Effect of magnetic field on the reconstruction of the defect-impurity state and сathodoluminescence in Si/SiO₂ structure
Impurity states in Si/SiO₂ structure have been studied using cathodoluminescence (CL). It has been found that intrinsic structure defects in Si/SiO2 are sensitive to the action of magnetic field, which can be revealed due to changes in Si/SiO₂ optical properties. The most sensitive to magnetic...
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| Цитувати: | Effect of magnetic field on the reconstruction of the defect-impurity state and сathodoluminescence in Si/SiO₂ structure / L.P. Steblenko, O.V. Koplak, I.I. Syvorotka, V.S. Kravchenko // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2011. — Т. 14, № 3. — С. 334-338. — Бібліогр.: 20 назв. — англ. |
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Steblenko, L.P. Koplak, O.V. Syvorotka, I.I. Kravchenko, V.S. 2017-05-26T16:01:06Z 2017-05-26T16:01:06Z 2011 Effect of magnetic field on the reconstruction of the defect-impurity state and сathodoluminescence in Si/SiO₂ structure / L.P. Steblenko, O.V. Koplak, I.I. Syvorotka, V.S. Kravchenko // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2011. — Т. 14, № 3. — С. 334-338. — Бібліогр.: 20 назв. — англ. 1560-8034 PACS 07.57.-c, 61.43.Dq, 61.72.Dd, 68.35.Dv, 78.60.Hk, 78.66.-w https://nasplib.isofts.kiev.ua/handle/123456789/117754 Impurity states in Si/SiO₂ structure have been studied using cathodoluminescence (CL). It has been found that intrinsic structure defects in Si/SiO2 are sensitive to the action of magnetic field, which can be revealed due to changes in Si/SiO₂ optical properties. The most sensitive to magnetic field (about 35 per cent) is the intensity of the 1.9 eV CL band attributed to non-bridge oxygen atoms. en Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України Semiconductor Physics Quantum Electronics & Optoelectronics Effect of magnetic field on the reconstruction of the defect-impurity state and сathodoluminescence in Si/SiO₂ structure Article published earlier |
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| title |
Effect of magnetic field on the reconstruction of the defect-impurity state and сathodoluminescence in Si/SiO₂ structure |
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Effect of magnetic field on the reconstruction of the defect-impurity state and сathodoluminescence in Si/SiO₂ structure Steblenko, L.P. Koplak, O.V. Syvorotka, I.I. Kravchenko, V.S. |
| title_short |
Effect of magnetic field on the reconstruction of the defect-impurity state and сathodoluminescence in Si/SiO₂ structure |
| title_full |
Effect of magnetic field on the reconstruction of the defect-impurity state and сathodoluminescence in Si/SiO₂ structure |
| title_fullStr |
Effect of magnetic field on the reconstruction of the defect-impurity state and сathodoluminescence in Si/SiO₂ structure |
| title_full_unstemmed |
Effect of magnetic field on the reconstruction of the defect-impurity state and сathodoluminescence in Si/SiO₂ structure |
| title_sort |
effect of magnetic field on the reconstruction of the defect-impurity state and сathodoluminescence in si/sio₂ structure |
| author |
Steblenko, L.P. Koplak, O.V. Syvorotka, I.I. Kravchenko, V.S. |
| author_facet |
Steblenko, L.P. Koplak, O.V. Syvorotka, I.I. Kravchenko, V.S. |
| publishDate |
2011 |
| language |
English |
| container_title |
Semiconductor Physics Quantum Electronics & Optoelectronics |
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Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
| format |
Article |
| description |
Impurity states in Si/SiO₂ structure have been studied using
cathodoluminescence (CL). It has been found that intrinsic structure defects in Si/SiO2
are sensitive to the action of magnetic field, which can be revealed due to changes in
Si/SiO₂ optical properties. The most sensitive to magnetic field (about 35 per cent) is the
intensity of the 1.9 eV CL band attributed to non-bridge oxygen atoms.
|
| issn |
1560-8034 |
| url |
https://nasplib.isofts.kiev.ua/handle/123456789/117754 |
| citation_txt |
Effect of magnetic field on the reconstruction of the defect-impurity state and сathodoluminescence in Si/SiO₂ structure / L.P. Steblenko, O.V. Koplak, I.I. Syvorotka, V.S. Kravchenko // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2011. — Т. 14, № 3. — С. 334-338. — Бібліогр.: 20 назв. — англ. |
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| fulltext |
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2011. V. 14, N 3. P. 334-338.
