ВПЛИВ СУПЕРПАРАМАГНІТНИХ НАНОЧАСТИНОК Fe3O4 НА СПЕКТРАЛЬНО-ЛЮМІНЕСЦЕНТНІ ВЛАСТИВОСТІ СФОРМОВАНИХ В СТАЦІОНАРНИХ МАГНІТНИХ ПОЛЯХ МЕЗОСТРУКТУРНИХ ПЛІВОК SiO2/P123/Rh6G/Fe3O4
The effect of superparamagnetic Fe3O4 nanoparticles (NPs) on the spectral luminescence properties of homogeneous optically transparent mesostructured silica films of SiO2/P123/Rh6G/Fe3O4, containing {P123 (Rh6G)} micelles consisting of Pluronic 123 with encapsulated Rh6G, a...
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| Date: | 2020 |
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| Main Authors: | , , , , , |
| Format: | Article |
| Language: | English |
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V.I.Vernadsky Institute of General and Inorganic Chemistry
2020
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| Online Access: | https://ucj.org.ua/index.php/journal/article/view/123 |
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Ukrainian Chemistry Journal| _version_ | 1871465409325039616 |
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| author | Grebennikov, Volodimir Leonenko , Evgen Manorik, Petro Romanovska, Natalia Kobylinska, Natalia Shulzhenko, Olexandr |
| author_facet | Grebennikov, Volodimir Leonenko , Evgen Manorik, Petro Romanovska, Natalia Kobylinska, Natalia Shulzhenko, Olexandr |
| author_institution_txt_mv | [
{
"author": "Volodimir Grebennikov",
"institution": "L.V. Pisarzhevskii Institute of Physical Chemistry of National Academy of Science of Ukraine, Nauki av. 31, Kyiv, Ukraine"
},
{
"author": "Evgen Leonenko ",
"institution": "L.V. Pisarzhevskii Institute of Physical Chemistry of National Academy of Science of Ukraine, Nauki av. 31, Kyiv, Ukraine"
},
{
"author": "Petro Manorik",
"institution": "L.V. Pisarzhevskii Institute of Physical Chemistry of National Academy of Science of Ukraine, Nauki av. 31, Kyiv, Ukraine "
},
{
"author": "Natalia Romanovska",
"institution": "L.V. Pisarzhevskii Institute of Physical Chemistry of National Academy of Science of Ukraine, Nauki av. 31, Kyiv, Ukraine "
},
{
"author": "Natalia Kobylinska",
"institution": "Taras Shevchenko National University of Kyiv., 64\/13, Volodymyrska str., Kyiv, Ukraine"
},
{
"author": "Olexandr Shulzhenko",
"institution": "L.V. Pisarzhevskii Institute of Physical Chemistry of National Academy of Science of Ukraine, Nauki av. 31, Kyiv, Ukraine"
}
] |
| author_sort | Grebennikov, Volodimir |
| baseUrl_str | https://ucj.org.ua/index.php/journal/oai |
| collection | OJS |
| datestamp_date | 2026-07-22T08:23:42Z |
| description | The effect of superparamagnetic Fe3O4 nanoparticles (NPs) on the spectral luminescence properties of homogeneous optically transparent mesostructured silica films of SiO2/P123/Rh6G/Fe3O4, containing {P123 (Rh6G)} micelles consisting of Pluronic 123 with encapsulated Rh6G, and formed in stationary magnetic fields (MF) with an induction of less than 500 mT, was investigated. It was shown that, unlike SiO2/P123/Rh6G, the spectral and luminescent properties of SiO2/P123/Rh6G/Fe3O4 films depend on the MF used during their formation, and a gradual decrease in the band intensities in Rh6G spectra and quenching of luminescence with increasing of MF induction was observed. It is associated with a decrease in the monomer fraction and an increase in the fraction of non-luminescent Rh6G H-aggregates in micelles due to the interaction intensifying in the MF (formation of Fe3+ -O bonds) of superparamagnetic NPs with micelles {P123 (Rh6G)}, oriented in the MF, which leads to a gradual deformation of micelles and accumulation in them of H-aggregate. The dependences of the changes in the absorption bands intensity and fluorescence of the monomeric form of Rh6G in the spectra of the films on the changes in the magnetic induction of the MF are described by an exponential function, and the ratio of the fluorescence intensities of the SiO2/P123/Rh6G films to the fluorescence intensities of the SiO2/P123/Rh6G/Fe3O4 films linearly depends on the induction of MF, which they are able to "remember", which is manifested in the values of fluorescence intensities. |
| doi_str_mv | 10.33609/0041-6045.86.2.2020.78-96 |
| first_indexed | 2025-09-24T17:43:23Z |
| format | Article |
| fulltext |
Фізична хімія
© V.N. Grebennikov, E.A. Leonenko, P.A. Manorik, N.I. Romanovska, N.G. Kobylinska,
A.V. Shulzhenko , 2020
78 ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2
УДК 535.373.2 doi: 10.33609/0041-6045.86.2.2020.78-96
V.N. Grebenni kov*, E.A. Leonenko, P.A. Manori k, N.I. Romanovska, N.G.
Kobyli nska**, A.V. Shul zhenko
THE INFLUENCE OF SUPERPARAMAGNETIC Fe3O4 NANOPARTICLES ON
SPECTRAL AND LUMINESCENT PROPERTIES OF MESOSTRUCTURED
SiO2/P123/Rh6G/Fe3O4 FILMS FORMED IN STATIONARY MAGNETIC FIELDS
*L.V. Pisarzhevsky Institute of the Physical Chemistry of the National Academy of Science of
Ukraine, Prospect Nauki 31, Kyiv, Ukraine.
** Taras Shevchenko National University of Kyiv 64/13, Volodymyrska Street, City of Kyiv,
Ukraine, 01601
* E-mail: _vng@ukr.net
The effect of superparamagnetic Fe3O4 nanoparticles (NPs) on the spectral luminescence
properties of homogeneous optically transparent mesostructured silica films of
SiO2/P123/Rh6G/Fe3O4, containing {P123 (Rh6G)} micelles consisting of Pluronic 123
with encapsulated Rh6G, and formed in stationary magnetic fields (MF) with an
induction of less than 500 mT, was investigated. It was shown that, unlike
SiO2/P123/Rh6G, the spectral and luminescent properties of SiO2/P123/Rh6G/Fe3O4
films depend on the MF used during their formation, and a gradual decrease in the band
intensities in Rh6G spectra and quenching of luminescence with increasing of MF
induction was observed. It is associated with a decrease in the monomer fraction and an
increase in the fraction of non- luminescent Rh6G H-aggregates in micelles due to the
interaction intensifying in the MF (formation of Fe3+ -O bonds) of superparamagnetic
NPs with micelles {P123 (Rh6G)}, oriented in the MF, which leads to a gradual
deformation of micelles and accumulation in them of H-aggregate. The dependences of
the changes in the absorption bands intensity and fluorescence of the monomeric form of
Rh6G in the spectra of the films on the changes in the magnetic induction of the MF are
described by an exponential function, and the ratio of the fluorescence intensities of the
SiO2/P123/Rh6G films to the fluorescence intensities of the SiO2/P123/Rh6G/Fe3O4
films linearly depends on the induction of MF, which they are able to "remember", which
is manifested in the values of fluorescence intensities.
