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intensive research has been conducted to explore other materials as p-type TCOs. Here, we have
examined the fundamental physics of TCOs and performed a comprehensive material-wise
literature survey of p-type transparent conductors, including synthesization methods, deposition
techniques, and their optoelectronic properties.
1.1 Fundamental Material Physics of TCOs
1.1.1 Electrical properties
The simultaneous existence of excellent electrical conductivity alongwith high optical | [
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] |
The simultaneous existence of excellent electrical conductivity alongwith high optical
transparency in stoichiometric oxide materials is not feasible. The electrical conductivity
mechanism in TCO material can be explained based on classical mechanics on charge transport
in metals, i.e., Drude theory. The free charge carriers generated due to doping can be considered
as free-electron gas. Hence, their conductivity is directly related to the density of charge carriers
and their effective mass:
e
e
e
e | [
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] |
and their effective mass:
e
e
e
e
m
n e
n e
2
=
=
(1)
where σ is the electrical conductivity, ne is the number of charge carriers, me is the effective mass
of charge carriers, μe is the mobility of charge carriers, e is the electronic charge, and τ is
relaxation time. The conduction band cannot be thermally populated at room temperature due to | [
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] |
relaxation time. The conduction band cannot be thermally populated at room temperature due to
the wide optical band of TCO materials. Hence, stoichiometric TCO materials are insulating in
nature. In the case of intrinsic TCO materials, availability of conduction electrons or holes is
mainly due to unintentional defects such as cation interstitials or anion vacancies (in case of n-
type) and cation vacancies or anion interstitials (in case of p-type). This type of defects may | [
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] |
type) and cation vacancies or anion interstitials (in case of p-type). This type of defects may
create shallow donor and acceptor levels close to conduction and valence band, respectively (as
shown in figure 1). And these excess generated charge carriers can be thermally ionized at room
temperature and impart conduction within the material. To further enhance its electrical
properties, extrinsic doping can be introduced into TCO materials. | [
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properties, extrinsic doping can be introduced into TCO materials.
Hence, the basic idea in TCO materials is to generate high mobile free charge carriers
(whether it is electrons or holes) into wide optical band gap semiconductors/insulators by using
appropriate dopants. Considering the example of highly effective n-type TCO, i.e., Indium-tin
oxide (ITO), the substitution of Sn4+ cations at the In3+ cationic sites lead to the formation of | [
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] |
oxide (ITO), the substitution of Sn4+ cations at the In3+ cationic sites lead to the formation of
donor-defects below the conduction band minimum (CBM). Apart from that, doping of Sn into
In2O3 material also leads to the dispersion of conduction band, which can reduce the effective
mass of charge carriers and impart conductivity to the material. Therefore, Sn-doping into In2O3
material results in high electrical conductivity of the order of 104 S/cm at room temperature with | [
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] |
material results in high electrical conductivity of the order of 104 S/cm at room temperature with
minimal effect on its optical transparency [6]. Hence, TCO material exhibits excellent electrical
conductivity alongwith optical transparency in the visible region.
One thing common in highly effective TCO materials (such as ITO, ZnO, SnO2, and
CdO) is their similar structural, chemical, and electronic properties. For instance, post-transition | [
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] |
metal oxides have (n-1)d10ns2 outer shell orbitals with closely packed dense structures. There is a
strong interaction between metal ns orbital and oxygen 2p orbital. The conduction band is
formed by the hybridization of anti-bonding metal ns orbitals and oxygen p orbitals. In contrast,
the valence band is shaped by interaction between bonding and non-bonding oxygen 2p states.
Interaction between metal ns and oxygen 2p orbitals leads to the forbidden gap between the | [
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] |
Interaction between metal ns and oxygen 2p orbitals leads to the forbidden gap between the
valence band and conduction band. As s-orbital is highly delocalized in spatially spread, it leads
to the large dispersion of conduction band by overlapping with oxygen 2p orbitals. Besides,
cations having octahedral coordination with oxygen anions results in further dispersion of
conduction band. Considering the case of rocksalt CdO, large dispersion is observed due to | [
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] |
conduction band. Considering the case of rocksalt CdO, large dispersion is observed due to
octahedral coordination with oxygen anions, leading to the lowest effective mass of electrons [7].
Hence, all highly effective TCOs demonstrate excellent electrical conductivity at room
temperature due to the low effective mass of charge carriers. Their electrical properties can
further be modified by introducing appropriate counter cations or anions. Replacement of host | [
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] |
further be modified by introducing appropriate counter cations or anions. Replacement of host
cation with suitable aliovalent cation can result in the generation of free charge carriers, which
can impart conductivity to the material. Most highly effective TCOs doped with suitable
countercation (without affecting its crystal structure) lead to remarkable optoelectronic properties
in a single material.
Besides, removing or replacing oxygen anions from its lattice sites can also provide more | [
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] |
Besides, removing or replacing oxygen anions from its lattice sites can also provide more
electrons within the crystal system, in the case of n-type TCO material. On the contrary, in the
case of p-type TCOs, incorporation of oxygen at the interstitial positions generates excess charge
carriers (holes) into the lattice [8]. These generated charge carriers may be free or localized
around the vacant site, ascribed to the formation energy of oxide material. Conventional TCO | [
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] |
around the vacant site, ascribed to the formation energy of oxide material. Conventional TCO
materials have low formation energy, exhibit a higher density of free charge carriers. On the
other hand, most of the p-type TCOs are attributed to higher formation energy. Hence, the charge
carrier generated localized around oxygen 2p states, which leads to the formation of a deep
acceptor level [9].
1.1.2 Optical properties | [
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0.10335467755794525
] |
acceptor level [9].
