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content increased from 0.04 to 0.12, the conductivity of the thin films increases considerably
from 3.1×10-3 to 67.7×10-3 S/cm. Beyond this, the conductivity somewhat decreases as the
concentration of Mg increases. Hall measurements revealed changes in hole concentration and
carrier mobility with varying Mg-content. Furthermore, the doped thin films exhibited high
optical transmittance in the visible spectrum.
Lately, Keerthi et al. (2020) achieved excellent hole conductivity in AgInGaO2 thin film | [
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] |
Lately, Keerthi et al. (2020) achieved excellent hole conductivity in AgInGaO2 thin film
[80]. They have deposited AgGaO2 and AgInGaO2 thin films evaporation technique followed by
post-thermal annealing. The highest conductive value of 61 S/cm in Ag-deficient AgInGaO2
thin-film, whereas optical transparency was only 25% despite having a wide optical band gap of
3.77 eV. Hall measurements results confirmed the p-type nature of as-deposited thin films, and at | [
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] |
3.77 eV. Hall measurements results confirmed the p-type nature of as-deposited thin films, and at
maximum conductivity value, Hall mobility and carrier concentration were 0.017 cm2/V-s and
2.2×1024 cm-3, respectively.
1.4.3 Spinel-based oxides as p-type TCOs
The spinel structure has a general formula of AB2O4, where A is divalent cation occupies the
tetrahedral site, and B is trivalent cation occupies the octahedral site. Windisch et al. (2001) | [
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] |
tetrahedral site, and B is trivalent cation occupies the octahedral site. Windisch et al. (2001)
deposited the first spinel oxide-based p-type TCO thin film by spin coating technique in the form
of NiCo2O4 [81]. Pristine NiCo2O4 illustrated excellent transmittance in the visible range and
found to be decreased when the ratio (x) of Co/(Co + Ni) was increased. In this material, the
trivalent cation (Co3+) substitution by divalent ion (Ni2+) increased the hole conductivity, as | [
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] |
trivalent cation (Co3+) substitution by divalent ion (Ni2+) increased the hole conductivity, as
shown in table 3. Minimum value of resistivity (~0.06 Ω-cm) was obtained at x = 0.67. Below
this ratio, there is a formation of NiO, which increased the resistivity. Above that ratio, the
compound was spinel only and increased Co-content also enlarged the resistivity value.
However, several cations such as Al, Cu, and Zn were also introduced in the starting precursor | [
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] |
However, several cations such as Al, Cu, and Zn were also introduced in the starting precursor
solution. But obtained results were not upto the mark, and oxide films demonstrated a low
conductivity value compared to pristine NiCo2O4 film.
Zinc-based spinel oxides have also been explored by different researchers in the form of
ZnM2O4 (where M is transition-metal ions such as Co, Rh, and Ir). As these ions exhibit | [
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] |
ZnM2O4 (where M is transition-metal ions such as Co, Rh, and Ir). As these ions exhibit
octahedral symmetry and acquire nd6 electronic configuration, behave as "quasi-closed shell"
configuration in a low-spin state. Mizoguchi et al. (2002) reported p-type conductivity in
ZnRh2O4 thin film deposited using RFMS technique [82]. The thin film's conductivity was found
to be 0.7 S/cm at room temperature with an optical band gap of 2.1 eV. Narushima et al. (2003) | [
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] |
to be 0.7 S/cm at room temperature with an optical band gap of 2.1 eV. Narushima et al. (2003)
also deposited a thin film of ZnRh2O4 on a glass substrate by a similar technique, but it was
amorphous. The optical band gap value was observed to be the same. But conductivity was
increased to 2 S/cm at room temperature [83]. They have also fabricated a p-n junction in the
form of Au/ZnRh2O4/InGaZnO4/ITO. I-V characteristics demonstrated the rectifying behavior | [
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] |
form of Au/ZnRh2O4/InGaZnO4/ITO. I-V characteristics demonstrated the rectifying behavior
with an on/off current ratio of 103 and threshold voltage was 2.1 V. In addition, Ohta et al.
(2003) also fabricated a p-n junction in view of Au/ZnRh2O4/ZnO/ITO but in an epitaxial single-
crystalline form [84]. The same rectifying behavior was observed with a threshold voltage of 2
eV. Conduction in amorphous ZnRh2O4 thin film was explained by Kamiya et al. (2005) [85]. | [
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] |
eV. Conduction in amorphous ZnRh2O4 thin film was explained by Kamiya et al. (2005) [85].
They investigated that conduction in amorphous ZnRh2O4 type material emerges from the
isotropic nature of spinel oxide’s structure and networks of edge-sharing RhO6 octahedra. And
these are hardly effective by structural distortion and remain stable even in an amorphous state.
After this, H J Kim et al. (2004) deposited ZnCo2O4 thin film by reactive magnetron | [
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] |
After this, H J Kim et al. (2004) deposited ZnCo2O4 thin film by reactive magnetron
sputtering technique [86]. The optical band gap of the as-deposited thin film was 2.63 eV.
Talking about the electrical properties, it was found to be entirely dependent on oxygen partial
pressure. At low oxygen partial pressure, ZnCo2O4 thin film was n-type in nature with a carrier
concentration of 1.37×1020 cm-3. But, as the O2 partial pressure raised, conduction changed to p- | [
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concentration of 1.37×1020 cm-3. But, as the O2 partial pressure raised, conduction changed to p-
type with a carrier concentration of 2.81×1020 cm-3 with Hall mobility of 0.2 cm2/V-s, as shown
in figure 7. Excess oxygen can result in diminishing O-vacancies and electron concentration. The
activation energy was found to be 41 meV for p-type ZnCo2O4 thin film.
In 2007, Dekkers et al. deposited thin films of ZnRh2O4, ZnCo2O4, and ZnIr2O4 by PLD | [
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] |
In 2007, Dekkers et al. deposited thin films of ZnRh2O4, ZnCo2O4, and ZnIr2O4 by PLD
technique [57]. Among these three materials, ZnIr2O4 illustrated a wide optical band gap of 2.97
eV. However, the optical band gap of 2.74 eV was observed for ZnRh2O4, which was higher than
the earlier reported value [82]. All thin films were p-type in nature, as determined by the Seebeck
coefficient. The observed conductivities values for ZnRh2O4, ZnCo2O4, and ZnIr2O4 were | [
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coefficient. The observed conductivities values for ZnRh2O4, ZnCo2O4, and ZnIr2O4 were
0.39/0.61, 2.75/2.83, and 3.39/2.09 S/cm, respectively (Previous conductivity value is for
polycrystalline and later for the epitaxial thin film). After that, S Kim et al. (2010) deposited
ZnCo2O4 thin film on the sapphire substrate by PLD technique [87]. They observed a high
conductivity value of 21.8 S/cm (at room temperature) by optimizing oxygen pressure, which | [
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conductivity value of 21.8 S/cm (at room temperature) by optimizing oxygen pressure, which
was higher than previously reported values [57]. The carrier concentration and Hall mobility
values were found to vary with oxygen pressure. The optical band gap was found to be 2.3 eV.
They have also deposited a p-n junction, but no satisfying results were found.
Using an inverse design approach, researchers identified Cr2MnO4 as a promising | [
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] |
Using an inverse design approach, researchers identified Cr2MnO4 as a promising
candidate for a new p-type transparent conducting oxide [88]. Using lithium as dopant, they
significantly enhanced its p-type electrical conductivity at room temperature. High-temperature
measurements confirmed its behavior as a band conductor, indicating potential improvements in
its electrical properties with methods like single crystal growth or thin film deposition. However, | [
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] |
the introduction of lithium reduced its optical transparency due to the formation of certain
species and increased hole content within the material.
Hong-Ying Chen and Po-Chun Chen (2020) utilized the sol-gel process to fabricate thin
films of p-type spinel ZnCo2O4 [89]. The films were produced through annealing at temperatures
between 300 and 400°C in an oxygen atmosphere. The wide optical band gap of 3.95–3.99 eV | [
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] |
between 300 and 400°C in an oxygen atmosphere. The wide optical band gap of 3.95–3.99 eV
was determined for the thin films. The films demonstrated resistivity of the order of 102-103 Ω-
cm. In the recent study, Z. Chi et al. (2021) successfully deposited both p-type ZnGa2O4 thin
films by precisely controlling deposition parameters. The deposited p-type thin film was found to
be highly resistive. But the hole conductivity in p-ZnGa2O4 was found to be enabled by ZnGa | [
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be highly resistive. But the hole conductivity in p-ZnGa2O4 was found to be enabled by ZnGa
anti-site defects. This study provides valuable insights into the conductivity mechanisms of
ZnGa2O4, contributing to a deeper understanding of its electrical properties [90].
Various theoretical studies were also conducted on the electronic structure of spinel-
based oxide materials [91–93]. But theoretical calculations were not well-consistent with | [
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] |
based oxide materials [91–93]. But theoretical calculations were not well-consistent with
experimental results, whether in terms of optical band variation or its magnitude. As discussed
above, Dekkers et al. (2007) found that the optical band gap increased with a quantum number
[57]. But different trends were observed in theoretical evaluation. In the case of spinel oxides,
their p-type conductivity can be enhanced by creating acceptors like anti-site disorder and | [
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their p-type conductivity can be enhanced by creating acceptors like anti-site disorder and
divalent cation vacancy. But theoretical studies explained that there was no noteworthy
dispersion of VBM observed in spinel oxides, which lead to a large effective mass of holes and
limiting hole conductivity. However, p-type conductivity was improved by oxygen intercalation.
But this is significant upto some extent only, subsequently, it started diminishing. Hence, spinel- | [
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based oxide materials do not show great potential as p-type TCOs.
1.4.4 Binary metal oxides as p-type TCOs
As discussed early in the introduction part, the first p-type TCO was NiO with a transparency
and electrical conductivity of 40% and 7.1 S/cm (at room temperature), respectively. Table 4
illustrates the optical and electrical results of various binary oxide materials as p-type TCO.
However, the optical band energy of single-crystal NiO was reported between 3.6 to 4 eV [5]. In | [
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] |
However, the optical band energy of single-crystal NiO was reported between 3.6 to 4 eV [5]. In
NiO material, both factors, such as Ni vacancies and oxygen interstitial, are responsible for its p-
type conductivity, as described by Antolini in 1992 [94]. Its valence band is comprised of
hybridized Ni 3d orbital and O 2p orbital. Therefore, conduction is expected in NiO material.
However, Li was also tried as a dopant to enhance the conductivity of NiO [95]. As substitution | [
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] |
However, Li was also tried as a dopant to enhance the conductivity of NiO [95]. As substitution
of Li+ into Ni2+ introduced a hole into the system, no satisfactory results were found. In 2014,
Chen et al. deposited a thin film of NiO on the glass substrate [96]. They studied the effect of
oxygen ion beam current on NiO thin films' optical and electrical properties. Stoichiometric NiO
thin films were highly resistive of the order of 1013 Ω-cm (at 50% O-content). Reduction in | [
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] |
thin films were highly resistive of the order of 1013 Ω-cm (at 50% O-content). Reduction in
resistivity was observed when excess oxygen was introduced during the growth process. The
lowest resistivity value of 0.11 Ω-cm was determined at a discharge current of 0.42 A.
Alongwith that, carrier concentration was also raised with oxygen ion beam discharge current,
but Hall mobility decreased from 28.56 to 6.12 cm2/V-s when the discharge current increased | [
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] |
but Hall mobility decreased from 28.56 to 6.12 cm2/V-s when the discharge current increased
from 0.22 to 0.42 A. Considering the optical properties, NiO thin film exhibited average
transparency of 69% in the visible range. But as the discharge current raised, transmittance was
diminished to 22%.
In addition, Yang et al. (2012) also tried to enhance the hole conductivity in NiO through
K-doping [97]. The highest conductivity of 4.25 S/cm was achieved at 25 at% of K-doping and | [
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] |
K-doping [97]. The highest conductivity of 4.25 S/cm was achieved at 25 at% of K-doping and
noteworthy average optical transmission of 60% in the visible region. Hall measurements
confirmed the p-type nature of as-deposited thin films. Another dopant Cu has also been
introduced into p-type NiO thin films by Chen et al. in 2013 [98]. Cu-dopant was added at 10
and 18 at% into NiO thin films. The optical band gap energy was reduced with Cu-doping. The | [
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] |
and 18 at% into NiO thin films. The optical band gap energy was reduced with Cu-doping. The
lowest value of resistivity was observed at 18 at.% of Cu-doping, i.e., 0.07 Ω-cm (see figure 8).
Despite having low conductivity and transparency, NiO is mostly used as a p-type TCO
for transparent p-n junction and TFTs. One benefit of NiO is its simple rocksalt structure that
may be found more compatible with other n-type TCOs. Ohta et al. (2003) deposited | [
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] |
may be found more compatible with other n-type TCOs. Ohta et al. (2003) deposited
NiO/ZnO/ITO on (111) YSZ substrate by using the PLD technique [99]. The p-n diode
illustrated the rectifying characteristics with a threshold voltage of 1 V and an ideality factor of
2. In 2009, Gupta et al. also fabricated the same p-n junction in the form of Au/ZnO/NiO/Au on
via PLD technique [100]. They also showed rectifying behavior under the I-V characteristics | [
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] |
via PLD technique [100]. They also showed rectifying behavior under the I-V characteristics
curve with a barrier height of 0.33 eV and ideality factor of 4. The p-type NiO also finds
applications in resistive-switching memory, electrochromic windows, and hole transport layer in
thin-film solar cells [3,101]. Recently, begum et al. (2024) also tried to enhance the
optoelectronic properties of NiO by doping with Zn and Mn, but no satisfactory results were | [
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] |
optoelectronic properties of NiO by doping with Zn and Mn, but no satisfactory results were
obtained [102]. However, optical transmittance of NiO film was good as compared to previous
results.
Moving ahead from NiO, some serious efforts have been made to develop ZnO as a p-
type TCO. ZnO is n-type in nature and exhibits excellent optoelectronic properties. Hence,
fabrication of transparent p-n homojunction can lead to a spectacular achievement in the field of | [
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fabrication of transparent p-n homojunction can lead to a spectacular achievement in the field of
“invisible electronics”. Doping elements such as B, F, Al, Ga, and In incorporated into ZnO
lattice lead to n-type conductivity, and they are widely used in optoelectronic applications
[16,103]. Lander performed the very first try in 1960 [104]. He doped Li into ZnO and studied its
reactions as donor and acceptor. The main conclusion drawn from this report was that too high | [
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reactions as donor and acceptor. The main conclusion drawn from this report was that too high
oxygen pressure is needed to develop p-type conductance in ZnO, which is impractical.
Yuichi Sato and Susumu Sato made another considerable effort in 1996 by mixing
oxygen and nitrogen gas during ZnO thin film deposition on a sapphire substrate using reactive
evaporation technique [105]. Films deposited under the O2 environment were highly c-axis | [
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evaporation technique [105]. Films deposited under the O2 environment were highly c-axis
oriented and exhibited greater transparency in the visible region. Whereas the film deposited in
the N2 environment was amorphous in nature and reddish-brown in color with very poor
transmittance. After that, mixing of both gases were done at a ratio of N2/(N2 + O2) 25, 50, and
75% at two different deposition temperatures of 300 and 400 ⁰C. But no noticeable change in | [
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75% at two different deposition temperatures of 300 and 400 ⁰C. But no noticeable change in
transmittance spectra has been observed. Hall mobility was increased, but all thin films were n-
type in nature.
Following the above concept, Minegishi et al. demonstrated the realization of p-type ZnO
film on c-cut sapphire substrate by using a chemical vapor deposition technique in 1997 [106].
They illustrated the simultaneous incorporation of ammonia (NH3) in carrier hydrogen and the | [
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They illustrated the simultaneous incorporation of ammonia (NH3) in carrier hydrogen and the
surplus of Zn in ZnO powder. However, the resistivity was found in the order of ~100 Ω-cm.
They suggested a model that introducing nitrogen into ZnO can lead to p-type with reasonable
conductivity by optimizing temperature for thermal annealing. Similar electrical properties of
undoped ZnO were observed with N-doing without excess of Zn. Also, they did not detect the | [
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] |
undoped ZnO were observed with N-doing without excess of Zn. Also, they did not detect the
presence of nitrogen in ZnO thin film at Zn/ZnO ratio of 0 mol%, indicating that incorporating N
into ZnO lattice is not easy. However, at Zn/ZnO ratio of 10 mol%, the existence of N was
confirmed. Hence, excess Zn was required to add nitrogen, as Zn likely to be combined with
oxygen rather than nitrogen. sThe carrier density was found to be decreased and conduction | [
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] |
oxygen rather than nitrogen. sThe carrier density was found to be decreased and conduction
transformed into p-type. This indicated the successful substitution of oxygen (O) by nitrogen (N)
and results in the formation of acceptor level, estimated at nearly 0.1 eV above the top of the
valence band. The activation of acceptor depends upon the substrate temperature region as low-
temperature results in electrically inactive acceptor and intermediate temperature lead to | [
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] |
temperature results in electrically inactive acceptor and intermediate temperature lead to
activation of acceptor and reduced carrier density, which in turn, convert conduction into p-type.
But high temperature broke the N-H bond of ZnNH before the addition of nitrogen into ZnO
film. The control of temperature in that narrow range (where conduction nature is inversed) is
complicated. That's why the resistivity of N-doped ZnO films was found to vary with substrate | [
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complicated. That's why the resistivity of N-doped ZnO films was found to vary with substrate
temperature. High resistive samples were obtained between 650 to 750 ⁰C. Such high resistivity
value is not significant for optoelectronic applications.
Guo et al. (2000) also introduced nitrogen into ZnO thin film deposited using the PLD
technique [107]. During the deposition, pure Zn metal was ablated under N2O plasma | [
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] |
technique [107]. During the deposition, pure Zn metal was ablated under N2O plasma
environment. They were successful in achieving the p-type conduction in ZnO thin films by
optimizing N2O partial pressure and micro-wave input power. A significant value of resistivity
was achieved. The conduction nature of p-type ZnO was confirmed by the Seebeck coefficient.
Optical transparency achieved in p-type ZnO was very similar to n-type ZnO. | [
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] |
Optical transparency achieved in p-type ZnO was very similar to n-type ZnO.
Another homoepitaxial N-doped ZnO thin film was deposited by Look et al. (2002) using
the molecular beam epitaxy [108]. Both O2 and N2 gases were introduced (with varying ratios) in
r.f. plasma source. A thin film of N-doped ZnO was deposited on Li-doped, semi-insulating ZnO
substrate to prevent the influence of conduction from the substrate. The resistivity value of 40 Ω- | [
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] |
substrate to prevent the influence of conduction from the substrate. The resistivity value of 40 Ω-
cm along with carrier concentration and Hall mobility of 9×1016 cm-3 and 2 cm2/V-s was
obtained, respectively. No optical properties of as-deposited thin films were studied in this
report.
Ammonia doped ZnO effort was also made by Wang et al. (2003). They deposited thin
films of NH3-doped ZnO by metalorganic chemical vapor deposition on
0224
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] |
films of NH3-doped ZnO by metalorganic chemical vapor deposition on
0224
oriented
sapphire substrate [109]. They also demonstrated hole conductivity in ZnO thin film with a
resistivity of 102 Ω-cm and carrier concentration and Hall mobility of 1.69×1016 cm-3 3.6 cm2/V-
s, respectively. The mechanism behind ZnO film's conductivity is that the concentration of N-
acceptor was more than self-compensated native donors such as Zn-interstitials and O-vacancies. | [
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] |
acceptor was more than self-compensated native donors such as Zn-interstitials and O-vacancies.
But after a certain extent, conduction nature again reverted to n-type with increasing NH3 flux.
Because hydrogen content was also rising with NH3 flux, and hydrogen atom can also act as a
donor. No comments on the optical properties of NH3-doped ZnO films were highlighted in this
report.
Moving ahead of N-doping, Ryu et al. (2000) tried arsenic (As) as a dopant to introduced | [
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] |
report.
Moving ahead of N-doping, Ryu et al. (2000) tried arsenic (As) as a dopant to introduced
hole conductivity in ZnO [110]. Thin films of As-doped ZnO were grown on (001) GaAs
substrates under O2 environment by PLD technique. Dopant arsenic (As) act as a better
acceptor, and its binding energy was found to be near about 100 meV. Post-annealing of thin
films demonstrated the conversion of p-type conductivity from n-type due to diffusion of As- | [
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] |
films demonstrated the conversion of p-type conductivity from n-type due to diffusion of As-
atom from the substrate to ZnO thin film. The p-type ZnO films exhibited carrier density around
1018-1021 cm-3, and Hall mobility was in the range of 0.1-50 cm2/V-s. However, these values
have significant uncertainties, as the contribution was not well-understood from interface layer
between GaAs substrate and ZnO thin film. They have also not reordered optical properties of | [
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between GaAs substrate and ZnO thin film. They have also not reordered optical properties of
as-deposited and post-annealed thin films.
The concept of co-doping was also tried to develop ZnO as a p-type TCO. Yamamoto
and Yoshida (1999) performed a first-principle study on Ga and N doped ZnO, in which Ga was
assumed to act as donor and N as acceptor [111]. However, the concentration of N was twice that
of Ga to achieve p-type conductivity in ZnO. The idea behind this approach was to decrease the | [
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of Ga to achieve p-type conductivity in ZnO. The idea behind this approach was to decrease the
repulsive N-N interaction, which in turn, creates a shallow acceptor level. Various reports were
published by researchers following the above approach and claimed the lack of reproducibility of
p-type ZnO using the co-doping technique [112–114]. The conclusion drawn from the above
reports is that production of p-type ZnO is not a trivial task. Even hole conductivity obtained | [
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reports is that production of p-type ZnO is not a trivial task. Even hole conductivity obtained
from the above reports was not outstanding from the application point of view. Furthermore, the
main concern about its reproducibility may be due to lack of using proper growth conditions, or
there may be a formation of unwanted impurity in ZnO matrix.