K e y w o r d s: hybrid mesostructured silica films, spectral luminescent properties,
Rhodamine 6G, Pluronic 123, nanoparticles, magnetite, a magnetic field.
INTRODUCTION. Interest in nanostructured materials is due to a noticeable change in
mailto:_vng@ukr.net
V.N. Grebennikov, E.A. Leonenko, P.A. Manorik, Romanovska, N.G. Kobylinska, A.V. Shulzhenko
ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2 79
their physical and physico-chemical
properties compared to the bulk material. In
this regard, nanocomposites from two or
more phases and hybrid materials with a
certain spatial mesostructure are attracting
attention. From the practical point of view,
the condensed mediums in the form of hybrid
organo-inorganic mesostructural films
containing molecules of fluorescent dye [1, 2]
and follow-up firmware nanodimensional
particles of subgroup of iron and their oxides
as a magnetic component of such hybrid
materials [3, 4] capable to interact with the
constant magnetic fields (MF) with an
induction < 500 mT are interesting. The use
of such NPs as the magnetic component of a
hybrid material is due to their unique
properties associated with a change in the
domain structure of such magnetically
ordered systems, acquisition of
superparamagnetic properties that appear
when particle sizes are reduced [5, 6], and
also with the presence of a hysteresis curve,
which plays an important role in
magnetization of reversal processes.
The influence of an external magnetic
field is manifested in changes in several
physical and physicochemical properties of
hybrid materials. Thus, the introduction of
NP γ-Fe oxide into the matrix of mesoporous
SiO2 allows obtaining materials with different
structural and magnetic properties [7]. The
use of MP makes it possible to improve the
sensory characteristics of some composite
materials with nickel NPs [8] and to propose
a sensitive element for a magnetically con-
trolled sensor. When studying the
photophysical properties of some organic flu-
orescent probes [3], an increase in the lumi-
nescence intensity was detected in the pres-
ence of an external constant magnetic field
with an induction of 1–20 mT.
The influence of local magnetic fields of
superparamagnetic magnetite NPs on the
spectral-kinetic properties of the triplet exci-
tation of Rh6G dye molecules embedded in
the polyvinyl alcohol polymer matrix was
shown in [4]. Changes in the absorption and
luminescence spectra of the dye are explained
by the formation of charge-transfer complex-
es.
The choice of magnetite as one of the
components of such hybrid materials is be-
cause magnetite particles behave like ferro-
magnetic only at temperatures below the
blocking temperature TB, which depends on
the particle volume and anisotropy value. A
decrease in the particle size to a single-
domain level at a temperature higher than TB
allows the magnetization vector of a single-
domain particle to fluctuate from one direc-
tion of the easy magnetization axis to another,
by analogy with an ideal paramagnet [9, 10].
Fe3O4 nanoparticles with sizes less than 24
nm at a temperature T = 300 K, which is
somewhat higher than TB and characterized
by a small relaxation time (<5·10 -2 s), ac-
quire superparamagnetic properties [9, 10]
and behave like paramagnet. Thus, in the ab-
sence of an external magnetic field at room
temperature, such a system of nanosized par-
ticles of magnetite behaves like an ensemble
of paramagnetic atoms with zero resulting
magnetization.
At the stages of preparation and for-
mation of thin hybrid mesostructured films
containing fluorescent dye molecules, the in-
troduction of magnetic NPs can affect the
spectral-luminescent and magnetic properties
of such materials, giving them new properties
The influence of superparamagnetic Fe3O4 nanoparticles on spectral…
80 ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2
that can change under the influence of an ex-
ternal magnetic field.
The aim of this work was to study the ef-
fect of superparamagnetic Fe3O4 NPs on the
spectral luminescence properties of homoge-
neous optically transparent mesostructured
silica SiO2/P123/Rh6G/Fe3O4 thin films con-
taining {P123 (Rh6G)} micelles consistent of
Pluronic 123 (R126) and incapsulated Rh6G
dye molecules and formed in stationary mag-
netic fields with an induction of less than 500
mT.
EXPERIMENT AND DISCUSSION OF
THE RESULTS. The following reagents
were used in the work: Iron chloride
tetrahydrate (FeCl2·4H2O; 98,0 %, Merck),
Iron chloride hexahydrate (FeCl3·6H2O;
99,0 %), tetraethoxysilane (TEOS), triblock
copolymer Pluronic P123 (Sigma-Aldrich),
hydrochloric acid (HCl 37%), EtOH (etha-
nol, anhydrous), Rh6G (Rhodamine 6G for
microscopy), distilled water.
X-ray diffractometry of the NPs was car-
ried out using a Panalytical X’Pert Prо pow-
der diffractometr with CuKα-radiation (λ =
1.540598 Å), monochromatized Ni-filter, at
room temperature in the range of angles 2θ
5-120° in increments of 0.040. The crystal-
line phases were identified using the JCPDS
(Joint Committee on Powder Diffraction
Standards) file cabinet. The morphology of
the NPs samples was studied using a JSM-
6610 LV scanning electron microscope
(JEOL, Japan) at a voltage of 20 kV with an
increase of up to 50.000 times. To enhance
the optical contrast, the samples were
sprayed with gold using the JFC-1600 Auto
Fine Coater (JEOL, Japan), an ultra-thin
spraying device.
FTIR-spectra of NPs and films as films
coated on КВr crystal plate were recorded on
spectrometer Perkin-Elmer Spectrum One.
The absorption and luminescence spec-
tra of the films before and after exposure to
an external magnetic field were recorded on
a Specord 210 spectrophotometer (Analytic
Jena) and a spectral setup in the "photon
counting" mode, respectively (wavelength of
exciting light 406 nm). The thickness of the
films was measured by the results of AFM
studies on atomic force microscopy
(Nanoscope IIIa (Nanoscope Digital Instru-
ment, USA). The magnitude of the magnetic
induction of the magnetic field was meas-
ured using a universal device Teslameter
43205/1 (Ukraine).
Synthesis of Magnetit (Fe3O4) nanopar-
ticles were obtained by chemical
coprecipitation of FeCl2 and FeCl3 salts in an
ammonia medium according to the modified
previously described method [11] by mixing
the salt solutions in the ratio 1:2 at a temper-
ature of 55°C and the subsequent addition of
25% ammonia solution. The resulting pre-
cipitate was separated by magnetic separa-
tion and washed thoroughly with EtOH. The
obtained magnetite nanoparticles were
stored in an ethanol solution without drying.
