Electronic Materials Letters

https://doi.org/10.1007/s13391-019-00161-8

ORIGINAL ARTICLE - ENERGY AND SUSTAINABILITY

High‑Performance Amorphous Silicon Thin Film Solar Cells Prepared

at 100 °C: Toward Flexible Building‑Integrated Photovoltaics
Dong‑Won Kang1   · Jun Ryu1 · Makoto Konagai2

Received: 30 May 2019 / Accepted: 26 June 2019

© The Korean Institute of Metals and Materials 2019

Abstract
For low-cost and lightweight polymer/plastic substrates in flexible building-integrated photovoltaic (BIPV) modules, low-
temperature processing is essential. Amorphous silicon (a-Si:H) requires processing at a temperature of 200–250 °C by
plasma-enhanced chemical vapor deposition to obtain satisfactory optoelectronic properties, which limits such substrates
in terms of thermal budget. This study is focused on the fabrication of p–i–n-type a-Si:H solar cells at relatively low tem-
peratures (100 °C). Intrinsic a-Si:H films with large optical gaps (1.83 eV) were prepared at 100 °C using a high hydrogen
dilution ratio. In addition, p-type amorphous silicon oxide and n-type microcrystalline silicon oxide films with large optical
gaps and suitable conductivities were prepared at 100 °C using a gas mixture containing the dopant B ­ 2H6 or P
­ H3 and C
­ O 2.
Finally, an a-Si:H p–i–n cell was fabricated at 100 °C; it exhibited an excellent power conversion efficiency of 9.0%, which
was higher than those reported for a-Si:H thin film photovoltaics prepared at 100 °C. We believe that this study will open
promising routes for the development of high-performance and flexible BIPVs.
Graphic Abstract

Keywords  Amorphous silicon · Low temperature · Thin film · Solar cells · Chemical vapor deposition

* Dong‑Won Kang 1 Introduction

kangdwn@cau.ac.kr
1
Recently, the use of fossil fuels has considerably increased,
School of Energy Systems Engineering, Chung-Ang
incurring the generation of large amounts of carbon diox-
University, Seoul 06974, Republic of Korea
2
ide ­(CO2) gas and thereby accelerating climate change,
Advanced Research Laboratories, Tokyo City University,
including global warming [1]. Therefore, renewable energy
Tokyo 158‑0082, Japan

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Vol.:(0123456789)
 Electronic Materials Letters

solutions are required. Among the various renewable energy

resources, building-integrated photovoltaics (BIPVs), may (a)

Raman intensity (Arb. units)

potentially resolve power generation issues without harmful R=20
gas emission [2–5]. BIPV systems can be easily installed on
Amorphous
home windows and the exterior surfaces of various build-
(480 cm-1)
ings, making them efficient renewable power generation R=16
tools [6]. Several studies have been recently performed on
semitransparent solar cells. Dye-sensitized solar cells and/or
organic-material-based solar cells have disadvantages such
R=13
as low outdoor stability and heat resistance. On the other
hand, stabilized hydrogenated amorphous silicon (a-Si:H)
solar cells are relatively free from such issues [7]. Further- R=10
more, the large-area fabrication, non-toxicity, and feasible
control of semitransparent properties of a-Si:H make it
200 250 300 350 400 450 500 550 600 650 700
highly suitable for BIPV applications [8–11]. -1
To achieve satisfactory electronic properties, a-Si:H thin Wavenumber (cm )
films and solar cells are generally fabricated by plasma-
enhanced chemical vapor deposition (PE-CVD) at tempera- (b) Crystalline
tures in the range 200–250 °C [12–14]. However, such high- (520 cm-1)

Raman intensity (Arb. units)

