Influence of Mn doping on ZnO defect-related emission
Defect-related emission in undoped and doped with manganese ZnO ceramics was investigated. Mn concentration Nᴹⁿ was varied from 10¹⁹ to 10²¹ cm⁻³. The samples were sintered for 3 hours in air at 1100 °C. The color of ZnO:Mn ceramics changed from yellow to reddish-brown with increasing Mn content. Ph...
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Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
2017
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| Cite this: | Influence of Mn doping on ZnO defect-related emission / T.R. Stara, I.V. Markevich // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 1. — С. 137-141. — Бібліогр.: 27 назв. — англ. |
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| citation_txt | Influence of Mn doping on ZnO defect-related emission / T.R. Stara, I.V. Markevich // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 1. — С. 137-141. — Бібліогр.: 27 назв. — англ. |
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| description | Defect-related emission in undoped and doped with manganese ZnO ceramics was investigated. Mn concentration Nᴹⁿ was varied from 10¹⁹ to 10²¹ cm⁻³. The samples were sintered for 3 hours in air at 1100 °C. The color of ZnO:Mn ceramics changed from yellow to reddish-brown with increasing Mn content. Photoluminescence (PL) spectra of the prepared samples were measured at room temperature and analyzed by Gaussian fitting. PL of undoped ceramics exhibited itself as an intense broad band peaking at about 550 nm. Two effects were shown to occur as a result of Mn doping: i) drastic quenching of self-activated PL accompanied by a gradual red-shift of the spectral boundary of the quenching with increasing the Mn content; ii) appearance of a new emission band peaking at 645 nm that becomes dominant in the PL spectrum at Nᴹⁿ = 10²⁰ cm⁻³. The observed effects were believed to be due to reabsorption of self-activated ZnO emission by Mn-related centers. The following recombination in excited centers was supposed to occur by both radiative and nonradiative ways, the former being responsible for the 645 nm PL band.
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Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 137-141.
doi: https://doi.org/10.15407/spqeo20.01.137
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
137
PACS 81.05.Dz, 81.05.Je
Influence of Mn doping on ZnO defect-related emission
T.R. Stara, I.V. Markevich
V. Lashkaryov Institute of Semiconductor Physics, NAS of Ukraine,
41, prospect Nauky, Kyiv 03028, Ukraine
Phone: +38(044)525-72-34; e-mail: stara_t@ukr.net
Abstract. Defect related emission in undoped and doped with manganese ZnO ceramics
was investigated. Mn concentration NMn was varied from 1019 to 1021 cm–3.The samples
were sintered for 3 hours in air at 1100 °C. The color of ZnO:Mn ceramics changed from
yellow to reddish-brown with increasing the Mn content. Photoluminescence (PL)
spectra of prepared samples were measured at room temperature and analyzed by
Gaussian fitting. PL of undoped ceramics exhibited itself as intense broad band peaking
at about 550 nm. Two effects were shown to occur as a result of Mn doping: i) drastic
quenching of self-activated PL accompanied by gradual red-shift of spectral boundary of
the quenching with increasing the Mn content; ii) appearance of a new emission band
peaking at 645 nm that becomes dominant in the PL spectrum at NMn = 1020 cm–3. The
observed effects were believed to be due to re-absorption of self-activated ZnO emission
by Mn-related centers. The following recombination in excited centers was supposed to
occur by both radiative and nonradiative ways, the former being responsible for 645 nm
PL band.
Keywords: ZnO ceramics, photoluminescence.
Manuscript received 11.10.16; revised version received 25.01.17; accepted for
publication 01.03.17; published online 05.04.17.
1. Introduction
Zinc oxide doped with manganese attracts much
attention due to the influence of this dopant on ZnO
varistor behavior and magnetic properties. Thus, the
majority of research is focused on the electrical and
magnetic characteristics of this material, whereas
information on ZnO:Mn light emission is rather scarce.
