Research Article

Cite This: ACS Appl. Mater. Interfaces 2018, 10, 21985−21990 www.acsami.org

Spectral Dependence of Degradation under Ultraviolet Light in

Perovskite Solar Cells
Amjad Farooq,*,† Ihteaz M. Hossain,†,‡ Somayeh Moghadamzadeh,‡ Jonas A. Schwenzer,‡
Tobias Abzieher,‡ Bryce S. Richards,†,‡ Efthymios Klampaftis,† and Ulrich W. Paetzold*,†,‡
†
Institute of Microstructure Technology, Karlsruhe Institute of Technology, Hermann-von-Helmholtz-Platz 1, 76344
Eggenstein-Leopoldshafen, Germany
‡
Light Technology Institute, Karlsruhe Institute of Technology, Engesserstrasse 13, 76131 Karlsruhe, Germany
*
S Supporting Information
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ABSTRACT: Perovskite solar cells (PSCs) demonstrate excellent power conversion

efficiencies (PCEs) but face severe stability challenges. One key degradation mechanism is
exposure to ultraviolet (UV) light. However, the impact of different UV bands is not yet well
established. Here, we systematically study the stability of PSCs on the basis of a
methylammonium lead iodide (CH3NH3PbI3) absorber exposed to (i) 310−317 (UV-B
range) and (ii) 360−380 nm (UV-A range), under accelerated conditions. We demonstrate
that the investigated UV-B band is detrimental to the stability of PSCs, resulting in PCE
degradation by more than 50% after an exposure period >1700 sun-hours. This finding is valid
for architectures with a range of electron transport layers, including SnO2, compact-TiO2,
electron-beam TiO2, and nanoparticle-TiO2. We also show that photodegradation is apparent
for high, as well as for low illumination intensities of UV-B light, but not for illumination with
UV-A wavelengths. Finally, we show that degradation of PSCs is preventable at the cost of a
small fraction of photocurrent by using UV-filtering or luminescent downshifting layers.
KEYWORDS: perovskite solar cells, UV degradation, spectral dependence, electron transport layers, luminescent downshifting layers,
stability

■ INTRODUCTION
Perovskite solar cells (PSCs) are a potential disruptive
technology in the field of photovoltaics (PV) because of
their excellent power conversion efficiencies (PCEs), and
promise of low costs due to the ease of solution processing.1
However, any PV manufacturer today that wishes to be
competitive in large-scale solar power generation needs to
guarantee that their PV module will produce more than 80% of
its original rated power after a period of 25 years.2 This is the
key aspect of PSCs in which they fall far behind their inorganic
market-dominating counterpartssuch as silicon (Si), copper
indium gallium diselenide (CIGS), or cadmium telluride
(CdTe)because of the intrinsic material instability at
elevated temperatures3 and their vulnerability to degrade
during prolonged light exposure,4 humidity,5 and oxygen.6 The
underlying degradation processes occur not only within the
perovskite absorber itself, but rather they are cumulative
phenomena originating from other layers and interfaces as well.
For instance, the most commonly used hole transport layer
(HTL) 2,2′,7,7′-Tetrakis[N,N-di(4-methoxyphenyl)amino]-
9,9′-spirobifluorene (C81H68N4O8, or commonly known as
spiro-OMeTAD) is neither moisture stable nor can it
withstand elevated temperatures.7 Since exposure to moisture
and oxygen can be effectively prevented via proper
encapsulation5 as other successful technologies (e.g., CIGS
solar cells) have overcome susceptibility to water vapors
through encapsulation,8 light-induced degradation remains as a
key challenge that needs to be tackled in order to realize more
stable devices.
Reports discussing the light-induced instability of PSCs
emphasize different causes of light induced degradation so far,
however the majority conclude that ultraviolet (UV) radiation
is the most damaging region of the solar spectrum.9,10 In
particular, the most commonly used electron transport layer
(ETL), titanium dioxide (TiO2), is reported to reduce device
stability under UV illumination in two ways. First, the
photocatalytic effect at the surface of the titanium dioxide
surface is reported to decompose the methylammonium lead
iodide (CH3NH3PbI3) perovskite to PbI2 in an irreversible
process.11−13 Second, upon UV exposure, deep trapping at
oxygen vacancies on the TiO2 surface is reported to strongly
enhance recombination and, thus, decreases performance of
the PSC. The oxygen vacancies originate from holes in the
valence band which recombine with adsorbed oxygen causing
desorption and leaving positively charged trap states of long
lifetime.14,15 To overcome these problems various approaches
have been suggested:9,16−18 (i) replacing TiO2 with another
ETL material; (ii) insertion of interfacial layers between the
Received: February 20, 2018
Accepted: June 11, 2018
Published: June 11, 2018