Preparation of film-forming sol Hybrid
silica films received by method of sin-
gle -stage sol-gel synthesis by the technique
described earlier [1]. To film-forming sol
with a molar ratio of reagents:
TEOS : Pluronic P123 : HCl : EtOH : H2O =1
: 6∙10-3 : 0,2 : 30 : 9,2 the calculated amount of
Rh6G dye (1∙10-3 M) and a magnetite (7,5∙10-3
g/ml) was added. For dispersion of compo-
nents the sol was subjected to ultrasonic pro-
cessing (10 min.), aged for 72 hours. Films
were obtained by applying a film-forming sol
V.N. Grebennikov, E.A. Leonenko, P.A. Manorik, Romanovska, N.G. Kobylinska, A.V. Shulzhenko
ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2 81
on a pre-cleaned substrate (glass 25 mm×20
mm) by spin-coating at a substrate rotation
speed of 1800 rpm-1 for 5 s. Films formed in a
constant magnetic field with the known induc-
tion. Thickness of the prepared films accord-
ing to the atomic forces microscopy (AFM)
was 200 ± 5 nanometers.
The magnetic field at which silica hy-
brid mesostructured films of the composi-
tion SiO2/P123/Rh6G and (#)SiO2/P123/
Rh6G/Fe3O4 were formed was created us-
ing N38 (Ni) permanent magnets made of
NdFeB alloy with the characteristics listed
in Table 1, in the form of a magnetic com-
posite module of a cylindrical shape (Fig. 1
а). To visualize the lines of magnetic in-
duction around the magnetic module the
program Vizimag 3.18 was used. In Fig. 1
а shows the locations of the formed hybrid
mesostructured (#) SiO2/P123/Rh6G/Fe3O4
films, where # is the number of the sample
that corresponds to the position (Fig. 1 а)
of the film in the field during its formation.
Samples of hybrid films of
(0) SiO2/P123/Rh6G/Fe3O4 and
(4) SiO2/P123/Rh6G were obtained outside
the field (B0 = 0).
Characterization of the obtained nano-
particles to investigate the phase content of
the Fe3O4, as well as to determine the aver-
age crystallite size, the method of XRD was
applied (Fig. 1 b).
T a b l e 1
The main characteristics of permanent magnets
brand N38 (Ni).
Residual induction, T 1,24
Induction coercive force, kA / m 915
Magnetization coercive force, kA / m 955
Diameter of a disk, mm 60
Height of disk, mm 15
The diffraction patterns identified seven
peaks at: 18.4 (111), 30.2 (220), 35.6 (311),
43.3 (400), 53.7 (422), 57.7 (511) and 62.9
(442). These peaks are typical for a phase
like spinel of the composition Fe3O4, i.e.,
for magnetite (250540-JCPDS). Iron oxides
nanoparticles are prone to oxidation, but the
absence of g-Fe2O3 (40142-JCPDS) peaks
and the intense black color of the powders in
the diffractogram indicate the absence of
significant impurities of this oxide in the
phase of the obtained Fe3O4.
On the diffractograms of the obtained
magnetite, there is a slight decrease in inten-
sity and broadening of the peaks, but no ad-
ditional peaks observed (Fig. 1 b). The aver-
age crystallite size of the obtained magnetite
calculated by the Scherrer formula [12] is 10
nm. In Fig. 1 c,d shows the data of electron
microscopy and the corresponding size dis-
tributions of the NPs of the obtained magnet-
ite. It is known that iron oxide nanoparticles
are prone to aggregation due to the high sur-
face energy inherent in finely dispersed
structures, which is confirmed by transmis-
sion microscopy (Fig. 1 d ).
An analysis of CEM microphotographs
of Fe3O4 (Fig. 1 c) indicates that the synthe-
sized materials, after drying are aggregates
consisting of smaller particles. The magnet-
ite NPs were obtained at a reaction solution
temperature of 55 °C and stored in an etha-
nol suspension. They are characterized by an
average particle size of ~ 9–11.0 nm (Fig. 1
d ), which is consistent with the calculation
data from XRD data.
As follows from the Fig. 1 e, curve 1 ) in
NPs spectra Fe3O4 together with the bands,
which can be attributed to valence and band-
ing vibrations of ethanol’s different groups
The influence of superparamagnetic Fe3O4 nanoparticles on spectral…
82 ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2
4000 3000 2000 1000
70
75
80
85
90
95
4
6
5
3
2
Т
, %
ν, cм-1
1
Fig. 1 а) Visualized lines of magnetic induction of the module of a cylindrical shape; 1, 2, 3 - loca-
tion of the formed hybrid mesostructured (#) SiO2/P123/Rh6G/Fe3O4 films in a magnetic field,
which correspond to the values of magnetic induction B, mT: 1 (B1 = 15), 2 (B2 = 100), 3 (B3 =
300). b) Diffraction patterns of magnetite and standard samples of magnetite (JCPDS file No.
250540) and hematite (JCPDS file No. 40142). ;. c)d) Microphotographs of scanning (c) and trans-
mission (d) electron microscopy with the corresponding size distribution curve of magnetite nano-
particles; e) FTIR-spectra of the samples (NPs and films) as films precipitated on КВr crystal plates:
1- Fe3O4 NPs; 2- P123/ Fe3O4 (60/1); 3- P123/Fe3O4 (30/1 ); 4- P123/ Fe3O4 (60/1 in MF); 5-
SiO2/P123/Rh6G/Fe3O4 (without MF); 6 -SiO2/P123/Rh6G/Fe3O4 (in MF).
20 40 60 80 100 120
0
50
100
150
200
250
40142-ICSD data
250540-ICSD data
Fe3O4
Ин
те
нс
ив
но
ст
ь
2 θ
2
1
3
50 mm
a b
c
e
d
V.N. Grebennikov, E.A. Leonenko, P.A. Manorik, Romanovska, N.G. Kobylinska, A.V. Shulzhenko
ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2 83
[ 13 ], there are a few bands (640,589,565
см-1) forming summary conture in region
500-700 см-1 , which according to [13, 14]
may be attributed to Fe-O valence stretching
bands (O of ethanol and in Fe3O4).
Analysis of the absorption spectra of
aqueous solutions of Rhodamine 6G and the
obtained films (Fig. 2 ) shows that in the
concentration range from 1∙10-6 M to 1∙10-4
M, the dye is in monomeric form. At the
used concentration of Rhodamine 6G
(>1∙10-4 M) both in solution and when its
molecules included in the solid matrix, two
main types of dimers formed as a result of
dimerization of dye molecules: H-dimer and
J-dimer [15]. The configuration of H-type
dimers is energetically more favorable than
the configuration of J-type dimers [16] with
a relatively small difference in energy ≤ 3
kT, which indicates the joint presence of
these configurations at room temperature.
The aggregation mechanism during the for-
mation of H dimers is explained by π-π in-
teraction of aromatic π systems of two
Rhodamine 6G molecules [2].
The influence of the aggregation of
Rhodamine 6G dye molecules (Rh6G) and
the concentration of Pluronic 123 in the
film-forming sol (SiO2 + P123 + Rh6G) on
the spectral-luminescent properties of the
formed silica hybrid films without magnetite
NPs is studied in [17].
Fig. 2 shows the absorption and fluores-
cence spectra of a film without NPs magnet-
ite (SiO2/P123/Rh6G), as well as the spectra
of thin hybrid films of the same composition
(SiO2/P123/Rh6G/Fe3O4), formed by dif-
ferent MF induction in the places shown in
Fig. 1a.