temperature processes cannot be used for the fabrication of Amorphous
BIPV solar modules with flexible substrates (low-cost plas- (480 cm-1)
tics/polymer-based substrates), because the substrates would R=32
become deformed [15, 16]. Hence, to utilize low-cost plastic
or flexible polymer substrates, PE-CVD must be performed
at temperatures below 150 °C.
R=24
This study is focused on the fabrication of amorphous
silicon thin films by PE-CVD at a very low temperature of
100 °C. Firstly, we fabricated (and optimized) intrinsic and
R=22
doped thin films (i-a-Si:H, p-μc-SiOx:H, and n-μc-SiOx:H)
at 100 °C, which is a lower temperature than that commonly
200 250 300 350 400 450 500 550 600 650 700
used (150 °C) [16, 17]. After optimizing the optical and -1
Wavenumber (cm )
electronic characteristics of the p–i–n layers, we fabricated
a p–i–n superstrate-type a-Si:H solar cell at 100 °C and
assessed its efficiency. The solar cell exhibited a power con- Fig. 1  Raman spectra of a-Si:H films deposited by PECVD at differ-
ent R (= H2/SiH4) values: a 10–20 and b 22–32. Microcrystallization
version efficiency (PCE) of 9.0%, which is, to the best of occurred in films prepared at R > 22 with a substrate temperature of
our knowledge, higher than any reported in the literature 100 °C
(5.0–6.0%) [16, 18, 19]. We believe that this advanced tech-
nology will pave the way for the development of a-Si:H-
based flexible and wearable devices, and BIPVs employing loss at the doped layers, which could promote enhanced
low-cost plastic/polymer substrates. light absorption in the intrinsic layer. To obtain a p-type
amorphous silicon oxide (p-a-SiOx:H) window layer with
suitable conductivity and a wide optical gap, the synthesis
2 Experimental was optimized by using different ­B2H6/SiH4 (0.012–0.0167)
and ­H2/SiH4 (30–40) ratios. Moreover, to optimize the con-
In this study, p- and i- layers were deposited by very high ductivity (σ), crystallinity, and optical gap ­(Eopt) of the
frequency (VHF) PE-CVD, and the n-layer was deposited n-type μc-SiOx:H layer, an n-type seed layer (R = 100) and
by radio frequency (RF) PE-CVD at a substrate temperature a μc-SiOx:H (R = 72) film were sequentially deposited using
of 100 °C. To produce an amorphous absorber layer, the different ­CO2/SiH4 ratios from 0.6 to 1.73.
deposition of the intrinsic a-Si:H (i-a-Si:H) layer on glass at The crystalline phases of the deposited thin films were
a pressure of 50 Pa was optimized by using different values analyzed by Raman spectroscopy (JASCO, RS-1000). The
for the dilution ratio (R = H2/SiH4) from 10 to 32. Regard- photoconductivity (σph) and dark conductivity (σd) of the
ing the p- and n- doped layer, silicon oxide materials were samples were determined by current–voltage measurements;
employed instead of silicon to reduce parasitic absorption before the measurements were taken, Al electrodes (3 mm

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Electronic Materials Letters
Fig. 2  Dark conductivity and
photoconductivity data for 1E-4
a-Si:H films prepared at dif-
ferent R (= H2/SiH4) values
1E-5
Conductivity (S/cm)
(10–32). The increase in the
conductivity (especially dark
conductivity) indicates phase 1E-6
change from a-Si:H to μc-Si:H
1E-7
1E-8
1E-9
1E-10
1E-11
1E-12
8 10
width and 200 μm spacing) were deposited on the surface
of the thin films by thermal evaporation. The film thickness
and ­Eopt were determined by spectroscopic ellipsometry (J.
A. Woollam Co. Inc., EC-400).
For the solar cell fabrication, typically, an Al-doped
ZnO (ZnO:Al) film of 30 nm thickness was first deposited
on a ­SnO2:F substrate. Next, p-a-SiOx:H (10 nm)/i-a-Si:H
(150 nm)/n-μc-SiOx:H (40 nm) layers were deposited by
PE-CVD. Then, thermal evaporation of Ag (200 nm)/Al
(100 nm) was carried out using a shadow mask to define the
effective cell area (0.086 cm2). The current–voltage charac-
teristics (EKO, LP-50B) and external quantum efficiencies
(EQE; Bunkohkeiki, CEP-25MLT) of the fabricated devices
were measured under a standard 1 sun illumination condition
(100 mW/cm2, 25 °C).
3 Results and Discussion
Because the PE-CVD processing temperature was 100 °C,
the defect density in the a-Si:H films was expected to be
much higher than that of conventional film deposited at
higher temperatures (200–250 °C) [20]. Therefore, to sup-
press the formation of defects and microcrystallites from the
dilution of a too-high hydrogen content, we aimed to find
optimal ­H2/SiH4 ratios. It is to be noted that the presence of
microcrystallites in a-Si:H films can result in a significant
drop in the open circuit voltage (­ Voc) of the solar cells [21].
Microcrystalline
Amorphous
Dark conductivity
Photo conductivity
12 14 16 18 20 22 24 26 28 30 32 34
R ratio
The structural properties of the i-a-Si:H films prepared
at different values of R from 10 to 32 at 100 °C were inves-
tigated by Raman spectroscopy (Fig. 1). As observed in
Fig. 1a, the films prepared at an R from 10 to 20 show amor-
phous peaks at 480 cm−1. However, the films prepared at
higher R values (22–32) show crystalline peaks at 520 cm−1,
as shown in Fig. 1b [22, 23]. Notably, with an increasing R
value from 22 to 32, the crystalline peak intensity increases,
indicating that the proportion of the crystalline phase in the
films is significantly higher than that of the amorphous
phase. Thus, the Raman results show that to obtain an amor-
phous absorber layer, an R value of < 20 must be used.
We determined the electrical conductivities (σd and σph)
of the fabricated intrinsic absorber layers, as depicted in
Fig. 2. With an increasing R, σd and σph increase; particu-
larly, σd increases more drastically than σph, indicating phase
transformation from a-Si:H to μc-Si:H when the hydrogen
dilution is high. Here we need to consider the factor of
photosensitivity (= σph/σd) to anticipate a suitable photo-
voltaic response for the a-Si:H solar cells. Notably, as R
increases from 10 to 16, the a-Si:H film photosensitivity
decreases from ~ 6 × 105 to ~ 3 × 104 because of the dominant
increase in σd; however, ­Eopt increases from 1.79 to 1.83 eV
(extracted from Tauc’s plot, which was obtained by spectro-
scopic ellipsometry [24, 25]) because of the high hydrogen
dilution. The a-Si:H films prepared at R values between 24
and 32 exhibit photosensitivity in the range ­102–103, indicat-
ing microcrystallite formation in the deposited silicon layer.
Although the sample prepared at R = 20 contains amorphous
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 Electronic Materials Letters

