I¹²⁷ NQR spectra of Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ of mixed layered semiconductors
The results of studying the concentration and temperature dependences of NQR spectrum parameters inherent to I¹²⁷ in mixed layered semiconductors Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ are presented for x ≤ 0.30 and T = 77…150 K. It has been shown that, for the low content x ≤ 0.08 Pb₂ for (BiI₃)₍₁₋ₓ₎(Pb...
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Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
2017
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| Cite this: | I¹²⁷ NQR spectra of Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ of mixed layered semiconductors / I.G. Vertegel, E.D. Chesnokov, O.I. Ovcharenko, L.S. Ivanova, Yu.P. Gnatenko, I.I. Vertegel // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 3. — С. 340-343. — Бібліогр.: 15 назв. — англ. |
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Digital Library of Periodicals of National Academy of Sciences of Ukraine| _version_ | 1860301533875273728 |
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| author | Vertegel, I.G. Chesnokov, E.D. Ovcharenko, O.I. Ivanova, L.S. Gnatenko, Yu.P. Vertegel, I.I. |
| author_facet | Vertegel, I.G. Chesnokov, E.D. Ovcharenko, O.I. Ivanova, L.S. Gnatenko, Yu.P. Vertegel, I.I. |
| citation_txt | I¹²⁷ NQR spectra of Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ of mixed layered semiconductors / I.G. Vertegel, E.D. Chesnokov, O.I. Ovcharenko, L.S. Ivanova, Yu.P. Gnatenko, I.I. Vertegel // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 3. — С. 340-343. — Бібліогр.: 15 назв. — англ. |
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| container_title | Semiconductor Physics Quantum Electronics & Optoelectronics |
| description | The results of studying the concentration and temperature dependences of NQR spectrum parameters inherent to I¹²⁷ in mixed layered semiconductors Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ are presented for x ≤ 0.30 and T = 77…150 K. It has been shown that, for the low content x ≤ 0.08 Pb₂ for (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ and x ≤ 0.02 CdI₂ for Pb₁₋ₓCdₓI₂, the temperature coefficients of NQR frequency don’t undergo significant changes, which is indicative of conservation of the quasi-two-dimensional nature of the vibration states. The possibility of forming nanoclusters of Pb₂ and CdI₂, and their influence on NQR spectral parameters, has been discussed.
|
| first_indexed | 2026-03-21T19:36:33Z |
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Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 3. P. 340-343.
doi: https://doi.org/10.15407/spqeo20.03.340
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
340
PACS 76.60.Gv
I127 NQR spectra of Pb1–xCdxI2 and (BiI3)(1–x)(PbI2)x
of mixed layered semiconductors
I.G. Vertegel1, E.D. Chesnokov1, O.I. Ovcharenko1, L.S. Ivanova1, Yu.P. Gnatenko1, I.I. Vertegel2
1Institute of Physics, NAS of Ukraine,
46, prospect Nauky, 03680 Kyiv, Ukraine
2National Technical University “KPI”,
37, prospect Peremohy, 03056 Kyiv, Ukraine
Abstract. The results of studying the concentration and temperature dependences of
NQR spectrum parameters inherent to I127 in mixed layered semiconductors Pbx–1CdxI2
and (BiI3)(1–x)(PbI2)x are presented for x ≤ 0.30 and T = 77…150 K. It has been shown
that, for the low content x ≤ 0.08 PbI2 for (BiI3)(1–x)(PbI2)x and x ≤ 0.02 CdI2 for Pb1–
хCdxI2, the temperature coefficients of NQR frequency don’t undergo significant changes,
which is indicative of conservation of the quasi-two-dimensional nature of the vibration
states. The possibility to form nanoclusters of PbI2 and CdI2 as well as their influence on
the parameters of the NQR spectra has been discussed.
Keywords: nuclear quadrupole resonance, layered semiconductors, asymmetry para-
meter, nanoclusters.
Manuscript received 18.05.17; revised version received 10.07.17; accepted for
publication 06.09.17; published online 09.10.17.
1. Introduction
In this work, the temperature dependences of parameters
inherent to NQR spectra of the layered semiconductor
crystals (BiI3)(1–х)(PbI2)х and Pb1–xCdxI2 have been
studied. The temperature coefficients of the NQR
spectrum parameters are highly sensitive to changes in
the crystal dynamic parameters (amplitudes, frequencies)
[1, 2]. The urgency of studies of solid solutions of
layered semiconductor crystals (BiI3)(1–х)(PbI2)х and Pb1–
хCdxI2 is first of all associated with the possibility of
formation of cluster structures in these crystals, which
significantly affects their properties. Recently, the
interest significantly increased in finding of
semiconductor materials that are suitable for
development on their base the detectors with high
radiation energy distribution, which can operate at room
temperature. The promising materials are those that have
a layered structure with relatively high atomic number of
components. The absorption and reflectance spectra as
well as X-ray structural analysis of (BiI3)1–x(PbI2)x mixed
crystals, photoluminescence spectra were studied in
[3, 4]. The I127 nuclear quadrupole resonance (NQR)
spectra of chemically pure BiI3 crystals and mixed
layered semiconductor were studied in [5-8].
At the same time, NQR investigations are of
episodic character and don’t completely explain the
dynamic character of these crystals. In this work, for the
first time, the authors fulfilled studying the temperature
dependence of NQR frequencies in crystals under
consideration.
2. Experimental
The I127 NQR spectra of the crystals under investigation
were measured within the temperature range 77 to 150 K
and the frequency range 5…300 MHz by using quasi-
coherent NQR spectrometer. Accuracy was determined
by the half-width of the NQR lines, and for the crystals
(BiI3)(1–х)(PbI2)х and Pb1–хCdxI2, it was limited by the
interval ±100 kHz. Crystals with PbI2 contents of x =
0.0, 0.05, 0.08, 0.2, 0.3 and CdI2: х = 0, 0.02, 0.1 were
studied. Measurements of the I127 NQR frequencies ν
corresponding to the ±1/2↔±3/2 and ±5/2↔±3/2
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 3. P. 340-343.
doi: https://doi.org/10.15407/spqeo20.03.340
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
341
transitions enabled to determine the temperature and
concentration dependences of the quadrupole interaction
constans e2Qqzz(x) and the asymmetry parameter η(х) of
the electric-field-gradient tensor ( ) zzyyxx qqq −=η
(η = (qxx–qyy)/qzz) (EFGT). The accuracy of
determination of the asymmetry parameter and
quadrupole interaction constant depended on the line
width and was no worse than ±1.5% and ±0.1% of their
absolute values, respectively. At temperatures above the
Debye one, TD, the NQR frequency usually exhibits a
linear dependence [1]. When studying the temperature
dependence of the NQR frequencies of the lines within
the temperature range 77 to 150 K, it was found that the
NQR frequency of those lines varied linearly with
temperature. The experimental results obtained for the
NQR lines ν made it possible to determine the
temperature coefficients of the NQR spectrum
parameters: k1 = dν/dТ (±1/2↔±3/2), k2 = dν/dТ
(±3/2↔±5/2). The accuracy of determination of the
specified parameters was defined by the width of the
NQR lines and precision of sample temperature
stabilization and was no worse than ±10% for all lines.
The data of our measurements are summarized in Table.
3. Experimental results and discussion
With increasing the PbI2 content in the crystal (BiI3)(1–
х)(PbI2)х and CdI2 in Pb1–хCdxI2, the line width of the
NQR I127 (±3/2↔±5/2) is significantly increased. With
increasing PbI2 and CdI2 content x in the crystals under
investigation from 0 up to 0.30, the width Δν of lines ν
of I127 NQR in the same range of content x varies by
about an order of magnitude: Δν|x=0 ~ 0.24,
Δν|x=0.3 ~ 2,30 MHz, Δν1|x=0 ~ 0.2, Δν1|x=0.1 ~ 1.40 MHz.
It must be noted that the value of the constants e2Qqzz
in the crystal (BiI3)(1–х)(PbI2)х in the range of content x
(0 ≤ x ≤ 0.10) does not change within the measurement
error [5]. For crystals PbI2 at Т = 77 K, it was revealed
that the value of e2Qqzz is 29.83 MHz, and the
asymmetry parameter of the (EFGT) is equal to zero.
The quadrupole constant of interaction is 30.708 MHz
for solid solutions Pb1–xCdxI2 (x = 0.02), and the
asymmetry parameter EFGT is equal to 14%. In this
case, the ratio of NQR line width to the NQR frequency
is 0.052. Proceeding from the obtained results, it can be
considered that there is violation of axial symmetry of
electric field gradient at the resonant nuclei I127 during
formation of solid solutions with a low content of Cd
component. This may be due to the fact that the
introduction of Cd atoms in the matrix PbI2 leads to
minor violation of internally layer anisotropy due to the
fact that ionic radius Pb2+ and Cd2+ are significantly
different (1.21 and 0.97Ǻ, respectively). This leads to
emergence of internal layer mechanical stresses of
crystalline lattice, and, as consequence, to the decrease
in the axial symmetry of the electric field gradient
along the axes qxx and qyy that are inside the crystal
layer.
Thus, for the range of content 0 ≤ x ≤ 0.1, introduc-
tion of groups of atoms PbI2 and CdI2 causes the minor
change of symmetry of layers and does not change the
layered structure of crystals. For that, the symmetry of
studied layered crystals in the range of content
0 ≤ x ≤ 0.1 can remain unchanged 2
3C i . This assumption
is based on the fact that the x and y axes of components
qxx and qyy of the electric field gradient tensor lie in the
plane of the crystal layers and z-axis are perpendicular to
the layers [6]. Therefore, when analyzing the NQR I127
spectra, it can be concluded that in the interval of PbI2
and CdI2 content 0 < x < 0.1 layered structure of crystals
(BiI3)(1–x)·(PbI2)x and Pbx–1CdxI2 is remained and PbI2 and
CdI2 groups are located within the crystal layers. In
addition, the PbI2 and CdI2 groups may form the layer
clusters of island type, the size of which increases with
increasing the content x [8, 9]. A further growth of
cadmium component content in crystals Pb1–xCdxI2 up to
x ≥ 0.1 causes a significant broadening of NQR line. The
relative broadening of NQR line is 0.33, the quadrupole
interaction constant increases up to 43.429 MHz, and
parameter EFGT – to 63%.
It should be also noted that the shape of NQR lines
for crystals Pb0.9Cd0.1I2 at T = 77 K is complex and
includes a number of vague lines [10]. Existence of this
structure in the NQR lines may indicate formation of an
“island” (heterophase) structure.
It is known that for the chemically pure samples
with sufficiently high degree of perfection of the crystal
lattice, as a rule, the width of the NQR spectra line Δν
must be very small in comparison with the NQR line fre-
quency Δν/ν ~10–3 [11]. It is known that for the chemi-
cally pure samples with sufficiently high degree of per-
fection of the crystal lattice as a rule the width of the
NQR spectra line Δν must be very small in comparison
with the NQR line frequency Δν/ν ~ 10–3 [11]. Really,
lattice distortions result in that the intermolecular distan-
ces r of the same type in the crystal are not accurately
identical, i.e., a spread of distances r emerges. In turn it
lead to certain divergence of values for the components
of the electric-field-gradient tensor, Δqxx, Δqyy and Δqzz
and to increasing the NQR spectrum line width Δν. In
the work [11], it was also shown that the ratio Δν/ν
(~Δ r/r) increases to about 10–1, and lines of the spect-
rum become unobservable. It is also known [1] that the
product of the width and the intensity of the NQR line is
proportional to the number of resonance nuclei that form
this line. Therefore, the fact that, in the range of content
CdI2 0.1 < x < 1 in crystals Pb1–xCdxI2 and in the range of
content PbI2 х ≥ 0.2 in crystals (BiI3)(1–х)(PbI2)х the line ν
with the parameters e2Qqzz = 682.18 MHz and η = 0.29
was not observed, can testify to a considerable reduction
of the number of I127 resonance nuclei that are
responsible for this line. It was received [5] that for
chemically pure crystal BiI3 (х = 0) at 77 K I127 NQR
frequencies of two transitions ν(1/2↔±3/2) and ν(±3/2↔±5/2)
are accordingly equal to 111.320 and 210.380 MHz. The
constant of the quadrupole interaction e2Qqzz =
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 3. P. 340-343.
doi: https://doi.org/10.15407/spqeo20.03.340
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
342
682.18 MHz and asymmetry parameter of the electrical
field gradient tensor η = 0.29 ± 0.01 correspond to given
values of frequencies at 77 K.