After this, a new p-type TCO material came into the picture in the form of SnO due to its | [
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] |
After this, a new p-type TCO material came into the picture in the form of SnO due to its
abundancy, non-toxic nature, and comparatively high hole mobility. Various theoretical studies
on the band structure of this material were investigated [115–117]. They revealed greater hole
mobility in SnO material, due to its valence band structure and low-defect formation energy of
Sn vacancies (VSn). The valence band of SnO mainly consists of hybridization of Sn 5s and O 2p | [
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-0.03726014122366905
] |
Sn vacancies (VSn). The valence band of SnO mainly consists of hybridization of Sn 5s and O 2p
orbitals, which lead to the large dispersion of VBM and Sn vacancies act as acceptors. All these
intrinsic properties motivated other researchers to explore its optoelectronic properties by
depositing a thin film of SnO. However, before investigating the p-type SnO, most of the
research activities were attentive to SnO2 material, which is n-type in nature and acquires | [
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] |
research activities were attentive to SnO2 material, which is n-type in nature and acquires
applications like active electronics, transparent passive, and gas sensing [118–120]. For the very
first time, Ogo et al. (2008) deposited epitaxial thin films of SnO and also fabricated a better top-
gated p-type TFTs based on SnO [121]. The as-deposited thin film illustrated an optical band of
2.7 eV. They achieved Hall mobility of 2.4 cm2/V-s at room temperature. Epitaxial SnO channels | [
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2.7 eV. They achieved Hall mobility of 2.4 cm2/V-s at room temperature. Epitaxial SnO channels
in TFTs demonstrated a reasonable performance with on/off current ratio of 102, a threshold
voltage of 4.8 V, and field-effect mobility of 1.3 cm2/V-s.
Liang et al. (2010) also deposited a thin film of SnO on quartz and silica substrate
followed by rapid-thermal annealing via e-beam evaporation technique [122]. They have also | [
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followed by rapid-thermal annealing via e-beam evaporation technique [122]. They have also
fabricated a p-type TFT using SnO as a channel. But not satisfactory results were obtained. In the
same year, Fortunato et al. (2010) deposited thin films of SnOx (where x <2) and bottom gated
TFTs using RFMS technique [123]. XRD patterns determined the polycrystalline thin films,
ascribed to β-Sn and α-SnOx phases. Average transparency was around 85% in the visible and IR | [
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] |
ascribed to β-Sn and α-SnOx phases. Average transparency was around 85% in the visible and IR
range. Electrical resistivity varied between the range of 10-100 Ω-cm. SnOx based TFT
demonstrated on/off current ratio of 103 with field-effect mobility of >1 cm2/V-s.
Besides, Kwok et al. (2022) investigated Ga and Na doping to improve conductivity in
SnO thin films [124]. While Ga doping increased conductivity, Na doping achieved significantly | [
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] |
SnO thin films [124]. While Ga doping increased conductivity, Na doping achieved significantly
lower resistivity but with lower transparency (<50%). Both dopants act as effective acceptors.
The study suggested that Na-doped SnO has potential for TCO applications, but further research
is needed to improve transparency.
SnO material can be a suitable candidate for p-type TCO to acquired transparent devices-
based applications. But the main concern is about its stability, as it can be simply oxidized to | [
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based applications. But the main concern is about its stability, as it can be simply oxidized to
SnO2 (n-type) or reduced to metallic Sn. Therefore, it is challenging to grow single-phase SnO
thin film from the device fabrication point-of-view.
Although SnO2 is n-type in nature, efforts were made by various researchers to convert
its conduction into p-type by introducing Al, Ga, and In cations at the Sn-lattice sites, as shown | [
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] |
its conduction into p-type by introducing Al, Ga, and In cations at the Sn-lattice sites, as shown
in figure 9 [62]. Varley et al. (2009) performed the first-principle study and revealed that SnO2
material has low formation enthalpy, i.e., -5.42 eV (lower than ZnO). Besides, SnO2 also has
smaller ionization potential as compared to ZnO [125]. After that, Singh et al. (2008) concluded
that SnO2 material acquires significant chances to act as p-type TCO to render optoelectronic | [
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] |
that SnO2 material acquires significant chances to act as p-type TCO to render optoelectronic
applications [126]. However, before these theoretical studies, Ji et al. in 2003 already reported
the p-type conductivity in In-doped SnO2 thin films deposited on quartz substrate using dip-
coating technique [127]. All thin films were found to be n-type below 450 ⁰C processing
temperature, and above this, conduction changed to p-type. The lowest value of resistivity (i.e., | [
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] |
temperature, and above this, conduction changed to p-type. The lowest value of resistivity (i.e.,
20.4 Ω-cm) was determined at 525 ⁰C processing temperature with carrier concentration and Hall
mobility of 1.85×1018 cm-3 and 1.57 cm2/V-s, respectively. All thin films demonstrated the large
optical band gap of 3.8 eV. Besides that, Lekshmy and Joy (2014) also shown optoelectronic
properties of In-doped SnO2 thin films by the same technique on same substrate as that of Ji et al. | [
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] |
(2003) [128]. Upto 3 mol% In-doping into SnO2, films exhibited n-type conductivity, whereas
above 5 mol%, p-type conducting behavior was observed. Average transparency of more than
80% was reflected in UV-Vis spectra.
Huang et al. (2007) also reported the p-type conductivity in SnO2 thin films with Ga-
doping [129]. Considering the optical properties, thin film was highly transparent in the visible
region with an average transmittance of >85%. On the other hand, the nature of conduction | [
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] |
region with an average transmittance of >85%. On the other hand, the nature of conduction
depended upon the oxidation temperature; too low or high temperature was not favorable for
hole conductivity. They have achieved the p-type conductivity in the optimized temperature
range of 600-650 ⁰C.
The rare-earth element (Eu) was also doped into SnO2 thin film [130]. Undoped SnO2
thin film was n-type in nature, but the inversion of conduction was observed with Eu-doping. | [
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] |
thin film was n-type in nature, but the inversion of conduction was observed with Eu-doping.
The minimum value of resistivity (15.9 Ω-cm) was observed at 0.2 mM of Eu-doping. Carrier
concentration was increased as Eu3+ cations at Sr4+ lattice sites act as acceptors in SnO2 thin
films. Simultaneously, a drastic reduction in Hall mobility was demonstrated from 57.2 to 2.71
cm2/V-s due to the degradation of crystallinity and charge carrier's scattering, as depicted in | [
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] |
cm2/V-s due to the degradation of crystallinity and charge carrier's scattering, as depicted in
figure 10. Talking about the optical properties, increment in the transparency was illustrated with
Eu-doping, due to the Moss-Burstein shift. They have also prepared a bottom-gated TFT by
using Eu-doped SnO2 thin film as a p-type channel. The I-V characteristics curve demonstrated
an ohmic behavior due to the low resistivity of thin film. | [
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] |
an ohmic behavior due to the low resistivity of thin film.
Apart from the above dopants, Al-dopant has also been tried to achieve better p-type
conductivity in SnO2 material. Mohagheghi and Saremi (2004), Ahmed et al. (2006), and
Ravichandran and Thirumurugan (2014) demonstrated p-type conductivity in Al-doped SnO2
thin films deposited on glass substrates [131–133]. Mohagheghi and Saremi (2004) and
Ravichandran and Thirumurugan (2014) used the spray pyrolysis technique, whereas Ahmed et | [
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] |
Ravichandran and Thirumurugan (2014) used the spray pyrolysis technique, whereas Ahmed et
al. (2006) used the dip-coating technique for the growth of Al-doped SnO2 thin films. They have
observed that undoped and Al-doped SnO2 thin films (at low Al-content) exhibited n-type
conductivity. After a particular doping-content of Al, conduction was changed to p-type. Among
all three reports, Mohagheghi and Saremi (2004) illustrated the lowest resistivity of 0.036 Ω-cm | [
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] |
all three reports, Mohagheghi and Saremi (2004) illustrated the lowest resistivity of 0.036 Ω-cm
at 8.4 at% of Al-doping with carrier concentration and Hall mobility of 6.7×1018 cm-3 and 25.9
cm2/V-s, respectively. However, Ravichandran and Thirumurugan (2014) observed the better
carrier concentration (3×1019 cm-3) and Hall mobility (more than 50 cm2/V-s) value, but still, the
resistivity was found to be high (0.38 Ω-cm). It is worth mentioning that Mohagheghi and | [
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] |
resistivity was found to be high (0.38 Ω-cm). It is worth mentioning that Mohagheghi and
Saremi (2004) and Ravichandran and Thirumurugan (2014) showed a decrement in the optical
band gap with Al-doping. But, in Ahmed et al. (2006), optical band gap was increased from 3.87
to 4.21 eV. They have claimed that due to a decrease in particle size and some traces of Al-O
bonding (particularly at grain boundary) observed in FTIR spectra responsible for the widening | [
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] |
bonding (particularly at grain boundary) observed in FTIR spectra responsible for the widening
of optical band gap. The concept of co-doping was introduced into SnO2 material to improve its
optoelectronic properties. Duong et a. (2020) deposited Al and N doped SnO2 thin films DC
magnetron sputtering technique [134]. The optimized content of 6 wt% Al2O3 (with a mixture of
50% N2 and 50% Ar gas) demonstrated the minimum resistivity value of 7.1×10-3 Ω-cm with | [
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50% N2 and 50% Ar gas) demonstrated the minimum resistivity value of 7.1×10-3 Ω-cm with
high Hall mobility and carrier concentration of 14.1 cm2/V-s and 6.24×1019 cm-3, respectively.
Apart from that, good optical transparency ~80% observed in as-deposited thin films.
Another binary oxide material explored as p-type TCO was Cu2O. In 1966, Fortin et al.
demonstrated an excellent value of Hall mobility in Cu2O, i.e., 100 cm2/V-s [135]. Because its | [
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] |
demonstrated an excellent value of Hall mobility in Cu2O, i.e., 100 cm2/V-s [135]. Because its
VBM mainly consists of Cu 3d and O 2p orbital, which lead to the delocalization of holes and
low holes' effective mass. Furthermore, Cu cations have tetrahedral coordination with O-ligands,
which in turn, decreases the nonbonding nature of O2- anions and promotes further
delocalization. Low formation energy of Cu-vacancies is responsible for its p-type nature [136– | [
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] |
delocalization. Low formation energy of Cu-vacancies is responsible for its p-type nature [136–
139]. Matsuzaki et al. (2008) reported the growth of p-type Cu2O thin films as TFTs [140]. The
films were grown by PLD technique and reflected high Hall mobility of 90 cm2/V-s at room
temperature. But results obtained from TFTs were not reasonable with low on/off current ratio
and field-effect mobility. Li et al. (2009) also prepared thin films of Cu2O by using RFMS | [
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] |
and field-effect mobility. Li et al. (2009) also prepared thin films of Cu2O by using RFMS
technique [141]. They have investigated the effect of low-temperature buffer (LTB) layer of
Cu2O on the deposition of Cu2O thin films and observed increment in grain size. They have
achieved Hall mobility of 256 cm2/V-s by optimizing the flow rate of oxygen during deposition
(illustrated in figure 11), which is the highest reported value to date. No concern about optical | [
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] |
(illustrated in figure 11), which is the highest reported value to date. No concern about optical
properties was highlighted in this report.
Various deposition techniques have been employed to study the electrical properties of
Cu2O. There is only material (i.e., Cu2O) whose Hall mobility varied from 0.05 to 256 cm2/V-s.