As follows from the Fig. 2 a, the absorp-
tion spectra of hybrid films correspond to the
monomeric form of Rh6G, which are charac-
terized by a vibronic shoulder [18 ] at λ1 =
501 nm [2,15,19,20] and the central maxi-
mum at λ2 = 534 nm, the intensity of which
depends on the amount of dye. The fluores-
cence spectra of hybrid films (Fig. 2 2Гр c)
are characterized by a band at λ = 562 nm,
which corresponds to the monomeric form
of the Rh6G molecule.
It follows from the experimental data
that an increase in the induction of the exter-
nal MF, in which films are formed, leads to a
sequential decrease in the intensity of the
absorption and fluorescence bands (Fig. 2 a,
Fig. 2 c and Table 2). However, in the pres-
ence of MF, such changes in the spectra of
samples of hybrid SiO2/P123/Rh6G films
without NPs were not observed, which indi-
cates the presence of interaction of Rh6G
molecules with superparamagnetic magnetite
NPs in samples of hybrid
SiO2/P123/Rh6G/Fe3O4 films.
Differential absorption and fluorescence
spectra of samples of hybrid films in Fig. 2 b
and fig. 2 d obtained by subtracting from the
spectrum of a SiO2/P123/Rh6G film the cor-
responding spectra of SiO2/P123/Rh6G/
Fe3O4 films formed at different values of
magnetic induction. On differential absorp-
tion spectra, as shown in Fig. 2 b, bands ap-
pear at λ1 = 501 nm and λ2 = 534 nm.
The numerical values for the difference
in the intensities of the absorption bands in
the electronic spectra of the film samples at
these wavelengths are given in Table 2, from
which it follows that the magnitudes of the
difference increase in the series under con-
sideration without changing the position of
the maxima of the absorption bands. An
The influence of superparamagnetic Fe3O4 nanoparticles on spectral…
84 ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2
Fig. 2. Absorption spectra (a), fluorescence (c) of hybrid mesostructured films (4) SiO2/P123/Rh6G
and (#) SiO2/P123/Rh6G/Fe3O4 (samples # = 0, 1, 2, 3) and the corresponding differential
absorption spectra (b) and fluorescence (d). Curves No.0, No.1, No.2, No.3 are obtained by
subtracting, respectively, the curves 0, 1, 2, 3 from curve 4 shown in Fig. 2 a and Fig. 2 c; λ1 = 501
nm, λ2 = 534 nm, λa = 542 nm; λ = 562 nm, λа = 604 nm.
exception is a sample No. 0 of the hybrid
mesostructured (0) SiO2/P123/Rh6G/Fe3O4
film, for which at B = 0, two broad bands of
low intensity with maximum peaks close to
505 and 542 nm appear in the differential
spectrum.
The appearance of a broad maximum in
the spectrum (at B = 0) in the region of 542
nm, as shown in Fig. 2 b indicates a change
in the environment of Rh6G monomeric
molecules encapsulated in micelles, possibly
as a result of donor-acceptor interaction or
interaction of micelles with super-
paramagnetic magnetite NPs with zero re-
sultant magnetization.
In the fluorescence spectra of the formed
hybrid mesostructured films (Fig. 2 c) bands
observed in the region λ = 562 nm, are char-
acteristic, according to [15,19], for Rh6G
monomeric molecules. This band is also pre-
sent in the differential fluorescence spectra
(Fig. 2 d). With an increase in the induction
V.N. Grebennikov, E.A. Leonenko, P.A. Manorik, Romanovska, N.G. Kobylinska, A.V. Shulzhenko
ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2 85
Fig. 3 . The effect of magnetic induction of MF on the difference in band intensities (No. 0, No. 1, No.
2, No. 3, see Fig. 2 b and Fig. 2 d) in the absorption spectra (ΔA) and luminescence (ΔI) of samples of
hybrid films with magnetite NPs; Changes in the absorption intensity A at λ2 = 534 nm (с) and the
fluorescence intensity I at λ = 562 nm (d) of the samples of hybrid mesostructured
SiO2/P123/Rh6G/Fe3O4 films as a function of magnetic induction (No. 0, No. 1, No. 2, No. 3, see Fig. 2
b and Fig. 2 d).
of MF, the intensity of the bands in the dif-
ferential fluorescence spectra of the film
samples decreases.
Fig. 3 shows the results of measure-
ments of the difference in the intensities of
the bands (No. 0, No. 1, No. 2, No. 3, see
Fig. 2 b and Fig. 2 d) in the absorption spec-
tra (ΔA, Fig. 3 a) and luminescence (ΔI, Fig.
The influence of superparamagnetic Fe3O4 nanoparticles on spectral…
86 ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2
T a b l e 2
The band intensities in the absorption and fluorescence spectra of hybrid films in MF and the dif-
ference between the band intensities in the spectrum of the SiO2/P123/Rh6G film and the band
intensities in the spectra of SiO2/P123/Rh6G/Fe3O4 films.
Sample of the
film
magnetic in-
duction B,
mТ
Bands intensity characteristics in the spectra of the films in magnetic
field:
absorption
(A λ, MFE, ΔA λ)
fluorescence
(I λ, MFE, ΔI λ)
λ1=501 nm λ2=534 nm λ=562 nm
A λ1 MFE,
% ΔAλ1 A λ2 MFE,
% ΔAλ2 I λ
MFE,
% ΔI λ
№0 (с Fe3O4) B0=0 0,092 0 0,009 0,147 0 0,009 15,624 0 2,69
№1(с Fe3O4) B1=15 0,091 1 0,010 0,140 5 0,016 14,392 7,9 3,92
№2(с Fe3O4) B2=100 0,088 4 0,013 0,132 10 0,024 12,304 21,2 6,01
№3(с Fe3O4) B3=300 0,085 8 0,016 0,125 15 0,031 11,600 25,8 6,72
SiO2/P123/Rh6G B0=0 0,101 - 0 0,156 - 0 18,312 - 0
3 b) samples of hybrid films with NP mag-
netite depending on the magnitude of the
magnetic induction. As can be seen from fig.
3, these curves tend to reach the shelf.
The magnitude of the magnetic field (MFE)
influence was estimated according to the ap-
proach proposed in [3] by changing in the
intensity of the bands in the absorption and
fluorescence spectra of the formed hybrid
films, which is caused by the magnetic field.
The MFE value was determined as
нн FFFMFE /%100)( ⋅−= λ , where λF and нF
are the intensities of the bands in the spectra
of the hybrid film in the magnetic field and at
B = 0 , respectively.
Moreover, for the intensity of the bands
in the absorption spectra of the hybrid film
λF = λA , нF = нA , and for the intensity in the
fluorescence spectra λF = λI , нF = нI . The cal-
culated MFE values are shown in table 2.