1.2E-8 phase (as confirmed by Raman spectroscopy), it would be

(a) within the region of amorphous-to-microcrystalline transi-
1.1E-8
Dark conductivity (S/cm)

tion [26], as the dark conductivity gradually increases with

1E-8 proximity to the microcrystalline region (Fig. 2). On the
basis of the experimental results, the optimal value of R
9E-9
was determined to be 16, as the amorphous phase is pref-
erably formed at high hydrogen dilution and low tempera-
8E-9
tures. Thus, an a-Si:H film with a large E
­ opt of approximately
1.83 eV and an adequate photosensitivity of ~ 3 × 104 can be
7E-9 (B2H6/SiH4=0.0167) obtained at 100 °C by fixing R at 16.
(B2H6/SiH4=0.012) Figure  3 exhibits the variations in dark conductivity
6E-9 and optical gap (­Eopt) of the p-a-SiOx:H films prepared
30 35 40 at 100 °C as a function of R. On the basis of the result
H2/SiH4 obtained for the conventional p-layer (marked with black
2.3 square), which was prepared at 150 °C using ­H2/SiH4 = 30
(b) and ­B 2H 6/SiH 4 = 0.012, we prepared p-a-SiO x:H films
using a higher ­B2H6/SiH4 ratio of 0.0167 to incorporate a
sufficient amount of B dopant atoms, because proper gas
Optical gap (eV)

2.2 decomposition may not occur at low substrate tempera-

tures. With the increase in the B ­ 2H6/SiH4 ratio to 0.0167,
the dark conductivity increases by approximately 60% (from
7.1 × 10−9 to 1.12 × 10−8 S/cm) at R = 30; however, the ­Eopt
2.1 of the p-a-SiOx:H film slightly decreases from 2.16 eV to
2.15 eV. In addition, with the increase in R, σd gradually
(B2H6/SiH4=0.0167) decreases because of the increased hydrogen incorporation,
(B2H6/SiH4=0.012) as expected; nonetheless, the increase in ­Eopt is rather lim-
ited. Thus, p-type a-Si:H window layers with high conduc-
2
30 35 40
tivity and large E­ opt for PV devices can be obtained by using
­B2H6/SiH4 and H ­ 2/SiH4 ratios of 0.0167 and 30, respectively.
H2/SiH4
We used n-μc-SiOx:H films as alternatives to the con-
ventional n-a-Si:H/ZnO films for enhanced rear reflection;
Fig. 3  a Dark conductivity and b optical bandgap of p-a-SiOx:H films moreover, the additional sputtering process (for ZnO) could
prepared at a B­ 2H6/SiH4 ratio of 0.0167 as a function of ­H2/SiH4. The
data for the film prepared at ­B2H6/SiH4 = 0.012 are included
be avoided. Because of the low-temperature processing, fine
tuning of the ­CO2/SiH4 ratio must be performed to achieve
the optimum conductivity and refractive index (n). Figure 4
presents the σd and Raman crystallinity of the n-μc-SiOx:H
films prepared with various C ­ O2/SiH4 ratios at 100 °C. As
50
observed, σd decreases from 1.39 × 10−2 to 2.1 × 10−5 S/cm
with an increase in the C ­ O2/SiH4 ratio from 0.6 to 1.73;
Raman crystallinity (%)
Dark conductivity (S/cm)