Different deposition techniques, substrates, and growth parameters are responsible for this | [
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] |
Different deposition techniques, substrates, and growth parameters are responsible for this
massive fluctuation [58,141,142]. But very few reports on its optical properties are available in
the literature. This drawback is the primary concern. Regardless of having an excellent mobility
value, this material cannot be found suitable for "invisible electronics" due to its low optical
band gap of 2.4 eV. This small optical band gap of Cu2O is due to the direct interaction of | [
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] |
band gap of 2.4 eV. This small optical band gap of Cu2O is due to the direct interaction of
neighboring Cu 3d10 electrons. As discussed in CuAlO2, the presence of Al3+ ions reduced the
Cu+-Cu+ interaction along c-axis, which is responsible for its large band gap. But this is not the
case with Cu2O, and not so much effort has been made to enlarge the band gap of Cu2O.
1.4.6 Chalcogen material as p-type TCOs
Chalcogenides such as S and Se were employed in layered structure of (RO)CuCh (where R is | [
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] |
Chalcogenides such as S and Se were employed in layered structure of (RO)CuCh (where R is
rare-earth elements and Ch is chalcogenides) thin films to develop p-type TCOs. The CMVB
technique employed for developing effective p-type TCOs also extended to these kinds of
materials. As the energy-filled level of S 3p and Se 4p lying below than O 2p level, responsible
for the widening of optical band gap. Furthermore, due to the presence of rare-earth element | [
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] |
for the widening of optical band gap. Furthermore, due to the presence of rare-earth element
(La), which is highly electropositive, there will be a high energy shifting of conduction band
minimum (CBM). The number of Cu-S bonds in unit cells also decreases, thereby promoting
dispersion at the top of the valence band maximum (VBM) and improving mobility, clearly
depicted in table 5. Therefore, this type of material showed great potential in the field of
“transparent electronics”. | [
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] |
“transparent electronics”.
This type of material was firstly developed by Palazzi in 1981, and its hole conductivity
was reported after a decade by Ishikawa et al. (1991) and Takano et al. (1995) [143–145]. Ueda
and co-workers were the first ones who prepared a thin of thin LaCuOS [53]. Thin films
deposited was highly transparent in the visible region (>70%). They have also doped Sr into
LaCuOS and conductivity was found to be increased from 1.2×10-2 to 0.26 S/cm. Similar Sr- | [
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] |
LaCuOS and conductivity was found to be increased from 1.2×10-2 to 0.26 S/cm. Similar Sr-
doped LaCuOS thin films were grown by Hiramatsu et al. in 2002 [146]. As-deposited thin films
were post-annealed in an evacuated silica tube comprising a small quantity of LaCuOS powder.
The electrical conductivity of films was increased from 6.4×10-5 S/cm (undoped) to 20 S/cm (3%
Sr doped). Optical transmittance of > 60% was reflected in the visible and NIR region. | [
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] |
Sr doped). Optical transmittance of > 60% was reflected in the visible and NIR region.
The same group made another effort in 2003 by substituting Se at the S anionic site in
LaCuOS thin film [54]. Hall mobility was found to be increased with Se doping and reached a
maximum value of 8 cm2/V-s. Epitaxial LaCuOSe thin film exhibited the maximum conductivity
value of 24 S/cm. As a significant change in carrier density was observed, improved mobility | [
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value of 24 S/cm. As a significant change in carrier density was observed, improved mobility
was responsible for high conductivity value. For the sake of increasing the conductivity value of
LaCuOSe, various divalent cations were also tried (such as Mg2+, Ca2+, and Sr2+). Mg-cation
came out as an effective dopant and increased the conductivity of epitaxial 20% Mg-doped
LaCuOS thin film to 140 S/cm, due to increased carrier concentration. On the other hand, | [
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] |
LaCuOS thin film to 140 S/cm, due to increased carrier concentration. On the other hand,
mobility was decreased to 4 cm2/V-s. The determination of the optical properties of as-deposited
thin films was missing in this report [56].
In 2020, Zhang et al. substituted rare-earth element (Y) at the rare-earth (La) cationic site
in LaCuOS material [147]. They have doped Y into LaCuOS at various contents. Electrical | [
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] |
in LaCuOS material [147]. They have doped Y into LaCuOS at various contents. Electrical
conductivity was found to have increased from 5.6 S/cm (x = 0) to 89.3 S/cm (x = 0.25), which is
highest till date in case of LaCuOS material. Furthermore, Hall mobility and carrier
concentration were improved with Y-doping. On the other hand, optical transparency was
slightly decreased with Y-doping, i.e., from 81.2% to 76.1%. They have also fabricated diode in | [
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] |
slightly decreased with Y-doping, i.e., from 81.2% to 76.1%. They have also fabricated diode in
the form of Y-doped LaCuOS/Al-doped ZnO and results in very high rectifying having on-to-off
ratio of 300 at ±3V and threshold voltage around 1.1 V alongwith very low leakage current of
5×10.7 A. Apart from that, this p-n junction exhibited greater transparency of more than 65% in
the visible range. Hence, this material can be a potential candidate in next-generation
“transparent electronics”. | [
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] |
“transparent electronics”.
Apart from La, various rare-earth elements such as Y, Pr, Nd, and Gd have also been
explored [148]. But they have studied structural properties and band structure. Their
optoelectronic properties still need to be investigated.