The observed effect of the influence of ex-
ternal MF induction on the change in the
Fig. 4. Dependence characterizing the
fluorescence quenching of magnetite-containing
hybrid mesostructured SiO2/P123/Rh6G/Fe3O4
films on the magnitude of the magnetic induction
(No. 0, No. 1, No. 2, No. 3 and Fig. 4d) used at
the formation of the films.
absorption intensity and luminescence intensity
0,00 0,05 0,10 0,15 0,20 0,25 0,30
0
10
20
30
40
No. 1
No. 2
No. 3
I*
/ (
I f
-I o
)
B, T
No. 0
V.N. Grebennikov, E.A. Leonenko, P.A. Manorik, Romanovska, N.G. Kobylinska, A.V. Shulzhenko
ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2 87
T a b l e 3
Parameters of the approximating curves describing the experimental data on the changes in the
maximum of absorption and fluorescence intensities in the spectra of hybrid mesoscopic
SiO2/P123/Rh6G/Fe3O4 films formed in MP.
λ,
nm
A0 Ан-A0 kA×103 λ,
nm
I0 Iн-I0 kI×103
501 0,084±0,001 0,008±0,001 7,0±0,9 562 11,68±0,19 3,86±0,24 20,8±4,6
534 0,124±0,001 0,021±0,001 12,0±0,9
of magnetite-containing mesostructured films
can be described by a general differential equa-
tion: )( 0FFkdBdF F −=− λλ in which λdF - is
the change in the intensity of the band (absorp-
tion, fluorescence), 0F - is the limiting value of
the change in intensity.
Integration of the differential equation
from the initial value нF (at B = 0) to λF , at
the current value of B, gives a logarithmic
response function
BkFFFF Fн −=−− )]/()ln[( 00λ that depends
linearly on the magnitude of the induction B,
in which the coefficient Fk characterizes the
sensitivity of magnetite-containing hybrid
mesostructured films to the influence of an
external MF.
By potentiating, we obtain general ex-
pressions for changing the band intensity in
the absorption and fluorescence spectra
)exp()( 00 BkFFFF Aн −−+=λ , which de-
scribe the experimental data in Fig. 6 with the
corresponding parameters of the approximat-
ing curves. The numbers of film samples in
Fig. 3 с and d correspond to their location in
a magnetic field during their formation, ac-
cording to Fig. 1 a. The calculated parameters
of the approximating curves are shown in Ta-
ble 3. Since for these films Ik are larger Ak ,
the sensitivity of the SiO2/P123/Rh6G/Fe3O4
hybrid film to the influence of an external MF
is maximum under fluorescence (MFE =
25.8%).
Dependence of the ratio of the fluores-
cence intensity of a film without magnetite
NPs in experimental value of the fluorescence
intensity of SiO2/P123/Rh6G/Fe3O4 films on
the magnitude of magnetic induction is
shown in Fig. 4. It can serve as a characteris-
tic of the degree of quenching of the fluores-
cence of these films by magnetite nanoparti-
cles.
Аs shown from the above results,
superparamagnetic magnetite NPs signifi-
cantly affect the spectral and luminescent
properties of mesostructured
SiO2/P123/Rh6G/Fe3O4 films formed in sta-
tionary magnetic fields with an induction of
less than 500 mT.
The observed effect of the magnetic field
used in the formation of hybrid (#)
SiO2/P123/Rh6G/Fe3O4 films on their spec-
tral-luminescent properties is due to the pres-
ence of Fe3O4 NPs in the films interacting
with magnetic field, since significant differ-
ences in the spectral-luminescent properties
of the SiO2/P123/Rh6G films, formed in the
MF and outside MF were not observed.
To understand the above facts and ex-
plain the possible mechanism of the effect of
the increasing magnitude of magnetic induc-
The influence of superparamagnetic Fe3O4 nanoparticles on spectral…
88 ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2
tion used in the formation of the studied hy-
brid (#) SiO2/P123/Rh6G/Fe3O4 films on
their spectral and luminescent properties,
some facts regarding the characteristics of the
Rh6G dye and its spectral – luminescent
properties, Fe3O4 NPs and other similar mate-
rials, and their interaction with MF were tak-
en into account.
From the analysis of the absorption spec-
tra of aqueous solutions [15] and hybrid films
[17] it is known that the dye (Rh6G) in the
concentration range from 1∙10-6 M to 1∙10-4
M is in monomeric form. In this case, a char-
acteristic band of the monomeric form (λ max
about 530 nm) with a vibronic arm (about
500 nm), which corresponds to a fluorescence
band with λ max about 560 nm, appears in the
spectrum.
With an increase in the concentration of
Rh6G both in solutions and in hybrid films,
two types of dimers H (λ max about 500 nm)
are formed, the band of which overlaps [18]
with a vibronic band (λ max about 500 nm),
and J (λ max about 550 nm), the relative con-
tent of which depends on various conditions
[15,18 ].
At room temperature, both types of di-
mers are formed due to the fact that the con-
figuration of H-type dimers is only slightly
energetically more favorable compared to the
configuration of J-type dimers (energy differ-
ence ≤ 3 kT) [16 ]. The aggregation mecha-
nism at the formation of H- dimers is ex-
plained by π-π interaction of aromatic π sys-
tems of two Rh6G molecules [2]. Along with
these dimers, so-called “intermediate”
(“oblique”) dimers (with angles of 0 о <θ
<90 о ) [15,20], having fluorescence spectra
are also formed. For Rh6G in the monomeric
form and in the form of oblique and J-type
dimers, in contrast to the H-type, lumines-
cence spectra are characteristic [15, 19, 20].
It was shown earlier that in the films
formed from a film-forming sol
(SiO2+Р123+Rh6G) (without magnetite
NPs), the formation of H- dimers is blocked
due to the encapsulation of Rh6G molecules
in micelles and such films retain luminescent
properties [17].
When films formed from the same film-
forming sol, but containing magnetite NPs,
in the absence of a MF, Fe3O4 NPs lose sol-
vent molecules (ethanol) during dip-coating,
which are both a dispersion medium and
NPs stabilizer, as a result of the interaction
of magnetite surface Fe3+ atoms with donor
atoms of oxygen of Pluronic 123. Indeed, the
Fe3+ atoms in the surface layer and in the
bulk of magnetite (Fe3+[Fe3+Fe2+]O4) are
nonequivalent, and the estimated number of
surface atoms, as shown in [21], depends on
the radius of the NPs and is 35 for NPs with
an average diameter of 10 nm.
In this case, to compensate for the sur-
face charge of NPs, apparently, new Fe3+ -О.
bonds should be formed. The more probable
areas where their formation is possible are
the more hydrophilic polyethylene oxide
fragments of P123 located on the periphery
of the micelle, in contrast to the more hydro-
phobic propylene oxide fragments that form
its core.
Moreover, Rh6G molecules can be lo-
cated both in polyethylene oxide and propyl-
ene oxide sites in the triblock copolymer mi-
celle, which is part of the
(0) SiO2/P123/Rh6G/Fe3O4 film.
