Nanocrystalline silicon carbide films for solar cells
Nanocrystalline silicon carbide (nc-SiC) films as protective coating and as solar cell material for a harsh environment, high temperatures, light intensities and radiation, were investigated. p- and n-types 100-mm silicon wafers with (100) orientation were used as substrates for SiC films deposition...
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irk-123456789-1215992017-06-15T03:04:17Z Nanocrystalline silicon carbide films for solar cells Vlaskina, S.I. Mishinova, V.I. Rodionov, V.E. Svechnikov, G.S. Nanocrystalline silicon carbide (nc-SiC) films as protective coating and as solar cell material for a harsh environment, high temperatures, light intensities and radiation, were investigated. p- and n-types 100-mm silicon wafers with (100) orientation were used as substrates for SiC films deposition. The films were deposited using HighFrequency Plasma Enhanced Chemical Vapor Deposition (HF-PECVD) with CH₃SiCl₃ gas as a silicon and carbon source. Hydrogen supplied CH₃SiCl₃ molecules in the field of HF discharge. Deposition was carried out on a cold substrate. The power density was 12.7 W/cm². Deposition conditions were explored to prepare films with a controlled band gap and a low defect density. Formation of nc-3C-SiC films has been confirmed by the high resolution-transmission electron microscopy analysis, optical band gap values ETauc, conductivity, charge carrier activation energy and Hall measurements. The efficiency of photoconductivity was calculated for evaluating the photoconductivity properties and for the correlations with technology. For p-n junction creation in solar cell fabrication, the ntypes nc-SiC films were doped with Al. Employing Al as a doping material of nc-n-SiC, the open-circuit voltage as high as 1.43 V has been achieved. 2016 Article Nanocrystalline silicon carbide films for solar cells / S.I. Vlaskina, G.N. Mishinova, V.I. Vlaskin, V.E. Rodionov, G.S. Svechnikov // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2016. — Т. 19, № 3. — С. 273-278. — Бібліогр.: 6 назв. — англ. 1560-8034 DOI: 10.15407/spqeo19.03.273 PACS 64.70.K-,77.84.Bw, 81.30.-t http://dspace.nbuv.gov.ua/handle/123456789/121599 en Semiconductor Physics Quantum Electronics & Optoelectronics Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
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Nanocrystalline silicon carbide (nc-SiC) films as protective coating and as solar cell material for a harsh environment, high temperatures, light intensities and radiation, were investigated. p- and n-types 100-mm silicon wafers with (100) orientation were used as substrates for SiC films deposition. The films were deposited using HighFrequency Plasma Enhanced Chemical Vapor Deposition (HF-PECVD) with CH₃SiCl₃ gas as a silicon and carbon source. Hydrogen supplied CH₃SiCl₃ molecules in the field of HF discharge. Deposition was carried out on a cold substrate. The power density was 12.7 W/cm². Deposition conditions were explored to prepare films with a controlled band gap and a low defect density. Formation of nc-3C-SiC films has been confirmed by the high resolution-transmission electron microscopy analysis, optical band gap values ETauc, conductivity, charge carrier activation energy and Hall measurements. The efficiency of photoconductivity was calculated for evaluating the photoconductivity properties and for the correlations with technology. For p-n junction creation in solar cell fabrication, the ntypes nc-SiC films were doped with Al. Employing Al as a doping material of nc-n-SiC, the open-circuit voltage as high as 1.43 V has been achieved. |
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Vlaskina, S.I. Mishinova, V.I. Rodionov, V.E. Svechnikov, G.S. |
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Vlaskina, S.I. Mishinova, V.I. Rodionov, V.E. Svechnikov, G.S. Nanocrystalline silicon carbide films for solar cells Semiconductor Physics Quantum Electronics & Optoelectronics |
| author_facet |
Vlaskina, S.I. Mishinova, V.I. Rodionov, V.E. Svechnikov, G.S. |
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Vlaskina, S.I. |
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Nanocrystalline silicon carbide films for solar cells |
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Nanocrystalline silicon carbide films for solar cells |
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Nanocrystalline silicon carbide films for solar cells |
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Nanocrystalline silicon carbide films for solar cells |
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Nanocrystalline silicon carbide films for solar cells |
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nanocrystalline silicon carbide films for solar cells |
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Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
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2016 |
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Nanocrystalline silicon carbide films for solar cells / S.I. Vlaskina, G.N. Mishinova, V.I. Vlaskin, V.E. Rodionov, G.S. Svechnikov // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2016. — Т. 19, № 3. — С. 273-278. — Бібліогр.: 6 назв. — англ. |
| series |
Semiconductor Physics Quantum Electronics & Optoelectronics |
| work_keys_str_mv |
AT vlaskinasi nanocrystallinesiliconcarbidefilmsforsolarcells AT mishinovavi nanocrystallinesiliconcarbidefilmsforsolarcells AT rodionovve nanocrystallinesiliconcarbidefilmsforsolarcells AT svechnikovgs nanocrystallinesiliconcarbidefilmsforsolarcells |
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2025-07-08T20:11:56Z |
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Semiconductor Physics, Quantum Electronics & Optoelectronics, 2016. V. 19, N 3. P. 273-278.