1.4.7 Cr-based oxides as p-type TCOs
Recently, chromium oxide (Cr2O3) received tremendous attention as p-type TCOs. Due to low
formation energy of Cr-vacancies (VCr), Cr2O3 is p-type in nature [149]. The optical band gap | [
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] |
formation energy of Cr-vacancies (VCr), Cr2O3 is p-type in nature [149]. The optical band gap
energy of Cr2O3 is 3.1 eV. Apart from that, two kinks were always observed at 2 and 2.6 eV,
which ascribed to dipole-forbidden d-d transition [150]. However, these transitions are very
weak in thin-film form and barely affect the transparency in the visible region. Stoichiometric
Cr2O3 is insulating in nature, and its conductivity was found to be increased by introducing | [
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] |
Cr2O3 is insulating in nature, and its conductivity was found to be increased by introducing
suitable dopants. In 1996, Uekawa and Kaneko investigated that Li, Mg, and Ni dopants can
increase conductivity [151]. They have illustrated only resistance-temperature study and
observed that resistance decreases with Li, Mg, and Ni doping. The reduction of resistance in Li-
doped samples was marginal. On the other hand, a rise in absorption intensity was demonstrated | [
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] |
doped samples was marginal. On the other hand, a rise in absorption intensity was demonstrated
with Mg-doping, as addition of Mg into Cr2O3 leads to the formation of mix valence state of Cr3+
and Cr6+ ions. And the charge was also transferred from O2- 2p to Cr6+ 3d, known as ligand-to-
metal charge transfer (LMCT), and the color of as-deposited thin films changed from green to
brownish.
Arca et al. (2011) were the first ones who investigated the optoelectronic properties of | [
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] |
Arca et al. (2011) were the first ones who investigated the optoelectronic properties of
Mg-doped Cr2O3 thin films [152]. They have also tried to prevent the formation of Cr mixed-
valence state by introducing co-doping of nitrogen alongwith Mg. The optical transparency of
undoped and Mg-doped Cr2O3 thin films was very ordinary, as shown in table 6. However,
increment in transparency was demonstrated with Mg and N co-doping, and maximum | [
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] |
increment in transparency was demonstrated with Mg and N co-doping, and maximum
transmittance of 65% was observed in the NIR region, as shown in figure 12. On the other hand,
electrical resistivity was drastically reduced from 400 Ω-cm to 15 Ω-cm. They have achieved the
best results with an optimized ratio of Cr:Mg 9:1 and Cr:N 1:4. The lowest resistivity achieved in
this report was 3 Ω-cm. All thin films were p-type in nature. | [
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] |
this report was 3 Ω-cm. All thin films were p-type in nature.
This study was further extended by the same group in 2013. They have investigated the
role of different chemical precursors on the optoelectronic properties of Mg and N-doped Cr2O3
thin films [150]. The smallest value of resistivity 4 Ω-cm was determined using nitrate precursor
at 0 pH value, whereas thin films deposited using chloride and acetate precursor results in high | [
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] |
at 0 pH value, whereas thin films deposited using chloride and acetate precursor results in high
resistive film. The optical band gap was increased with N-doping because introduction of
nitrogen reduced the concentration of Cr6+ ions. They have also explained the mechanism of
conduction in epitaxial Mg-doped Cr2O3 thin films deposited using molecular beam epitaxy
(MBE) technique followed by post-annealing in an oxygen environment [153]. They have | [
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] |
(MBE) technique followed by post-annealing in an oxygen environment [153]. They have
reported that conductivity of as-deposited thin films can be increased with post-thermal treatment
under oxygen flow, illustrated in figure 13. However, conductivity of epitaxial Mg-doped Cr2O3
thin films wouldn’t surpass their previous result.
A similar group in 2017 reported the optical and electrical properties of Ni-doped Cr2O3 | [
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] |
A similar group in 2017 reported the optical and electrical properties of Ni-doped Cr2O3
thin films deposited using the PLD technique [154]. Significant p-type conductivity in Cr2O3 thin
film was achieved by Ni doping (28 S/cm). They have also performed DFT calculations, which
stated that the introduction of Ni promoted the delocalization of VB of Cr2O3, and it is
experimentally proved that Ni has a higher solubility as compared to Mg. Due to these two | [
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] |
experimentally proved that Ni has a higher solubility as compared to Mg. Due to these two
advantages, Ni was found to be more effective dopant in Cr2O3 material. However, optical
transparency was not too high, varying between 35 to 55% in the visible region.
We have also used Cr2O3 as a host material and Mg, Al, and Ni as substituents to enhance
the optoelectronic properties of Cr2O3. We have deposited thin films of Cr2O3, MgxCr2-xO3 (x = | [
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] |
the optoelectronic properties of Cr2O3. We have deposited thin films of Cr2O3, MgxCr2-xO3 (x =
0.1, 0.2, and 0.3), AlxCr2-xO3 (x = 0.1, 0.2, and 0.3) and NixCr2-xO3 (x = 0.03, 0.05, and 0.1)
nanomaterial using PLD technique [155,156]. All thin films were found single crystalline and
epitaxially grown on c-cut sapphire substrates. And crystal structure of Cr2O3 thin films remains
unaffected with Mg, Al, and Ni-substitution. All thin films illustrated the excellent optical | [
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] |
unaffected with Mg, Al, and Ni-substitution. All thin films illustrated the excellent optical
transparency in the visible range, suitable for optoelectronic applications. The incorporation of
Mg and Ni leads to the improvement in the electrical conductivity of Cr2O3 thin film, without
much degrading its optical transparency. On the contrary, Al-substitution into Cr2O3 thin film
further degraded its electrical properties. Comparing the NixCr2-xO3 and MgxCr2-xO3 thin films, | [
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] |
further degraded its electrical properties. Comparing the NixCr2-xO3 and MgxCr2-xO3 thin films,
nickel came out as an effective dopant for improving the electrical conductivity of Cr2O3
material. Because its higher energy-filled 3d orbital can destroy the robust localization around
oxygen 2p states, reduces the effective mass of holes and increases conductivity. It was also
reflected in Hall measurement results, where hole mobility was increased to 2 cm2/V-s from 0.1 | [
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