If one assume that the reason for the
changes in the electronic spectra of
SiO2/P123/Rh6G/Fe3O4 films is the interac-
V.N. Grebennikov, E.A. Leonenko, P.A. Manorik, Romanovska, N.G. Kobylinska, A.V. Shulzhenko
ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2 89
tion of Fe3+ ions (which in an amount of
about 15 are present on the surface of mag-
netite NPs with an average size of 10 nm
[21]), for example, with amine nitrogen of
Rh6G look-like observed interaction of
magnetite NPs with humic acids [22] upon
their adsorption, then a shift in the maximum
of the dye absorption band observed. How-
ever, as it is evidenced by the results of the
experiment, this does not happen. Direct in-
teraction of Fe3O4 NPs with dye molecules
encapsulated in a micelle with P123 seems
unlikely.
In the absence of MF at room tempera-
ture, the magnetic moments of spherical
magnetite nanoparticles (10 nm) located in a
film-forming sol with micelles
{P123 (Rh6G)} are randomly oriented due to
thermal fluctuations.
Taking into account the above consider-
ations, the reasons for the changes in the
spectral-luminescent properties of the
(0)SiO2/P123/Rh6G/Fe3O4 film as compared
to the (4)SiO2/P123/Rh6G film that does not
contain magnetite NPs (Fig. 2 a, curves 0
and 4), Fig. 2 c, curves 0 and 4; Fig. 2 b,
curve No. 0, Fig.2 d, curve No. 0) become
clear. It should be noted that the intensity of
the vibronic shoulder (or the band corre-
sponding to the H-dimer) and the band cor-
responding to the monomer (Fig. 2 b, No. 0),
in contrast to the spectra for
(4)SiO2/P123/Rh6G (Fig. 2 a, No. 4) and
(0)SiO2/P123/Rh6G/Fe3O4 (Fig. 2 a, No. 0)
are comparable.
The formation of new Fe3+ - О bonds, in
which Fe atoms on the surface of Fe3O4 NPs
and oxygen donor atoms of P123 micelles
with Rh6G molecules encapsulated in them
in monomeric form participate, can cause mi-
celle deformation and contribute to the for-
mation of both intermediate and H- dimers.
This is consistent with a decrease in the in-
tensity of both bands (vibronic and related to
the monomeric form) both in the differential
absorption spectra (Fig. 2 b, No. 0) and in the
differential fluorescence spectra (Fig. 2 d, No.
0).
However, in contrast to the differential
absorption spectra (Fig. 2 b, curve No. 0),
where ∆А (λ max ≈562 nm) ≈ ∆А (λ max ≈604
nm), in the differential fluorescence spectra
(Fig. 2 d, curve No. 0) ∆Ι (λ max ≈562 nm) <
∆Ι (λ max ≈604 nm) and the observed decrease
in the intensity of the vibronic band is very
insignificant in contrast to the decrease in the
intensity of the monomer band.
This may indicate that, against the back-
ground of a noticeable decrease in the content
of the Rh6G monomeric form, the so-called
“oblique” dimers (with angles of 0о<θ<90о)
are formed in the system [15,19,20], having
fluorescence spectrum. The formation of the-
se dimers instead of H-dimers occurs appar-
ently due to insufficiently strong deformation
of the micellar structure.
When a film-forming sol with
superparamagnetic magnetite particles is
placed in a MF, NPs acquire additional poten-
tial energy, and their magnetic moments tend
to orient themselves along the lines of mag-
netic field induction.
As a result of the orienting action of
the constant magnetic field in the film-
forming ash (in the process of film for-
mation), the number of magnetite NPs with a
smaller angle formed between the magnetic
induction vectors and the magnetic moment
increases, as well as the number of NPs for
which the directions of the vectors coincide.
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90 ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2
The formation of a hybrid mesostructured
SiO2/P123/Rh6G/Fe3O4 film ends with a
“freezing” of the magnetic moments of the
NPs, which are oriented under the action of
the magnetic field, not randomly, but in a cer-
tain direction. The formation of a hybrid
mesotructured film with a larger magnetic
induction also ends with “freezing”, but with
a larger number of NPs oriented along the
lines of magnetic field induction.
Thus, the number of magnetite NPs in the
film-forming sol, for which the directions of
the vectors coincide, should increase with in-
creasing of magnetic field induction. In the
presence of a weak permanent MF at the
formation of a hybrid film from a film-
forming sol, a small part of the magnetite
NPs is magnetized, being oriented and
aligned along the lines of magnetic induction.
Considering the fact that, apparently,
Fe3O4 NPs are connected via surface iron at-
oms to donor oxygen atoms of P123 micelles,
such an orientation of NPs and their increas-
ing “aggregation” in the magnetic field with
increasing magnetic induction should lead to
increasing micelle deformation, which should
contribute to a decrease in fractions of Rh6G
monomers and their dimerization.
According to the calculations, the num-
ber of micelles in the reaction mixture was
1.4. 1016 (the calculation used the concentra-
tion of P123 and the known [23] content
(250 molecules) of P123 in one micelle), and
the amount of magnetite NPs was 6.16. 1016
(in the calculation we used a weight of Fe3O4
NPs, its density (5.17 g / cm3) and average
size (10 nm) of NPs). That is, in the resulting
reaction mixture, 4.4 NP Fe3O4 are account-
ed for one micelle. Despite the fact that this
value is an estimate, it gives an idea of the
ratio of the numbers of NPs and micelles in
the film. It follows that, with the formation
of “linear aggregates” of NPs and an in-
crease in their linear dimensions with in-
creasing magnetic field induction, micelle
deformations can be enhanced by increasing
z, q and p in the resulting complexes {{(NP)
q} Fez ... Op {Pluronic123 ( Rh6G) n} m]. Ac-
cording to the results of FTIR- spectra (Fig.
1e), the interaction of iron atoms on the sur-
face of Fe3O4 NPs with P123 oxygen atoms
(curve 2) leads to redistribution of the band
intensities observed in the spectrum of Fe3O4
NPs (curve 1). The band in the region of
1200-950 cm-1 with a maximum of about
1107 cm-1 is, according to [24 ], the total
contour, consisting of a group of bands that
can be attributed to νas and νs С-О-С and С-
С of the ether group P123. The band in the
region of 500–700 cm – 1 with a maximum of
about 590 cm– 1 consists of three bands
(640.589, 565 cm – 1), which according to
[13,14] can be attributed to the Fe – O
stretching vibrations with the participation of
O in Fe3O4 and P123. With a twofold in-
crease in the ratio of NPs to P 123, the mag-
nitude of the ratio of the intensities of the
bands with maxima near 590 cm-1 and 1107
cm-1 (Fig. 3, curves 2 and 3) increases from
0.15 to 0.18. In the spectra of SiO2
{Pluronic123 (Rh6G)} Fe3O4 films obtained
outside the magnetic field (curve 4) and in
the magnetic field (curve 5), the ν (Fe-O)
band with a maximum of about 590 cm-1 is
retained, however, with insignificant chang-
es in its total contour due to the redistribu-
tion of the intensities of its constituent
bands. Moreover, comparing its intensity
with the band intensity in the region of
1200–950 cm– 1 with a maximum of about
V.N. Grebennikov, E.A. Leonenko, P.A. Manorik, Romanovska, N.G. Kobylinska, A.V. Shulzhenko
ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2 91
1107 cm– 1 becomes impossible due to the
overlapping of the latter with more intense
bands, which can be attributed [14] to Si-O
stretching vibrations.