© 2018 American Chemical Society 21985 DOI: 10.1021/acsami.8b03024

ACS Appl. Mater. Interfaces 2018, 10, 21985−21990
ACS Applied Materials & Interfaces Research Article

TiO2 ETL and perovskite absorber; and (iii) the use of UV-
absorbing filters and introduction of luminescent downshifting
(LDS) layers to improve UV stability.
Despite the general understanding of the degradation
mechanism at the TiO2 surface upon UV illumination, the
literature remains inconclusive in defining the harmfulness of
UV degradation for PSCs.19−21 This is due to the multitude of
coexisting degradation mechanisms occurring across different
layers and interfaces of the PSC, including metal infiltration
from top contact to perovskite,4 deterioration of chemical
bonding between HTL and gold (Au) electrode,10 photo-
induced oxidation of spiro-OMeTAD22 and the dependence of
perovskite film thickness variation on photoinduced perform-
ance degradation.23 In addition, there is a lack of standardized
long-term illumination test conditions for PSC. Even the “class
A” spectral match of the standardized test conditions (STC)
for solar simulators does not provide an intensity specification
for UV light of wavelengths shorter than 400 nm.24 As a
consequence, the literature reports use of different UV spectra,
ranging from studies with light stress of one sun to studies
using only UV light stress.9,14,16 Moreover, various illumination
levels are used ranging from 1000 W m−2 of a 325 nm UV laser
light (>250 suns) to simulated one-sun and 100-suns spectra
without specifying in detail the UV content.18,25,26 The existing
standardized test with regard to UV stress is the International
Electrotechnical Commission (IEC) qualification test 61215,
which uses the air-mass 1.5 global (AM 1.5G) spectrum, but
this test does not ensure that a PV module will withstand >20
years of UV radiation.27 Thus, a comparative study of the
spectral dependence of the UV photostability of PSCs with
different device architectures is missing, as it is not clear which
UV wavelengths and at what intensities are detrimental to
device stability.

■ MATERIALS AND CHARACTERIZATION

In this Research Article, we present an extensive study of different
ETLs under different UV spectra to ascertain the spectral dependence
of UV degradation mechanisms within PSCs. Out of wide range of
ETLs used in PSCs28,29 (TiO2, SnO2, ZnO, ZrO2, BaSnO3, CdSe);
the studied ETLs are selected on the basis of their usage frequency in
PSC research and provided the fact that they bear the potential of low
temperature processability and high device stability (for example
SnO2) or yield the record-high efficiency (for example most widely
used TiO2).28,29 The devices used in this study are based on solution-
processed methylammonium lead iodide (CH3NH3PbI3 or MAPbI3)
employing five different kinds of ETLs: (i) tin oxide (SnO2); plus four
made from TiO2: (ii) post annealed at 500 °C compact (c-TiO2)
Figure 1. (a) Schematic illustration of perovskite solar cells under UV
illumination. UV spectral ranges are highlighted in red and blue along
with AM 1.5G spectrum; (b) short-circuit current density (JSC) values
for ITO/SnO2/MAPbI3 based solar cells exposed to 311 nm UV
(left) and 370 nm UV (right); (c) Stabilized PCEs of the reference
and UV-exposed devices with different ETLs illuminated with 311 nm
UV (left) and 370 nm UV (right).
glovebox. A schematic illustration of the UV exposure experiments is
presented in Figure S1.