The latter can be accounted for by the fact that ZnO:Mn,
contrary to some other II-VI compounds (ZnS:Mn,
ZnSe:Mn, CdS:Mn), exhibits quite weak emission. It has
been shown that doping ZnO with Mn results in
suppression of self-activated luminescence [1-6]. This
effect, however, was not investigated in detail, and its
mechanism was not decisively established. In addition,
the presence of Mn-related band in ZnO:Mn emission
spectrum is still a matter of debate. Some authors believe
that a new emission band arises due to Mn doping [7-
10], while the others assert that only redistribution of the
intensities of initially present emission bands occurs [2-
5]. Thus, to understand the mechanisms of the processes
that result in modification of ZnO emission by the Mn
doping further study is required. One can expect that the
clarification of these mechanisms will give the
possibility to control the emission in this material. In this
work, the influence of Mn content on defect-related
photoluminescence (PL) in ZnO:Mn ceramics was
investigated in order to clarify the origin of suppression
of ZnO emission by Mn doping.
2. Experimental procedure
Undoped and doped with manganese ZnO ceramics were
prepared. The samples were formed of the mixture of
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 137-141.
doi: https://doi.org/10.15407/spqeo20.01.137
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
138
Fig. 1. PL (a) and PLE (b) spectra of ZnO:Mn ceramics with NMn = 0 (1); 1·1019 (2); 1·1020(3) and 1·1021cm–3 (4).
ZnO powder (99.99% purity) with distilled water or
MnSO4 aqueous solution. Mn content NMn was varied
from 1019 to 1021 cm–3. The samples were dried at room
temperature, sintered in air for 3 hours at 1100 °C and
cooled with the furnace. Firm and dense ceramics with
the average sizes 8×3×2 mm were obtained. The color of
the doped samples changed from yellow to reddish-
brown with increasing the Mn content. The ceramics
were cut transversally, and PL spectra in the
400…800 nm range as well as PL excitation (PLE)
spectra in 250…500 nm range were measured from the
cleft surface at room temperature. Xe-lamp light passing
through grating monochromator was used as an exciting
source.
3. Results and discussion
The PL spectra of undoped and doped with Mn samples
manifest themselves as unstructured broad bands
(Fig. 1a). It is seen that drastic weakening of emission
and gradual red-shift of PL band maximum occur with
increasing the Mn content. PLE spectra of the observed
bands exhibit the only maximum whose position
coincides with that of free exciton (Fig. 1b), which is
characteristic for defect-related emission in ZnO [11]. A
slight red-shift of this maximum from 3.26 to 3.22 eV
takes place with increasing NMn from 0 to 1021 cm–3.
Such an effect is usually observed in ZnO:Mn samples at
a low Mn content (< 2 mol.%) and has been attributed to
bandgap decrease caused by exchange interaction
between d electrons of Mn and s and p electrons of the
host bands [7, 12].
It should be noted that quenching the visible
emission as well as its red-shift as a result of Mn doping
were earlier observed in ZnO ceramics, films and
nanostructures [1-6] and were often ascribed to
redistribution of green and orange PL bands intensities
due to suppression of self-activated green emission [2-
6]. This suppression was accounted for by the decrease
of concentrations of zinc interstitials Zni and/or oxygen
vacancies VO as a result of Mn incorporation [2-5, 13].
However, it is known that, in addition to self-activated
green band peaked at about 2.40 eV (510-520 nm) [14-
16], another one peaked at about 2.30 eV (530-540 nm)
and related to residual Cu impurity is usually present in
PL spectrum of intentionally undoped ZnO [14-16]. The
intensity of this Cu-related band in the samples prepared
in air or oxygen ambient is usually higher than that of
the self-activated one [15, 16]. Besides, as Fig. 1a
shows, quenching the visible emission by Mn doping
takes place not only in green but also in orange spectral
region.
It was stated that in undoped ZnO defect-related
emission consisted of several overlapping bands,
namely, of two abovementioned green ones as well as
self-activated orange at 2.03 eV (610 nm) and red at
1.72 eV (720 nm) [14, 16]. To clarify modification of
each of these bands due to Mn doping, deconvolution of
PL spectra by Gaussian fitting was made for both
undoped and Mn-doped samples (Fig. 2).
It is seen that in undoped samples the self-activated
green band is rather weak and the Cu-related one
dominates in the PL spectrum (Fig. 2a). In the samples
with NMn = 1·1019cm–3, the self-activated green band
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 137-141.
doi: https://doi.org/10.15407/spqeo20.01.137
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
139
1.6 2.0 2.4 2.8
0
10
20
30
40
1.6 2.0 2.4
0
5
10
15
1.5 2.0 2.5
0.0
0.5
1.0
1.5
2.0
1.6 2.0 2.4 2.8
0
10
20
30
40
b
c
PL
in
te
ns
ity
, a
.u
.