With this in mind, and since solvents,
including alcohol, are removed during the
formation of the film, it can be assumed that
at least part of the bands in the region of
500–700 cm– 1 is due to stretching Fe – O
vibrations involving iron atoms on the NPs
surface, bound to ether oxygen donor atoms
of P123.
According to experimental data, the use of
MF in the preparation of
(#) SiO2/P123/Rh6G/Fe3O4 films enhances the
manifestation of the influence of NPs on their
spectral and luminescent characteristics. As
can be seen from the fluorescence spectra
(Fig. 2 c) and the differential fluorescence
spectra (Fig. 2 d), as the magnetic flux density
increases, the intensities of the fluorescence
bands (λmaxс≈ 562 nm) and the shoulder
(λmaxс≈ 604 nm) decrease.
When using a weak magnetic field of 100
mT (Fig. 2 d, curve No. 1) in the differential
fluorescence spectrum, as well as the differen-
tial absorption spectrum (Fig. 2 b, curve No.
1), with a slight decrease in the intensity of the
vibronic (dimeric, λmax≈ 604 nm) band again
there is a significant decrease in the band in-
tensity (λmax≈ 562 nm) compared to sample
No. 0 (Fig. 2 d, curve No. 0) with insignificant
changes in the band (λmax≈ 604 nm) intensity
compared to sample No. 0 (Fig. 2 d , curve
No. 0 and Fig. 2 b, curve No. 0 respectively,).
Based on this, it can be assumed that a
significant decrease in the intensity of the
band of the monomeric form of Rh6G in the
differential fluorescence spectrum when us-
ing a weak (100 mT) MF (Fig. 2 d, curve
No. 1) is apparently due to further defor-
mation of micelles containing Rh6G due to
an increase in the number of nanoparticles
“linear aggregates” oriented in the field with
a nonzero magnetic moment and an increase
in their size, which leads to a further in-
crease in the number of fluorescent
“oblique” dimers due to a decrease in the
number of the monomeric form Rh6G.
As can be seen from fig. 2 d, the ob-
served difference in the intensity of the dif-
ferential spectra of the samples (No. 0, No.
1, No. 2, No. 3) is significantly larger at
λmaxс≈ 562 nm compared to λmaxс≈ 604 nm.
However, in this case, with an increase in
the magnetic induction of the magnetic field
from 100 mT (Fig. 2 d, curve No. 1) to 200
mT (Fig. 2 d, curve No. 2), a sharp drop
(jump) in the intensity of the bands (λmaxс≈
562 nm and λmaxс≈ 604 nm ) occurs and
starting from sample No. 2 with an increase
in the magnetic induction of MF from 200
mT to 300 mT (samples No. 2, No. 3), the
decrease in band intensity (λmaxс≈ 562 nm)
exceeds the decrease in band intensity
(λmaxс≈ 562 nm) ∆Ι (λmaxс≈ 562 nm) < ∆Ι
(λmaxс≈ 562 nm) in contrast to samples No. 0
and No. 1, for which ∆Ι (λмакс≈562 nm) < ∆Ι
((λмакс≈562 nm). This is apparently due to a
stronger deformation of micelles due to an
increase in the size and number of “linear
aggregates” of Fe3O4 NPs oriented in the
magnetic field with a nonzero resulting
magnetic moment in which surface Fe3+ at-
oms are bonded to oxygen donor atoms in
{Pluronic123 (Rh6G)n}m, that is, under these
conditions, the formation of complexes
[{(NP)q}Fez…Op{Pluronic123 (Rh6G)n}m]
of variable composition (q, z and p), which
will depend on the magnitude of the magnet
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92 ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2
ic field induction, is possible. This leads to a
sharp decrease in the amount of Rh6G mon-
omeric form in the films, which forms
“oblique” dimers and, partially, H-dimers.
Thus, in the SiO2/P123/Rh6G film, when
it is formed both in MF and without MF, in
the absence of magnetite NPs, a certain mu-
tual arrangement of dipoles of dye molecules
encapsulated in Pluronic123 micelles incor-
porated into a SiO2 matrix is “frozen”, which
determines the observed spectra absorption
(Fig. 2 a, curve 4) and luminescence (Fig. 2
c, curve 4).
During the formation of a
(#)SiO2/P123/Rh6G/Fe3O4 film containing
magnetite NPs, in the absence of MF, Fe3+
iron ions located on the surface of the nano-
particles form the complexes
[{(NP)q}Fez…Op{Pluronic123 (Rh6G)n}m],
as a result of which a deformation of the mi-
celle structure can occur, leading to the for-
mation of H-aggregates configuration that are
energetically more favorable than a J-type
configuration [16]. As a result, the intensity
of the absorption and luminescence bands of
the film should change (decrease), which is
observed in the experiment (Fig. 2 a and Fig.
2 c, spectral curve 0, as well as Fig. 2 b and
Fig. 2 d, spectral curve No. 0).
The above-described features of the ef-
fect of magnetic induction of MF used in the
process of formation of
(#)SiO2/P123/Rh6G/Fe3O4 (# = 1-3) film
samples on their luminescence spectra (Fig. 2
c, d) can be considered as a result of a de-
crease in the fraction of Rh6G monomers
(λmax≈ 534 nm) and the increase in the frac-
tion of “oblique” dimers and H-dimers (λmax≈
501 nm) due to the interaction of “linear ag-
gregates” of Fe3O4 nanoparticles oriented in
MF associated with Rh6G-containing mi-
celles with MP and formation complexes
[{(NP)q}Fez…Op{Pluronic123 (Rh6G)n}m].
Therefore, upon application of a magnetic
field, Fe3O4 NPs associated with micelle
fragments form “linear aggregates” (chains)
consisting of several spherical Fe3O4 NPs
with nonzero resulting magnetic moment (un-
like individual NPs), sizes of which increase
with increasing magnetic induction. This, in
turn, leads to more efficient deformation of
micelles and their closer contact (between
layers) due to the increasing interaction of
magnetic fields oriented by
superparamagnetic Fe3O4 NPs with micelles
(formation of complexes
[{(NP)q}Fez…Op{Pluronic123 (Rh6G)n}m])
and, in fact, to a specific orientation of mi-
celles in a magnetic field due to such an in-
teraction. At the same time, part of Rh6G
molecules encapsulated in micelles can be
forced to come into close contact both inside
the micelle and with Rh6G molecules of
neighboring micelles. This creates the condi-
tions for the formation of non-fluorescent H-
aggregates. However, it should be noted that
such a compression effect of micelles and
their layers has a limit due to the geometric
dimensions of the molecules.