deposited via spin coating; (iii) nanoparticles (np-TiO2) grown via
wet-chemical synthesis; (iv) TiO2 deposited via electron-beam
evaporation (e-TiO2); and (v) post annealed at 450 °C meso-TiO2
on top of compact TiO2. We have provided further details on device
fabrication in the Supporting Information (SI). The two different UV
spectra used are 310−317 nm (emitted from a narrowband UV−B
fluorescent Philips lamp, hereafter referred to as 311 nm UV) and
360−380 nm (emitted from an actinic Philips UV lamp in the UV-A
region, hereafter referred to as 370 nm), shown in Figure 1a. The
choice of these UV lamps is justified as the scarcity of the UV sources
with broad spectral emission limits such degradation studies to span
over many UV spectral bands. Initial experiments are “‘accelerated”’
such that the UV light intensities are significantly greater than the
respective UV content in AM 1.5G spectrum (112 times for 311 nm
and 57 times for 370 nm UV light). However, in a later control
experiment, we also verify the findings for lower intensities (11 suns
for 311 nm). In order to isolate only the effects from light-induced
degradation, all experiments are carried out in nitrogen (N2) filled
21986
■
RESULTS AND DISCUSSION
The schematic illustration of a perovskite solar cell under UV
illumination, highlighting the two different UV illumination
spectra tested in this study, along with the AM 1.5G spectrum
are shown in Figure 1a. All the devices are exposed to UV light
from the glass/ETL side, while the light exposure times are
recorded in terms of sun-hours. The transmittance of the ETL
coated substrates varies in the two wavelength ranges of
interest (310−317 nm and 360−380 nm) as shown in Figure
S2. It should be noted that average transmission for all ETLs in
the former wavelength range is low (∼20% on average for all
ETLs) because of absorption by the soda lime glass substrate,
while in the longer wavelength range the transmission is >70%
on average. The stress tests are performed on a number of
devices always including two kinds of reference configurations:
DOI: 10.1021/acsami.8b03024
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(i) the dark reference devices (6 in total), which are wrapped
with aluminum foil so that they experience the same heat stress
as other samples, but are not exposed to any light; and (ii)
devices covered with optical long-pass filters (4 in total), which
cutoff wavelength of 400 nm. The third set of devices (6 in
total) are the ones exposed to UV light for degradation testing.
Both types of references (dark and UV filters covered) are used
here to isolate the temperature effects (if any) as some studies
report the decreased device performance due to adverse effect
of temperature cycles (20−70 °C) on spiro-OMeTAD/
perovskite interface.30
The results of the experiments demonstrate that the devices
exposed to 311 nm UV experience severe decrease in short-
circuit current density (JSC). In contrast, devices exposed to
370 nm UV experience no degradation in general and a light
soaking effect in the case of the c-TiO2 devices is prominent.
Light soaking generally describes the improved performance as
a result of photoinduced structural transformation due to trap
filling by photogenerated carriers upon prolonged light
exposure.31 Figure 1(b) shows JSC measured for devices with
SnO2. The reference devices do not exhibit any decrease in JSC,
while devices exposed to 311 nm UV experience a significant
decrease in JSC of up to 64% over the 1750 sun-hour testing
period. We attribute this reduction to the decomposition of the
perovskite absorber layer.32 Charge generation and extraction
remains unaltered for the devices exposed to 370 nm UV
wavelength for equal number of sun-hours. The observed loss
in JSC at 311 nm UV resulted in reduced PCEs, measured by
tracking the power output of the PSC for 5 min at constant
voltage close to the maximum power point (hereafter referred
to as PCE-5 min). The open circuit voltage (VOC) is less
affected as compared to JSC, while the fill factor (FF) decreased
due to the decrease in JSC as shown in Figures S3−S5.
Additional data on the devices, like RS, RSh, and cross-sectional
scanning electron microscope (SEM) images are presented in
Figures S6−S8. The initial and final values of PCE-5 min for all
the devices exposed to both UV spectra are given in Table S1.
A similar trend of decreased JSC under 311 nm UV light is
observed for all other ETLs (c-TiO2, e-TiO2, np-TiO2)
decreasing 70.3%, 72.2% and 81.8% respectively, as shown in
Figure S3. This underlines the fact that degradation under
UV−B light is present for all types of ETLs. Interestingly
among all the studied ETLs, SnO2 appeared to be 43% more
stable in terms of PCE-5 min as compared to np-TiO2 (the
least stable). The findings reported here are also applicable in
devices based on meso-TiO2 as ETL which do not have state
of the art PCE as shown in Figure S9.
The trend in JSC degradation for the devices based on SnO2
and tested under 311 nm UV radiation translates into