Energy, eV
d
a
PL
in
te
ns
ity
, a
.u
.
Fig. 2. Gaussian deconvolution of PL spectra for undoped (a) and doped samples with NMn = 1·1019 (b), 1·1020 (c) and
1·1021cm–3 (d).
disappears in fact, and the intensity of Cu-related band
becomes lower than that of the orange one;
simultaneously, a new red-orange band peaking at
1.92 eV (645 nm) appears (Fig. 2b). At NMn = 1020cm–3,
disappearance the Cu-related emission and weakening
the orange band with respect to the red one occur, while
the PL band at 1.92 eV (645 nm) becomes dominant in
PL spectrum (Fig. 2c). At NMn = 1·1021cm–3, only
1.72 eV (720 nm) and 1.92 eV (645 nm) bands are
observed, decreasing the intensity of the former with
respect to that of the later takes place (Fig. 2d). Thus,
two effects demonstrate themselves under Mn doping:
i) suppression of initial PL, the effect of enhancing and
extending from green to red spectral region with
increasing the Mn content; ii) appearance of a new PL
band at 1.92 eV (645 nm).
The reported data on ZnO:Mn materials show that
doping ZnO with Mn results in appearance of absorption
in the visible spectral region, which exhibits itself as an
unstructured “tail” in the absorption spectra [12, 17-22].
The intensity of this tail arises, and its spectral boundary
shifts toward lower energies with increasing the Mn
content [12, 17, 19, 21, 22], which produces at first
yellow, then orange and at last reddish-brown color of
the samples [2, 19, 22]. This effect was attributed to
absorption of incident photons by MnZn
2+ ions caused by
intra d-shell electron transitions from the ground to
excited states [17, 19]. The absence of any structure in
the absorption tail leads to supposition that these excited
states are located in some band continuum [17, 23, 24].
The origin of this absorption tail, however, requires
further study. One should expect that formation of this
absorption “tail” will result in re-absorption of self-
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 137-141.
doi: https://doi.org/10.15407/spqeo20.01.137
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
140
activated PL by Mn-related centers and, so, to quenching
the emission caused by native and Cu-related defects.
It is known that intense emission bands in the
spectral region of 2.07…2.14 eV (580…600 nm) appear
in ZnS, ZnSe, CdS and CdSe compounds due to doping
with Mn, which is ascribed to intra-shell 4T1–6A1
transitions in Mn2+ ions incorporated to the host lattice
[24]. At the same time, the presence of Mn-related
emission in ZnO:Mn is thus far a subject of debate.
Some authors affirm that this emission is completely
absent and only nonradiative recombination in excited
Mn-related centers occurs [2, 3, 24]. At the same time,
PL bands at 2.12 eV (586 nm) [25], 2.07 eV (600 nm)
[7], 1.95 eV (636 nm) [8] and 1.91 eV (650 nm) [9] were
found in doped with manganese ZnO thin films [8, 25],
ceramics [9] and nanopowders [7], which was ascribed
to the radiative intra-shell transitions in Mn ions. Intense
emission bands at 2.0 eV (620 nm) and 1.69 eV
(730 nm) were also observed in electroluminescence
spectra of ZnO:Mn ceramics [26]. Narrow green PL
bands at 2.36 eV (526 nm) and 2.34 eV (530 nm) with
specific PLE spectra were revealed in ZnO:Mn
nanopowders [8] and ceramics [1], accordingly. The
band at 2.34 eV appeared only after additional annealing
at 900 °C of sintered at 1200 °C ceramics, which was
ascribed to changes in the intrinsic defect concentration
[1]. The aforementioned PL band at 1.92 eV (645 nm) in
our ZnO:Mn ceramics should be also believed to be
caused by Mn-related centers. In fact, this emission
appears under doping ZnO with Mn and enhances with
increasing the Mn content side by side with suppression
of the other PL bands. The weakness of Mn-related
emission in ZnO:Mn can be accounted for by
supposition that recombination in excited Mn ions can
occur by both radiative and nonradiative ways, the later
being dominant.