doi: 10.15407/spqeo19.03.273
© 2016, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
273
PACS 64.70.K-,77.84.Bw, 81.30.-t
Nanocrystalline silicon carbide films for solar cells
S.I. Vlaskina1, G.N. Mishinova1, V.I. Vlaskin1,2, V.E. Rodionov1, G.S. Svechnikov3
1V. Lashkaryov Institute of Semiconductor Physics, NAS of Ukraine,
41, prospect Nauky, 03028 Kyiv, Ukraine; e-mail: businkaa@mail.ru
2Sensartech, 2540 Lobelia Dr., Oxnard, 93036 California, USA
3National Technical University of Ukraine, Peremohy Ave, 37, Kiev, Ukraine
Abstract. Nanocrystalline silicon carbide (nc-SiC) films as protective coating and as
solar cell material for a harsh environment, high temperatures, light intensities and
radiation, were investigated. p- and n-types 100-mm silicon wafers with (100) orientation
were used as substrates for SiC films deposition. The films were deposited using High-
Frequency Plasma Enhanced Chemical Vapor Deposition (HF-PECVD) with CH3SiCl3
gas as a silicon and carbon source. Hydrogen supplied CH3SiCl3 molecules in the field of
HF discharge. Deposition was carried out on a cold substrate. The power density was
12.7 W/cm2. Deposition conditions were explored to prepare films with a controlled band
gap and a low defect density. Formation of nc-3C-SiC films has been confirmed by the
high resolution-transmission electron microscopy analysis, optical band gap values ETauc,
conductivity, charge carrier activation energy and Hall measurements. The efficiency of
photoconductivity was calculated for evaluating the photoconductivity properties and for
the correlations with technology. For p-n junction creation in solar cell fabrication, the n-
types nc-SiC films were doped with Al. Employing Al as a doping material of nc-n-SiC,
the open-circuit voltage as high as 1.43 V has been achieved.
Keywords: silicon carbide, nanocrystalline film, photoconductivity, solar cell.
Manuscript received 14.03.16; revised version received 12.07.16; accepted for
publication 13.09.16; published online 04.10.16.
1. Introduction
SiC materials are extremely hard, very inert, and have
high thermal conductivity. Their properties such as the
breakdown electric field, saturated drift velocity, and
impurity ionization energies are unique for different
polytypes. β-SiC possesses the smallest band gap
(~2.4 eV) and has the highest electron carrier mobility as
compared with that of α-SiC, which makes it an
important SiC material in the microelectronics industry
[1-3]. In the tandem SiC/Si solar cell β-SiC is an ideal
top cell due to wide band gap. The SiC upper cell most
efficiently converts the shorter wavelength light into the
useful current, while the Si lower cell absorbs red and
near-infrared light [1]. To prepare films with a
controlled band gap and low defect density, it is
necessary to investigate different structural, electro-
physical and optical properties of films. Because of these
excellent properties, SiC is a perfect material in the
electronics industry, with a wide application in the areas
of high-temperature, high-power, high-frequency, and
optoelectronic devices [2].
This paper presents the results of investigations of
nanocrystalline SiC films obtained using the HF-PECVD
method to allow making SiC solar cells at low
temperatures with higher open circuit voltages on large
substrates.
2. Experiment and discussion
In this paper, the plasma–enhanced chemical-vapor
deposition method (High-Frequency Plasma Enhanced
Chemical Vapor Deposition HF-PECVD) was used to
fabricate the nanocrystalline (nc-SiC) films.