reduction of PCE as illustrated in Figure 1c. The PCE-5 min
decrease is proportional to the JSC decrease for the same
devices. All devices with other ETLs (c-TiO2, e-TiO2, np-TiO2,
meso-TiO2) also show a decrease in stabilized PCE-5 min with
increasing exposure times when illuminated with 311 nm UV
light. In contrast, all the devices exposed to 370 nm UV show
no degradation in PCEs-5 min when compared to the
reference devices kept in dark or stored under UV filters.
For the PSCs prepared with SnO2, e-TiO2, and c-TiO2, the
initial PCE-5 min is maintained throughout the testing period.
A degradation in PCE-5 min is only observed for PSCs with
np-TiO2 ETL and stressed under 370 nm UV, as shown in
Figure 1c. However, this decrease is not caused by the UV
stress, as it is also apparent from the reference devices kept in
21987
Research Article
dark and under UV filters. It should be noted that the devices
with np-TiO2 ETL appear intrinsically less stable with regard
to PCE-5 min, although the PCE from voltage−current scan is
not degraded (see Figure S3). Furthermore, all TiO2 ETL
based devices exhibit similar performance degradation under
311 nm UV. Thus, it can be concluded that devices fabricated
using any of the ETLs investigated here exhibit similar
degradation trends when exposed to 311 nm UV irradiance,
while the reference devices retain their initial PCEs-5 min.
Having demonstrated a strong spectral dependence of the
UV degradation for PSCs with TiO2 and SnO2 ETLs for high
UV exposure intensities at 311 nm, the impact of UV intensity
is investigated. Since the intensities of both UV light sources
used in this study are high, ranging from 50 to 100 times more
than respective UV content in the AM 1.5G spectrum, it is
important to understand whether the observed degradation is
also present at lower intensities. To demonstrate that this
degradation is solely caused by the photon energy instead of
the high UV light intensity, polymer based UV long-pass filters
were used allowing only the 10% of incoming 311 nm UV light
(11 times of 311 nm UV content in AM 1.5G spectrum) to be
transmitted toward the devices under test. As demonstrated in
Figure 2, the degradation trend remains the same under 90%
Figure 2. UV degradation of perovskite solar cells based on a SnO2 as
ETL under ∼11 suns UV irradiation. Reference devices covered with
optical long-pass filters (left) are compared with the devices exposed
to UV light (right).
less intense 311 nm UV radiation, indicating that the UV light
intensity itself is not playing a major role here. Assuming a
linear degradation rate with respect to intensity, a PSC will
degrade at a rate of 1.27% /100 sun-hours of exposure time to
311 nm UV light. Due to their impact, these UV−B photons
cannot be ignored, since sunlight contains ∼1.6 W m−2 in the
UV−B band of 300−320 nm. This observation suggests that
this degradation trend may be the cause of instability of PSCs
under simulated one-sun solar irradiance.
The remedies suggested to prevent this 311 nm UV-
stimulated degradation include the employment of a UV filter
or a LDS layer. The former approach is already commonly
employed in PV applications. For example, the front glass sheet
of PV modules in extra-terrestrial applications is doped with
trivalent cerium (Ce3+) ions to minimize the impact of high
energy radiation,33 while for terrestrial applications UV
absorbers are used in commercial PV encapsulants like
ethylene vinyl acetate (EVA).34 However, while UV filtering
will protect devices from photodegradation, but the energy
content of the UV photons is not harnessed.
The addition of a LDS layer will also protect the devices
assuming total absorption of the harmful photons. However, it
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ACS Applied Materials & Interfaces
affords the advantage of not wasting the energy content of the
UV photons, but instead downshifting these via photo-
luminescence to longer wavelengths, hence harvesting a
fraction of the available photocurrent.9,35 The ideal case here
would be a LDS material with strong absorption in the UV
region of the spectrum and emission near the peak external
quantum efficiency (EQE) of the solar cells, in the range 600−
800 nm. However, it must be noted that the introduction of a
LDS layer also results in new loss mechanisms.36 The most
important are those arising from a subunity photolumines-
cence quantum yield (PLQY)defined as the number of
lower-energy photons emitted per the number of higher-energy
incident photonsand emission of light to directions other
than that of the solar cell (from the top and the edges of the
LDS layer). Additionally, the LDS materials can either be made
of organic or inorganic materials, and thus exhibit their own
UV stability issues. Thus, a trade-off between current gain and
increased device stability versus added complexity due to a
newly introduced layer and cost arises.36
To examine the potential of LDS layers for mitigating JSC
losses compared to UV filtering, a detailed calculation of total