PACS 07.57.-c, 61.43.Dq, 61.72.Dd, 68.35.Dv, 78.60.Hk, 78.66.-w
Effect of magnetic field on the reconstruction of the defect-impurity
state and сathodoluminescence in Si/SiO2 structure
L.P. Steblenko1, O.V. Koplak2, I.I. Syvorotka3, V.S. Kravchenko1
1Taras Shevchenko Kyiv National University, Department of Physics,
64, Volodymyrs’ka str., 01601 Kyiv, Ukraine,
2Research and Training Center “Physical and Chemical Materials Science”
under Taras Shevchenko Kyiv National University and NAS of Ukraine
64, Volodimirska str., 01033 Kyiv, Ukraine, е-mail: o.koplak@gmail.com
3Scientific Research Company “CARAT”, 202, Stryis’ka str., 79031 Lviv, Ukraine
Abstract. Impurity states in Si/SiO2 structure have been studied using
cathodoluminescence (CL). It has been found that intrinsic structure defects in Si/SiO2
are sensitive to the action of magnetic field, which can be revealed due to changes in
Si/SiO2 optical properties. The most sensitive to magnetic field (about 35 per cent) is the
intensity of the 1.9 eV CL band attributed to non-bridge oxygen atoms.
Keywords: silicon, defects, magnetic field, cathodoluminescence.
Manuscript received 30.12.10; accepted for publication 14.09.11; published online 21.09.11.
1. Introduction
The Si/SiO2 system is a basis of modern
microelectronics. The growth of thermal oxide on the
silicon surface is accompanied by occurrence of a
number of diverse physico-chemical processes, nature of
which has not been elucidated yet. Nevertheless, the
physical properties of the formed phase boundary, which
determine the parameters of planar devices, are
reflection of the oxide film structure [1]. One of the most
informative methods for diagnostics of structural defects
and impurities in thermal oxide films on silicon is the
cathodoluminescence (CL) [2]. As indicated in [2], CL
using a focused beam of high-energy electrons for
luminescence excitation has a number of advantages
over photoluminescence. First of all, high energy of
electrons (1 keV and higher) provides excitation of all
luminescence centers present in the oxide. Secondly,
there is a possibility to obtain spectra from different
depths of the film, since the penetration depth is a
function of electron energy [3]. At the energy of 1 keV
electrons penetrate SiO2 into a depth of 200 Å.
The CL spectra of thermal oxide films on silicon
are determined by the type of substrate and the film
formation conditions [2, 4]. Nowadays, for efficient
application of Si/SiO2 systems in optoelectronics, used
are various techniques of silicon dioxide modification.
The authors of [4] have found a high-power-electron-
beam-induced modification of silicon dioxide, which
consists in appearance of additional CL bands attributed
to structural defects, specifically, to Si clusters. In this
case, the source for formation of Si clusters is SiO2
irradiated by electrons. According to [4], Si clusters
appear as a result of irradiation and local heating-up of
silicon dioxide by electron beam, which cause changes
in the cathodoluminescent properties of microvolume.
The authors of [5] have found that CL bands in the green
spectral region (2.0–2.5 eV) are observed when the
energy transferred to a unit volume (e.g., under action of
electron beam) exceeds certain threshold. In [5] it is
shown that irradiation by electrons creates interstices,
which are present in silicate systems, free Si
nanoclusters. The authors of [5] suppose that appearance
of green luminescence in this case can be related to
Si/SiO2 phase boundary. In literature, there is also
evidence for the effect of electric field on the charge
state of ion-implanted Si/SiO2 structures [6]. The work
[7] reports a change in the intensity of the 2.8 eV CL
band in nanocomposit glass after treatment of initial
samples in electric field. Taking into account the
importance of the problem related to the structure of
silicon dioxide, in our opinion, it is worthwhile
searching for and developing the other methods of its
modification.