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2016. V. 19, N 3. P. 273-278.
doi: 10.15407/spqeo19.03.273
© 2016, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
274
Methyltrichlorosilane (MTS, CH3SiCl3) was used as a
source precursor, because it has an equivalent ratio of Si
to C and is decomposed at a low temperature in a high-
frequency (40 MHz and 13.56 MHz) electric field with a
power density (0.5…12.7) W/cm2. nc-SiC films were
deposited on the Si (100 mm), glass, ceramic and metal
substrates at the temperatures 20 to 1000 °C. Hydrogen
carried out the role both of a gas carrier, which supplied
CH3SiCl3 molecules in the field of the HF discharge, and
regulator of the mixture concentration of MTS in the
carrier gas. The dc bias voltage (200…600) V during
precipitation was supplied to substrate for increasing the
drift of charged particles near the substrate surface.
Deposition of SiC films results in solely cubic nc-SiC
with average grain sizes of several tens of nanometers,
as it is determined by XRD measurements. The
stoichiometry of the deposited film was, therefore,
continuously controlled using the Raman measurements.
The steady-state electron photoconductivity is
given by:
ημτμph eGen ==σ .
Here, n is the photocarrier concentration, η – the
quantum efficiency, μ and τ are the electron mobility and
lifetime, respectively, G is the volume generation rate of
carriers.
( ) ( )[ ] ddRFG α−−−= exp11 ,
where F is the flux of incident photons, α – absorption
coefficient, R – reflectivity, and d – sample thickness.
To improve the efficiency, it is necessary to choose
parameters of deposition, which will increase electron
mobility. Hall measurements showed that the films
deposited from CH3SiCl3 were characterized by
sufficiently high values of the free carrier mobility and
that specially undoped films possess n-type conductivity.
The free carrier mobility in SiC-films deposited from
CH4+SiH4 mixture was significantly lower. Fig. 1 shows
the temperature dependence of the free electron
concentration in films grown by using CH3SiCl3. Hall
measurements were performed with SiC films deposited
on p-Si.
The figure below shows that the concentration of
electrons at room temperature for different samples
varies within the small range (2.7…4.5).1017 cm–3.
The conductivity of nc-SiC is determined by the
nitrogen impurity ionization. Nitrogen enters together
with carrying out gas into the chamber by CH3SiCl3
decomposition during growth of single β-SiC crystals.
Nitrogen is a shallow donor impurity with the ionization
energy ΔEN = 0.05 eV.
The temperature dependence of the Hall mobility
shows a clear distinction between values of mobility
caused by the bias voltage applied to the substrate during
film growth (Fig. 2). These electrical properties of the
films obtained within the temperature range
200…600 °C are shown in Table. Formation of nc-SiC
at the temperature 200 °C is confirmed by obtained
electrophysical and X-ray data [4-6].
Formation of nc-SiC films has been confirmed not
only by high resolution-transmission electron
microscopy analysis but by optical band gap
measurements. The optical band gap values Eg were
measured using the Tauc optical method. According to
Tauc’s model, the optical band gap was obtained from
the plot by linear extrapolation to zero.
Table. Electrical properties of SiC films.
N Structure Ubias,
V
Tsubst.,
°C
Sisubst.
(hkl) n (cm–3) μ,
cm2V–1s–1
1 –600 920 (100) 2.4.1017 40
2 –600 920 (111) 3.7.1017 25
3 –400 620 (111) 2.4.1019 12
4
Poly-
crystalline
–600 500 (100) 1.2.1017 200
5 Nano-
crystalline –200 200 (100) 3.3.1017 190
Fig. 1. Temperature dependence of the free electron
concentration in films grown by using CH3SiCl3: Ubias =
+400 V (1), +200 V (2), –100 V (3), –600 V (4).
Fig. 2. Temperature dependence of the Hall mobility in SiC
films: Ubias = +400 V (1), +200 V (2), –100 V (3), –600 V (4).
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2016. V. 19, N 3. P. 273-278.
doi: 10.15407/spqeo19.03.273
© 2016, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
275
(αhν)1/2 = B(hν – Eg).
Here, α is the absorption coefficient Eg is the optical gap,
and B is the constant for the given sample that
characterizes the degree of order. To obtain Eg we
measured the spectral dependence of the absorption
coefficient and plotted the function (αhν)1/2 vs hν. Then,
extrapolation of the linear section of the curve to zero
gives Eg. The thickness of nc-SiC films was 1 μm. The
calculation of Eg was performed as follows. The
reflection from the silicon substrate and then from the
film SiC was recorded (Fig. 3).
