Individual glow bands of Mn²⁺ ions photoluminescence in plastically deformed ZnS single crystals
The spectra of a photoluminescence (PL) in plastically deformed (PD) ZnS:Mn single crystals are investigated. It is shown that the PD processes cause change of a quantitative ratio between separate types of glow manganese centres (MC) as a result of their local symmetry rearrangement. After decompos...
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Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
2004
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| Цитувати: | Individual glow bands of Mn²⁺ ions photoluminescence in plastically deformed ZnS single crystals / T.A. Prokofiev, A.V. Kovalenko, B.A. Polezaev, M.F. Bulanyi, A.A. Gorban, O.V. Hmelenko // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2004. — Т. 7, № 1. — С. 63-67. — Бібліогр.: 24 назв. — англ. |
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Prokofiev, T.A. Kovalenko, A.V. Polezaev, B.A. Bulanyi, M.F. Gorban, A.A. Hmelenko, O.V. 2017-05-28T17:41:37Z 2017-05-28T17:41:37Z 2004 Individual glow bands of Mn²⁺ ions photoluminescence in plastically deformed ZnS single crystals / T.A. Prokofiev, A.V. Kovalenko, B.A. Polezaev, M.F. Bulanyi, A.A. Gorban, O.V. Hmelenko // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2004. — Т. 7, № 1. — С. 63-67. — Бібліогр.: 24 назв. — англ. 1560-8034 PACS: 78.55.Et https://nasplib.isofts.kiev.ua/handle/123456789/118114 The spectra of a photoluminescence (PL) in plastically deformed (PD) ZnS:Mn single crystals are investigated. It is shown that the PD processes cause change of a quantitative ratio between separate types of glow manganese centres (MC) as a result of their local symmetry rearrangement. After decomposing of PL integral spectra by individual PL bands using the cumulative distribution Gauss function, the nature of a ratio change between PL MC of different types is established. The individual with the peaking in the range 618-620 nm is discovered. en Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України Semiconductor Physics Quantum Electronics & Optoelectronics Individual glow bands of Mn²⁺ ions photoluminescence in plastically deformed ZnS single crystals Article published earlier |
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Digital Library of Periodicals of National Academy of Sciences of Ukraine |
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| title |
Individual glow bands of Mn²⁺ ions photoluminescence in plastically deformed ZnS single crystals |
| spellingShingle |
Individual glow bands of Mn²⁺ ions photoluminescence in plastically deformed ZnS single crystals Prokofiev, T.A. Kovalenko, A.V. Polezaev, B.A. Bulanyi, M.F. Gorban, A.A. Hmelenko, O.V. |
| title_short |
Individual glow bands of Mn²⁺ ions photoluminescence in plastically deformed ZnS single crystals |
| title_full |
Individual glow bands of Mn²⁺ ions photoluminescence in plastically deformed ZnS single crystals |
| title_fullStr |
Individual glow bands of Mn²⁺ ions photoluminescence in plastically deformed ZnS single crystals |
| title_full_unstemmed |
Individual glow bands of Mn²⁺ ions photoluminescence in plastically deformed ZnS single crystals |
| title_sort |
individual glow bands of mn²⁺ ions photoluminescence in plastically deformed zns single crystals |
| author |
Prokofiev, T.A. Kovalenko, A.V. Polezaev, B.A. Bulanyi, M.F. Gorban, A.A. Hmelenko, O.V. |
| author_facet |
Prokofiev, T.A. Kovalenko, A.V. Polezaev, B.A. Bulanyi, M.F. Gorban, A.A. Hmelenko, O.V. |
| publishDate |
2004 |
| language |
English |
| container_title |
Semiconductor Physics Quantum Electronics & Optoelectronics |
| publisher |
Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
| format |
Article |
| description |
The spectra of a photoluminescence (PL) in plastically deformed (PD) ZnS:Mn single crystals are investigated. It is shown that the PD processes cause change of a quantitative ratio between separate types of glow manganese centres (MC) as a result of their local symmetry rearrangement. After decomposing of PL integral spectra by individual PL bands using the cumulative distribution Gauss function, the nature of a ratio change between PL MC of different types is established. The individual with the peaking in the range 618-620 nm is discovered.
