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\begin{document}

\title{High Mobility Hafnium and Hydrogen Co-Doped Indium Oxide Transparent
Conductive Films and Application in High Efficiency Silicon
Heterojunction Solar Cell}



\author[1]{Jiacheng Shang}%
\author[2]{Qi Wang}%
\author[3]{Shuai Zhou}%
\author[4]{Wanwu Guo}%
\author[1]{Rong Zhou}%
\author[1]{Yuqin Zhou}%
\author[1]{Fengzhen Liu}%
\affil[1]{University of the Chinese Academy of Sciences}%
\affil[2]{Suzhou Maxwell Technologies Co Ltd}%
\affil[3]{Weiqiao-UCAS Science and Technology Park}%
\affil[4]{Jetion Solar (China) Co Ltd}%


\vspace{-1em}



  
  \date{May 04, 2024}


\begingroup
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\selectlanguage{english}
\begin{abstract}
In this work, high quality hafnium and hydrogen co-doped In
\textsubscript{2}O \textsubscript{3} (IHfO:H) transparent conductive
films are developed via a reactive plasma deposition (RPD) technique
followed by air atmosphere annealing. Crystallinity, valence states, and
opto-electronic properties of the IHfO:H films under different H
\textsubscript{2} concentration (0-1.5 \%) and different annealing
temperature (100-250 \selectlanguage{ngerman}°C) are systematically investigated. The effects of
hydrogen doping and annealing temperature on the properties of the
IHfO:H films are discussed. The high average transmittances (400-800 nm:
87.92 \%; 800-2300 nm: 86.68 \%), a sheet resistance of 27.53 \selectlanguage{greek}Ω/\selectlanguage{english}#, \selectlanguage{english}and a
Hall mobility of 102.92 cm \textsuperscript{2}V \textsuperscript{-1}s
\textsuperscript{-1} are achieved on the optimized IHfO:H thin film
fabricated using 0.8 \% H \textsubscript{2} concentration with a 200 \selectlanguage{ngerman}°C
annealing temperature. Finally, the IHfO:H films are applied to the
bifacial silicon heterojunction (SHJ) solar cells to serve as the
front-side transparent electrode. The significant improvement in the
long wavelength spectral response compared to the control SHJ device
with an indium tin oxide (ITO) front-side transparent electrode leads to
an increase of about 0.3 \% in the efficiency and an efficiency of over
25 \% is achieved on the SHJ solar cell with an IHfO:H front-side
transparent electrode.%
\end{abstract}\selectlanguage{ngerman}%



\sloppy


\textbf{1 Introduction}

In recent decades, silicon heterojunction (SHJ) solar cells based on
intrinsic amorphous silicon passivation layers and doped amorphous or
microcrystalline silicon carrier selective layers have attracted more
and more attention due to their advantages of high efficiency, weak
light attenuation and low temperature
coefficient.\textsuperscript{1-2}The SHJ technology has succeeded in
bringing the conversion efficiency of monocrystalline silicon solar
cells to over 26 \%.\textsuperscript{3}Due to the relatively low carrier
diffusion length of doped amorphous or microcrystalline silicon films,
transparent conductive oxide (TCO) electrodes are essential for
achieving efficient lateral carrier collection in the SHJ solar cells.
High quality TCO layers with good optical and electrical properties are
crucial for SHJ solar cells to realize high fill factor (FF) and high
short-circuit current density (J\textsubscript{sc}). Indium tin oxide
(ITO) thin film is widely used in the industrial production of SHJ solar
cells because of its high electrical conductivity. So far, in many
reported high-efficiency SHJ solar cells, the ITO films were utilized as
the front or bifacial transparent conductive
electrodes.\textsuperscript{4-5} Different deposition techniques,
including direct current (DC) or radio frequency (RF)
sputtering,\textsuperscript{6} thermal\textsuperscript{7} or electron
beam evaporation,\textsuperscript{8} plasma-enhanced reactive thermal
evaporation,\textsuperscript{9} and pulsed laser
deposition,\textsuperscript{10} etc., have been successfully employed to
deposit ITO films with high conductivity. However, the Hall mobility of
the ITO films prepared by these methods mentioned above is typically
below 50
cm\textsuperscript{2}V\textsuperscript{-1}s\textsuperscript{-1}. The
high conductivity characteristic of ITO mainly benefits from the high
carrier concentration (usually in the order of
10\textsuperscript{21}cm\textsuperscript{-3}) which causes serious
parasitic absorption in the near-infrared (NIR) region and limits the
short-circuit current density of the SHJ solar
cells.\textsuperscript{11} To explore TCO films with both high
transmittance and high mobility, so as to improve the
J\textsubscript{sc} to catch up with the Tunnel Oxide Passivated Contact
(TOPCon) solar cells, is one of the main research directions of the high
efficiency SHJ solar cells.