In recent years, the researchers’ attention has been
attracted by the possibility of modification of the
© 2011, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
334
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2011. V. 14, N 3. P. 334-338.
structure and the structure-dependent, e.g., optical
properties of non-magnetic materials and structures
based on them by using weak (B ≤ 1 T) magnetic fields
[8-11]. In this relation, the aim of this work was to study
the changes in the cathodoluminescent properties of
amorphous silicon dioxide grown on silicon under action
of weak constant magnetic field.
2. Experimental
Experimental samples were Si/SiO2 structures obtained
by thermal oxidation of p-Si(111) boron-doped single-
crystal silicon wafers in dry oxygen atmosphere at
1050 °C. The thickness of SiO2 oxide layer was
measured ellipsometrically and comprised 250 nm. As-
grown samples were then stored under room conditions
for a year. Cathodoluminescence of Si/SiO2 structures
was studied in a vacuum cryostat ( ) at liquid
nitrogen temperature. The experimental setup is shown
in Fig. 1.
Pa10 4−=P
© 2011, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
Cathodoluminescence of the samples was excited
by electron gun pulses. The parameters of electron beam
were as follows: electron energy 10 keV, beam current
100 μA, pulse duration 2 μs, repetition rate 30 Hz. The
electron beam was focused on the sample surface into a
round spot 1 mm in diameter. The luminescence spectra
were recorded using the diffraction grating
monochromator DMR-4 and detected by a
photomultiplier tube of type within the
spectral region 1.0 to 5.0 eV. Magnetic treatment (MT)
was carried out by exposing the Si/SiO
106FEU −
2 structures to a
weak constant magnetic field with an induction
B = 0.17 T for t1MT = 7 days and t2MT = 15 days. Studied
in this work was a relative effect of magnetic field on the
CL spectra. The CL spectra of Si/SiO2 structures were
measured in the identical conditions (energy of electrons
in the beam, current value, pulse duration, etc.) at the
same temperature.
Fig. 1. Experimental setup for studying cathodoluminescence
of Si/SiO2 structure: 1 – electron gun power supply; 2 – pulsed
generator; 3 – electron gun; 4 – Si/SiO2 sample; 5 – cryostat;
6 – monochromator; 7 – photomultiplier tube; 8 – PM tube
power supply; 9 – preamplifier; 10 – roughing-down pump;
11 – recording device; 12 – lock-in amplifier.
3. Results and discussion
The results of CL study in Si/SiO2 structures are
presented in Fig. 2 ca − . The CL spectra of the samples
after MT for both MT durations used are similar in their
shape to the spectra of the reference samples, they are
well reproducible and consist of 6 bands, too. The CL
bands of Si/SiO2 structure after action of magnetic field
showed, in general, the same peak positions as for the
reference samples and were well described by Gaussian
shapes, although their intensities were different (Fig. 2c).
1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.
-0.1
0.0
0.1
0.2
0.3
0.4
0.5
0.6
0
In
te
ns
ity
, a
.u
.
E,eV а
1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0
-0.05
0.00
0.05
0.10
0.15
0.20
0.25
0.30
0.35
0.40
In
te
ns
ity
, a
.u
.
E,eV b
1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0
0.0
0.1
0.2
0.3
0.4
0.5
0.6
after MT
before MT
E, eV
In
te
ns
ity
, a
.u
.
с
Fig. 2. Cathodoluminescence spectra of Cz-р-Si/SiO2 structure:
a – before magnetic treatment (MT), b – after MT (B = 0.17 T
for tMT = 15 days), c –CL spectra before and after MT.
335
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2011. V. 14, N 3. P. 334-338.
Identification of the bands in the CL spectra was
carried out by comparing them with the respective bands
taken from literature. In this work, we have identified
the intrinsic-defect-related bands with the peaks at
1.90 ± 0.05, 2.65 ± 0.10 and 4.40 ± 0.07 eV in the
reference samples. These bands were well approximated
by Gaussian shapes with the half-widths of 0.14 ± 0.02,
0.17 ± 0.01 and 0.29 ± 0.01 eV, respectively (Fig. 2a).
It is suggested in [2, 6, 12] that the red emission
band at 1.9 eV may be related to excitation of non-
bridge oxygen atom. Non-bridge oxygen produces a
luminescence band with the peak at 1.9 eV which
corresponds to absorption bands at 2.0 and 4.75 eV.
