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2021 AnandA - Introduction of A Novel Figure of Merit For The Assessment of Transparent Conductive Electrodes
2021 AnandA - Introduction of A Novel Figure of Merit For The Assessment of Transparent Conductive Electrodes
2021 AnandA - Introduction of A Novel Figure of Merit For The Assessment of Transparent Conductive Electrodes
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Adv. Energy Mater. 2021, 11, 2100875 2100875 (1 of 16) © 2021 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH
16146840, 2021, 26, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/aenm.202100875 by Universidade Nova De Lisboa, Wiley Online Library on [03/11/2023]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
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T 10 1
φTC = ,[φTC ] = = Ω −1 (4)
R Ω −1
Metal
oxides with φTC being the figure of merit in units of Ω−1, where T is
the transmittance at 550 nm, and R□ is the sheet resistance.
Dielectric
/Metal/ Ultra thin This modification yielded the best value of φTC for a given con-
Dielectric metals ductivity when the transmittance was surpassing 90%.
After the turn of the millennium, Dressel and Grüner sug-
gested a dimensionless figure of merit by comparing, respec-
tively dividing, the zero-frequency (DC) conductivity with the
TCEs conductivity in the optical regime. The transmittance and the
optical conductivity can be related as[23,24]
Graphene Metal
nanowires −2
T = 1 + o σ OPt
Z
(5)
2
T %
φTC = , [φTC ] = = % Ω −1 (1) where σDC is the direct conductivity, R□ is the sheet resistance
R Ω −1 and t is the thickness of the film. Solving for t and putting in
Equation (5), the transmittance can be written as
with φTC being the figure of merit in units of % Ω−1 where
according to the Lambert–Beer law, the transmittance T is a Z σ
−2
In the FOM defined by Fraser and Cook, the transmittance is σ DC 188.5 σ Scm −1
φTC =
σ OP
= , [φTC ] = σ DC = Scm −1 = 1 (8)
only considered at 550 nm, corresponding to the maximum of − 12 OP
R T − 1
photopic vision. R□ is the sheet resistance, which is defined as
the resistance of one square-shaped tile of the electrode. Gener-
ally, the sheet resistance is a size-independent magnitude with with φTC being dimensionless, and T and R□ as defined above.
unit ohm square−1 (Ω □−1), where □ signifies a square-shaped However, De et al. and Jacobs et al. showed that the figure of
area of an electrode with arbitrary edge length and thus size. merit defined by Dressel and Grüner is restricted in its appli-
For a square tile, the length (l) and the width (w) equate, and cation to thin uniform layers, as it overestimates the value of
only the thickness (t) remains in the classical formula for calcu- having a low sheet resistance when at the same time the trans-
lation of the resistance of a conductor mittance is low.[24,25]
Recently, Cisneros-Contreras et al. showed in their work that
l 1 1 Haacke’s figure of merit was unfortunately inefficient for TCEs
R = · = (3)
w·t σ t·σ with low transmittance and slightly modified the proposed equa-
tion to increase the resolution of the figure of merit by up to two
Therefore, the sheet resistance does not depend on the size of orders of magnitude by assigning more importance to the trans-
the area through which current is transported but rather on its mittance against the sheet resistance. As a result, the figure of
geometry.[18,19,21] The choice of Fraser and Cook was simple and merit, named “FOM Haacke High Resolution,” was defined as[26]
straightforward and thus efficient: The FOM indicates higher
T 1
values for higher transmittance and lower sheet resistance, φTC = , [φTC ] = = Ω −1/n (9)
being mediated by a simple ratio between these two quantities.
n
R (Ω )
−1 1/n
Adv. Energy Mater. 2021, 11, 2100875 2100875 (2 of 16) © 2021 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH
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One of the other major concerns about all figures of merit did analyze with the novel figure of merit for a given constant
discussed so far is the limitation of the value of transmittance transmittance, where the critical transition for suitable sheet
to a single point (550 nm), which makes analysis of broad-range resistances can be found, which may be used to direct the TCE
light transmission impossible. It should be noted that the latter materials development goals consciously.