According to the literature, the relatively low mobility of ITO is
mainly related to the low doping efficiency of
tin.\textsuperscript{12}Substitutional doping of Sn\textsuperscript{4+}
with smaller ionic radius may cause lattice distortion in ITO and, as a
less efficient dopant,\textsuperscript{13} relatively high doping
concentration of tin impurities is required to achieve low
resistivity.\textsuperscript{14}To obtain TCO films with high mobility
and low carrier concentration, various metal elements with higher ionic
valence or more matched ionic radius with In\textsuperscript{3+}, such
as W,\textsuperscript{15}Mo,\textsuperscript{16} Ce\textsuperscript{17}
and Hf,\textsuperscript{18} etc., were proposed to replace Sn as the
dopant elements of indium oxide films to reduce the impurity
concentration without compromising film conductivity. Among them, indium
oxide doped with Hf (IHfO) presents excellent opto-electronic properties
and great application potential. A Hall mobility of 79.6
cm\textsuperscript{2}V\textsuperscript{-1}s\textsuperscript{-1}, a
carrier concentration of
5.04\selectlanguage{ngerman}×10\textsuperscript{20}cm\textsuperscript{-3} and a resistivity of
3.76×10\textsuperscript{-4}\selectlanguage{greek}Ω\selectlanguage{ngerman}·cm were achieved on IHfO thin film grown by
magnetron sputtering technique.\textsuperscript{19} The IHfO films have
been successfully applied on amorphous silicon germanium thin film solar
cells and SHJ solar cells and obtained conversion efficiencies of 8.3\%
and 19.08\%, respectively.\textsuperscript{18-19}

In recent years, reactive plasma deposition (RPD) technology, also named
as hollow cathode discharge deposition, has been used to prepare TCO
films and has received wide attention of the researchers in the field of
heterojunction solar cells.\textsuperscript{20} During the RPD process,
the substrate is not directly exposed to the plasma and the damage
related to the ion bombardment is greatly
reduced.\textsuperscript{20}Thereby, RPD is considered to be a suitable
technique for the devices such as heterojunction solar cells with
extremely high-quality interface requirements. Furthermore, RPD is
actually an ion-plating method working in the arc discharge plasma
regime with low-voltage and high-current. The high ionization yield is
conducive to promote the gas phase reaction and improve the
opto-electronic properties of the grown TCO films. Previously, some TCO
films including ZnO,\textsuperscript{21} Ce-doped
In\textsubscript{2}O\textsubscript{3} (ICO),\textsuperscript{22} W-doped
In\textsubscript{2}O\textsubscript{3} (IWO)\textsuperscript{23} and W
and Ti co-doped
In\textsubscript{2}O\textsubscript{3}(IWTO)\textsuperscript{24} have
been successfully grown by RPD and have exhibited excellent
opto-electronic properties. However, more research work is still needed
in IHfO films prepared using RPD technique and application of IHfO films
in high efficiency SHJ solar cells is also expected.

In this work, hydrogen doped IHfO thin films (IHfO:H) were prepared by
RPD technique. The effects of hydrogen concentration and post-annealing
temperature on the crystallinity, opto-electronic properties, and
valence states of the IHfO:H thin films were investigated. Under the
conditions of H\textsubscript{2} concentration of 0.8 \% and
post-annealing temperature of 200 °C, the IHfO:H films with the best
comprehensive properties were obtained. The IHfO:H thin film prepared
under the optimized condition was applied to the bifacial SHJ solar cell
as the front TCO layer and a conversion efficiency of more than 25 \%
has been achieved.

\textbf{2 Experimental details}

2.1 Preparation of IHfO:H thin films:

IHfO:H thin films were deposited on glass and polished silicon wafers by
RPD to investigate their micro-structure, morphology, opto-electronic
properties, and chemical valence states. HfO\textsubscript{2}-doped
In\textsubscript{2}O\textsubscript{3} particles (4 wt \%
HfO\textsubscript{2}, 99.99 \% purity) were used as the target.
High-purity argon with the fixed flow rate of 30 sccm and argon-hydrogen
mixture (30 \% hydrogen) with the varied flow rate between 0 and 1.5
sccm were used as the working gas. The chamber pressure was controlled
to be at 0.4-0.5 Pa and the working current of power was set at 60 A.
The thicknesses of all the IHfO:H films are around 100 nm (±5 nm). The
post-annealing process was carried out in air with the annealing time of
20 minutes and the annealing temperature of 50-250 °C.