1.1.2 Optical properties
Maxwell’s equation of electromagnetic (EM) waves demonstrated that electrical properties and
optical properties are entirely contradictory to each other. When EM waves traveled through a
semiconducting material (uncharged), the solution to Maxwell's equation determines the value of
the refractive index in the form of real and imaginary parts, given below [10,11]:
+
+
=
1
2
1
2
12
2
2
n | [
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] |
+
+
=
1
2
1
2
12
2
2
n
(2)
−
+
=
1
2
1
2
12
2
2
k
(3)
where, n is refractive index of material, ϵ is dielectric constant, σ is electrical conductivity, k is | [
0.3123522102832794,
0.3545597791671753,
0.9752746820449829,
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0.0652448907494545,
0.26500943303108215,
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0.5544334053993225,
0.3665260672569275,
0.6970277428627014,
0.4178086519241333,
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0.4377206265926361,
0.3053789734840393,
0.05046620965003967,
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0.005092398729175329,
0.4817313849925995,
0.23395904898643494,
0.3152309060096741,
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0.22926677763462067,
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0.5991197228431702,
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] |
extinction coefficient, and ν is the frequency of EM waves. Considering the case of insulating
material, where electrical conductivity (σ) → 0, refractive index (n) → ϵ1/2 and then, extinction
coefficient (k) → 0. It concludes that insulating material is transparent to EM radiations. On the
other hand, in perfect conductors, Maxwell's equation solution for transmitted and reflected
components of the electric field vector is IT = 0 and EI = - ER. Hence, excellent conductors are | [
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] |
components of the electric field vector is IT = 0 and EI = - ER. Hence, excellent conductors are
opaque to EM radiations. When EM waves incident on the surface of a perfect conductor, it gets
reflected with 180⁰ out-of-phase. So, from the solution of Maxwell's equation, it is concluded
that insulators are transparent to EM waves, whereas conductors are not.
Also, Drude's model (free electrons in metals) explained the absorption of TCO material | [
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] |
Also, Drude's model (free electrons in metals) explained the absorption of TCO material
in the infra-red (IR) region [12–14]. The equation for the dielectric constant of a free electron gas
can be written as:
( )
i
m
ne
+
−
=
2
2
4
1
(4)
where, ϵ is dielectric constant, τ is relaxation time, and ω is frequency of EM waves. From | [
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0.3272060751914978,
0.07229756563901901,
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0.917119026184082,
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0.2720320224761963,
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1.0970770120620728,
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0.11914908140897751,
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0.32981985807418823,
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0.7638171315193176,
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0.08634500950574875,
0.9585888385772705,
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0.6322789192199707,
0.6039398908615112,
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0.6059243679046631,
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0.17201754450798035,
0.5246173143386841,
-0.49202412366867065,
0.9207454919815063,
-0.5408245325088501,
0.5579764246940613,
-0.6108366847038269,
-0.15370886027812958,
0.6490659713745117,
0.14681679010391235,
-0.111103855073452,
-0.14414703845977783,
0.13120493292808533,
-0.14334867894649506,
0.5161573886871338,
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-0.3926914930343628,
-0.5842614769935608,
0.69866544008255,
0.37210768461227417,
0.09644877910614014,
0.08094034343957901,
0.4453326463699341,
-0.0019056687597185373,
-0.02200748212635517,
-0.1619729995727539,
0.641903281211853,
-0.16461630165576935,
-0.3229266107082367,
0.809780478477478,
-0.5174282789230347,
0.1906401664018631,
-0.05579008907079697,
0.23324376344680786,
-0.08709879219532013,
-0.32807087898254395,
-0.004759195260703564,
-0.0036493423394858837,
-0.27678683400154114,
0.5533209443092346,
0.1533292531967163,
0.3093773126602173,
-0.12188723683357239,
-0.4603133499622345,
-0.6431966423988342,
0.4323657751083374,
0.11007354408502579,
-0.41967225074768066,
-0.4655369222164154,
0.09163486957550049,
-0.4774405360221863,
-0.21415264904499054,
-0.006208705250173807,
0.0099902069196105,
0.3760877549648285,
0.026065202429890633
] |
where, ϵ is dielectric constant, τ is relaxation time, and ω is frequency of EM waves. From
Drude's theory, it is revealed that EM waves cannot travel through a material with a negative
value of dielectric constant because its wave vector is imaginary and decays exponentially. The
EM waves incident on that material gets reflected. The plasma frequency or cut-off frequency
can be determined by:
2
1
*
2
=
o
p
m
ne
| [
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0.6019123792648315,
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0.7621206045150757,
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0.26897621154785156,
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0.4704464375972748,
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0.48908963799476624,
0.28811001777648926,
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0.25102701783180237,
0.13330048322677612,
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0.26724863052368164,
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0.2188655585050583,
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0.09271949529647827,
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0.10133577138185501,
0.15895353257656097,
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0.38806870579719543,
-0.5378709435462952,
-0.3296929895877838,
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-0.3672040104866028,
0.5519767999649048,
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0.12810511887073517,
0.28797417879104614,
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0.12087786942720413,
0.6114758849143982,
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0.3026064336299896,
0.03772909194231033,
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0.2969002425670624,
0.02881833352148533,
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0.04680110514163971,
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0.15021871030330658,
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1.5294276475906372,
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] |
can be determined by:
2
1
*
2
=
o
p
m
ne
(5)
where, ωp is a plasma or cut-off frequency, ϵo is permittivity of free space, n is the number
density of charge carriers, and m* is its effective mass. The material is transparent to those EM
radiations whose frequency is greater than plasma frequency. Hence, TCO materials are | [
0.5756602883338928,
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] |
radiations whose frequency is greater than plasma frequency. Hence, TCO materials are
transparent in visible and near infra-red (NIR) regions and reflect IR radiation (below plasma
frequency), as shown in figure 2. The material is transparent in the range between the shorter
wavelength band gap (λg) to the higher plasma wavelength (λp). Plasmon frequency and mobility
are governed by the effective mass of charge carriers and optical band gap. When the energy of | [
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] |
are governed by the effective mass of charge carriers and optical band gap. When the energy of
incident photons is higher than that of band gap of material, it is being absorbed by the material,
while if it is less than the plasmon frequency, then it is being reflected. Because at a frequency
higher than plasma frequency, electrons did not react to EM radiations with a varying electric
field and hence, act as transparent dielectrics. Most of the TCO materials exhibit plasma | [
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] |
field and hence, act as transparent dielectrics. Most of the TCO materials exhibit plasma
frequencies in the NIR region and accordingly, render high optical transparency in the visible
part. The plasma frequency is directly proportional to the concentration of free electrons. The
plasma frequency and carrier concentration vary similarly to that of resistivity values. Therefore,
by tailoring the plasmon frequency, the infra-red region can be blocked or transmitted by TCO
materials [15]. | [
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materials [15].
When a material is degenerately doped with suitable counter cation, excess generated
charge carriers occupy the lower energy level of conduction band and push the Fermi level to a
higher energy state. In this case of degenerate doping, an electron can only be excited to a higher
energy level if it has sufficient energy to surpass the bottom filled energy levels of occupied
conduction band and reside in unoccupied conduction band energy level. It results in the rise of | [
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] |
conduction band and reside in unoccupied conduction band energy level. It results in the rise of
band gap of material, which is advantageous for its optical properties. This shift in optical band
energy is known as Burstein-Moss shift or BM shift and can be determined by:
(
) 3
2
2
*
2
3
2
n
m
EBM
=
(6) | [
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] |
where, ΔEBM is magnitude of BM-shift, n is carrier concentration, and m* is effective mass. If
transparent material is heavily doped and concentration of charge carriers is high enough, then
the plasma edge will shift towards the red region of visible spectrum.
Alongwith that, when the bottom energy states of conduction band are completely
occupied, then there is a probability that electrons at Fermi level (EFL) may have sufficient | [
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occupied, then there is a probability that electrons at Fermi level (EFL) may have sufficient
energy to jump into the adjacent unoccupied energy band (next to above the conduction band).
This difference in the two lowest conduction bands is known as 'secondary gap" (Esg), as shown
in figure 3. Hence, a high secondary band gap (must be greater than 3.1 eV) is also necessary for
TCO materials. Because material with a large value of secondary band gap (Esg) can forbid the | [
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] |
TCO materials. Because material with a large value of secondary band gap (Esg) can forbid the
intra-band transition and illustrates high optical transparency. A similar discussion can equally
apply for p-type TCO material, where holes rather than electrons cause conduction.
Therefore, it is concluded that physical properties of TCO materials are interconnected,
and it is very improbable that a single material can pull off all the requirements. Contradictions | [
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] |
and it is very improbable that a single material can pull off all the requirements. Contradictions
will always be there for some points to improve the physical properties of TCO materials. But
the most important property of materials is their charge carrier type, as it is hard to modify. The
basic functionalities can be determined from a device having a single charge carrier type
material. Whereas most electronic devices require manipulation of both charge carrier types (i.e., | [
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] |
material. Whereas most electronic devices require manipulation of both charge carrier types (i.e.,
p-type and n-type) to function.
1.1.3 Optical and electrical performance or Figure of merit (FOM)
Better performance TCOs comprise significant optical and electrical properties, which are
inversely related to each other. Hence, researchers have developed a reliable parameter, i.e.,
figure of merit (FOM), which is used for assessing the performance of TCO materials. FOM | [
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] |
figure of merit (FOM), which is used for assessing the performance of TCO materials. FOM
value can be determined by using the following equation:
T
R
FOM
sh ln
−1
=
=
(7)
where, σ is electrical conductivity and α is absorption coefficient of TCO material. The term Rs
is the sheet-resistance (thickness-independent parameter) of TCO material’s thin-film and T is
the transmittance in visible region. FOM value is also used to quantify the performance of | [
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the transmittance in visible region. FOM value is also used to quantify the performance of
different TCO materials, as it provides a single number by combining both properties in a
particular combination. And that value can be set as a benchmark for comparison of all TCO
materials.
However, several issues need to be taken care of while considering the FOM value as a
performance parameter. In research articles, maximum transmittance peak values are used rather | [
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] |
performance parameter. In research articles, maximum transmittance peak values are used rather
than average transmittance values over the visible range (1.6–3 eV) for solar cells and displays
applications. Thus, various low optical band gap materials with a high FOM value have been
reported, regardless of acquiring limited optical transparency in the visible region. Another issue
is that two materials can have the same FOM value despite having different optoelectronic | [
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] |
is that two materials can have the same FOM value despite having different optoelectronic
properties. For example, one material with optical transparency of 20% and another material
exhibiting optical transparency of 80% can have the same FOM value because the former's
conductivity is higher enough. This amount of optical transparency (20%) is not acceptable for
optoelectronic device-based applications. Hence, FOM values can be compared for those | [
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] |
optoelectronic device-based applications. Hence, FOM values can be compared for those
materials that exhibit considerable optical transparency in visible region.
1.2 Types of TCOs
TCOs are classified into two categories, i.e., n-type and p-type, depending upon the nature of
conduction in the material. The detail explanation of both types of TCOs is discussed below:
1.2.1 n-type TCOs
High optical transparency in the visible region and high electrical conductivity at room | [
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] |
High optical transparency in the visible region and high electrical conductivity at room
temperature are usually believed to be incompatible within a single material. Since the material
has a wide optical band equal to or more than 3.1 eV makes extrinsic doping very difficult. But
TCOs can acquire high conductivity even close to that of metal (104 S/cm) and excellent
transparency (80%) as that of ceramics in the visible region by introducing dopants and/or non- | [
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] |
transparency (80%) as that of ceramics in the visible region by introducing dopants and/or non-
stoichiometry. This kind of technique was also employed in oxides of Cd, In, Sn, and Zn thin
films by using different deposition techniques. Above mentioned materials are insulating in
nature without extrinsic doping and acquired an optical band gap of ≥ 3 eV [16]. These materials
were degenerately doped with appropriate countercation to lift the Fermi level into conduction | [
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were degenerately doped with appropriate countercation to lift the Fermi level into conduction
band, demonstrating large carrier mobility and low absorption in the visible region of
electromagnetic spectrum. An increase in carrier concentration will also increase the optical
absorption, while improvement in mobility has no adverse effect on the transparency of
materials. Therefore, the focus is to develop TCO material with large carrier mobility and high | [
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materials. Therefore, the focus is to develop TCO material with large carrier mobility and high
optical transparency. The very first n-type transparent conductor was realized in 1907 by
Badekar in the form of CdO, whose thin film was deposited by sputtering of target Cd metal
experienced incomplete thermal oxidation upon post-annealing heating in an ambient
environment [7]. Hence, technological interest has been generated after the discovery of CdO as | [
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environment [7]. Hence, technological interest has been generated after the discovery of CdO as
the first transparent conductor. Though CdO is not widely used nowadays as it is toxic in nature
but still receives great interest due to its great carrier mobility. Afterward, extensive work has
been done to develop better performance TCO so that they can render a wide variety of
optoelectronic devices-based applications. There are various highly effective and commercially | [
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optoelectronic devices-based applications. There are various highly effective and commercially
used TCOs available, such as Sn/F/Sb/Mo-doped In2O3, In/Al/F/B/Ga-doped ZnO, Sb/F-doped
SnO2, MgIn2O4, Cd2SnO4, Y-doped CdSb2O6, Sn-doped CdIn2O4, Zn2SnO4, Zn2In2O5, ZnSnO3,
ZnGa2O4, In4Sn3O12, Ge/Sn-doped GaInO3, Sn-doped AgInO2, BaSnO3 etc. [4, 15–40]. In most
of the n-type oxide, the ionic character of host acquires a valence band comprising O 2p orbital, | [
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] |
of the n-type oxide, the ionic character of host acquires a valence band comprising O 2p orbital,
and conduction band consist of metal ns orbital, which are spatially distributed, exhibit excellent
n-type conductivity and large optical band gap as well. Out of these, ITO (Indium-tin oxide) is
the best performance TCO reported in 1954, exhibits transparency of 80%, and conductivity of
the order of 104 S/cm [6]. Hence, its unique optoelectronic properties extend applications in solar | [
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] |
cells and flat panel display devices as transparent electrodes [41]. Besides, ITO is considered as
the best n-type TCO to date and accounts for more than 90% of the optoelectronic market due to
its ease of fabrication along with high transparency and conductivity. However, due to low
abundancy and regularly increasing price from the past three decades, forced researchers to
explore other materials as possible alternatives to ITO.
1.2.2 p-type TCOs | [
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] |
explore other materials as possible alternatives to ITO.
1.2.2 p-type TCOs
The struggle for achieving p-type TCOs with comparable performance to n-type is due to their
valence band structure. Because in n-type oxides, conduction band minimum (CBM) mainly
consists of metal ns-orbitals. And it is a well-known fact that s orbital is highly delocalized or
spatially distributed and may lead to enough hybridization even in the amorphous crystal | [
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] |
spatially distributed and may lead to enough hybridization even in the amorphous crystal
structure. This highly dispersed or delocalized CBM results in the low effective mass of charge
carriers (i.e., electrons) and great mobility. On the contrary, there is a lack of conductivity in p-
type TCOs due to the following reasons: (i) production of charge carriers (i.e., holes) is limited
by high formation energy of intrinsic acceptors that create holes like cation vacancies (Vc), | [
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] |
by high formation energy of intrinsic acceptors that create holes like cation vacancies (Vc),
oxygen interstitials (Vi) and (ii) low formation energy of intrinsic donors that can act as “hole
killers” like oxygen vacancies (Vo) (iii) holes transport pathways in valence band maximum
(VBM), as there is strong localization around oxygen 2p orbitals, which results in the larger
effective mass of holes and impart low mobility (iv) Dispersion of valence band is so small that | [
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effective mass of holes and impart low mobility (iv) Dispersion of valence band is so small that
VBM level lies so deep, making hole doping unfavorable [9,42,43].
All the drawbacks mentioned above extend to the fact that the development of highly
effective p-type TCOs is not a trivial task. But in 1997, Kawazoe et al. introduce the concept of
chemical modulation of the valence band (CMVB) technique, as shown in figure 4 [42]. | [
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] |
chemical modulation of the valence band (CMVB) technique, as shown in figure 4 [42].
Following this concept, p-type TCOs conductivity can be improved by introducing appropriate
countercation, whose energy-filled levels must be comparable or more than oxygen 2p levels. It
can promote the delocalization around oxygen 2p orbitals by hybridizing metal-cation s, p or d
orbital with oxygen 2p orbital to form a covalent bond and thus, lead to the dispersion of valence | [
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orbital with oxygen 2p orbital to form a covalent bond and thus, lead to the dispersion of valence
band minimum (VBM), which in turn, reduce the effective mass of holes and improve carrier's
mobility.
The research for p-type TCOs was accelerated when a breakthrough was given by
Kawazoe and co-workers in 1997, in which they invented a good performance p-type TCO in the
form of CuAlO2 [4]. In CuAlO2 thin film, Cu+ has 3d10 electronic configuration, and its energy | [
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] |
form of CuAlO2 [4]. In CuAlO2 thin film, Cu+ has 3d10 electronic configuration, and its energy
level is just above the O 2p level, which is responsible for significant improvement in hole
conductivity. Besides, the closed-shell configuration of Cu+ ions avoided coloration and ascribed
to a wide optical band gap. However, the electrical conductivity obtained from this material is
still very low as compared to highly effective n-type TCOs. But this report makes other | [
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still very low as compared to highly effective n-type TCOs. But this report makes other
researchers realize that the development of better p-type TCOs is not an invincible goal. After
that, a series of p-type TCOs were invented that can lead to the development of novel “invisible
electronics” devices.
Following the concept of the CMVB technique, various oxide materials with
degenerately doping were identified as p-type TCOs such as CuMO2 (where M is Al, Mg, Cr, In, | [
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degenerately doping were identified as p-type TCOs such as CuMO2 (where M is Al, Mg, Cr, In,
Sc, Y, and Ga) and SrCu2O2 [44–50]. The development of p-type TCOs demonstrated that the
fabrication of transparent p-n junction is possible. After investigating the Cu-based p-type TCO
materials, the concept of CMVB technique was also employed to chalcogens based materials. In
this type of material, oxygen was intended to be replaced by chalcogens like S, Se, and Te. So | [
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] |
this type of material, oxygen was intended to be replaced by chalcogens like S, Se, and Te. So
that, there will be a hybridization between metal d orbital and chalcogen p-orbital. Layered
Sr3Cu2Sc2O5S2, LaCuOS, LaCuOSe and LaCuOTe were also identified as a potential candidate
for p-type TCOs [51–55]. In addition, Mg-doped LaCuOS exhibits the highest p-type
conductivity of 910 S/cm to date [56]. But its optical transparency is limited due to a low optical | [
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band gap of 2.8 eV. Lately, the CMVB technique was also employed on oxide materials with
quasi-closed shell configuration like d6 and d3. This results in the realization of new TCO
materials such as ZnM2O4 (where M is Co, Rh, and Ir) and chromium-based oxides [57,58].
1.3 Why p-type TCOs are required?
The history of TCO is more than a century ago, when Badekar invented the first TCO in the form
of CdO in 1907 [7]. TCOs are extensively utilized in various optoelectronic applications. Still, | [
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] |
of CdO in 1907 [7]. TCOs are extensively utilized in various optoelectronic applications. Still,
active devices are absent such as bipolar diodes and transistors, due to lack of better performance
p-type TCOs. Active electronic devices cannot be fabricated without p-n junctions. But the
majority of TCOs available in the market are n-type in nature. Therefore, optoelectronic
applications are limited to n-type TCOs based unipolar devices only. Furthermore, applications | [
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] |
applications are limited to n-type TCOs based unipolar devices only. Furthermore, applications
like solar water splitting and photovoltaics are also looking for p-type TCOs as electrodes for a
better efficient collection of holes [59]. The difficulty encountered in p-type TCOs is intrinsic
band structure of oxides. As oxygen is a relatively small atom with high electronegativity.
Hence, it is responsible for the struggle to form a shallow acceptor level and results in a large | [
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] |
Hence, it is responsible for the struggle to form a shallow acceptor level and results in a large
effective mass of holes. However, attempts are also being made to develop acceptor level defects
in the previously existing n-type TCOs for fabricating transparent p-n homojunction. But
unfortunately, no TCO material has been invented yet, which can demonstrate ambipolarity.
Materials like ZnO and SnO2 were tried to convert their conduction from n-type to p-type by | [
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] |
Materials like ZnO and SnO2 were tried to convert their conduction from n-type to p-type by
introducing different dopants but failed. DFT study revealed that intrinsic defects like oxygen
vacancies and cation interstitials act as donor defects, which abolish the p-type dopants [60–62].
Besides, Theoretical investigations have shown that band structure requirement for n-type and p-
type dopability is completely contradictory to each other. | [
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] |
type dopability is completely contradictory to each other.
If p-type TCOs with equally good performance will be available, then transparent p-n
junction and highly efficient energy circuits with more complexity can be fabricated. For
instance, alike silicon technology, a transparent complementary metal-oxide-semiconductor
(CMOS) device with effective performance and similar complex circuits can be realized. Hence, | [
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] |
(CMOS) device with effective performance and similar complex circuits can be realized. Hence,
the development of highly effective p-type TCOs became a major research topic in “invisible
electronics”.
1.4 Development of p-type TCOs
Since the groundbreaking work by Kawazoe et al. in 1997, there has been a surge in research on
p-type transparent conducting oxides (TCOs) for applications in transparent electronics. This | [
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] |
p-type transparent conducting oxides (TCOs) for applications in transparent electronics. This
review investigated the scientific output in this field, focusing on the evolution of published
papers between 1997 and 2024. Figure 5 illustrates a bar chart categorizing published research
on p-type TCOs by material type: binary oxides, spinel oxides, chromium (Cr)-based oxides, and
delafossite. Notably, the number of publications escalated significantly after 2003, exceeding | [
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delafossite. Notably, the number of publications escalated significantly after 2003, exceeding
500 publications by 2010 and so on.
Initially, research focused immensely on delafossite structures; however, there has been a
gradual shift towards exploring binary oxides over the years (discussed later). The increase in
publications and the evolving focus of research show up the dynamic nature of the field and the
ongoing efforts for highly effective p-type TCO materials. | [
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] |
ongoing efforts for highly effective p-type TCO materials.
This review provides a comprehensive survey of p-type TCO materials explored in
previous studies. We have examined various host materials that have been investigated for their
potential in p-type TCO applications. This examination considered crucial factors such as optical
transparency, electrical conductivity, chemical stability, and the deposition processes of p-type
TCO materials.
1.4.1 Cu-based materials as p-type TCOs | [
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] |
TCO materials.
1.4.1 Cu-based materials as p-type TCOs
CuAlO2 material received great interest due to its wide optical band gap and significant p-type
conductivity. After that, various Cu-based delafossite structures have been studied and their
optoelectronic properties are highlighted in table 1. However, hole conductivity in CuAlO2 was
firstly reported in 1984 by Benko and Koffyberg [63]. But they have examined optoelectronic | [
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] |
firstly reported in 1984 by Benko and Koffyberg [63]. But they have examined optoelectronic
properties of powder sample compacted into a disk. The disk sample exhibited the resistivity of
5.9 Ω-cm with a very low value of Hall mobility of 10-5 cm2/Vs at room temperature. A detailed
structural study of CuAlO2 was reported by Ishiguro et al. [64]. They have also determined the
electron-energy distribution in crystals of CuAlO2 [65]. Thereafter, Kawazoe et al. in 1997 | [
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] |
electron-energy distribution in crystals of CuAlO2 [65]. Thereafter, Kawazoe et al. in 1997
prepared a transparent thin film of CuAlO2 material and studied its optoelectronic properties.
Following the CMVB technique by introducing Cu+ cation, other Cu-based delafossite
structures were reported as p-type TCO material in the form of CuGaO2 and CuInO2. The optical
and electrical properties of CuGaO2 thin film were studied [49]. As-deposited CuGaO2 was | [
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] |
and electrical properties of CuGaO2 thin film were studied [49]. As-deposited CuGaO2 was
found epitaxial in nature, confirmed by cross-sectional HRTEM. UV-Vis optical transmission
spectra demonstrated that CuGaO2 thin film was highly transparent in the visible region with an
average transparency of 80%. The observed electrical conductivity at room temperature was very
low compared to CuAlO2. However, the conduction mechanism is similar in both materials, i.e.,
variable-range hopping. | [
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] |
variable-range hopping.
Thereafter, the optoelectronic properties of doped CuInO2 thin film was explored by
introducing counter-cation and optimized thin-film deposition parameters [46]. Two different
dopants, such as Ca and Sn were used, resulting in p-type and n-type thin film conduction. The
PLD technique was used to deposit a thin film of Ca and Sn doped CuInO2. All parameters were
kept the same except O2 partial pressure, which is 1 Pa for Ca CuInO2 and 1.5 Pa for Sn doped | [
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] |
kept the same except O2 partial pressure, which is 1 Pa for Ca CuInO2 and 1.5 Pa for Sn doped
CuInO2 thin film, as the conductivity of Sn:CuInO2 thin film is susceptible to O2 partial pressure
during deposition. Both Sn:CuInO2 and Ca:CuInO2 were highly transparent in the visible range
with a direct optical band gap of 3.9 eV. However, thickness of Sn:CuInO2 thin film was 280 nm
and 170 nm for Ca:CuInO2 thin film. Considering the electrical properties of n-type Sn:CuInO2 | [
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] |
and 170 nm for Ca:CuInO2 thin film. Considering the electrical properties of n-type Sn:CuInO2
and p-type Ca:CuInO2 thin film, low conductivity value (of the order of 10-3 S/cm) was observed
at room temperature. The nature of conduction was demonstrated by sign of Seebeck coefficient,
which was -50 μV/K for Sn:CuInO2 and +480 μV/K for Ca:CuInO2 thin film. The substitution of
Ca2+ ions at In3+ cationic sites result in p-type conductivity, whereas Sn4+ ions at In3+ attributed to
n-type conduction. | [
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] |
n-type conduction.
They have also fabricated a transparent p-n homojunction composed of Sn:CuInO2 and
Ca:CuInO2 films [66]. Initially, ITO film with a thickness of 600 nm was epitaxially grown on
(111) yttria-stabilized zirconia (YSZ) substrate by using the PLD technique. Subsequently, p-
type and n-type CuInO2 thin film having a thickness of 400 nm was deposited on ITO. At last,
again ITO film (act as a cathode) deposited on multi-layered film with a thickness of 400 nm. | [
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] |
again ITO film (act as a cathode) deposited on multi-layered film with a thickness of 400 nm.
The characteristics I-V curve of transparent p-n homojunction illustrated the rectifying behavior,
i.e., current in forward biasing was 10 times higher than the reverse one in the voltage range
from –4 to +4 V. The diode in thin-film form was also showed good transparency in the visible
region, varying in the range of 60 to 80%. However, the transmission was very poor in the NIR | [
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] |
region, varying in the range of 60 to 80%. However, the transmission was very poor in the NIR
region due to ITO carrier electrons.
As desired hole conductivity was not achieved in pristine Cu-based delafossite structure.
Therefore, various dopants have been tried in Cu-based p-type TCOs such as Fe-doped CuGaO2,
Mg-doped CuScO2, Mg-doped CuCrO2, and Ca-doped CuYO2 [67]. A thin film of CuGa1-xFexO2
was deposited via PLD technique, and conductivity was found to be increased from 0.02 to 1 | [
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] |
was deposited via PLD technique, and conductivity was found to be increased from 0.02 to 1
S/cm. The idea was to combine the optical properties of CuGeO2 and electrical properties of
CuFeO2. As Benko et al. in 1986 already determined the optoelectronic properties of CuFeO2 in
powder form and found a minimum resistivity value of 0.11 Ω-cm at 2% of Mg-doped CuFeO2,
which was 0.65 Ω-cm in pure form with low mobility value of 0.27 cm2/V-s. But on the contrary, | [
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] |
which was 0.65 Ω-cm in pure form with low mobility value of 0.27 cm2/V-s. But on the contrary,
a reduction in transparency was observed with Fe doping, and the optical band gap reduced from
4.3 eV to 3.4 eV, which is very near to the band gap of CuFeO2 [68].
Transition metal (Sc) was also employed in Cu-based delafossite structure and prepared a
thin film of CuScO2+x by sputtering technique [47]. Polycrystalline CuScO2 film was found | [
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] |
thin film of CuScO2+x by sputtering technique [47]. Polycrystalline CuScO2 film was found
insulating in nature with a large optical band gap of 3.3 eV, illustrating higher optical
transparency. Afterward, as-deposited thin films were post-annealed under the O2 environment
for 2 hours at 450 ⁰C. This oxygen intercalation results in an improvement in conductivity value
to 15 S/cm (at room temperature). But transparency of thin film was degraded to 40% in the | [
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to 15 S/cm (at room temperature). But transparency of thin film was degraded to 40% in the
visible spectrum. However, they have also achieved a conductivity value of 30 S/cm by
increasing intercalation pressure, as shown in figure 6. Still, this conductivity value is lower than
n-type TCOs, but this report paved another way for increasing the p-type conductivity.
Optoelectronic properties of oxygen intercalated Mg-doped CuScO2+x thin film was also | [
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] |
Optoelectronic properties of oxygen intercalated Mg-doped CuScO2+x thin film was also
examined [69]. Mg-doping improved the conductivity to 0.48 S/cm of CuMgySc1-yO2+x pallet. On
the other hand, oxygen intercalation enhanced thin film's p-type conductivity to 25 S/cm.
However, Mg incorporation didn't affect the optical transparency, but oxygen intercalation
darkened the thin film.
After the transition metal, rare earth element (Y) was also employed by Jayaraj et al. in | [
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] |
After the transition metal, rare earth element (Y) was also employed by Jayaraj et al. in
2001 [48]. They have deposited the thin film of CuY1-xCaxO2 by thermal co-evaporation
technique. They have prepared thin films on different substrates, i.e., glass, Si, and single crystal
(100) MgO. As-deposited thin films were non-conductive, turn into conductive, followed by
rapid thermal annealing in the O2 atmosphere, and improved transparency as well. Still, no | [
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] |
rapid thermal annealing in the O2 atmosphere, and improved transparency as well. Still, no
exciting results were obtained from this material, exhibited conductivity of 1 S/cm with Ca
doping (which was 0.03 S/cm without Ca) and transparency varying between 40-50% in the
visible range. Highly oriented thin film on the MgO substrate didn't illustrate any improved
optoelectronic properties over polycrystalline thin films deposited on glass and Si substrate. | [
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optoelectronic properties over polycrystalline thin films deposited on glass and Si substrate.
They have also fabricated a transparent p-n diode in the form of glass/ITO/Zn1-xAlxO /CuY1-
xCaxO2/In by r.f. magnetron sputtering technique and demonstrated rectifying behavior.
In 2001, when a wide variety of Cu-based delafossite structures have been explored,
Nagarajan et al. developed a p-type CuCr1-xMgxO2 material with the excellent value of hole | [
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] |
Nagarajan et al. developed a p-type CuCr1-xMgxO2 material with the excellent value of hole
conductivity [45]. They have synthesized CuCr1-xMgxO2 material, both in bulk and thin-film
form. Undoped bulk CuCrO2 material was found to be black, with an average value of
conductivity. And conductivity observed in undoped CuCrO2 thin film was of the order of 0.1
S/cm. When 5% Mg was introduced into CuCrO2, its conductivity was increased by a factor of | [
0.35533419251441956,
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] |
S/cm. When 5% Mg was introduced into CuCrO2, its conductivity was increased by a factor of
103, i.e., 220 S/cm, which was highest at that time for any p-type TCO material. However, this
material's optical transparency was low in the visible region, i.e., only 30% for 250 nm thick
film. They have also post-annealed the thin film at different temperatures. No significant change
in crystallinity, conductivity, and transparency has been observed upto 600 ⁰C. But at 900 ⁰C, | [
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] |
in crystallinity, conductivity, and transparency has been observed upto 600 ⁰C. But at 900 ⁰C,
transparency was improved to 40%, whereas the resistivity value also increased to ~1 Ω-cm.
They have even attempted oxygen intercalation of as-deposited thin films, but that experiment
turned out to be a failure. Due to the low lattice volume of CuCrO2 compound, no oxygen intake
was there at any temperature upto 1200 ⁰C, indicated by thermogravimetric analysis (TGA) | [
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] |
was there at any temperature upto 1200 ⁰C, indicated by thermogravimetric analysis (TGA)
results. After this temperature, oxygen intake leads to the formation of CuCr2O4.
In 2015, Farrell et al. prepared the Cu-deficient CuCrO2 thin film by spray pyrolysis
technique [70]. They have achieved maximum conductivity of 12 S/cm alongwith good
transparency of 55% for 80 nm Cu-deficient CuCrO2 thin film. The experiment of co-doping of | [
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] |
transparency of 55% for 80 nm Cu-deficient CuCrO2 thin film. The experiment of co-doping of
Mg and N into CuCrO2 thin films was conducted by Ahmadi et al. in 2018 [71]. Mg and N doped
CuCrO2 thin films were prepared by RF sputtering technique on the quartz substrate. A
tremendous increase in electrical conductivity was observed from 0.01 S/cm (undoped CuCrO2)
to 277.7 S/cm (2.5% Mg, N doped CuCrO2) alongwith better optical transparency of 69.1% in | [
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] |
to 277.7 S/cm (2.5% Mg, N doped CuCrO2) alongwith better optical transparency of 69.1% in
the visible region and band gap of 3.52 eV. Besides, 2.5% Mg, N co-doped CuCrO2 thin film
illustrated the highest hole conductivity to date despite having very poor Hall mobility of 0.006
cm2/V-s.