The reported data on ZnO:Mn emission show that
the intensity and spectral position of Mn-related PL band
in different samples depend essentially on the
preparation technique. This effect was accounted for by
different sites of Mn ions in the host lattice [8] as well as
their interaction with Zni [2, 5, 13] and VO [1-5]. The
possibility of Mn cluster formation also should be taken
into account [6, 27]. To elucidate the influence of native
defects on Mn-related emission in ZnO:Mn ceramics
further investigations are planned.
4. Conclusion
To elucidate the effect of Mn doping on ZnO defect-
related emission, PL spectra of ZnO ceramics undoped
and doped with manganese were measured and analyzed
using Gaussian fitting. As a result of Mn doping,
quenching all the self-activated PL bands was observed,
gradual red-shift of spectral boundary of this quenching
from the green to red spectral region taking place with
increasing the Mn content from 1019 to 1021 cm–3.
Simultaneously, it was found appearance of a new PL
band peaking at 1.92 eV (645 nm) that became dominant
in PL spectra at NMn = 1020 cm–3. As ZnO doping with
Mn is known to cause formation of the absorption “tail”
in the visible spectral range, the quenching effect can be
accounted for by the re-absorption of self-activated PL
by Mn-related centers. This explanation is in accordance
with the change of sample color from yellow to reddish-
brown with increasing the Mn content, which is
accompanied by the red shift of PL quenching boundary.
Recombination in the excited Mn-related centers has
been supposed to occur by both radiative and
nonradiative ways. The former was believed to be
responsible for 1.92 eV (645 nm) PL band. The
weakness of this emission leads to the conclusion that
the nonradiative process is dominant.
Acknowledgment
This research has been financially supported by National
Academy of Sciences of Ukraine (project III-4-16).
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|
| id | nasplib_isofts_kiev_ua-123456789-214902 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 1560-8034 |
| language | English |
| last_indexed | 2026-03-21T12:40:17Z |
| publishDate | 2017 |
| publisher | Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
| record_format | dspace |
| spelling | Stara, T.R. Markevich, I.V. 2026-03-03T11:00:52Z 2017 Influence of Mn doping on ZnO defect-related emission / T.R. Stara, I.V. Markevich // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 1. — С. 137-141. — Бібліогр.: 27 назв. — англ. 1560-8034 PACS: 81.05.Dz, 81.05.Je https://nasplib.isofts.kiev.ua/handle/123456789/214902 https://doi.org/10.15407/spqeo20.01.137 Defect-related emission in undoped and doped with manganese ZnO ceramics was investigated. Mn concentration Nᴹⁿ was varied from 10¹⁹ to 10²¹ cm⁻³. The samples were sintered for 3 hours in air at 1100 °C. The color of ZnO:Mn ceramics changed from yellow to reddish-brown with increasing Mn content. Photoluminescence (PL) spectra of the prepared samples were measured at room temperature and analyzed by Gaussian fitting. PL of undoped ceramics exhibited itself as an intense broad band peaking at about 550 nm. Two effects were shown to occur as a result of Mn doping: i) drastic quenching of self-activated PL accompanied by a gradual red-shift of the spectral boundary of the quenching with increasing the Mn content; ii) appearance of a new emission band peaking at 645 nm that becomes dominant in the PL spectrum at Nᴹⁿ = 10²⁰ cm⁻³. The observed effects were believed to be due to reabsorption of self-activated ZnO emission by Mn-related centers. The following recombination in excited centers was supposed to occur by both radiative and nonradiative ways, the former being responsible for the 645 nm PL band. This research has been financially supported by the National Academy of Sciences of Ukraine (project III-4-16). en Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України Semiconductor Physics Quantum Electronics & Optoelectronics Influence of Mn doping on ZnO defect-related emission Article published earlier |
| spellingShingle | Influence of Mn doping on ZnO defect-related emission Stara, T.R. Markevich, I.V. |
| title | Influence of Mn doping on ZnO defect-related emission |
| title_full | Influence of Mn doping on ZnO defect-related emission |
| title_fullStr | Influence of Mn doping on ZnO defect-related emission |
| title_full_unstemmed | Influence of Mn doping on ZnO defect-related emission |
| title_short | Influence of Mn doping on ZnO defect-related emission |
| title_sort | influence of mn doping on zno defect-related emission |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/214902 |
| work_keys_str_mv | AT staratr influenceofmndopingonznodefectrelatedemission AT markevichiv influenceofmndopingonznodefectrelatedemission |