2.2 Fabrication of SHJ solar cells:

The n-type Cz crystalline silicon wafers with the thickness of 170 \selectlanguage{greek}μ\selectlanguage{english}m
and resistivity of 1 \selectlanguage{greek}Ω\selectlanguage{ngerman}·cm were used as the substrates. Alkaline
texturing, chemically polishing and RCA cleaning procedures were
performed prior to the fabrication of the SHJ solar cells. The SHJ solar
cells adopt a bifacial light incident structure of Ag
grids/IHfO:H/\selectlanguage{greek}μ\selectlanguage{english}c-Si:H(n\textsuperscript{+})/a-Si:H(i)/n type c-Si/
a-Si:H(i)/a-Si:H(p\textsuperscript{+})/ITO/Ag grids, as specifically
shown in Figure 1. The intrinsic hydrogenated amorphous silicon
(a-Si:H(i)) passivation layers with the thickness of 7 nm were deposited
on both sides of the n-type crystalline silicon by plasma enhanced
chemical vapor deposition (PECVD). A 10 nm p-type amorphous silicon
(a-Si:H(p\textsuperscript{+})) layer and a 7 nm n-type micro-crystalline
silicon \selectlanguage{greek}µ\selectlanguage{english}c-Si:H(n\textsuperscript{+}) layer, also deposited by PECVD,
serve as the hole transport layer (emitter) and electron transport
layer, respectively. A 100 nm IHfO:H film, as both the transparent
conductive layer and the antireflection layer, was prepared by RPD. A 70
nm ITO film was prepared by the magnetron sputtering method on the back
side of the SHJ solar cells. The silver grids on both sides of the
device were prepared by screen printing technology. After electrode
printing was completed, the whole solar cells were annealed in air at a
temperature of 200 \selectlanguage{ngerman}°C for 20 minutes.

2.3 Characterization:

The thickness of the IHfO:H films was measured by a step profiler
(Bruker DektakXT). X-ray diffraction (Rigaku Smartlab SE) measurement
was carried out to analyze the crystal structure of the IHfO:H thin
films using a Cu-K\selectlanguage{greek}α \selectlanguage{english}radiation source (\selectlanguage{greek}λ \selectlanguage{english}= 1.5405 \selectlanguage{ngerman}Å), scanned in 2\selectlanguage{greek}θ \selectlanguage{english}mode,
with the diffraction angles ranging from 10 to 80 \selectlanguage{ngerman}°. The square
resistance of the IHfO:H films was measured by the four-probe method,
while the carrier concentration and Hall mobility were obtained from the
Hall measurement (PSAICSwin Hall 8686). A UV-Vis-NIR spectrophotometer
(Perkin-Elmer Labmda 750) was used to obtain the optical transmission
spectra of the films. The chemical state characterization of the IHfO:H
films was determined using X-ray photoelectron spectroscopy (XPS, Kratos
Axis Supra+). In order to exclude the effect of adsorbed air on the
surface, all samples were etched with Ar ion beam for 1 minute before
the XPS measurement. The light current-voltage (I-V) curves of the solar
cells were obtained using a solar simulator under standard conditions
(100 mW/cm\textsuperscript{2}, AM 1.5 G, 25 °C). The external quantum
efficiency (EQE, BENTHAM INSTRUMENT PVE300-IVT) was measured to study
the spectral response of the solar cells.\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image1/image1}

\end{center}
\end{figure}

Figure 1 Schematic of the bifacial SHJ solar cells based on n-type
monocrystalline silicon wafers.

\textbf{3 Results and discussion}

3.1 Effect of hydrogen concentration on the IHfO:H thin films

Hydrogen doping has been proved to be an effective strategy to modify
the performance of the TCO films, such as reducing the square resistance
and improving the mobility, by influencing the crystallinity, forming
shallow donor states, and passivating the structural
defects.\textsuperscript{25-27} We investigated the effects of hydrogen
doping on the IHfO:H films by varying the
H\textsubscript{2}concentrations (gas flow ratio of hydrogen to argon: 0
\%, 0.5 \%, 0.8 \%, 1.2 \% and 1.5 \%) during the deposition process.
Referring to the fabrication process of traditional SHJ solar cells, the
series of IHfO:H films were all annealed at 200 \selectlanguage{ngerman}°C in air for 20
minutes.