So, red emission with the peak at 1.9 eV excited
within absorption bands at 2.0 and 4.75 eV is attributed
to the centers related to defects of silicon-oxygen
tetrahedron (i. e., non-bridge oxygen). As noted in [12],
the emission band that corresponds to a 4.75-eV
absorption band may be caused by the presence of
hydroxyl impurity. The centers of red luminescence are
non-bridge oxygen atoms ( ), i. e., oxygen radicals 0
1O
© 2011, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
)( ) ( OSiO
|
,OSi
|
30 −≡−−
which are formed on the breakage of oxygen-hydrogen
bonds in hydroxyl groups. The neutral center of a free
radical of non-bridge oxygen atom ( ) is an
elementary intrinsic defect in glassy silica. In the
crystalline state (the long range ordering), this kind of
defects cannot be stabilized [12]. Therefore, the
luminescence band peaked at 1.9 eV and excited at
4.75 eV is identified as that related to non-bridge
oxygen.
0
1O
According to [4, 5], the appearance of intense
emission in the green region with a peak at 2.2–2.3 eV is
due to the presence of silicon nanoclusters in SiO2. It
should be noted that there are alternative interpretations
of the origin of the green 2.3 eV band in the CL spectra
of thermal films. Thus, in [13] this band is related to the
existence of Si/SiO2 interface, while in [12] this band is
attributed to exciton emission. In the latter case, under
high-energy excitation the autolocalised exciton
emission is observed at 2.6 eV for quartz, at 2.3 eV for
amorphous SiO2, and at 2.2 eV for cristobalite [14].
The blue band at 2.65 eV, which was observed in
the CL spectra, is due to forbidden singlet-triplet
transitions in the molecular complex of twofold-
coordinated silicon atom [4]. Most likely, this defect is a
silicon atom that has only two neighbouring oxygen
atoms [4].
The 4.4-eV band that we observed in the CL
spectra, according to the authors of [15], is also related
to twofold-coordinated silicon (O2 = Si:), a defect known
as a silylene center. Silylene centers are believed to be
formed as a result of displacement of atoms from the
sites of SiO2 lattice [15] in the process of ion
implantation or in the processes of growth and
theatments [16]. Also, there are alternative opinions on
the mechanism inherent to formation of twofold-
coordinated silicon. Thus, the authors of [17] suggest
that ion implantation results in formation of that kind of
defects due to breakage of two bonds in the same OSi −
OSi − tetrahedron during the implantation process.
In the UV region, we have observed the band at
3.1-3.2 eV that is attributed to a small content of boron
impurity in the Si/SiO2 interface [4]. Appearance of this
band is caused by the presence of boron dopant in the
single-crystal silicon used as substrate.
As our experiments have shown, a weak magnetic
field influences the CL spectra (Fig. 2 cb − ).
Comparison of the CL spectra presented in Fig. 2c
shows that magnetic treatment decreases the intensity of
all the CL bands considerably (from 23 up to 35
per cent). Especially strong are the changes in the
intensities of the CL bands at 1.9 eV (attributed to non-
bridge oxygen) and 4.4 eV (twofold-coordinated
silicon). In our opinion, the decrease in the CL intensity
may be caused by the reconstruction in the centers of
radiative recombination, which are intrinsic structural
defects in Si/SiO2. Our previous studies [18, 19] have
shown that magnetic treatment of single-crystal silicon
wafers with a natural silicon dioxide film results in
changes in the structure of both silicon and oxide film,
which, in turn, alters the defect-impurity state of the
near-surface layer of the crystal. From the literature [8,
10, 11], it is known that action of a weak magnetic field
on non-magnetic materials initiates the processes of
chemical bond breakage in structural defect
nanoclusters, stimulates processes of diffusional
instability and adsorption, increases the rate of
interdefect solid state reactions.