|
| issn |
1560-8034 |
| url |
https://nasplib.isofts.kiev.ua/handle/123456789/118114 |
| citation_txt |
Individual glow bands of Mn²⁺ ions photoluminescence in plastically deformed ZnS single crystals / T.A. Prokofiev, A.V. Kovalenko, B.A. Polezaev, M.F. Bulanyi, A.A. Gorban, O.V. Hmelenko // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2004. — Т. 7, № 1. — С. 63-67. — Бібліогр.: 24 назв. — англ. |
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| first_indexed |
2025-11-24T06:14:25Z |
| last_indexed |
2025-11-24T06:14:25Z |
| _version_ |
1850844156897787904 |
| fulltext |
63© 2004, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
Semiconductor Physics, Quantum Electronics & Optoelectronics. 2004. V. 7, N 1. P. 63-67.
PACS: 78.55.Et
Individual glow bands of Mn2+ ions photoluminescence
in plastically deformed ZnS single crystals
T.A. Prokofiev, A.V. Kovalenko, B.A. Polezaev, M.F. Bulanyi, A.A. Gorban, O.V. Hmelenko
Dnipropetrovsk National University, 13, Naukova str., Dnipropetrovsk, Ukraine
Phone: +380 (562) 7768378, E-mail: tichonprok@yahoo.de, tichon@mail.dsu.dp.ua
Abstract. The spectra of a photoluminescence (PL) in plastically deformed (PD) ZnS:Mn
single crystals are investigated. It is shown that the PD processes cause change of a quantita-
tive ratio between separate types of glow manganese centres (MC) as a result of their local
symmetry rearrangement. After decomposing of PL integral spectra by individual PL bands
using the cumulative distribution Gauss function, the nature of a ratio change between PL
MC of different types is established. The individual with the peaking in the range 618�620 nm
is discovered.
Keywords: spectra of photoluminescence, plastical deformation, manganese centres, individual
band, decomposition of integral spectra.
Paper received 05.11.03; accepted for publication 30.03.04`.
The photoluminescence (PL) researches of ZnS:Mn single
crystals at small plastical deformations (PD) (ε ~ 1�2%)
have shown that there is an increase of PL integral spec-
trum intensity by 10�15 % from an intensity level of a
undeformed single crystal with a shift of the peak posi-
tion into short wave side by 2�3 nm. At further increase
of up to 5.3 %, there is a decrease of the glow intensity
with the shift of PL peak into long wave range by 5�7 nm
(Fig. 1).
This experimental fact predetermines more detail
analysis of manganese centres (MC) glow behaviour in
ZnS single crystals in the range of values 0 < ε < 5.3 % in
PD process. Each of them is characterised by the intrin-
sic local symmetry of Mn2+ ions and features of excita-
tion causing MC glow. The types of these centres were
offered after electroluminescence (EL) and PL researches
of spectra in ZnS:Mn single crystals under different con-
ditions of excitation [1�6]. Being based on the obtained
data, individual bands are interpreted as follows: the band
λmax = 557 nm � ions Mn2+ in tetrahedrons of the cubic
grating; λmax = 578 nm � ions Mn2+ near to dislocations
or dot defects; max = 600 nm � ions Mn2+ in octahedral
interstices. The band peaking at λmax = 635 nm is con-
nected to formation of α-MnS phase in ZnS. If somehow
it will be possible to execute decomposing of integral PL
spectra and to receive the information on a behaviour of
individual PL bands at various values of PD, it means,
that we shall receive the information on change of a ratio
between different types of MC glow, and consequently
we shall obtain some comprehension of changes taking
place in the crystalline structure of ZnS:Mn chips as a
whole. Now there are some methods enabling to make
similar decomposition. The most effective of them are
based on the analysis of integral spectra changes accom-
panying variations in experimental conditions: the in-
tensity [7] or wavelength [7, 8] of excitation, concentra-
tions of centres of glow [9], the temperature [10], the ad-
ditional illumination from damping area of one bands
[11]. Using the results obtained with the Alentsev-Fok
method [11] allows to determine, in a number of cases,
the shape of an contour of a individual band, quantity of
these bands in an integral spectrum without any prior
assumption about their form. The application of modu-
lation methods [12] enables to find a feeble structure of
composite bands. At the same time, it is necessary to note
that for today there is no universal method to decompose
integral spectra of the different form. Moreover, from
[11, 12] it follows that obtaining unambiguous and au-
thentic results about the structure of an integral PL spec-
trum decomposed is practically impossible. Each of listed
methods has both number of advantages and a number of
lacks and can be correctly applied only in specific condi-
tions. Some methods are tolerant to very feeble and nar-
row bandwidths located inside the broad and intensive
64
SQO, 7(1), 2004
T.A. Prokofiev et al.: Photoluminescence of Mn2+ ions individual bands of ...
individual bands [7, 8�11]. Besides, the known Alentsev-
Fok method is rather complex in operational use, as it
demands considerable changes of an integral spectrum,
which is often impossible without considerable changes
of experimental conditions. If we have large a number of
individual bands in intermediate spectra, it is very diffi-
cult to determine horizontal segments bound with coeffi-
cients of decomposition. Other methods [12], being su-
per-sensitive, allow to find out even phonon repetitions
[7, 13], thus the number of features in a differential lumi-
nescent spectrum can be larger then quantity of independ-
ent centres of glow [12]. As a result, we have to carry out
additional experiments. Therefore, selecting this or that
method of decomposing, or creating a new one, it is nec-
essary to aim it at specific features of integral PL spectra
and special conditions of experiment.
As the spectral shape of individual PL bands of Mn2+
ions is close to the form of a cumulative distribution of
the Gauss function, in our view, for decomposing similar
spectra it is convenient to use the following function:
]2)(exp[ 22
max0 w / xxA yy −−+= , (1)
where A is the amplitude of a maximum, w is the width of
a peak at the half of its amplitude, xmax � the maximum
position, y0 � level of zero point (Fig. 2).
The area under the curve, ∫=
2
1
)(
x
x
dxxyS will be pro-
portional to quantity of glow MC, accountable for radia-
tion of an integral spectrum. The limits of integrating x1
and x2 belong to a segment, where function y(x) ≠ 0. As at
the analysis of PL spectra, the area under a spectral curve
between the ordinate y = 0 and y0 level characterises the
noise signal and has no useful information, we can ac-
cept y0 = 0.
It is known that any �Gaussian� can be decomposed
by components also depicted by a cumulative distribu-
tion of the Gauss function, so
x yx y x y x y xy n )()()()()( 321 +…+++= , (2)
where y1 y2 y3 � yn are functions determining separate
individual bands included into a structure of an integral
PL spectrum.
In our case, the number of such components should be
limited by the number of individual bands shaped close
to �Gaussian� and found other methods [11, 14, 15]. As
the form of experimental spectra nevertheless differs a
little from the form of an approximating function, it is
necessary to allow for error of this approximation. So, it
is necessary to decide a return problem by having estab-
lished how great is the deviation of the sum of approxi-
mating functions describing individual bands, from an
experimental PL spectrum. As this relation has compos-
ite nature, we shall designate it as some function f(x).
Allowing the said above, we should obtain
)()()()()()( 4321 x fx yx yxyxyxy ++++= . (3)
In original sign of experimental PL spectra this for-
mula will accept the following view:
a
1
2
1 20 3 4 5 6
592
588
584
580
l
e, %
m
a
x
,
n
m
b
1
2
1 20 3 4 5 6
0.8
0.4
0.0
e, %
I
,
a
rb
.
u
n
.
Fig. 1. Relation of a peak position (à) and emission power (b) of the
integral PL spectrum in ZnS:Mn single crystals at different degrees
of plastic deformation ε. CMn = 1⋅10�2 (1) and CMn = 5⋅10 �3 (2)
g MnS / g ZnS (g/g).
0
500 600
l, nm
W
A/2
A
Y
0
I
,
a
rb
.
u
n
.
700
0.4
0.8
Fig. 2. PL spectra of ZnS:Mn single crystals with parameters
serving as constants of decomposition of an integral spectrum by
individual bands.
T.A. Prokofiev et al.: Photoluminescence of Mn2+ ions individual bands of ...
65SQO, 7(1), 2004
),(]2/)(exp[
]2/)(exp[
]2/)(exp[
]2/)(exp[)(
2
4
2
max44
2
3
2
max33
22
max22
2
1
2
max11
2
λλλ
λλ
λλ
λλλ
AwA
wA
wA
wAI
∆+−−+
+−−+
+−−+
+−−=
(4)
where I(λ) is the function describing the experimental spec-
trum, À1, À2, À3, À4 � amplitudes; w1, w2, w3, w4 � half
widths; λ1max, λ2max, λ3max, λ4max � abscissas of individual
peaks, accordingly; ∆A(λ) - some function describing how
great is the deviation of the sum of approximating func-
tions from an experimental PL spectrum � �function of
an error�.
So, the problem of decomposing the integral PL
spectrum is reduced to finding the functions y1(λ) = A1×
×exp[�(� λ1max)2 /2w1
2], y2(λ) = A2exp [�(�λ2max)2 /2w2
2],
y3(λ) =A3exp [�(�λ3max)2 /2w3
2], y4(λ) = A4exp[�(�λ4max)2/
/2w4
2], at some optimal value ∆A(λ). This problem can
be solved using mathematical methods of optimization,
for example, the least square method [16, 17]. In essence,
it is the minimisation of a special object function, which,
using directly the experimental notations, looks like:
min)]]([)([),( 2
200
1
4
1
=−=Φ ∑∑
==
ji
j
jj
i
ijij yIwA λλ . (5)
Allowing that wij values are in indexes of exponents
(4) and are carried up in a quadratic degree, the solution
of the given problem represents the minimization of a
non-linear model. In this case, the formula (5) has set of
solutions, the optimal of which should be selected. It is
rather difficult problem that often has no unequivocal
solutions. Therefore, it is better to make some assump-
tions.
From mathematical statistics [18], it is known that
for construction of normal �Gaussian� distribution of
probability:
]/2)[(exp2
1
)(
22
max mxxm
xP
−
=
π
, (6)
it is enough to know two constants: a maximum position
xmax and parameter of half width � m. For the given func-
tion, up to date vast tables are compounded [19]. If we
change only constants xmax the plot of the function dis-
places along the absciss axis by some value without any
changes of the form. As we need the information on the
relative contribution of individual bands into radiation
of an integral PL spectrum, we have to know also the
behaviour of the third value � amplitudes of the maxima
Ài versus PD degree.
The shape of integral spectra changed only with re-
distribution between the intensities of individual bands
in PD process. The temperature was fixed and half width
of PL spectra practically did not change (Fig. 2). So,
there are no basis to consider that the half width of PL
individual bands will be changed essentially. Therefore,
we attempt to fix this value and we shall assume that all
bands are elementary, are subject to distribution (1) and
have approximately identical half widths. It means that
w1 ≈ w2 ≈ w3 ≈ w4 = constant, and
/2 nwwi ≈ , (7)
where n is the number of bands.
This assumption is in accord to the same interaction
with crystal for different types of MC glow. However,
taking into account that this difference is shown that only
in the third layer of their local symmetry, in our opinion,
in this case we shall not make the big mistake. Finally,
we may correct this parameter by using experimental
data, keeping in such a manner the mathematical iden-
tity of the decomposition for all spectra.
The values λimax are found in [11, 14, 15], where four
steady individual bands with λmax = 557, 578, 600 and
635 nm were described. If these bands are individual, the
values λimax should be stable during decomposing. Now
our object function Ô(Ài) depends only on four variables
À1, À2, À3 and À4 � amplitudes of individual band maxima
that are vary within the limits from 0 up to yi(λimax). In
this case, the least square criterion demands that the fac-
tors Ài should be selected from the condition of a mini-
mum value for Ô(Ài) [16, 17]. Therefore,
,min)]]()(
)()([)([)(
2
43
21
200
1
=++
++−=Φ ∑
=
jj
jj
j
jji
yy
yyIA
λλ
λλλ
(8)
0
)(
=
∂
Φ∂
ka
a
r
. (9)
After that we use selected values wi, yi (λimax), Ài from
the indicated interval, parameter λimax from [11, 14, 15]
and we calculate values of functions yi(λ) using (8). For
this aim, after introducing the following notations we will
have the relations:
=
A
A
A
A
A
4
3
2
1
r
, B
wwww
wwww
wwww
=
−−−−−−−−
−−−−−−−−
−−−−−−−−
]
2
)(
exp[]
2
)(
exp[]
2
)(
exp[]
2
)(
exp[
]
2
)(
exp[]
2
)(
exp[]
2
)(
exp[]
2
)(
exp[
]
2
)(
exp[]
2
)(
exp[]
2
)(
exp[]
2
)(
exp[
2
4
2
max4
2
3
2
max3
2
2
2
max2
2
1
2
max1
2
4
2
max4
2
3
2
max3
2
2
2
max2
2
1
2
max1
2
4
2
max4
2
3
2
max3
2
2
2
max2
2
1
2
max1
λλλλλλλλ
λλλλλλλλ
λλλλλλλλ
MMMM
=
y
y
y
f
nλ
λ
λ
M
r
2
1
66
SQO, 7(1), 2004
T.A. Prokofiev et al.: Photoluminescence of Mn2+ ions individual bands of ...
In a vectorial form, we discover optimum values of the
matrix A conforming to minimum value Ô(Ài) in (8):
fAB
rr
=
fBABB tt
rr
= (10)
fBBBA tt
rr
1)( −=
where Bt � transpose of the matrix Â.
Using a personal computer, it is possible to take any
values yi(λimax) = Ai from the indicated interval sequen-
tially from the smaller to greater ones. However, allow-
ing the form of experimental PL spectra of ions Mn2+ in
ZnS:Mn chips and the plenty of the experimental results
of decomposing, obtained by us, the optimal ratio �
y(λmax)/ y(λimax) ≈ 1.14.
The PL spectra of ZnS:Mn single crystals, CMn = 5×
×10�3 and 1⋅10�2 gMnS/gZnS (g/g), at different values of
a degree of PD were used for checking the given method.
The obtained results are submitted in Fig. 3. According
to them, the most considerable changes of an emission
power in PD process is characteristic for the band with
λmax =578 nm. The general change of an emission power
of remaining individual bands is comparable to changes
of the given band. Let is take into account, that this per-
sonal band is connected with MC of glow arranged near
to defective places of crystal lattice � of dislocations and
dot defects undergoing the most considerable change in
PD process. The results of decomposition correlate well
with the known data [20-23].
The analysis of the �function of an error� � ∆A(λ)
view (Fig. 4) gives the completely definite result. This
function has the large values in a wavelength interval
λ = 510÷560 and 650÷670 nm conforming to boundaries
of an integral PL spectrum. The most likely, it is con-
nected with some little changes of the ratio �signal to
noise� during the experiment. The view of ∆A(λ) func-
tion completely coincides with the view of the Gauss func-
tion having a maximum in the range of 618÷620 nm, in
the interval of λ = 605÷630 nm. Also, we obtained the
appearance of the second maximum in PL spectra of the
deformed ZnS:Mn single crystals at λ = 606÷608 nm, the
temperature of experiment T = 77 K and concentration
of manganese CMn = 1⋅10�2 g/g. Most legibly, it was ob-
served at λexit = 396 nm (Fig. 5). All that gives the basis
to suppose availability in the given place at least one
more individual band.
The data of other works about existence of this band
are rather various. In [4], the given band observed at EL
and cathodoluminescence with a maximum in the range
5
20
0
10
15
20
25
30
4
4
3
1
2
8 106
S
,
a
rb
.
u
n
.
5
20
10
15
20
25
4
1
2
3
4
8 106
S
,
a
rb
.
u
n
.
b
Fig. 3. Relations of integral brightness of individual bands of ions
Mn2+ in ZnS:Mn single crystals at a different degree of PD � ε.
CMn = 5⋅10�3 g/g (a) and 1⋅10�2 g/g (b), λexit = 557 (1), 578 (2),
600 (3), 635 nm (4).
1
550
0
2
3
600
3
1
2
4
5
650
a
1
550
0
600 650
2
3
2
1
4
3
5
6
b
Fig. 4. The deviation of the sum of approximating functions from
an experimental PL spectrum of ZnS:Mn single crystals for vari-
ous degree of PD. CMn = 5⋅10�3 g/g (a), ε = 0 (1); 1.57 (2); 1.8 (3);
3.8 (4); 4.33 (5); 9.35 % (6) and CMn = 1⋅10�2 g/g, ε =0 (1); 1.57 (2);
1.78 (3); 3.8 (4); 4.63 (5); 8.7%(6) (b).
T.A. Prokofiev et al.: Photoluminescence of Mn2+ ions individual bands of ...
67SQO, 7(1), 2004
of 616±2 nm. In the authors opinion, it is conditioned by
the glow of MCs arranged in the bulk of the crystal lat-
tice with a small concentration of dot defects obtaining
excitation energy due to direct absorption. In [24], the
given band was secured with a maximum close to
λ = 606÷610 nm. According to [24], the glow in this area
of PL spectrum is conditioned by complex centres con-
sisting of two or more defects, structure of which could
include vacancy of sulphur. Here it is necessary to allow
that in [24] samples differed a little from the samples used
in [4] and in our researches. So, according to the data
[24], during growth of crystals ZnS:Mn from melt by the
Bridgeman method of the, the manganese was added into
the melt as MnS2. Its concentration was much larger
(1.9 mass %) than in our case. Therefore, formation of
complex centres at such activator concentrations is quite
possible.
Binding the obtained experimental results and data of
works [4, 11, 24] with results of our decomposition, it is
possible to say that in the spectral range including λmax =
= 618�620 nm without doubts exists at least one new ele-
mentary individual emission band. This indicates a view
of a �function of an error� close to the normal cumulative
distribution Gauss function in the range λ = 605�630 nm
and presence of the second peak in PL spectra.
References
1. M.F. Bulanyi, A.V. Kovalenko, V.I. Klimenko, B.A. Polezaev,
Features of crystal structure and luminescence ZnS:Mn //
Inorganic materials, 39(5), pp. 529-533 (2003), (in Russian).
2. M.F. Bulanyi, A.I. Gorban, A.V. Kovalenko, About reso-
nance transmission of excitation energy in ZnS:Mn crystals
in cases of photo- and electroluminescence // Optics and
spectr. (OAS), 94(3), pp. 436-440 (2003), (in Russian).
3. M.F. Bulanyi, B.A. Polezaev, T.A. Prokofiev, About the
nature of manganese centres of glow in single crystals of zinc
sulphide // Semicond. (St. Petersburg), 32(6), pp. 673-675
(1998).
4. N.D. Borisenko, V.I. Klimenko, B.A. Polezaev, Influencing
of a method of excitation on a radiation spectrum of manga-
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0
l, nm
I
,
a
rb
.
u
n
.
560 580 600 620 640
0.4
0.8
3
1
2
Fig. 5. PL spectra of ZnS:Mn single crystals � λexit = 396 nm,
Ò = 77 K, CMn = 1⋅10�2 g/g at a different degree of PD: ε = 0 (1),
1.57 (2); 1.78 % (3).
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