Figure 2 shows the XRD patterns of the IHfO:H films with different
hydrogen concentrations after annealing at 200 °C. According to the
standard comparison card (JCPDS No.06-0416), the diffraction peaks of
(211), (222), (332), and (444) belonging to the cubic bixbyite
polycrystalline structure of In\textsubscript{2}O\textsubscript{3} are
observed. The absence of diffraction peaks for
HfO\textsubscript{2}indicates that substitutional doping
(Hf\textsuperscript{4+} replacing In\textsuperscript{3+}) forms a solid
solution in which HfO\textsubscript{2} was dissolved into the
In\textsubscript{2}O\textsubscript{3} lattice during the film growth
process.\textsuperscript{28} The intensity of the diffraction peak (222)
in all samples is much higher than that of the other peaks, which
indicates that (222) is the preferential crystallization direction. We
calculated the average grain size D of the IHfO:H films corresponding to
the full width at half maximum (FWHM) of the (222) diffraction peak
according to the Scherrer formula,\textsuperscript{19} as included in
Figure 2.

It can be seen that the average grain sizes of all the samples are in
the range of 50±5 nm, which implies that the
H\textsubscript{2}concentration hardly affects the crystallinity of the
films. Annealing can greatly improve the crystallinity of the IHfO:H
films, thus weakening the effect of hydrogen doping on the crystallinity
of the films, as will be discussed below.\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image2/image2}

\end{center}
\end{figure}

Figure 2 Normalized XRD patterns of the IHfO:H films with 0 \%, 0.5 \%,
0.8 \%, 1.2 \% and 1.5 \% H\textsubscript{2} concentration after
post-annealing at 200 .

The electrical properties of the IHfO:H films prepared with different
hydrogen concentrations are shown in Figure 3. It can be seen that the
sheet resistance of the IHfO:H films decreases first and then increases
as the increase of the hydrogen concentration, reaching a minimum of
27.53 \selectlanguage{greek}Ω/\selectlanguage{english}# \selectlanguage{english}at a hydrogen concentration of 0.8 \%. For TCO films with the
same thickness, the sheet resistance is mainly affected by the mobility
and the carrier concentration. In order to clarify the influence
mechanism of the hydrogen concentration on the sheet resistance of the
IHfO:H films, the Hall mobility and the carrier concentration of the
IHfO:H films were studied, also depicted in Figure 3.\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image3/image3}

\end{center}
\end{figure}

Figure 3 Sheet resistance, carrier concentration and Hall mobility of
the IHfO:H films prepared with 0 \%, 0.5 \%, 0.8 \%, 1.2 \% and 1.5 \%
H\textsubscript{2} concentration after post-annealing at 200 .

The Hall mobility increases at first and then decreases with increasing
the H\textsubscript{2} concentration, reaching a maximum of 102.92
cm\textsuperscript{2}V\textsuperscript{-1}s\textsuperscript{-1}at a
H\textsubscript{2} concentration of 0.8 \%. Three carrier scattering
mechanisms including acoustical phonon scattering, ionized impurity
scattering, and grain boundary scattering are generally considered as
the main mechanisms to affect the mobility of the TCO
films.\textsuperscript{29} Considering that the electrical properties
were measured at the room temperature and no significant crystallinity
difference can be determined (as Figure 2 shows), phonon scattering and
grain boundary scattering should not be the main factors that cause the
mobility difference in the IHfO:H films with different
H\textsubscript{2} concentrations. Therefore, it can be inferred that
the variation of Hall mobility is mainly caused by the difference in the
intensity of ionized impurity scattering. The roughly opposite variation
tendency of the carrier concentration and the Hall mobility in Figure 3
proves the above analysis, since the carrier density is strongly related
to the impurity concentration.\textsuperscript{29}

Oxygen vacancies, substitution high~valence~metallic~ions for indium,
and H doping are all the important sources of conducting electrons in
hydrogenated indium oxide films.\textsuperscript{25,30} XPS measurement
was carried out to investigate the valence states of Hf and oxygen
elements in the IHfO:H films prepared with different
H\textsubscript{2}concentration. The significant Hf 4f XPS line and the
element ratio of Hf/In (3.87\selectlanguage{ngerman}±0.04 \%, calculated from the XPS peaks)
similar to the evaporation target indicate effective and similar Hf
doping in all the IHfO:H films (Figure S1). Varying the
H\textsubscript{2} concentration during the IHfO:H film deposition does
not seem to change the doping effect of Hf elements. According to
literature, hydrogen doping enables the replacement of double-electron
donors (oxygen vacancy Vo) for single-electron donors (interstitial
H\textsubscript{i}\textsuperscript{+} or substitutional
H\textsubscript{O}\textsuperscript{+})\textsuperscript{26,31} and
passivation of structural defects,\textsuperscript{32} which may reduce
the scattering intensity and thus improve the Hall mobility of the TCO
films. Thereby, the following discussion will focus on the influence of
the H\textsubscript{2} concentration on the oxygen elements.\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image4/image4}

\end{center}
\end{figure}

Figure 4 The decomposed O 1s XPS lines of the IHfO:H films deposited
with different H\textsubscript{2} concentrations of (a) 0 \%, (b) 0.5
\%, (c) 0.8 \%, (d) 1.2 \%, and (e) 1.5 \%. All the IHfO:H films were
annealed at 200 \selectlanguage{ngerman}°C.

Figure 4 illustrates the O 1s core level peaks of the XPS spectra for
the IHfO:H films deposited with different hydrogen concentrations. The O
1s XPS lines can be decomposed to three peaks of O\textsubscript{A},
O\textsubscript{B}, and O\textsubscript{C}, with the corresponding
binding energies of \textasciitilde{}530.0 eV, \textasciitilde{}531.1
eV, and \textasciitilde{}532.1 eV, respectively. The
O\textsubscript{A}peak with the lowest binding energy of
\textasciitilde{}530.0 eV corresponds to the O\textsuperscript{2-} ions
in the In\textsubscript{2}O\textsubscript{3} lattice. The
O\textsubscript{B}peak at \textasciitilde{}531.1 eV corresponds to the
oxygen vacancy Vo. The tiny O\textsubscript{C} peak at
\textasciitilde{}532.1 eV can be attributed to the hydroxyl bonds
appearing in In(OH)\textsubscript{3} or InOOH.\textsuperscript{27}

It can be seen that, the content of oxygen vacancies
(O\textsubscript{B}peak) in different IHfO:H films shows a slightly
decrease as the H\textsubscript{2} concentration increasing from 0 \% to
0.8 \% and then a rapid increase when the H\textsubscript{2}
concentration rises from 1.2 \% to 1.5 \%. The trend of the oxygen
vacancy content varied with the H\textsubscript{2} concentrations is
similar to that of the carrier concentration as shown in Figure 3, which
demonstrates the influence of H doping on the oxygen vacancy content and
thus the carrier concentration. However, a less than 5 \% change in
oxygen vacancy does not seem to be sufficient to explain the more than
60 \% increase in carrier concentration as the hydrogen concentration
rises from 1.2 \% to 1.5 \%. The contribution of hydrogen as a donor to
the carrier concentration should also be considered. As mentioned above,
hydrogen in TCO films exists in the forms of
H\textsubscript{i}\textsuperscript{+}and
H\textsubscript{o}\textsuperscript{+}. The amount of the interstitial
hydrogen H\textsubscript{i}\textsuperscript{+} can be equated with the
amount of hydroxyl (O\textsubscript{C}peak)\textsuperscript{31} which
exhibits an increase with increasing the hydrogen concentration as
observed by Huang et al.\textsuperscript{27}The sharp rise in the
carrier concentration can also be attributed to the sudden rise in the
interstitial hydrogen content. In addition, the substitutional hydrogen
from the excess hydrogen doping during the deposition would also cause
an increase in the carrier concentration.\textsuperscript{31}\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image5/image5}

\end{center}
\end{figure}

Figure 5 Transmittance in the wavelength range of 400-2300 nm for the
IHfO:H films deposited with H\textsubscript{2} concentrations of 0 \%,
0.5 \%, 0.8 \%, 1.2 \%, and 1.5 \% after post-annealing at 200  in air.

Figure 5 shows the transmittance of the IHfO:H films with different
H\textsubscript{2} concentrations in the wavelength range from 400 nm to
2300 nm. The hydrogen concentration does not significantly affect the
transmittance of the IHfO:H films in the visible region (400-800 nm)
with an average transmittance of \textasciitilde{}87 \%. In the NIR
region (800-1500 nm), the average transmittance is in the range of
\textasciitilde{}85 \% to \textasciitilde{}88 \%, which is much higher
than \textasciitilde{}79 \% for the ITO films with the same
thickness,\textsuperscript{33} thanks to the weaker NIR free carrier
absorption (FCA) effect.\textsuperscript{34} When the hydrogen
concentration is higher than 0.8 \%, the average transmittance of the
IHfO:H films increases slightly in the range of 1500-2300 nm which,
however, is beyond the optical absorption range of crystalline silicon.
Considering the application in crystalline silicon solar cells, it can
be said that the hydrogen doping concentration (0-1.5 \%) hardly effect
the optical properties of the IHfO:H films at an annealing temperature
of 200 .