The absorption coefficient α was calculated using
the formula
I = I0 exp (–αd),
where I is the intensity of light reflected from the nc-
SiC film, and I0 – intensity of light reflected from the
substrate. The magnitude d was taken to be 2 μm, since
the light passed twice through the amorphous film.
Fig. 4 shows that for the films deposited from
CH4+SiH4 mixture the results of Eg calculations are
equal Eg = 2.55±0.05 eV. Measurements of the
stoichiometric composition of this sample were carried
out using an Auger spectrometer showed that the Si:C
ratio is 1:1.5. This result shows that the stoichiometry
of Si:C is changed from 1:1 to 1:1.5 by increasing
carbon atom concentration, which leads to formation of
the hexagonal polytypes of SiC films with a high Eg
value. Cubic SiC films with stoichiometric composition
Si:C ratio 1:1 deposited from CH3SiCl3 showed Eg =
2.30±0.05 eV (β-SiC).
Raman spectra of nanocrystalline films (Fig. 5)
consist of a broad band with a peak at 800 cm–1,
corresponding to the maximum density of phonon states.
The bright line with the frequency of 775 cm–1 is
observed on the background of this broad band. The
appearance of this line is also indicative of nanocrystal’
occurance. Local heating the silicon substrate occurs
with the bombardment of the silicon substrate with high-
energy electrons, which leads to the growth of
nanocrystals. Decreasing the substrate temperature down
to the room one with increasing the plasma power
should enhance photoconductivity.
The efficiency of photoconductivity was calculated
for evaluating the photoconductivity properties and for
the correlations with technology. Neff is a very suitable
value for evaluating the photoconductivity properties of
films, because there are no much difficulties in its
measurement. In fact, it plays the role of the quantum
photocurrent yield because Neff points out how many
electrons participating in the photoconductivity are
generated per 1 s by 100 photons of the full incident
light focused flux on the film area 1 cm2. The parameters
of photoconductivity depend on each other, and it is very
difficult to measure them separately. The spectral
dependence of the photocurrent (difference between the
light and dark current) for SiC film is shown in Fig. 6.
Fig. 3. Reflection from nc-SiC film (1) and from silicon
substrate (2).
Fig. 4. Definition of Eg according to Tauc’s formula.
Fig. 5. Raman spectra of SiC film.
Fig. 6. The spectral dependence of photocurrent for SiC
samples (1, 2, 3, 4).
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2016. V. 19, N 3. P. 273-278.
doi: 10.15407/spqeo19.03.273
© 2016, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
276
Fig. 7. Efficiency of photoelectron yield for some SiC samples.
To quantitatively characterize the incident light
flux, it should be normalized to the density of photons
per 1 cm2; then Neff is related to 100 photons of such a
normalized light flux. In this case, expression for the
photoconductivity may be rewritten as:
100μ JNe effp =σ ,
then Neff can be calculated for the full spectral range
(Fig. 7).
The maximum of Neff occurs at λ = 540 nm
(2.3 eV), which coincides with the band gap. The large
halfwidth of this band is a positive peculiarity of SiC
films, because in optoelectronic devices using these
films photoelectrons are generated in the broad spectrum
range. A small peak is located in 900…1000-nm region
(~1.2 eV) and is caused by the network of defects. Thus,
Neff measurements allowed selecting these technological
parameters, which provides the highest open-circuit
voltage in the manufactured solar cell.
Boron and aluminum were tried to create a p-layer
in the nc-SiC film. More attention was paid to the
development of p-n junction in films obtained from
CH3SiCl3, since those films had better optical and
electro-physical parameters for solar cells. But Boron
doped SiC films showed too low value Voc. Boron-doped
SiC films were widely used in the development of
optical windows in the SiC-Si solar cell, but open-circuit
voltage values for Boron-doped SiC film were less than
1.04 V [3].
The highest Voc =1.5 V was demonstrated by
NASA Glenn Research Center, but on a small area
(0.48 cm2) SiC epilayers grew at a very high
temperature. This result was obtained for n-types SiC
films doped with Al. Employing Al as a doping material
of SiC films gives Voc = 1.43 V.
Fig. 8. Low Temperature Photoluminescence Spectra (LTPLS) according to the structural imperfection and impurity
concentration in nc-SiC crystals. Zero phonon parts: SF1 – (2.853-2.793) eV, DL1 – (2.73-2.625) eV, GB – (2.95-2.89) eV.