is a very important criterion for solar cell performance. In addition, recently demonstrated semi-transparent elec-
As a consequence, in 2016 Mendez-Gamboa et al. took an alter- trodes were assessed using the established and the exact FOMs
native approach to calculate the figure of merit for TCEs, and for a given spectral range from 350 to 800 nm. For that, the
instead of the transmission they simply took the resulting photo- transmittance and sheet resistance data were extracted from lit-
voltaic magnitude into account, namely, the maximum attainable erature using an online tool.[28] We note that many alternative
photocurrent density by including the whole spectral information approaches to the state-of-the-art transparent conductive elec-
of the transmittance of the TCEs and using the air mass 1.5 global trodes like indium tin oxide (ITO) and fluorine tin oxide (FTO)
photon flux spectrum. The FOM was defined as[27] already exist that are very suitable for application in photovol-
taics. In summary, it is demonstrated that the exact figure of
( JPH )max mA cm −2 merit provides decisive information for the application-specific
φTC =
R
, [φTC ] = Ω −1
= mA cm −2 Ω −1 (10)
development of transparent conductive material systems.
Adv. Energy Mater. 2021, 11, 2100875 2100875 (3 of 16) © 2021 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH
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arising from the sheet resistance. For the otherwise ideal solar observed, as pursued by the originators (see above). However,
cell, the parallel resistance is assumed to be infinite as it is a and most intriguingly, the gap between the standard values for
property of the entire photovoltaic layer stack and, thus, not a TCEs (transmittance: 90% and sheet resistance: 100 Ω □−1)
direct consequence of the TCE. and the ideal value (transmittance: 100% and sheet resistance:
Our novel and exact figure of merit is thus defined as the 0.0001 Ω □−1) was huge for the FOMs (a)–(d) (Fraser and Cook;
ratio of the power generated by an ideal solar cell having a Haacke; Dressel and Grüner; Gamboa et al.), whereas FOM
bandgap EG and length l for a particular TCE defined by its (e) (Contreras et al.) depicted only a factor of two between the
spectral transmittance and sheet resistance, to the power gener- same. Owing to the complexity of calculation, the exact FOM
ated by the same ideal solar cell with an ideal TCE (where R□ (f) captures the proper balance of impacts between transmit-
is for practical reasons set to be 0.0001 Ω □−1 and the transmit- tance and sheet resistance of TCEs, which is also indicated by
tance throughout the spectral range is 100%) a linear dependency on the transmittance for most of the R□
range. More details about the FOM values in higher resolu-
tion owing to smaller sheet resistance ranges can be found in
PMPP (E G , T ( λ ) , RS (R ) , l ) Figures S3–S8 (Supporting Information).
φTCE,exact = ,
PMPP (E G ,T = 100%∀λ , R = 0.0001 Ω −1 , l ) (13) For an improved understanding of the dependencies of
W the various FOMs on the sheet resistance, the different FOM
[φTCE,exact ] = W = 1 values were replotted in a cross section for transmittance of
90%, which is, in practical terms both, a desirable and a (nearly)
The bandgap (EG) and the solar cell length (l) are principally achievable value. The comparison for other hypothetical TCEs
system-specific parameters. Note that as long as only the series with various transmittance values can be found in Figure S9a–j
resistance is concerned, the solar cell width (perpendicular to (Supporting Information).
the current transport direction) does not influence the perfor- At first, it can be noted that FOMs (a)–(d) (Figure 3) show
mance of the device in the case of a classical overlapping stripe identical behavior on the double logarithmic plot. They span a
layout of the solar module. The transmittance spectrum T(λ) range of five orders of magnitude for an equal change in sheet
and the sheet resistance (resulting in an effective series resist- resistance but are shifted from each other by certain prefactors.
ance RS) can thus be seen as variables in terms of the develop- This is indeed not surprising, as they are all proportional to
ment of transparent conductive electrodes. 1/R□ and only vary in their proportionality factor. In contrast to
Admittedly, this exact FOM appears to be both, i) a trivial these ones, the FOM (e) suggested by Contreras et al. exhibits
choice as well as ii) not a proper choice at all, as the calcula- only a very weak dependence on the sheet resistance and varies
tional effort surpasses the established FOMs by far. However, by less than one order of magnitude. Upon comparison with
based on it, we will be able to assess the established FOMs in the exact FOM, it is evident that the functional dependence of
great detail, as it is an exact calculation of the influence of TCE the FOMs (a)–(d) is in good agreement for sheet resistances
properties on the attainable photovoltaic performance. The above 100 Ω □−1, whereas for values below 100 Ω □−1 the FOM
complete derivation of the exact figure of merit can be found (e) is showing a nice agreement even for the absolute value.