According~to~above~experimental results and discussion, adding a decent
H\textsubscript{2} gas when depositing IHfO:H films significantly
increases the carrier mobility and thus reduces its sheet resistance,
but hardly influences the film transmittance. Too much hydrogen can lead
to a significant degradation of the electrical properties of the IHfO:H
films. Comprehensive consideration of the optical and electrical
properties, the optimum H\textsubscript{2} concentration is determined
to be 0.8 \%.

3.2 The effect of post-annealing on IHfO:H films

Post-annealing is a conventional treatment to improve the
crystallinity\textsuperscript{28} and to activate the dopants of the TCO
films.\textsuperscript{35} XRD patterns of the IHfO:H films prepared
with 0.8 \% H\textsubscript{2} concentration annealed at 100-250  are
shown in Figure 6. The XRD pattern of an as-deposited sample is
included. Four diffraction peaks of (211), (222), (332), and (444)
belonging to In\textsubscript{2}O\textsubscript{3} can be determined
from the XRD patterns of all the samples. Increasing the annealing
temperature does not affect the dominant orientation of the (222)
crystal plane in the IHfO:H films, however, the FWHM of the (222)
diffraction peak is significantly reduced and the estimated average
grain size increases gradually as depicted in Figure 6. As the annealing
temperatures is above 200 \selectlanguage{ngerman}°C, the average grain size exceeds 50 nm
indicating better crystallinity of the IHfO:H films grown by RPD than
that by magnetron sputtering.\textsuperscript{19,36} It is worth noting
that the as-deposited IHfO:H film is also crystallized in the presence
of hydrogen during the deposition. Nevertheless, the as-deposited sample
without hydrogen doping is amorphous (Figure S2). That means both
post-annealing and hydrogen doping promote the film crystallization.\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image6/image6}

\end{center}
\end{figure}

Figure 6 Normalized XRD patterns of the IHfO:H films annealed at
different temperatures for 20 minutes. A H\textsubscript{2}concentration
of 0.8 \% was adopted during the deposition.

Figure 7 depicts the annealing temperature dependences of the electrical
properties of the IHfO:H films prepared with 0.8 \%
H\textsubscript{2}concentration. The sheet resistance, carrier
concentration, and Hall mobility of the as deposited IHfO:H film are
22.39 \selectlanguage{greek}Ω/\selectlanguage{english}#, \selectlanguage{english}6.11\selectlanguage{ngerman}×10\textsuperscript{20} cm\textsuperscript{-3}, and 41.48
cm\textsuperscript{2}V\textsuperscript{-1}s\textsuperscript{-1},
respectively. When the annealing temperature is lower or equal to 100
°C, no notable changes occur in the electrical properties of the IHfO:H
films. The sheet resistance increases slightly as the annealing
temperature increasing to 150 °C and then rapidly climbs to 44.97 \selectlanguage{greek}Ω/\selectlanguage{english}#
\selectlanguage{english}when the annealing temperature reaches 250 \selectlanguage{ngerman}°C, which is different from
the general observed rule that the sheet resistance of the TCO films
decreases with the increase of the annealing
temperature.\textsuperscript{21,23,25} The following analysis of Hall
mobility and carrier concentration varied with the post-annealing
temperature will help us understand this phenomenon.\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image7/image7}

\end{center}
\end{figure}

Figure 7 Annealing temperature dependences of sheet resistance, carrier
concentration and Hall mobility of the IHfO:H films prepared with 0.8 \%
H\textsubscript{2} concentration.

As can be seen from Figure 7, the Hall mobility of the IHfO:H films
increases rapidly from the as-deposited 41.48
cm\textsuperscript{2}V\textsuperscript{-1}s\textsuperscript{-1} to
102.92
cm\textsuperscript{2}V\textsuperscript{-1}s\textsuperscript{-1}with an
annealing temperature of 200 \selectlanguage{ngerman}°C. However, as the annealing temperature
is keep increasing to 250 °C, the Hall mobility decreases. The annealing
temperature dependence of mobility seems to be consistent with that of
the crystallinity, as shown in Figure 6, which implies the possible
relationship between the rise of the mobility and the reduced grain
boundary scattering.\textsuperscript{29} However, the carrier
concentration does not increase with the annealing temperature, but
shows an opposite tendency as depicted in Figure 7, although it is
generally believed that crystallization could promote the activation of
dopants.\textsuperscript{35} The significant decrease of carrier
concentration with annealing temperature, which actually determines the
change of sheet resistance, represents the reduced concentration of
doping impurity. The weakened ionized impurity scattering and the
improved crystallinity together lead to the improvement of the mobility
of the IHfO:H films. The slight decrease of the mobility and the average
grain size at the annealing temperature of 250 °C are probably related
to the escaping of the hydrogen. \textsuperscript{34,35}\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image8/image8}

\end{center}
\end{figure}

Figure 8 The decomposed O 1s XPS lines of the IHfO:H thin films without
annealing (a) and annealed at (b) 150 \selectlanguage{ngerman}°C, (c) 200 °C, and (d) 250 °C.