For BiI3 crystals at 77 K with PbI2 contents
x = 0.20 and 0.3, the line ν′ was observed in the I127
NQR spectrum, the parameters of which differed
significantly from the parameters of the I127 line ν for
pure BiI3 (Figure) [5]. For example, at x = 0.2, the ν′ line
at 77 K is characterized by the following values of
parameters: ν(±1/2↔±3/2) = 104.35 MHz, ν(±5/2↔±3/2) =
204.20 MHz, eQqzz′ = 684.01 MHz and η′ = 0.15. It’s
important to note that the asymmetry parameter η for
this new line ν′ in the I127 NQR spectrum is decreased
about twice: from η = 0.29 down to η′ = 0.15. The value
of the constant e2Qqzz′ of the electric field gradient at the
I127 nuclei does not change considerably, herewith:
e2Qqzz = 682.18 MHz and e2Qqzz′ = 684.01 MHz. We
think that, with increasing x, symmetry of the electric
field gradient increases.
It is known that for an intracrystalline field with the
asymmetry parameter η = 0 [1]
( )12
3
ν
2
3
2
5 −
=
±↔± IhI
qQe zz ,
where Q is the nuclear quadrupole moment, e – electron
charge, I – the nucleus spin, zzq – time-averaged EFGT,
averaged by lattice vibrations. Note that qzz is defined by
contributions from the covalent bonds of the ion and
from the point charges of the lattice ions qi
zz [12]. It was
shown [2, 13] that the temperature dependence of the
NQR frequency in the case of zero EFGT asymmetry
parameter and if qi
zz contribution from the point charges
can be neglected and this may be used to interpret long
wave low-frequency phonon spectra of crystals. The
vibrations with frequencies not exceeding 200 cm–1 are
the most efficient in averaging qzz.
For layered semiconductor crystals, the contribu-
tion of lattice point charges to temperature dependence
of the NQR frequencies can be significant [14], which
leads to inability of using the dual frequency model for
averaging GEF. If symmetry of EFGT differs from the
axial one (for BiI3, crystal, η = 29%) for the spin
I = 5/2, the NQR frequency, eQqzz, and η are related by
the solutions of the corresponding secular equations
[15]. The absolute values of the temperature
coefficients of the NQR frequencies in crystals of
alkaline halogens are mainly due to fluctuations of
isolated alkaline halogens; while in layered crystals –
by interlayer vibrations and oscillations of the crystal
lattice point charges.
Like PbI2 and BiI3 crystals, (BiI3)1–x(PbI2)x layered
crystals are characterized by structural anisotropy, which
should lead to the vibrational states of quasi-two-
dimensional character [6]. The vibrations that can
efficiently average the electric field gradient in the
studied crystals primarily include low-frequency
interlayer vibration associated with the weak interaction
between the layers. The temperature coefficients of the
frequency (k1 and k2) in (BiI3)1–x(PbI2)x for the line ν for
x = 0.05 and x = 0.08 do not differ from those for pure
BiI3 (x = 0) by more than 17%. Given the accuracy of
determining the studied parameters (±10%), we can
conclude that the experimental values at PbI2 contents
0 ≤ x≤ 0.08 remain constant. It suggests that, at these x
values, the low-frequency interlayer vibrations undergo
no significant changes and that the inclusion of PbI2
groups does not lead to the significant change in the
degree of two-dimensionality of the crystal structure.
The temperature coefficients of the frequency
(dν/dT) increased in comparison with the line ν′ (table)
for this new line ν in the NQR spectrum. For example,
for the line ν′ at x = 0.3 dν/dT = –74.6 kHz/K, whereas
for the line ν at х = 0 dν/dT = –15.3 kHz/K. As a result,
one can made the conclusion that, at the PbI2 content
range 0.2 ≤ x ≤ 0.6 as compared with range 0 ≤ x ≤ 0.08,
the degree of quasi-two-dimensionality of phonon
spectra becomes different (spectrum becomes ‘softer’).
Another possible assumption is that, in (BiI3)1–x(PbI2)x
crystals with PbI2 contents of x = 0.2 and x = 0.3, the
interlayer spacing accommodates one or more PbI2
layers. It causes a change in the degree of quasi-two-
dimensionality of the phonon spectrum and a decrease in
the frequency of interlayer vibrations, which manifests
itself through a considerable change in the value of
temperature coefficient of the NQR frequency. At the
same time, for the PbI2 content range 0 < x ≤ 0.08,
changes in dν/dT are insignificant. It’s possible to state
that PbI2 nanoclusters are created within the content
range 0≤ x ≤ 0.08, when they are located only within the
layers of the crystal.
Crystals k1/ν1 (10–3K–1)±1/2↔±3/2 k2/ν2 (10–3K–1)±3/2↔±5/2 η Spectral lines
BiI3 –0.1402 –0.0819 0.29 ν
(BiI3)0.95(PbI2)0.05 –0.1543 –0.090 0.287 ν
(BiI3)0.92(PbI2)0.08 –0.1316 –0.089 0.285 ν
(BiI3)0.8(PbI2)0.2 * –0.1523 0.15 ν′
(BiI3)0.7(PbI2)0.3 * –0.1754 0.15 ν′
PbI2 * –0.030 0.00 ν1
Pb0.98Cd0.02I2 * –0.032 0.014 ν1
* The temperature dependence was not investigated.
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 3. P. 340-343.
doi: https://doi.org/10.15407/spqeo20.03.340
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
343
4. Conclusions
In the mixed layered semiconductors (BiI3)(1–х)(PbI2)х
and Pb1–хCdxI2, the values of the temperature coefficients
of the NQR frequency has been defined, which changes
within the content range of PbI2 0 ≤ х ≤ 0.08 and CdI2
x ≥ 0.2 are insignificant, indicating conservation of
nature of quasi-two-dimensional vibrational states for
x ≤ 0.08 in the case of PbI2 and х ≤ 0.08 – of CdI2 The
measurements of the temperature dependences of the
NQR spectrum parameters at the PbI2 content x > 0.2
and that for CdI2 х > 0.1 show that the synthesized
crystals (BiI3)(1–х)(PbI2)х and Pb1–хCdxI2 are glassy solid
solutions of the substitution type. At this, the synthesized
PbI2 and CdI2 groups (intercalates) are fully or partially
ordered into the semiconductor crystal system. It leads to
changes in the temperature coefficients of the frequency
and ‘softening’ the vibrational states, which causes
changing the quasi-two-dimensionality of the crystal
structure.
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| id | nasplib_isofts_kiev_ua-123456789-214948 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 1560-8034 |
| language | English |
| last_indexed | 2026-03-21T19:36:33Z |
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| publisher | Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
| record_format | dspace |
| spelling | Vertegel, I.G. Chesnokov, E.D. Ovcharenko, O.I. Ivanova, L.S. Gnatenko, Yu.P. Vertegel, I.I. 2026-03-05T12:03:28Z 2017 I¹²⁷ NQR spectra of Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ of mixed layered semiconductors / I.G. Vertegel, E.D. Chesnokov, O.I. Ovcharenko, L.S. Ivanova, Yu.P. Gnatenko, I.I. Vertegel // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 3. — С. 340-343. — Бібліогр.: 15 назв. — англ. 1560-8034 PACS: 76.60.Gv https://nasplib.isofts.kiev.ua/handle/123456789/214948 https://doi.org/10.15407/spqeo20.03.340 The results of studying the concentration and temperature dependences of NQR spectrum parameters inherent to I¹²⁷ in mixed layered semiconductors Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ are presented for x ≤ 0.30 and T = 77…150 K. It has been shown that, for the low content x ≤ 0.08 Pb₂ for (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ and x ≤ 0.02 CdI₂ for Pb₁₋ₓCdₓI₂, the temperature coefficients of NQR frequency don’t undergo significant changes, which is indicative of conservation of the quasi-two-dimensional nature of the vibration states. The possibility of forming nanoclusters of Pb₂ and CdI₂, and their influence on NQR spectral parameters, has been discussed. en Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України Semiconductor Physics Quantum Electronics & Optoelectronics I¹²⁷ NQR spectra of Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ of mixed layered semiconductors Article published earlier |
| spellingShingle | I¹²⁷ NQR spectra of Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ of mixed layered semiconductors Vertegel, I.G. Chesnokov, E.D. Ovcharenko, O.I. Ivanova, L.S. Gnatenko, Yu.P. Vertegel, I.I. |
| title | I¹²⁷ NQR spectra of Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ of mixed layered semiconductors |
| title_full | I¹²⁷ NQR spectra of Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ of mixed layered semiconductors |
| title_fullStr | I¹²⁷ NQR spectra of Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ of mixed layered semiconductors |
| title_full_unstemmed | I¹²⁷ NQR spectra of Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ of mixed layered semiconductors |
| title_short | I¹²⁷ NQR spectra of Pb₁₋ₓCdₓI₂ and (BiI₃)₍₁₋ₓ₎(PbI₂)ₓ of mixed layered semiconductors |
| title_sort | i¹²⁷ nqr spectra of pb₁₋ₓcdₓi₂ and (bii₃)₍₁₋ₓ₎(pbi₂)ₓ of mixed layered semiconductors |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/214948 |
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