in Section S1 (Supporting Information). As a check-up for the The drastic change in the behavior of the FOM (f) can be char-
reliability of our calculations, we initially reproduced the effi- acterized by a critical sheet resistance R□,c, at which half the
ciency limit (Figure S2, Supporting Information), following the maximum value of the attainable performance can be reached
approach by Shockley and Queisser,[31] for the global AM1.5G and where the function undergoes a change in curvature, i.e., it
sun spectrum and indeed found convincing agreement with shows a deflection point. This characteristic change in behavior
the results published by Rühle.[32] located at 140 Ω □−1 is unfortunately not captured by any of
the other FOMs, owing to the simplicity of the formulas. The
inset figure shows the critical sheet resistance extraction from
3. Results and Discussion the curve of (our exact) FOM (f) and can be found enlarged in
Figure S10 (Supporting Information). For materials scientists
3.1. Comparing and Assessing Established Figures of Merit and developers of novel TCEs, the critical sheet resistance R□,c
is important information, because it indicates whether a mate-
To compare with and assess the established figures of merit, rial system is suitable or not for a given solar cell length l and
we ran a simulation program for hypothetical TCEs having whether the interesting region of conductivity is in close reach.
transmittances running from 10% to 100% (throughout the Intrigued by the FOM (e) to closely follow the exact calcula-
spectral range from 280 to 1100 nm) and sheet resistances run- tion, we were searching for an even better suitable parameter
ning from 0.1 to 1000 or 10 000 Ω □−1. Figure 2 shows con- n in the formula of Contreras et al. After short optimization,
tour plots which provide an initial comparison between the we identified n = 100 to be close enough to optimal accordance
different figures of merit suggested by a) Fraser and Cook, b) with the exact calculation (Figure S11, Supporting Information).
Haacke, c) Dressel and Grüner, d) Gamboa et al., e) Contreras By using this modified FOM (e) and by renormalizing FOMs
et al., and f) our exact FOM, respectively, the exact calculation (a)–(d) to the exact calculation, it was possible to construct the
of the impact on the performance of otherwise ideal solar cells. established FOMs as tangents to our novel and exact FOM and
It is evident from the plots that FOMs (a)–(d) show a very pro- to identify another interesting transition: θR□, the transition
nounced dependency on the sheet resistance, whereas FOMs sheet resistance above which the validity of FOM (e) is get-
(e) and (f) depict a milder impact of the same. Among FOMs ting worse, and where any of the renormalized FOMs (a)–(d) is
(a)–(d) some variation in the impact of the transmittance can be closely following the exact calculation. This fact is illustrated in
Adv. Energy Mater. 2021, 11, 2100875 2100875 (4 of 16) © 2021 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH
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Figure 2. Comparison between established figures of merit: a) Fraser and Cook, b) Haacke, c) Dressel and Grüner, d) Gamboa et al., and e) Contreras
et al., and f) our exact figure of merit, respectively, the exact calculation for the impact of transmittance and sheet resistance on photovoltaic perfor-
mance for the spectral range from 280 to 1100 nm and a solar cell length of 5 mm.
the following Figure 4. Clearly, the transition sheet resistance crossing point between renormalized FOMs (a)–(d) and FOM
separates two regimes of operation: the transmittance and the (e). For comparison and completeness, the critical sheet resist-
sheet resistance limited regime. ance obtained from the exact figure of merit is also depicted.
As a result, for the hypothetical case of 90% transmittance To learn more about the functional dependence of the
and an absorption range from 280 to 1100 nm, the transition transition sheet resistance, the solar cell length was varied
sheet resistance (θR□) was identified as 80 Ω □−1 by taking the between 2.5 and 20 mm and the transition sheet resistance was
Adv. Energy Mater. 2021, 11, 2100875 2100875 (5 of 16) © 2021 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH
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∆V
RS = (14)
∆I
VOC − 0 V
RS = = OC (15)
0 − ( −ISC ) ISC,SRL
l
RS = R · (16)
3w
with l and w being the length and the width of the solar cell, we
Figure 3. Comparison between different figures of merit versus sheet
finally obtain the power output of the solar cell under SRL
resistance for a hypothetical TCE having a transmittance of 90%
throughout the spectrum considered (280–1100 nm).
VOC 3 w V 2
evaluated as described above for a TCE having 90% transmit- PMPP,SRL = ISC ·VOC ·FF = ·VOC ·25% = · · OC (17)
l 4 l R
tance throughout the spectral range from 280 to 1100 nm. The R·
3w
results are depicted in Figure S12a–d (Supporting Information),
which already indicates a rather simple dependency of θR□ on In the special case of series resistance limited IV-character-
the length of the solar cell. istics (or in other words, conductance limitation), the fill factor
To find a mathematical way of deriving the transition sheet is strictly 25% (compare with Figure 5 above). And thus, we
resistance, we reflected upon the power output of a solar cell, obtain for the approximate figure of merit in the SRL regime
which is completely limited by the series resistance (RS). The
following Figure 5 displays such a series resistance limited PMPP, SRL
φTCE,SRL = (18)
(SRL) situation, where RS dictates the shape of the IV character- PMPP, SQL AM1.5
istics in the fourth quadrant.
It is now easy to note down the power output of such a whereas for the transmittance limited (TL) regime, we can
device. Because in general simply choose for approximation (thanks to the normalization
of the exact FOM)
3 w VOC 2 1 (21)
⇔ Tavg = · · ·
4 l θ R ISC,max·VOC·FFmax
Figure 4. Definition of the transition sheet resistance, θR□, which separates 3 w 1 VOC (22)
the regions of validity: below the FOM of Contreras et al. is valid if n = 100 is ⇔ θ R = · · ·
4 l Tavg ISC,max·FFmax
set and above any of the FOMs of either Fraser and Cook; Haacke; Dressel
and Grüner; or Gamboa et al. can be used. The latter were renormalized to
show their equivalence with the exact FOM. The calculation was done for a
3 w 1 VOC
hypothetical TCE having a transmittance of 90% throughout the spectrum ⇔ θ R = · · · (23)
considered (280–1100 nm) and a solar cell length of 5 mm. 4 l Tavg w··
l JSC,max·FFmax
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Adv. Energy Mater. 2021, 11, 2100875 2100875 (7 of 16) © 2021 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH
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Photovoltaic material systems Wavelength range Δλ [nm] Bandgap [eV] Efficiency SQL AM1.5G [%]
c-Si, m-Si, nc-Si, CIGS, CZTS 280–1100 1.13 33.4
GaAS, CdTe, InP, PbS QD 280–900 1.38 33.6
Dye/TiO2 (DSSC) 280–830 1.49 32.2
Typical OPV, perovskite 280–800 1.55 31.4
a-Si, GaInP 280–700 1.77 27.7
AgrOPV (OPV for Agrivoltaics) 700–1100 1.13 17.4
to switch between those equivalent formulations of FOM for (a-Si) and the gallium indium phosphide (GaInP) material
TCEs. system.[35]
Behind the real dependence of the photovoltaic performance Based on the SQL at AM1.5G conditions, all photovoltaic
on the two factors, transmittance and sheet resistance, there parameters were computed and are displayed in Figure 7. The
is just one lingering question: which of the two parameters is values can also be found in Table S2 (Supporting Information)
currently limiting the device function? Sufficiently well below and can be used to calculate the transition sheet resistance for
the transition sheet resistance, it is simply the transmittance, the TCE system of interest. The results for the exact figure
whereas, above the same, the situation is reversed. The latter of merit for combinations of the transmittance and the sheet
can be also understood as being the case, where photovoltaic resistance for different photovoltaic material systems can be
performance is limited by the conductance of the transparent found in Figure S13 (Supporting Information) and are gener-
conductive electrode as conductance is the reciprocal of resist- ally similar to Figure 2f.
ance, whose unit is the mho (℧) or Siemens (S). To clearly understand the impact of the bandgap of dif-
ferent photovoltaic material systems, the exact figure of merit
was plotted over the sheet resistance for various photovoltaic
3.2. Assessment of Photovoltaic Material System Requirements materials for a TCE having a transmittance of 90% throughout
by the Exact Figure of Merit the spectral range (Figure 8). Smaller absorption ranges, cor-
respondingly larger bandgaps, and thus smaller photocur-
As solar cells based on different photovoltaic material sys- rents result in lower sheet resistance requirements, implying
tems will exhibit different requirements concerning the that larger sheet resistances are possible. Figure 8 furthermore
TCEs, we have analyzed various material systems with regard depicts the critical sheet resistance, being evaluated at half the
to their maximal photovoltaic parameters under AM1.5G in average transmittance value (0.45), and the threshold FOM for
the SQL. the target sheet resistance, which is 0.85 for the case of 90%
Table 1 summarizes properties of typical PV material sys- transmittance.
tems according to their absorption wavelength range, their Table 2 lists the critical sheet resistance (R□,c), the transi-
electronic bandgap, and their attainable SQL AM1.5G perfor- tion sheet resistance (θR□) calculated by Equation (24), and the
mance. We have named in particular for agrivoltaics suitable target sheet resistance (R□, target) calculated by Equation (25).
material system “AgrOPV” (OPV for Agrivoltaics), as it can While the critical and transition sheet resistances were intro-
potentially be realized owing to the very specific property of duced via meaningful mathematical definitions, the target
organic semiconductors to exhibit limited absorption bands. sheet resistance is somewhat more arbitrarily defined and has a
When the latter is tuned into the near-infrared (NIR) region more practical purpose. It is meant to direct researchers in the
(700–1100 nm), the light absorption of plants is basically unaf- process of designing TCEs for a particular photovoltaic mate-
fected.[33] The spectral wavelength range from 280 to 1100 nm rial system. The calculational effort is much lower than for the
generally includes PV systems such as crystalline silicon exact FOM, since here experimentally obtained photovoltaic
(C-Si), monocrystalline solar cell (m-Si), copper zinc tin sulfide parameters can be applied to predict sheet resistance require-
(CZTS), and copper indium gallium selenide solar cells (CI(G) ments to limit the conductivity related losses to below 5%.
S) solar cells which are among the reported high-efficiency
solar cells.[34,35] The spectral wavelength range from 280 to
900 nm includes thin-film semiconductors, multijunction 3.3. Assessment of State-of-the-Art Transparent Conductive
solar cells such as gallium arsenide solar cells (GaAs), cad- Electrodes by Exact FOM
mium telluride solar cells (CdTe), as well as indium phosphide
(InP), and lead sulfide quantum dots (PbS QD) PV systems.[35] In this section, we are going to compare various concepts for
Dye-sensitized solar cell (DSSC), a third-generation PV system, transparent conductive electrodes which were recently sug-
falls under the spectral wavelength range of 280–830 nm. gested for use in solar cells. To evaluate the performance of
The spectral wavelength range from 280 to 800 nm includes various electrodes, transmittance and sheet resistance data
organic photovoltaics (OPV) and hybrid perovskites which were extracted from the literature and their performances
are emerging PV systems.[34,36] The spectral wavelength range were rated based on established FOMs (only in the Supporting
from 280 to 700 nm includes amorphous silicon solar cells Information) and the exact FOM. Figure 9 displays the sheet
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Figure 7. Absorption wavelength range of different photovoltaic material systems versus a) short-circuit current density, b) open-circuit voltage, c) fill
factor, d) maximum power point, e) dark saturation current density, and f) power loss at maximum power point due to series resistance.
resistance values of various TCEs investigated in this study, A very well-known standard for TCEs, being generally used
while Figure 10 shows the transmittance spectra of the TCEs for the most efficient solar cell devices, is ITO.[36] It displays
sorted into different subgroups. It must be stated though, a state-of-the-art material in the field of TCEs, to which new
that transmittances above 90% are to be taken with caution as concepts are generally compared.[37,38] ITO exhibits a very
already bare glass slabs provide a maximum transmittance of high charge carrier concentration of ≈1021 cm−3 and a high
92% owing to the inevitable reflectance losses. Experimentally, conductivity in the range of 104 S cm−1. The wide gap of
higher transmittances are to be achieved by using anti-reflec- ITO (≈3.75 eV) leads to a transmittance of more than 80%
tion layers. To enable a comparative study between the dif- in the visible range, which makes it the first choice for the
ferent TCEs, transparency losses owing to glass were included electrodes.[39] Several drawbacks, such as the use of rare ele-
(i.e., added) explicitly in cases of extraordinarily high transmit- ment indium, low mechanical and chemical stability, energy-
tance. The transmittance spectra of bare glass can be found in intensive processing, and high costs trigger the steadily rising
Figure S14 (Supporting Information). interest in new and alternative material systems (Figure 1).[1]
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Figure 8. Exact figure of merit versus sheet resistance computed for dif-
ferent photovoltaic material systems, having a transmittance T = 90% Figure 9. Summary of sheet resistance values for different TCEs evalu-
throughout the spectral range and a solar cell length of 5 mm. Further- ated in this work.
more, the critical sheet resistance is evaluated and the FOM for the target
sheet resistance is depicted as well. Originally developed in the 1970s,[45] conductive polymers
have gained great popularity within the field of optoelectronics
In this study, commercially available ITO substrates used in owing to their versatile applicability. Among all, poly(3,4-ethylene
our lab were assessed. dioxythiophene):polystyrene sulfonate (PEDOT:PSS) is the most
FTO also marks a state-of-the-art electrode apart from ITO. popular and commercially most successful conductive polymer,
FTO, being a nontoxic material, is often considered for thin- which is broadly used for transparent electrodes and charge
film solar cells and modules. For the DSSC PV system, FTO transport layers in the field of photovoltaics. PEDOT:PSS con-
is the most widely used electrode because of its good stability sists of a conductive part, the conjugated polymer PEDOT, and
at high temperatures and under acidic conditions.[40] In this an insulating polyelectrolyte PSS that encapsulates the former.[46]
work, an FTO fabricated by using horizontal ultrasonic spray PSS is generally used in formulations to bring PEDOT into an
pyrolysis deposition[40] was evaluated exemplarily. aqueous processable form. While as-prepared PEDOT:PSS
Ultrathin metal films (≈10–25 nm thick) like gold (Au), alu- films have low conductivity, doping or post-processing treat-
minum (Al), silver (Ag), copper (Cu), etc., and combinations of ments with solvents, surfactants, salts, etc., have shown to
them have been widely explored as electrodes for photovoltaics. increase the conductivity of PEDOT:PSS films.[46] For example,
Owing to very low film thickness, these metal layers are semi- dimethyl sulfoxide (DMSO) is a commonly used polar solvent
transparent to visible light. Although thin metal films permit for inducing enhanced phase separation between PEDOT and
light to be transmitted through it, maintaining the smooth mor- PSS. This leads to increased interactions between individual
phology of the films is crucial as it governs the conductivity of PEDOT chains and decreases the interaction with the PSS seg-
the films.[41] Surface modifications via surfactants[42] and the use ments, which yields an overall improved phase connectivity of
of metal seed layers[43] are often carried out to fabricate smooth the charge conducting PEDOT.[47,48] We included our own pro-
films which can yield good conductivity and optical transpar- cessed PEDOT:PSS (PH1000), modified by 5% v/v DMSO addi-
ency. In this work, TCEs based on metal films—Ag, Au, Ag/Au, tion, to this comparative evaluation. Various other PEDOT:PSS
and Au/Ag/Au and C60-surfactant/Ag[42–44]—were evaluated. modifications obtained by polyethylene oxide (PEO), sulfuric
Table 2. Critical, transition and target sheet resistances are summarized for the different photovoltaic material systems defined according to their
bandgap and spectral absorption range. The transmittance was assumed to be 90% throughout the spectral range, and the solar cell length was
5 mm.
Photovoltaic material systems Wavelength range Critical sheet resistance Transition sheet resistance Target sheet resistance
[nm] R□,c [Ω □−1] θR□ [Ω □−1] R□,target [Ω □−1]
c-Si, m-Si, nc-Si, CIGS, CZTS 280–1100 138.6 77.7 13.0
GaAS, CdTe, InP, PbS QD 280–900 224.9 123.7 20.6
Dye/TiO2 (DSSC) 280–830 281.7 155.7 25.9
OPV, perovskite 280–800 316.3 173.1 28.8
a-Si, GaInP 280–700 487.7 265.2 44.2
AgrOPV (OPV for Agrivoltaics) 700–1100 255.0 144.1 24.0
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Figure 10. Transmittance spectra of different groups of TCEs a) metal oxides, b) ultrathin metals, c) conductive polymers, d) carbon nanotubes,
e) graphene, f) metal nanowires, g) dielectric/metal/dielectric, and h) metal networks groups. The transmittance data were extracted from literature
using an online tool.[28]
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Table 3. Comparison of the exact FOM evaluated for different TCEs, done over a spectral range of Δλ = 350–800 nm and for a solar cell length of
5 mm.