The decomposed O 1s XPS lines of the IHfO:H films annealed at different
temperatures are shown in Figure 8. The relative intensities of the
three XPS peaks of O\textsubscript{A}, O\textsubscript{B}, and
O\textsubscript{C} are listed in Table 2. It can be seen that as the
annealing temperature increases to 250 °C, the relative integral area of
the O\textsubscript{B} peak, representing the oxygen vacancies,
gradually decreases from the as-deposited of 13.34 \% to 9.74 \% due to
the filling of the oxygen vacancies by oxygen in the air during the
annealing process, as studied by Meng et al.\textsuperscript{24} With
the same initial Hf and hydrogen doping concentrations, the decrease of
the oxygen vacancies is one of the reasons for the decrease of the
carrier concentration of the IHfO:H films. In addition, hydrogen might
escape during the annealing process as mentioned above, which is another
possible reason for the carrier concentration reducing at high annealing
temperature. Thereby, the excessively rapid decrease in carrier
concentration leads to an increase in the sheet resistance of the IHfO:H
films.\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image9/image9}

\end{center}
\end{figure}

Figure 9 TTe in the wavelength range of 400-2300 nm for IHfO:H films
annealed at different temperatures.

As the annealing temperature increases, both the transmission and
reflection spectra change significantly due to the change in refractive
index caused by the rise in crystallinity (Figure
S3).\textsuperscript{37} In order to eliminate the effect of reflection
on transmission, the effective total transmittance (TTe) spectra are
used instead of the transmission spectra to evaluate the optical
properties of the IHfO:H films annealed at different
temperatures,\textsuperscript{38} as shown in Figure 9. TTe is defined
as \(\text{TTe}=\frac{T}{(1-R)}\), where T is the transmittance and R is the
reflectance. When the annealing temperature is below or equal to 150 \selectlanguage{ngerman}°C,
the TTe of the IHfO:H films remains almost unchanged in the visible
region while slightly increases in the NIR region. After the annealing
temperature increases to 200 °C, the average TTe of the IHfO:H films
increases from 88.54 \% to 91.16 \% in the visible region which can be
related to better crystallization with less defects.\textsuperscript{39}
Meanwhile, the average TTe significantly increased from 77.14 \% to
95.61 \% in the NIR region. According to the Drude model, FCA is
proportional to carrier concentration.\textsuperscript{34} Thereby, the
IHfO:H films annealed at temperature above 200 °C behave higher
transmittance as they have lower carrier concentration as shown in
Figure 7.

Overall, the post-annealing treatment shows a significant impact on the
crystallinity, the electrical properties, and the optical transmission
of the IHfO:H films. Considering the above opto-electronic
characteristics comprehensively, the appropriate annealing temperature
is about 200 °C which is within the temperature tolerance range of the
SHJ solar cells.

3.3 Application of the IHfO:H films on SHJ solar cells\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image10/image10}

\end{center}
\end{figure}

Figure10 (a) The light I-V curves and (b) EQE spectra of the SHJ solar
cells with IHfO:H (Cell 1) or ITO (Cell 2) as the front-side TCO under
optimal conditions.

Finally, a bifacial SHJ solar cell with an area of 274.15
cm\textsuperscript{2} was fabricated using IHfO:H film deposited with a
H\textsubscript{2} concentration of 0.8 \% as the front-side TCO (Cell
I). And a control bifacial SHJ cell with ITO on both sides (Cell II) was
also assembled as a comparison. Post annealing was carried out in air
under a temperature of 200 \selectlanguage{ngerman}°C for 20 minutes for the whole devices. The
light I-V and EQE curves of Cell \selectlanguage{english}I and Cell \selectlanguage{english}II are shown in Figure 10.
The two solar cells do not show significant differences in open circuit
voltage (V\textsubscript{oc}) or FF. The improvement of 0.3 \% in
efficiency (Eff) for Cell \selectlanguage{english}I (25.03 \%) compared with Cell II (24.73 \%)
is mainly brought by the increase of 0.84 mA/cm\textsuperscript{2} in
J\textsubscript{sc}. The significant increase in EQE in the long
wavelength range (\textgreater{}850 nm) indicates reduced FCA for Cell I
using IHfO:H compared with Cell I using ITO as the front-side TCO layer.
The excellent device performance indicates that the IHfO:H films
prepared by RPD have the great application potential in high efficiency
SHJ solar cells.