A possible mechanism of magnetic field effect on
the evolution of metastable complexes that are present in
Si/SiO2 structure and have been detected in our study is
rearrangement of valence electrons in the atoms of point-
defect complexes ( OHSi − , , ,HSi − SiOSi −− xOSi −
precipitates, etc.) due to spin-dependent processes. The
force and energy UM, imposed by magnetic field with an
induction of B ∼ 1 T on a structural element in
magnetically disordered medium is negligible and at
room temperature (ТR = 300 K) comprises
UM ≈ gμB << kTBB R, where g is the Lande factor, μBB is the
Bohr magneton, and k is the Boltzmann constant. In such
a situation, the magnetic field cannot affect the
equilibrium state of the thermodynamic system.
Consequently, a weak magnetic field can influence
effectively only non-equilibrium systems (spin systems),
which pass in their evolution through short-lived excited
states, in which multiplicity can be changed. A constant
magnetic field is able to alter the multiplicity of non-
equilibrium spin-correlated pairs of paramagnetic
defects only if the energy difference between their
singlet and triplet states ES – ET is of the same order of
magnitude as the energy UM, that is, when the covalent
bond is weakened. Being in such a magnetosensitive
336
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2011. V. 14, N 3. P. 334-338.
state, point defect complexes are expected to show a
weaker covalent bond, for which the energy difference
between singlet and triplet states is of the same order as
UM and such a “weak” magnetic field can cause S–T
transitions. A result of spin conversion is weakening and
breakage of chemical bonds in point defect complexes.
These and other processes that are initiated by the
action of magnetic field are followed by the processes of
structural relaxation, which, in turn, result in structural
modification. In this relation, it is reasonable to suppose
that non-bridge oxygen (1.9 eV band), twofold-
coordinated silicon (2.3 and 4.4 eV), boron impurity
(3.1 eV band) and other defects that are present in
silicon dioxide film, due to action of magnetic field
undergo interdefect reactions with, e.g., vacancies and
form complexes of oxygen-vacancy ( ) type,
which are referred to as type A defects, and complexes
type (type E defects), complexes, etc. It is
binding of isolated defects, responsible for the red,
green, blue, UV and other CL bands, into
abovementioned point defect complexes that leads to
decreasing the concentration of the radiative
recombination centers and, correspondingly, to
quenching the cathodoluminescence. It is worth
mentioning that similar results related to a decrease in
the photoluminescence intensity in ZnS crystals under
action of pulsed magnetic field (B = 7 T) were obtained
by authors of [9].
VO −
VB − BSi −
It is not improbable that a magnetic-treatment-
induced decrease in the number of twofold-coordinated
silicon atoms, the emission centers responsible for the
2.3 and 4.4 eV bands, may occur due to closure of non-
saturated (broken in the magnetic treatment) bonds
between silicon and neighbouring under-coordinated
silicon and oxygen atoms or due to closure of broken
bonds of silicon by diffusing hydrogen atoms, which are
formed in the oxide layer due to magnetic-treatment-
induced dissociation of silylene ( ) and
hydroxyle (OH) groups.
OHSi −
And now let us say a few words about changes in
the green 2.3 eV emission band. As already noted above,
this band in the CL spectra may be due to emission of
autolocalized excitons in amorphous SiO2. The
magnetic-treatment-induced decrease in the intensity of
the 2.3 eV band may be explained as follows. Action of
magnetic field leads not only to breakage of chemical
bonds in nanoclusters, but also to a decrease in the
exciton binding energy, which results in exciton decay.
The latter leads to a rise in the number of free carriers
and to corresponding drop in the CL intensity. This
statement agrees with the results obtained by the authors
of [20] in studying the action of magnetic field with an
induction of 6 T on the kinetics of photoluminescence of
quantum dots in InAs/AlAs. Switching the magnetic
field on resulted in a faster decay kinetics [20]. The
results obtained are explained in the framework of a
model that takes into account a fine structure of exciton
levels and their exchange and Zeeman splitting in
magnetic field.
So, it may be concluded that the magnetic-
treatment-induced changes in the emission spectra
revealed in our study may be due to both magnetic-field-
stimulated interdefect reactions (and, as a result,
appearance of ‘new’ structural nanoclusters in silicon
dioxide itself) and processes in the electron subsystem.
A more detailed interpretation of the mechanism of
changing the intensities of Si/SiO2 structure
cathodoluminescence bands caused by action of
magnetic field requires further investigations, since this
fact depends on both a change in defect concentration
and a change in the efficiency of luminescence channels.
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© 2011, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
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