Another Cu-based delafossite materials were also investigated by Nagarajan’s research
groups such as CuM1-xM'xO2 (where M is Mg, Mn, Fe, Co, Ni, Zn and M' is Sb and V) [72]. | [
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groups such as CuM1-xM'xO2 (where M is Mg, Mn, Fe, Co, Ni, Zn and M' is Sb and V) [72].
Above mentioned Cu-based delafossite structures have been explored with doping (or even with
co-doping) in the hope to obtain desired optoelectronic properties of p-type TCOs. But all
materials were found to be highly resistive (in powder form) of the order of ~106 Ω-cm, and no
optoelectronic studies on the thin films of materials have been reported so far. However, the | [
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optoelectronic studies on the thin films of materials have been reported so far. However, the
same research group examined a thin film of Sn-doped CuNi1-xSbxO2 on a fused silica substrate.
Though transparency in the visible region was found to be reasonable, the conductivity of thin
film was 0.05 S/cm only at 10% of Sn doping.
Apart from the Cu-based delafossite structure, there is a material which is also Cu-based | [
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] |
Apart from the Cu-based delafossite structure, there is a material which is also Cu-based
but exhibits a non-delafossite structure in the form of SrCu2O2. Kudo et al. have deposited a thin
film of this material in 1998 [50]. Thin films of undoped SrCu2O2 and 3% K-doped SrCu2O2
were deposited. Both undoped and doped thin films (having a thickness of 150 and 200 nm,
respectively) were highly transparent in the visible and infra-red range. The electrical | [
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] |
respectively) were highly transparent in the visible and infra-red range. The electrical
conductivity of undoped thin film was found to be 3.9×10-3 S/cm, increased to 4.8×10-2 S/cm
with 3% K-doping. The positive sign of Seebeck and Hall coefficients confirmed the p-type
conductivity of both undoped and doped thin films.
In the recent past, various previously used Cu-based materials such as CuCrO2+x,
CuCrO2, CuGaO2 and CuAlO2 were explored using different deposition techniques and | [
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] |
CuCrO2, CuGaO2 and CuAlO2 were explored using different deposition techniques and
parameters to surpass the previous results, as shown in table 1. However, the optical
transparencies were found to be reasonably better than previous results, but no remarkable
improvement in electrical conductivity was demonstrated [73–76].
1.4.2 Ag-based materials as p-type TCOs
As suggested by Kawazoe et al. to follow the concept of CMVB technique to enhance p-type | [
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] |
As suggested by Kawazoe et al. to follow the concept of CMVB technique to enhance p-type
conductivity by introducing suitable counter-cation with nd10 configuration to promote
delocalization in the valence band. After that, various Cu based p-type TCOs have been studied,
as discussed above. But desired results were not achieved though they set a benchmark for other
researchers that it is not an impossible task. Afterward, some Ag-based delafossite structures | [
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researchers that it is not an impossible task. Afterward, some Ag-based delafossite structures
have been investigated as Ag+ ions also have a 4d10 closed-shell configuration and its energy
level is higher than Cu+ ions that can promote more delocalization [77].
However, the synthesization of Ag-based delafossite structures is not straightforward
through solid-state reactions and usually requires ion-exchange synthesis [67]. The first TCO | [
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] |
through solid-state reactions and usually requires ion-exchange synthesis [67]. The first TCO
thin film based on Ag-delafossite structure AgInO2 was reported in 1998 by Otabe et al., but it
was n-type [38]. They have deposited undoped and Sn-doped AgInO2 thin films by r.f. sputtering
technique. Both as-deposited thin films were post-annealed under O2 flow at 500 ⁰C for 12 hours.
Both thin films were highly transparent in the visible region, even upto near UV-region, and | [
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] |
Both thin films were highly transparent in the visible region, even upto near UV-region, and
acquired a wide optical band of 4.2 eV for pristine and 4.4 eV for 5% Sn-doped thin film.
Undoped AgInO2 thin film exhibited very poor conductivity at room temperature, i.e., 10-5 S/cm.
However, improvement in the Sn-doped AgInO2 thin film was marvelous (6 S/cm). But still, it
was very low as compared to the best-known n-type TCOs. A lower Hall mobility value of 0.47 | [
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was very low as compared to the best-known n-type TCOs. A lower Hall mobility value of 0.47
cm2/V-s was responsible for marginal n-type conductivity in Sn-doped AgInO2 thin film. And n-
type conduction was confirmed from the negative value of the Seebeck coefficient.
The synthesis and theoretical examination of Ag3VO4 was explored as potential p-type
TCO candidate [78]. Ag3VO4 is nearly transparent according to theoretical calculations, with | [
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] |
TCO candidate [78]. Ag3VO4 is nearly transparent according to theoretical calculations, with
optical absorption at 2.6 eV, which is in close agreement with experimental results. But, with a
conductivity limit of 0.002 S/cm and low hole concentration, making it undesirable for TCO
applications.
In 2017, Renhuai Wei et al. reported the synthesis and characterization of p-type TCO
thin films using AgCrO2 (ACO) delafossite structure [79]. They found that the stoichiometric | [
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] |
thin films using AgCrO2 (ACO) delafossite structure [79]. They found that the stoichiometric
ACO thin films showed a preferred c-axis orientation, with optimal properties achieved at 500°C
annealing temperature. To enhance conductivity, magnesium (Mg) doping was explored,
resulting in p-type conductivity for AgCr1-xMgxO2 thin films, as depicted in table 2. As the Mg-
content increased from 0.04 to 0.12, the conductivity of the thin films increases considerably | [
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