\textbf{Conclusions}

The IHfO:H films (Hf/In ratio=4 \% in target, \textasciitilde{}3.87+-0.04
\% in the films) with various H\textsubscript{2} concentrations (0-1.5
\%) were prepared at room temperature by a low-damage RPD method,
followed by post annealing in air atmosphere at different temperatures
(100\textasciitilde{}250 degC). Under an annealing temperature of 200 degC,
the hydrogen concentration hardly changes the crystallinity and the
optical properties of the annealed IHfO:H films. The Hall mobility
increases from 58.44
cm\textsuperscript{2}V\textsuperscript{-1}s\textsuperscript{-1} to
102.92 cm\textsuperscript{2}V\textsuperscript{-1}s\textsuperscript{-1}
as the H\textsubscript{2} concentration increases from 0 \% to 0.8 \%
mainly due to the hydrogen doping and the related reduction of the
oxygen vacancy concentration. However, higher H\textsubscript{2}
concentration of above 0.8\% makes the Hall mobility decrease and the
carrier concentration increase, which is probably due to the increasing
of the interstitial and substitutional hydrogen in the IHfO:H films.
Post annealing increases the crystallinity of the IHfO:H films and
reduces their oxygen vacancy, causing Hall mobility to rise from 41.8
cm\textsuperscript{2}V\textsuperscript{-1}s\textsuperscript{-1} to
102.92
cm\textsuperscript{2}V\textsuperscript{-1}s\textsuperscript{-1}and
carrier concentration to decrease from
6.11x10\textsuperscript{20}cm\textsuperscript{-3} to
1.75x10\textsuperscript{20}cm\textsuperscript{-3} after 200 degC annealing
for the IHfO:H films prepared with optimized 0.8\% H\textsubscript{2}
concentration. At meanwhile, the average TTe of the IHfO:H films
increases from 88.54 \% to 91.16 \% in the visible region and from 77.14
\% to 95.61 \% in the NIR region. The significant reduced FCA of the
IHfO:H films leads to the long wavelength response improvement in the
EQE and 0.84 mA/cm\textsuperscript{2} increase in J\textsubscript{sc}
for the SHJ solar cell. An efficiency of over 25\% was achieved on the
SHJ solar cells using IHfO:H films as the front-side TCO layer.

\textbf{Acknowledgements}

This work was supported by the State Key Program of the National Natural
Science Foundation of China (No. 62034001), the Fundamental Research
Funds for the Central Universities (No. E0E48919X2 and E1E41804X2),
Weiqiao-UCAS Special Projects on Low-Carbon Technology Development (No.
GYY-DTFZ-2022-019), and the International Partnership Program of the
Chinese Academy of Sciences (211211KYSB20180020).

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\end{enumerate}

Table 1

Relative intensities of the three XPS peaks of O\textsubscript{A},
O\textsubscript{B}, and O\textsubscript{C} obtained by integrating the
peak area of the IHfO:H films with different
H\textsubscript{2}concentrations.\selectlanguage{english}
\begin{longtable}[]{@{}llll@{}}
\toprule
H\textsubscript{2} concentration {[}\%{]} & O\textsubscript{A} {[}\%{]}
& O\textsubscript{B} {[}\%{]} & O\textsubscript{C}
{[}\%{]}\tabularnewline
\midrule
\endhead
0 & 83.19 & 10.81 & 6.01\tabularnewline
0.5 & 83.03 & 10.96 & 6.02\tabularnewline
0.8 & 83.28 & 10.10 & 6.61\tabularnewline
1.2 & 83.17 & 10.17 & 6.66\tabularnewline
1.5 & 81.52 & 10.67 & 7.81\tabularnewline
\bottomrule
\end{longtable}

Table 2

Relative intensities of the integral areas of the three XPS peaks of
O\textsubscript{A}, O\textsubscript{B}, and O\textsubscript{C} in the
IHfO:H films annealed at different temperature.\selectlanguage{english}
\begin{longtable}[]{@{}llll@{}}
\toprule
Annealing temperature {[}\selectlanguage{ngerman}°C{]} & O\textsubscript{A} {[}\%{]} &
O\textsubscript{B} {[}\%{]} & O\textsubscript{C} {[}\%{]}\tabularnewline
\midrule
\endhead
As-deposited & 80.32 & 13.34 & 6.33\tabularnewline
150 & 80.16 & 12.29 & 6.55\tabularnewline
200 & 83.28 & 10.10 & 6.61\tabularnewline
250 & 80.68 & 9.74 & 6.57\tabularnewline
\bottomrule
\end{longtable}\selectlanguage{english}
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\end{center}
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