loss in JSC and the potential regain of this lost JSC with
downshifting is done. It should be noted that this is an
estimation considering the favorable assumptions to realize the
potential use of LDS layers in Perovskite PV. A series of
experiments is required to explore the real practical gain
achieved from these luminescent layers. The estimated loss and
potential regain of the lost JSC is presented in Figure 3 showing
the JSC that will be lost by filtering the UV photons with
wavelength ranging from 300 to 400 nm with a step of 10 nm.
Figure 3. Loss and gain in integrated JSC by filtering out specific UV
wavelengths, maximum recoverable and the realistically recoverable
JSC via LDS materials.
These results show that if we cut off the photons of
wavelengths shorter than 360 nm, then the total lost JSC,
maximum recoverable JSC and realistically recoverable JSC are
0.53, 0.45, and 0.22 mA cm−2, respectively. Hence, it is
concluded that the LDS technology can afford the protection
from UV light and at the same time afford a small gain in terms
of photocurrent. This, however, is less than 0.3 mA cm−2 as
denoted by the realistic scenario in Figure 3, which still
includes favorable assumptions. Here, it should also be noted
that up-to-date there are no luminescent materials that will
exhibit 100% PLQY for the long period of time that a PV
module is expected to withstand sunlight exposure in the field
(>20 years). Hence, it is concluded that the approach of
filtering the UV light appears to be the simplest, leading to
protection of the devices at the cost of a very small fraction of
the available photocurrent.
21988
Research Article
■ CONCLUSIONS
In summary, spectral dependent UV degradation of PSCs is
studied for two kinds of UV light spectra: (i) a 310−317 nm
band, referred as 311 nm UV and (ii) a 360−380 nm band,
referred as 370 nm UV. We find that 370 nm UV radiation
only causes 64% degradation in stabilized PCE-5 min in PSCs
based on np-TiO2 ETLs. For other devices using SnO2 or TiO2
(c-TiO2 and e-TiO2) as ETLs no performance degradation is
observed. In contrast, 311 nm UV radiation heavily
deteriorates the JSC of all PSCs−regardless of whether SnO2
or TiO2 ETLs are utilized within the devices−already after 500
h. The overall quantification of degradation in PCE-5 min for
devices based on SnO2, c-TiO2, e-TiO2 and np-TiO2 as ETLs
is 50%, 69%, 83%, and 88%, respectively, after an exposure
period of >1700 sun-hours. To establish a global reference for
photostability studies of PSCs, the intensities of UV light are
translated to AM 1.5G spectral content for the respective UV
radiation bands. The degradation rate slightly depends on the
intensity of photon dose but, in general, similar stability issue
persists even with 10 times less intense UV radiations. To
address the UV light induced degradation of PSCs, the most
simple solution is to filter the UV photons with UV−B
wavelengths at the cost of a small fraction (0.53 mA cm−2) of
photocurrent. However, the implementation of LDS layer can
ideally recover photocurrent of up to 0.3 mA cm−2.
■
*
ASSOCIATED CONTENT
S Supporting Information
The Supporting Information is available free of charge on the
ACS Publications website at DOI: 10.1021/acsami.8b03024.
Materials and device fabrication methods; transmittance
of all used ETLs; schematic of UV exposure setup; initial
and final PCE values of all devices; plots of device
parameters like JSC, VOC, FF, RS, RSh; cross sectional
SEM images; details of the calculation of JSC loss and
gain using UV filtering and downshifting (PDF)
■ AUTHOR INFORMATION
Corresponding Authors
*E-mail: amjad.farooq@kit.edu.
*E-mail: ulrich.paetzold@kit.edu.
ORCID
Amjad Farooq: 0000-0002-8604-8536
Ihteaz M. Hossain: 0000-0001-6533-1757
Jonas A. Schwenzer: 0000-0001-8795-4875
Tobias Abzieher: 0000-0002-2733-0136
Bryce S. Richards: 0000-0001-5469-048X
Notes
The authors declare no competing financial interest.
■ ACKNOWLEDGMENTS
The authors would like to acknowledge financial support of the
German Federal Ministry for Education and Research (BMBF
project PeroSol FKZ 03SF0483B); the Helmholtz Association
for the Young Investigator Group of Dr. U. W. Paetzold;
Recruitment Initiative of Prof. B. S. Richards; the Helmholtz
Energy Materials Foundry (HEMF); and the Science and
Technology of Nanostructures research programme); as well
as the Karlsruhe School of Optics and Photonics (KSOP).The
authors express their gratitude to the great spirit of the “KIT
perovskite PV taskforce” and the KIT Young Investigator
DOI: 10.1021/acsami.8b03024
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ACS Applied Materials & Interfaces
Network. Mr. Amjad Farooq thankfully acknowledges the
financial support from DAAD (Deutscher Akademischer
Austauschdienst/German academic exchange service) for his
doctoral research work under personal reference number
91604868.
■
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21990 DOI: 10.1021/acsami.8b03024

ACS Appl. Mater. Interfaces 2018, 10, 21985−21990