-2 Dark conductivity 45
10
Raman crystallinity this decrease in σd is related to a decrease in the degree
40
of crystallinity of the microcrystalline films, resulting from
-3
10
35
­CO2 addition [27, 28]. Furthermore, n at a wavelength of
600 nm decreases from 3.0 to 2.7 with the increasing C ­ O 2/
10
-4 30
SiH4 ratio; however, ­E04 (the optical bandgap correspond-
25
ing to an absorption coefficient of ­104 for the microcrystal-
-5 line silicon oxide film [29]) increases from 2.15 to 2.43 eV
10 20
because of the increased incorporation of oxygen (from C ­ O2
15 gas). The rear reflection at the i/n interface can be enhanced
0.6 0.8 1.0 1.2 1.4 1.6 1.8 by the low n value of the n-μc-SiOx:H film. Additionally,
CO2/SiH4 ratio one must consider how the σd decreases with the addition
of ­CO2 to attain a low n value. When the ­CO2/SiH4 ratio
Fig. 4  Dark conductivity and Raman crystallinity of n-μc-SiOx:H increased to 0.85, the n value decreased from 3.0 to 2.77.
films as a function of C
­ O2/SiH4 ratio With further increase in the C ­ O2/SiH4 ratio from 0.85 to

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Electronic Materials Letters
(a) (b)
(c)
Fig. 5  a Schematic of the fabricated a-Si:H solar cell device structure, b current density–voltage curves, and c external quantum efficiency spec-
tra for a-Si:H PV devices fabricated at 100 °C and 150 °C
1.73, the n value decreased only from 2.77 to 2.70, whereas
σd decreased dramatically from 5.9 × 10−4 to 2.1 × 10−5 S/
cm. Hence, we could choose a ­CO2/SiH4 ratio of 0.85 for
n-μc-SiOx:H film to obtain a desirable n value without com-
promising σd, producing a σd of 5.9 × 10−4 S/cm, an n of
2.77, and an ­E04 of 2.3 eV.
Finally, using the optimized p–i–n layers (prepared at
100 °C), we fabricated a p–i–n-type a-Si:H solar cell and
assessed its performance. The device structure is described
in the experimental section and is depicted in Fig. 5a. The
current density–voltage characteristics and EQE spectrum
of the fabricated solar cell are given in Fig. 5b, c, respec-
tively. The solar cell exhibits a PCE of 9.0% ­(Voc = 0.985 V,
short-circuit current ­(Jsc) = 12.73 mA/cm2, and fill factor
(FF) = 0.716). We compared this performance with that of
a device fabricated under the conventional processing con-
dition (150 °C). As observed, the ­Jsc and FF values for the
device processed at 100 °C are lower than those for the cell
processed at 150 °C; this decrease in values is attributed to
the difference in the overall electronic quality of the p–i–n
layers of the cells. On the other hand, the V ­ oc of the solar
cell fabricated at 100 °C (0.985 V) is higher than that of
the device fabricated at 150 °C (0.948 V) because of the
larger ­Eopt value of the i-layer fabricated at 100 °C (1.83 eV)
than that of the one fabricated at 150 °C (1.75 eV). The
EQE spectra of the cells are given in Fig. 5c. The EQE peak
for the 100 °C sample is blue-shifted compared to that of
the 150 °C sample, which indicates a larger E ­ opt value in
the 100 °C sample. To the best of our knowledge, the PCE
of 9.0% is higher than those reported for a-Si:H solar cells
13

(5.0–6.0%) [16, 18, 19] prepared at 100 °C. Thus, we believe
that the output performance of flexible BIPV modules that
use low-cost plastic-based substrates can be effectively
increased by applying our technology.
4 Conclusion
In this study, the optoelectronic characteristics of intrinsic
a-Si:H, p-a-SiOx:H, and n-μc-SiOx:H films deposited at a
relatively low temperature of 100 °C were optimized for
application in flexible BIPVs employing low-cost polymer/
plastic-based substrates. Regarding i-a-Si:H, strong hydro-
gen dilution was performed using VHF PECVD before
microcrystallization, which produced a photosensitivity
of 3 × 104 and an ­Eopt of 1.83 eV. Moreover, a p-a-SiOx:H
thin film (as the window layer) with σd and ­Eopt values of
1.12 × 10−8 S/cm and 2.15 eV, respectively, and low parasitic
absorption was obtained. Furthermore, by using a ­CO2/SiH4
ratio of 0.85, we obtained an n-μc-SiOx:H film with a σd of
5.9 × 10−4 S/cm, an n of 2.77, and an ­E04 of 2.3 eV. Finally,
we fabricated a solar cell comprised of the optimized p–i–n
layers; it exhibited a high PCE of 9.0%, which was higher
than those reported for a-Si:H-based PVs prepared at
100 °C. We believe that this study will provide an effective
pathway for the development of inexpensive flexible BIPVs
employing low-cost plastic/polymer-based substrates.
Acknowledgements  This research was supported by the National
Research Foundation of Korea (NRF) Grant funded by the Korean Gov-
ernment (MSIT; NRF-2018R1C1B6008028) and was also supported
by the Chung-Ang University Research Scholarship Grants in 2019.
Compliance with Ethical Standards  parent a-Si: H pin solar cells for functional energy-harvesting
Conflict of interest  There are no conflicts of interest to declare.
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