Y-coordinate: most pure films – n ~ (1…5).1016 cm–3, lightly doped films – n ~ (5…8).1016 cm–3, samples with only
DL spectra – n ~ (2…7).1017 cm–3; X-coordinate: (δ-0) – perfect nanocrystal, (δ-I) – the disorientation between the
layers-blocks of the nanocrystal, (δ-II) –an increased one-dimensional disorder along the hexagonal axis c.
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2016. V. 19, N 3. P. 273-278.
doi: 10.15407/spqeo19.03.273
© 2016, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
277
Taking into account the results of the publications
in the present study, p-n junction was prepared using Al
for doping the SiC films. The Al doped SiC films were
heated to 600 °C despite the facts that the films were
deposited on the substrate at T = 200 °C at the power of
40 to 70 W, or on a cold substrate at the power 1000 W
(with decomposition of CH3SiCl3). The contacts were
made by sequential deposition of various metal layers at
a high temperature, too. In this case, phase
transformations of a cubic SiC to the hexagonal SiC
were observed in nanocrystals. The ability to produce
device-quality SiC is limited by inherent nanocrystalline
defects associated with SiC polytypism and their
associated electronic effects.
Fig. 8 shows LTPL spectra in films according to
structural imperfection and the impurity concentration of
nc-SiC.
The complex spectra were decomposed into similar
structure-constituting spectra shifted against each other
on the energy scale. These SFi type and DLi type spectra
are indicative of nanocrystals in films, namely:
i = 1 – SiC-14H1 〈4334〉,
i = 2 – SiC-10H2 〈55〉,
i = 3 – SiC-14H2 〈77〉,
i = 4 – SiC (N/A), probably – SiC-28H〈1414〉, the SF4
spectrum is difficult to determine. SF4 corresponds to the
unknown polytypes with lower percentage of
hexagonality (up to 7%).
i = 5 – SiC 33R 〈(3332)3〉,
i = 6 – SiC 8H 〈44〉.
Formation of a new nano-phase is indicator of
forming the corresponding motif.
Fig. 9. The binary tetrahedral structures of nc-SiC.
Perfect nanocrystal shows a typical spectrum of
nitrogen bound exciton complexes (PRS) together with
the linear ABC-spectrum related to Ti [(δ-0) – (a)] and
emission spectra of the donor-acceptor pairs. Another
spectrum with zero-phonon line (2.89…2.94 eV) was
found after identifying the SF [4] and DL spectra [5, 6].
GB spectra were observed simultaneously with the SF and
DL ones (Figs. 8a and 8b) in impurity cases. Zero-phonon
part of the GB spectra has a clear fine structure in the case
of low films doping. GB spectrum manifests through
interaction with phonons: TA-46, LA-77, TO-95, LO-104
at temperatures (4.2 – 40 K). At higher temperatures, there
is a synchronous thermal decay of all the elements of the
fine structure. Presumably, GB spectra display the border
nanocrystalline block or interconnect boundaries. In Fig.
9, transformation of the cubic structure (ABCABC) to the
hexagonal one (ABABAB) in nc-SiC films is shown.
Shockley Partial Dislocations with Burger’s vector bS =
1/6 〈112〉, | bS | = 1.788 Å as well as Frank Partial
Dislocation with Burger’s vector bF = 1/3 〈111〉, | bF | =
2.52 Å participate in transformations.
The nc-SiC without polytype transformation
(perfect crystal) were recommended for the manufacture
of solar cells, because any phase transformations
worsened values of short circuit current density and open
circuit voltage were observed.
The short-circuit current density Jsc and open
circuit voltage Voc on solar cells made on our
nanocrystalline films were less than those for single
crystals SiC. Namely, in the best case it was
9.78 mA/cm2 and 1.43 V, fill factor 0.71 in the case of
optimized deposition conditions. Jsc is not so good as in
[1] (Joc = 36.7 mA/cm2), but Voc is higher than 0.668V.
3. Conclusion
Films deposited using HF-PECVD with CH3SiCl3 gas as
silicon and carbon source have better advantages than
those deposited using CH4 and SiH4. Complex
investigations of structural, electro-physical and optical
properties allow choosing these technological
parameters, which are provided by deposition films on
large substrates (100 mm) at low temperatures (room
temperature).
Deeply understanding parameters of deposition and
properties of the layers allow achieving higher open
circuit voltage in SiC solar cell. The open-circuit voltage
as high as 1.43 V has been achieved for Al doped nc-
SiC. This work explores the potential possibility of
producing the large area solar cells based on SiC for
harsh environment, high temperature, light intensities
and radiation applications.
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