TCE Sheet resistance [Ω □−1] Average transmittance Substrate Exact figure of merit Reference
(350–800 nm) [%]
Metal oxides
• ITO 10 85.53 Glass 0.846 This work
• FTO 4.0 ± 0.14 83.81 Glass 0.849 [40]
Ultrathin metals
• Ag 15.7 49.79 Glass 0.479 [43]
• Au 7 43.50 Glass 0.447 [43]
• Ag/Au 7.8 50.70 Glass 0.486 [43]
• Au/Ag/Au ≈10.42 ± 0.5 48.43 Glass 0.467 [44]
• C60-surfactant/Ag 1.70 21.24 Glass 0.180 [42]
Conductive polymers
• PEDOT:PSS + DMSO 64 81.37 Glass 0.730 This work
• PEDOT:PSS + PEO 72 91.84 Glass 0.745 (0.803) [49]
• PEDOT:PSS + H2SO4 46.1 95.41 Glass 0.809 (0.873) [50]
• PEDOT:PSS + Zonyl 46 79.09 Glass 0.728 [51]
• PEDOT:PSS + CF3SO3H 32 85.99 PET 0.815 [52]
Carbon nanotubes
• Pristine CNT 17 78.92 Glass 0.778 [55]
• CNT/Cu 39 79.14 Glass 0.752 [56]
Graphene
• Graphene/PEDOT:PSS/ZnO 230 86.13 Glass 0.555 [60]
• TFSA-Graphene 185 87.29 PET 0.619 [61]
• Cu/Graphene ≈75 90.63 Glass 0.755 (0.812) [59]
• Cu-BHT 200 78.29 Glass 0.569 [62]
Nanowires
• AgNW1 10.3 88.10 Glass 0.869 [65]
• CuNW1 51.5 89.35 PET 0.821 [66]
• CuNW2 11.2 90.88 Glass 0.893 [67]
• AgNW2 8.5 89.15 Glass 0.880 [67]
• AgNW3 ≈10 76.30 Glass 0.783 [68]
Dielectric/metal/dielectric
• ZnS/Cu:Ag/WO3 31 78.98 Glass 0.752 [70]
• AZO/Ag/AZO 6 79.04 Glass 0.789 [71]
• MoO3/Ag/MoO3 5 86.11 Glass 0.860 [72]
• ZnS/Cu/Ag/ZnS 4.8 81.54 Glass 0.833 [73]
• AZO/Ag NW/AZO/Zn* 11.3 88.63 Glass 0.883 [74]
Metal network
• Ag metal mesh 10 85.89 Glass 0.842 [76]
• Cu nanotrough 15 95.45 Glass 0.856 (0.928) [77]
• Ag nanotrough 15 86.57 Glass 0.770 (0.842) [77]
• Al nanotrough 21 66.16 Glass 0.569 (0.641) [77]
• Au nanotrough 17 91.86 Glass 0.818 (0.890) [77]
Note: TCEs with a * were evaluated for Δλ = 400–800 nm due to insufficient data below 400 nm.
The values inside brackets represent FOM values of TCEs for which only film transmittance spectra were taken into account for the analysis.
a threshold of 80% of the theoretically maximum attainable approach constitutes the group of dielectric-metal-dielec-
performance. The technical standards, ITO, and FTO can be tric layer (DMD) layer stacks, where three examples can be
found clearly above this demarcation line. Gratifyingly, 12 found above 80%, and even the remaining ones were gen-
alternative approaches made it over this threshold as well. erally close to that. The group of “metal-nanotrough” layers
While unfortunately, all ultrathin metal layers failed to over- was another successful approach as two out of four materials
come this threshold, two of the highly conductive PEDOT:PSS exceeded the threshold. If only film transmittances were to
formulations reached upon treatments above a FOM of 80%. be considered, this approach would yield the highest FOMs
The group of metal nanowires generally showed high FOMs, among all studied. Last but not least, the silver-based “metal-
exceeding the 80% threshold in four out of five cases. In mesh” approach also surpassed the ITO performance for
the group of graphene, only one electrode yielded close to TCEs. For a comparison of the results obtained by the exact
80%, when considering glass in addition. A very successful FOM with the results obtained by the established FOMs, the
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reader is referred to Figures S15a–f and Table S3 (Supporting Characterization of PEDOT:PSS Films: The sheet resistance was
Information). measured using the SURAGUS sheet resistance tester—EddyCus TF
While this section is ultimately focusing on the material lab 2020SR. Transmittance was measured using the Avantes AvaSpec-
ULS3648-USB2-UA-25 fiber spectrometer.
properties of TCEs, it should also be noted that large-scale Simulation Methods: Different photovoltaic material systems[35]
photo voltaic production requires low material and fabrica- (Table 1) were accessed in this study. The evaluation of FOM for all
tion costs. The latter, of course, is an important factor to be TCEs was carried out using a MATLAB program. The program calculated
considered for the appropriate selection of transparent conduc- the photovoltaic power for a given solar cell length according to the
tive electrodes in real-life applications. Shockley–Queisser limit by using the photon flux descriptions of black
body radiation at 300 K and the AM1.5G solar spectrum, once for
optimal values of sheet resistance R□ = 0.0001 Ω □−1 and 100% light
transmission, and once for the conditions specified by transmittance
4. Summary and Conclusions spectra, the sheet resistance, and the photovoltaically active spectral
range, yielding the exact figure of merit. The transmittance data were
In this report, we have introduced two versions of a novel figure extracted from each publication using an online tool called web plot
of merit: one exact form based on computing the impact of digitizer.[28]
sheet resistance and transmittance spectra on the attainable
maximum performance according to the Shockley–Queisser
limit and one approximate form. While the computing effort Supporting Information
for the exact form requires a numerical approach, the simplified
and approximate form can be applied based on researchers’ own Supporting Information is available from the Wiley Online Library or
from the author.
experimental data. Furthermore, we have identified two more
parameters, which enabled us to formulate the exact figure of
merit: the solar cell length (l) and the spectral range (Δλ). Both
of these values show a strong effect on the sheet resistance of Acknowledgements
the transparent conductive electrode. The approximate FOM The authors gratefully acknowledge Dr. Gregory Welch, Dr. A. Markus
contains at least the same information as all the established Anton, Josef Bernd Slowik, Zhuo Xu, Philip Zimmer, Ju Hwan Kang,
FOMs so far, but it provides with the transition sheet resist- Prof. Yi Cui, Prof. Jooho Moon, and Dr. Xi Fan for their helping hands
ance a demarcation line between the observed two limiting and fruitful discussions. A.A. acknowledges financial support by DAAD
cases generally valid for TCE application in photovoltaics: a) the (Deutscher Akademischer Austauschdienst). H.H. and U.S.S. are
transmittance limited regime is found at the low end of sheet grateful to the Thüringer Ministerium für Wirtschaft, Wissenschaft und
Digitale Gesellschaft (TMWWDG) for funding the CEEC Jena. Part of the
resistances, whereas the b) conductance limited regime is natu- equipment used in this study was acquired within the “Innovation Center
rally found beyond the transition sheet resistance. CEEC Jena” project funded by the Free State of Thuringia under number
By analyzing the impact of photovoltaic material classes, 2016 IZN 0009 and co-financed by funds from the European Union within
we could demonstrate that the spectral range used plays an the framework of the European Regional Development Fund (ERDF).
important role in finding the true requirements concerning H.H. also acknowledges funding by Deutsche Forschungsgemeinschaft
the transparent conductive electrodes. An experimentally (DFG, German Research Foundation) - 431903417.
Open access funding enabled and organized by Projekt DEAL.
derivable target sheet resistance has been defined based on the
transition sheet resistance, which can serve as a guide for the
development goals of certain material systems for electrodes.
Finally, we have assessed more than 30 different novel Conflict of Interest
approaches for replacing the present state-of-the-art transparent The authors declare no conflict of interest.
electrodes based on ITO and FTO. An encouraging number of
12 already reported TCE approaches got very close to the tech-
nical standard, whereas even six candidates surpassed the exact
FOM for ITO and FTO. With the introduction of the novel Data Availability Statement
FOMs, we hope to make a contribution for guiding researchers’ The data that support the findings of this study are available from the
commitment to developing competitive approaches for high- corresponding author upon reasonable request.
performance TCEs for photovoltaic applications.
Keywords
5. Experimental Section figure of merit, photovoltaic devices, solar cells, transparent conductive
Materials: ITO-coated glasses were purchased from Xinyan electrodes, weighted balance
Technology Limited (China). The glasses were bought from Thermo
Scientific (Germany). PEDOT:PSS formulation (Clevios PH1000) was Received: March 15, 2021
purchased from Heraeus (Germany). Revised: May 11, 2021
Fabrication of PEDOT:PSS Films: Glass substrates were cleaned using Published online: June 1, 2021
toluene and isopropanol baths under ultrasonication for 15 min each. 5%
v/v DMSO was added to PEDOT:PSS formulation and was centrifuged
for 1 h before coating. The PEDOT:PSS films were spin-coated on top of
the glass at 1000 rpm for 60 s using a Berrytec PES 0.45 µm filter. The [1] W. Cao, J. Li, H. Chen, J. Xue, J. Photonics Energy 2014, 4, 040990.
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