­
connection was successful. However, further improvement of the mini­
module is necessary to achieve the 2% efficiency of the solar cell. An
optimized front contact should allow better electrical properties as well
as higher short circuit current due to improved light in-coupling and
reduced reflection losses, which are shown in Fig 6b. Further improve­
ment of the laser pattering of the AML and the optimized front contact
should lead to a higher serial resistance and improved VOC. In addition, a
cleaning of the p2 and p3 laser scribe was not performed in order to
avoid damage of the ultrathin AML. However, a cleaning procedure has
to be developed in order to remove residuals, which could also lead to a
reduced Voc and serial resistance. Furthermore, an adaption of the single
cell width and the distance between the three laser cuts can also improve
the cell performance [31]. With these improvements the FF of 50% and
an efficiency of 2% corresponding to the previously published spectrally
selective solar cell should be achievable [14].
4. Conclusion
In this work the development of a laser patterning approach for the
monolithic interconnection of mini-module based on ultrathin germa­
nium is presented. Green (532 nm) and IR (1064 nm) laser processes
with varied power were investigated regarding the possibility to ablate
different layers of the stack for monolithic interconnections stripes of a
spectrally selective solar cell based on ultrathin a-Ge:H nanoabsorber,
despite the challenge of a double metal layer in the spectrally selective
electrode. It was demonstrated that P1 scribes can be prepared with the
infrared laser, while the green laser is more appropriate for the P2 and
P3 scribes. From the successful serial connection of the cells, it can be
concluded that monolithic interconnection is a suitable approach for the
fabrication of spectrally selective mini-modules based on an ultrathin
germanium absorber. These results emphasize the promising industrial
scalability and electrical layout flexibility in production of the proposed
technology.
Supporting information
Declaration of competing interests
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgement
The authors thank L. Busch for support with the microscopy images.
The authors thank also C. Lattyak, M. Götz-Köhler, D. Berends, and U.
Banik for helpful discussion.
Supplementary materials
Supplementary material associated with this article can be found, in
the online version, at doi:10.1016/j.apsadv.2021.100206.
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