Therefore, in spite of the increasing ori-
entation of magnetite NPs along the lines of
force of the applied magnetic field, as the
magnetic induction increases, the ratios
ΔA/∆B and ΔI/∆B should gradually decrease,
tending to zero when certain values of mag-
netic induction are reached. This is consistent
with experimental results, namely, the de-
pendences of changes in the difference in
band intensities in the absorption spectra ΔA
and luminescence ΔI of samples of hybrid
V.N. Grebennikov, E.A. Leonenko, P.A. Manorik, Romanovska, N.G. Kobylinska, A.V. Shulzhenko
ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2 93
films with magnetite NPs (Fig. 3 a, b), and
with changes in the absorption intensity A at
λ2=534 nm and the intensity fluorescence I at
λ = 562 nm of samples of hybrid
mesostructured SiO2/P123/Rh6G/Fe3O4 films
of magnetic induction (Fig. 3 c, d ).
It is important here to note the manifes-
tation of the “memory” effect in
mesostructured SiO2/P123/Rh6G/Fe3O4
films formed in magnetic fields with differ-
ent magnitudes of magnetic induction. The
structure of the complexes
[{(NP)q}Fez…Op{Pluronic123 (Rh6G)n}m]
formed by Fe3+ ions located on the surface of
oriented in MF magnetite NPs ("linear ag-
gregates") during the formation of a
mesoporous film structure in a magnetic
field had a total magnetic moment of magni-
tude significantly superior to the magnetic
moment of one nano particle. In these com-
plexes, micelles with a deformed structure
retain a certain orientation of the dye mole-
cules incorporated into them.
CONCLUSIONS. Optically transparent
mesostructured silica films SiO2/Р123/Rh6G
and SiO2/Р123/Rh6G/Fe3O4 , containing
Fe3O4 NPs with superparamagnetic properties,
are formed in stationary magnetic fields with
known induction from a film-forming sol
mixed with Rhodamine 6G and Pluronic 123.
It was shown that the spectral-luminescent
properties of SiO2/P123/Rh6G films are inde-
pendent of the MF used at their formation. A
gradual decrease of the band intensity in the
spectra of Rhodamine 6G and quenching of
luminescence with an increase in the magnetic
field induction in SiO2/P123/Rh6G/Fe3O4
films, is associated with a decrease in the frac-
tion of monomer and an increase in the frac-
tion of non-luminescent H-aggregates of the
dye in micelles.
This effect is due to the formation of
complexes of variable composition
[{(NP)q}Fez…Op{Pluronic123 (Rh6G)n}m],
in which the interaction of Fe3+ atoms with
P123 micelle donor oxygen atoms increases
due to the increase in magnetic field induc-
tion. It occurs due to an increase in q as a
result of the formation of NPs “linear aggre-
gates” with the resulting nonzero magnetic
moment in the MF, and hence an increase in
z, as well as p. This in turn leads to the grad-
ual deformation of micelles and the accumu-
lation of H-aggregates, which can form both
within the micelle and between the micelle
layers in the film.
Changes in the intensity of the absorption
and fluorescence bands of the monomeric
form of Rh6G in the spectra of
SiO2/P123/Rh6G/Fe3O4 films depend on
changes in the magnetic induction and are de-
scribed by an exponential function, and the
ratio of the fluorescence intensity of the
SiO2/P123/Rh6G film to the fluorescence in-
tensities of SiO2/P123/Rh6G/Fe3O4 linearly
depends on the magnetic induction of the MF
at which they are formed. In this case, the ob-
tained films are capable of “memorizing” the-
se values (in terms of the intensity value),
which, apparently, is associated with a sequen-
tial increase in the number of magnetite nano-
particles oriented in the MF as the MF induc-
tion increases.
The detected ability of magnetite-
containing mesostructured films to “memo-
rize” the magnitude of magnetic induction af-
ter they are formed in a permanent magnetic
field can find practical application in sensor
technologies, as well as in the development of
new multifunctional organo-inorganic
The influence of superparamagnetic Fe3O4 nanoparticles on spectral…
94 ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2
mesostructured films and devices based on
them with magnetic and optical properties.
ВПЛИВ СУПЕРПАРАМАГНІТНИХ НАНО-
ЧАСТИНОК Fe3O4 НА СПЕКТРАЛЬНО-
ЛЮМІНЕСЦЕНТНІ ВЛАСТИВОСТІ СФОР-
МОВАНИХ В СТАЦІОНАРНИХ МАГНІТ-
НИХ ПОЛЯХ МЕЗОСТРУКТУРНИХ ПЛІ-
ВОК SiO2/P123/Rh6G/Fe3O4
В.Н. Гребенніков*, Є.В. Леоненко, П.А.
Манорик, Н.І. Романовська, Н.Г.
Кобилінська** , О.В. Шульженко
*Інститут фізичної хімії ім. Л.В. Пи-
саржевського НАН України просп.
Науки, 31, Київ 03028, Україна.
**Київський національний університет ім.
Тараса Шевченка (КНУ)
*Е-mail: _vng@ukr.net
Досліджено вплив суперпарамагнітних
наночастинок (НЧ) Fe3O4 на спектрально-
люмінесцентні властивості однорідних оп-
тично прозорих мезоструктурних кремне-
земних плівок SiO2/P123/Rh6G/Fe3O4, що
містять міцели {P123 (Rh6G)}, що склада-
ються з Pluronic 123 з інкапсульованими мо-
лекулами барвника родаміну 6Ж ( Rh6G), і
сформованих у стаціонарних магнітних по-
лях (МП) з індукцією менше 500 мТл. Пока-
зано, що на відміну від SiO2/P123/Rh6G,
спектрально-люмінесцентні властивості
плівок SiO2/P123/Rh6G/Fe3O4 залежать від
використаного при їх формуванні МП, а по-
ступове зменшення інтенсивності смуг в
спектрах Rh6G і гасіння люмінесценції зі
збільшенням індукції МП, що спостерыга-
эться для них, пов'язане зі зниженням частки
мономера і збільшенням долі не люминесц-
руючих Н-агрегатів Rh6G в міцелах
внаслідок посиленої в МП взаємодії (утво-
рення Fe3+ -O зв'язків) орієнтованих в МП
суперпарамагнітних НЧ з міцелами {P123
(Rh6G)}, що призводить до поступової
деформації міцел й накопичення Н-агрегатів.
Залежності змін інтенсивності смуг погли-
нання і флуоресценції мономерной форми
Rh6G в спектрах плівок від змін величини
магнітної індукції МП описуються
експоненціальною функцією, а відношення
інтенсивності флуоресценції плівки
SiO2/P123/Rh6G до інтенсивностей
флуоресценції плівок SiO2/P123/Rh6G/Fe3O4
лінійно залежать від використаних величин
магнітної індукції МП, які вони здатні
«запам'ятовувати», що проявляється в вели-
чинах інтенсивностей флуоресценції.
К л ю ч о в і с л о в а: гібридні мезо-
структурні кремнеземні плівки, спектрально-
люмінесцентні властивості, родамін 6Ж,
Pluronic 123, наночастинки, магнетит,
магнітне поле.
ВЛИЯНИЕ СУПЕРПАРАМАГНИТНЫХ
НАНОЧАСТИЦ Fe3O4 НА СПЕКТРАЛЬНО-
ЛЮМИНЕСЦЕНТНