Superlattices and Microstructures 107 (2017) doi: 10.1016/j.spmi.2017.04.

007

Analysis of the power conversion efficiency of perovskite solar cells with different
materials as Hole-Transport Layer by numerical simulations

G.A. Casas1,2, M.A. Cappelletti1,3,5, A.P. Cédola1,6, Bernabé Marí Soucase4 y E.L. Peltzer y
Blancá1,5
1
Grupo de Estudio de Materiales y Dispositivos Electrónicos (GEMyDE),
Facultad de Ingeniería, Universidad Nacional de La Plata, 48 y 116, CC. 91, La Plata (1900),
Buenos Aires, Argentina, Tel. 0221-4236690
2
Universidad Nacional de Quilmes, Roque Saenz Peña 352,
Bernal (1876), Buenos Aires, Argentina
3
Universidad Nacional Arturo Jauretche, Avenida Calchaquí 6200,
Florencio Varela (1888), Buenos Aires, Argentina
4
Department de Física Aplicada-ETSED, Universitat Politècnica de València, Camí de Vera
s/n, 46022 València, Spain
5
Comisión Nacional de Investigaciones Científicas (CONICET), Argentina
6
Comisión de Investigaciones Científicas, Provincia de Buenos Aires (CIC), Argentina

E-mail: [email protected]

Abstract

In this paper, a theoretical study of different p-p-n perovskite solar cells has been performed by means of
computer simulation. Effects of the offset level upon the power conversion efficiency (PCE) of these
devices have been researched using five different materials such as spiro-OMeTAD, Cu2O, CuSCN, NiO
and CuI, as Hole Transporting Layer (HTL). The Solar Cells Capacitance Simulator (SCAPS)-1D has
been the tool used for numerical simulation of these devices. A strong dependence of PCE has been found
with the difference between the Maximum of the Valence Band of the HTL and perovskite materials, and
with the doping level in p-type perovskite layer. A minimum value of hole mobility in the HTL has been
also found, below which the PCE is reduced. Efficiencies in the order of 28% have been obtained for the
Cu2O/Perovskite/TiO2 solar cell. Results obtained in this work show the potentiality of this promising
technology.

Keywords: Solar energy; Perovskite; Hole Transporting Layer (HTL); Numerical simulation

1. Introduction
In the last few years, the perovskite solar cells have had a significant increase in performance,
which has strongly encouraged many experimental and theoretical studies in order to optimize
the design of the structure and the selection of materials. These works are aimed at improving
the performance of a technology that promises to achieve high power conversion efficiencies
(PCE) at low cost. In particular, the development and progress of the perovskite solar cells,
regarding efficiency, stability, cost and commercialization, have been discussed in detail in
previous publications [1, 2]. Perovskite solar cells represent an emerging photovoltaic
technology, for which efficiencies have been increased substantially from 3.8% in 2009 [3] to
22.1% recently [4], confirming the upward trend of this promising technology.

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Superlattices and Microstructures 107 (2017) doi: 10.1016/j.spmi.2017.04.007

Figure 1 shows the planar structure of perovskite solar cells, where it can be seen that the
light is absorbed by the intermediate region called perovskite layer, whereas the hole-
transporting layer (HTL) and the electron-transporting layer (ETL) link the carrier generation
region with the electrodes. For the purpose of an efficient carrier collection in the electrodes,
the ETL must block the flow of holes but allow the free electrons flow towards the cathode.
On the contrary, the HTL must block the flow of electron but allow the free flow of holes
towards the anode, as shown in Figure 1. The effects of variations in the characteristics of the
perovskite layer and of the interfaces with the other two layers have been investigated
recently through modeling and simulation techniques [5-8]. In another works, a comparative
study using two different transparent conducting oxides such as TiO 2 and ZnO as electron
transporting materials have been recently researched [9, 10]. The ETL, HTL and the
perovskite layers are the path that photogenerated carriers must travel before being collected.
A good understanding of the effects of each of the layers in the performance of the devices is
critical for optimization. The most common material used for the HTL layer is spiro-
OMeTAD (2,2’,7,7’-tetrakis (N,N-di-p-methoxyphenylamine)-9,9’-spirobifluorene), which is
relatively expensive. In this work, a comparative study of the effects of replacing this organic
compound with four different inorganic materials such as Cu2O, CuSCN, NiO and CuI has
been carried out by means of computer simulation. These semiconductor materials have
different band gap energies (Eg) and electron affinities (Ӽe), which lead to different
alignments between the valence bands of both the HTL and the perovskite layer. All
inorganic compounds under consideration in this study are promising candidate for hole
transporting material and electron blocking layer [11, 12]. The authors have previously used
numerical simulations in order to study the behavior of solar cells and PIN photodiodes under
different operating conditions [10, 13-15].

Figure 1. The planar structure of a perovskite solar cell.

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Superlattices and Microstructures 107 (2017) doi: 10.1016/j.spmi.2017.04.007

Figure 2 illustrates typical values of energy in electron volts (eV) of the Minimum of the
Conduction Band (MCB) and of the Maximum of the Valence Band (MVB), with respect to
the vacuum energy level, for the alternative HTL materials spiro-OMeTAD, CuI, NiO,
CuSCN, and Cu2O, for the perovskite CH3NH3PbI3 and for TiO2 used as ETL region. The
subtraction between these two values is Eg, whereas the subtraction between the MCB and the
vacuum energy level gives Ӽe. Also, the offset level is referred as the difference between the
MVB of the HTL and perovskite materials (Offset = MVBHTL - MVBPerovskite).

Figure 2. Values of (eV) of the Minimum of the Conduction Band (on the top) and of the Maximum of the
Valence Band (on the bottom), with respect to the vacuum energy level, for all materials considered in this work.

2. Simulation Details

Numerical simulations of p-p-n perovskite solar cells exploiting the planar structure shown in
Figure 1 were performed with the one-dimensional code SCAPS-1D (Solar Cells Capacitance
Simulator) [16]. This simulation program solves numerically the three basic semiconductor
equations: the Poisson and the continuity equations for holes and for electrons. It has been
applied to the numerical simulation of perovskite solar cells recently [7, 10].

In this work, the heterojunction solar cells are simulated with three input layers, where p-type
spiro-OMeTAD, Cu2O, CuSCN, NiO and CuI are used separately in order to compare their
performance as HTL, low p-type doped perovskite (CH3NH3PbI3) is used as active layer, and
n-type transparent conducting oxide TiO2 is used as ETL. It is considered that solar energy is
entered through the ETL layer. The standard AM1.5G spectrum (1000 W/m2; T =300°K) has
been used.

Table 1 summarizes the physical parameters used for each layer in the numerical analysis,
where NC and NV are the effective density of states (DOS) in the conduction and the valence
bands, respectively; μn and μp are the electron and hole mobilities, respectively; ε is the
relative permittivity; and NA and ND are the acceptor and donor impurity concentrations,

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Superlattices and Microstructures 107 (2017) doi: 10.1016/j.spmi.2017.04.007

respectively. These values were extracted either from literature [6, 7, 10, 17-23] or estimated
as in the case of NC, NV, NA and ND for the inorganic HTL materials. Specifically, NC, NV, NA
and ND for spiro-OMeTAD were extracted from literature [6, 10]. These values are a good
first-approximation for each inorganic material considered in this work. Anyway, to verify the
validity of these parameters, theoretical values of NC and NV for the Cu2O calculated by ab
initio techniques [24] have been used in the simulations and no differences were found.
Additionally, no changes were found in the results when simulations for Cu2O, CuSCN, NiO
and CuI, with NC, NV in the range from 2.50 × 1018 to 2.50 × 1021 and NA in the range from
3.0 × 1016 to 3.0 × 1019 have been performed.

Typical thicknesses of each layer were fixed. In particular, 400 nm thick perovskite film
ensures a radiation absorption close to the maximum, without major recombination losses [6,
10]. Values extracted from literature were used for the absorption coefficients of TiO2 [25],
perovskite and spiro-OMeTAD [26], Cu2O [27], CuSCN [28] and NiO [29]. The absorption
coefficient of CuI is considered constant and equal to 1.00 × 105 cm-1 up to the wavelength
corresponding to the band gap of this material.

Table 1. Physical parameters used in the numerical analysis for each layer.

Cu2O CuSCN NiO CuI spiro-OMeTAD

Eg (eV) 2.17 3.6 3.8 3.1 3.06
Ӽe (eV) 3.2 1.7 1.46 2.1 2.05
-3
NC (cm ) 2.50 × 10 20
2.50 × 10 20
2.50 × 10 20
2.50 × 10 20
2.50 × 1020
NV (cm-3) 2.50 × 1020 2.50 × 1020 2.50 × 1020 2.50 × 1020 2.50 × 1020
HTL μn (cm2V-1s-1) 80 25 2.8 44 2.00 × 10-4
(400 nm) μp (cm2V-1s-1) 80 25 2.8 44 2.00 × 10-4
ε 6.6 5.1 11.7 6.5 3.0
-3
NA (cm ) 3.00 × 10 18
3.00 × 10 18
3.00 × 10 18
3.00 × 10 18
3.00 × 1018
ND (cm-3) 0 0 0 0 0
Offset (eV) 0.06 0.13 0.17 0.23 0.32
Eg (eV) 1.5
Ӽe (eV) 3.93
-3
NC (cm ) 2.50 × 1020
NV (cm-3) 2.50 × 1020
Perovskite
μn (cm2V-1s-1) 50
(400 nm)
2 -1 -1
μp (cm V s ) 50
ε 30
-3
NA (cm ) 2.10 × 1017
ND (cm-3) 0
TiO2 Eg (eV) 3.26

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Superlattices and Microstructures 107 (2017) doi: 10.1016/j.spmi.2017.04.007

(90 nm) Ӽe (eV) 4.2

-3
NC (cm ) 1.00 × 1021
NV (cm-3) 2.00 × 1020
μn (cm2V-1s-1) 1.00 × 10-3
μp (cm2V-1s-1) 1.00 × 10-3
ε 100
-3
NA (cm ) 5.00 × 1018
ND (cm-3) 5.00 × 1019

3. Results and Discussion

The results of PCE calculated by varying the HTL material and keeping fixed the ETL and
perovskite layers are summarized in Table 2. Recombination in the HTL layer has not been
considered, since the simulations show that recombination in this layer does not affect the PCE
values. In the case of spiro-OMeTAD, these results agree very well with experimental values
extracted from [30]. The last column of Table 2 corresponds to the simulated PCE values
assuming that the offset level is zero. This condition is obtained by adjusting the electron
affinity for each material.

Table 2. Performance of the solar cell obtained from simulations for each HTL material described in Table 1.

HTL Offset (eV) PCE (%) PCE (%) to Offset = 0

Cu2O 0.06 25.06 25.10
CuSCN 0.13 24.86 25.11
NiO 0.17 24.57 25.11
CuI 0.23 23.78 25.11
spiro-OMeTAD 0.32 21.79 24.37

Data taken from Table 2 are shown in Figure 3, where it can be seen that the PCE decreases
when the offset level is increased.

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Figure 3. Power conversion efficiency as a function of the offset level between the MVB of the
HTL and perovskite layers for the five HTL material considered in this work.

As it can also be observed in Table 2, the minimum value of PCE for the condition offset equal
to zero, was found for the spiro-OMeTAD (24.37%), whereas no differences were found for
the rest of the materials evaluated. The reduced performance of the spiro-OMeTAD is due to
the low hole mobility in this material (2.00 × 10-4 cm2V-1s-1). Since the mobility of other
materials varies from 2.8 (for NiO) to 80 cm2V-1s-1 (for Cu2O), by almost a factor of 30,
without affecting the PCE value (25.11%), therefore it is possible to assume that there is a
minimum value of mobility above which the change in the PCE is negligible. On the contrary,
the PCE is reduced when the mobility values are lower than this minimum value.

In order to fully understand the degradation in the PCE as a function of the hole mobility, new
simulations were made for the solar cell with spiro-OMeTAD as hole conductor for the
condition offset equal to zero. Specifically, with regard to parameters presented in Table 1, the
μp was varied from 2.00 × 10-4 to 2.00 × 10-1 cm2V-1s-1. The other values of Table 1 have
remained unchanged. Results obtained are shown in Figure 4(a). Also, the variation of the fill
factor (FF) with μp has been studied for the solar cell with spiro-OMeTAD, as can be seen in
Figure 4(b). In both cases, in Figure 4(a) and (b), an increase in PCE and FF is observed when
the hole mobility is increased. In particular, a value of PCE of 25.11% has been obtained by
μp = 2.00 × 10-1 cm2V-1s-1.

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Superlattices and Microstructures 107 (2017) doi: 10.1016/j.spmi.2017.04.007

(a)

(b)

Figure 4. Power conversion efficiency (a) and fill factor (b) versus hole mobility in the spiro-OMeTAD as Hole
Transporting Layer for the condition offset equal to zero.

The FF and PCE can be calculated as [31]:

FF  VMP  I MP  / VOC  I SC  (1)

and

PCE(%)  100 VOC  I SC  FF / PIN  (2)

where VMP, IMP, VOC and ISC represent the voltage at maximum power, the current at maximum
power, the open circuit voltage and the short-circuit current, respectively, whereas PIN is the
input power from the sun. Since VOC and ISC remain unchanged, it can be concluded that FF is
the cause of the increase in PCE when μp is increased.

In order to analyze the behavior of FF, in Figure 5 it is plotted the simulated current density–
voltage (J–V) characteristics of the solar cell with spiro-OMeTAD as HTL material for the
minimum and maximum values of the hole mobility considered. It is possible to observe in this
figure that, for the values of voltage close to VOC, the current is lower when μp is decreased.
The reason for this drop in the carrier collection at the electrodes can be explained by an

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increase of the recombination rate at voltages close to VOC. Therefore, the lower values of FF
(and of PCE) are a consequence of the decrease in the current for the values of voltage close to
VOC.

Figure 5. Current density-Voltage curves of the perovskite solar cell for two different hole
mobilities in the spiro-OMeTAD layer.

It has been previously mentioned in this work that with four different inorganic materials such
as Cu2O, CuSCN, NiO and CuI, if the electron affinity value is modified in order to remain
aligned the MVB of the perovskite and HTL materials (i.e. offset equal to zero), then the
performance is the same in all cases. This indicates that for the doping conditions shown in
Table 1, the band gap energies and the hole mobilities have no impact on the PCE for these
materials.

Since the Cu2O is the material with the lowest real offset (0.06 eV), the results obtained on the
Cu2O/Perovskite/TiO2 solar cell are analyzed in the rest of the work.
Figure 6 shows data obtained from simulation runs of the electrical parameters degradation
(VOC, ISC, FF and PCE) as a function of the offset level for the Cu2O/Perovskite/TiO2 solar cell.
The offset level was artificially modified by changing the electron affinity of Cu 2O. The values
presented are normalized to those corresponding to the offset level equal to zero, which are 1.22
V, 23.64 mA, 86.79 % and 25.10 %, for VOC, ISC, FF and PCE, respectively. The lines through
the data points are only intended to guide the eye. Positive offset values indicate that the MVB
of the HTL layer is over the MVB of the perovskite layer, such as is the case for the materials
considered in this work (Figure 2). Under this condition, according to equation (2), the

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decreasing of VOC is the main reason for the PCE degradation, whereas the fill factor FF is
slightly affected by the offset and ISC is remained approximately unchanged.
This behavior seems to be contradictory, since the positive offset (MVBHTL - MVBPerovskite > 0)
should involve an electric field that contributes to the flow of holes from perovskite to HTL. In
Figure 7 it has been plotted the MVB in the HTL/perovskite interface as a function of the
distance x from the front face of the Cu2O/Perovskite/TiO 2 solar cell, for two different offsets (0
and 0.5 eV). It is assumed that x = 0 is the location of the electrode closest to the HTL, and
therefore x = 400 nm is the location of the HTL/perovskite interface. In the case corresponding
to an offset level equal to 0.5 eV, it can be observed in x = 400 nm a potential barrier which
hinders the motion of holes from perovskite to HTL. Based on the results obtained from
simulations, the height of the potential barrier depends not only on the offset, but also on the
doping level in both regions and on the voltage (0.9 V in Figure 7). Furthermore, the carrier
recombination in the vicinity of HTL/perovskite interface increases when the height of the
potential barrier is greater, which causes lower VOC, FF and PCE. The increase of the carrier
recombination for an offset level equal to 0.5 eV and the comparison with an offset equal to
zero is shown in Figure 8.

Figure 6. Normalized electrical parameters as a function of the offset level between the MVB of
the HTL and perovskite layers for the Cu2O/Perovskite/TiO2 solar cell.

On the other hand, in the case of a negative offset (MVBHTL - MVBPerovskite < 0), the potential
barrier makes difficult the extraction of holes generated in the perovskite layer and the PCE
decreases rapidly due to the reduction of the FF, as can be observed in Figure 6.

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Superlattices and Microstructures 107 (2017) doi: 10.1016/j.spmi.2017.04.007

Figure 7. Maximum of the Valence Band as a function of the distance from front in the
HTL/perovskite interface for the Cu2O/Perovskite/TiO2 solar cell. Two different levels of offset
have been considered.

Figure 8. Carrier recombination as a function of the distance from front in the

HTL/perovskite interface for the Cu2O/Perovskite/TiO2 solar cell.
Two different levels of offset have been considered.

As it has been mentioned above, based on the simulation results, the height of the potential
barrier that causes the increase of the carrier recombination is dependent on the electron
affinities and bandgap, which determine the offset level. For a given offset level, the PCE
value increases when the acceptor concentration in the perovskite layer (NA) is larger. Thus, a
maximum value of PCE in the order of 28% has been obtained at NA = 5.00 × 1020 cm-3, for the

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Superlattices and Microstructures 107 (2017) doi: 10.1016/j.spmi.2017.04.007

offset equal to zero.

Figure 9 shows the simulated electrical parameters (VOC, ISC, FF and PCE) as a function of NA
in the perovskite layer, for the Cu2O/Perovskite/TiO2 solar cell. The values presented are
normalized with respect to the maxima, which are 1.32 V, 23.69 mA, 89.74 % and 28.07 % for
VOC, ISC, FF and PCE, respectively. The PCE and ISC values are the most and least increased
with NA, respectively.

Figure 9. Normalized electrical parameters as a function of the acceptor carrier concentration in

the perovskite layer for the Cu2O/Perovskite/TiO2 solar cell.

On the other hand, in the case of the Cu2O/Perovskite/TiO2 solar cell, the acceptor impurities
concentration in the HTL layer does not significantly affect the value of PCE. However, low
values of hole mobility in the HTL layer (below 3 cm2V-1s-1) reduce the PCE parameter up to
10% when this region is considered intrinsic (NA = 0) or is slightly doped, as can be seen in
Figure 10. From the data presented in Table 1, the hole mobility for spiro-OMeTAD is clearly
below 3 cm2V-1s-1. In opposition, the hole mobilities for Cu2O, CuSCN and CuI are well above
this value, whereas for NiO is close to 3 cm2V-1s-1, for which the degradation of the PCE is
still negligible.

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25.0

24.5

PCE (%)
24.0

23.5
Cu2O
23.0

22.5
0 1 2 3 4 5
2 -1 -1
Hole mobility (cm V s )

Figure 10. Power conversion efficiency as a function of the hole mobility in the HTL layer for the
Cu2O/Perovskite/TiO2 solar cell. The HTL layer is considered intrinsic.

4. Conclusion

The behavior of perovskite based solar cells with p-p-n planar structure has been studied
through computer simulation using an organic compound (spiro OMeTAD) and four different
inorganic materials (Cu2O, CuSCN, NiO and CuI) as Hole Transporting Layer (HTL). The
results obtained in this work show that the performance of these devices can be still
improved with respect to the prototypes reported in the literature, which have efficiencies in
the order of 20% when the HTL layer is the organic spiro OMeTAD. However, so far,
experimental results of efficiency of inorganic hole conductor-based perovskite solar cells is
still much lower than that of the traditional organic hole conductor-based cells. This
can be mainly due to the fact that both, the qualities of the manufacturing processes and HTL
layer, and the amount of defects in the HTL/perovskite interface, have a big influence in the
performance of perovskite devices. Data obtained from simulation runs also show that the most
decisive effect on the PCE is the potential barrier in the HTL/perovskite interface. The
alignment between the Maximum of the Valence Band (MVB) of the HTL and perovskite
materials (which is directly related to the band gap energy and the electron affinity of each
material), is a key factor to reduce the height of the potential barrier. The other major factor
involved is the doping level in p-type perovskite layer. For the maximum value of NA in the
perovskite region considered in this work (5.00 × 1020 cm-3), efficiency in the order of 28% has
been obtained for the Cu2O/Perovskite/TiO2 solar cell for the condition offset equal to zero.
The hole mobilities in the HTL play a fundamental role up to a certain minimum value (close
to 3 cm2V-1s-1), below which the PCE is reduced. The hole mobilities for Cu2O, CuSCN and

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CuI are well above the minimum value, for NiO coincides with this value, whereas for spiro-
OMeTAD is clearly below the minimum value. Since the most common material used
nowadays for the HTL layer is spiro-OMeTAD, results obtained in this work show that this
material can be replaced to improve the efficiency.

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Funding: This work was partially supported by the Universidad Nacional de Quilmes,
Argentina, by the Universidad Nacional Arturo Jauretche, Argentina, by the Universidad
Nacional de La Plata, Argentina, by the National Council Research (CONICET), Argentina, and
by the Ministerio de Economía y Competitividad (Grant ENE2016-77798-C4-2-R), Spain.

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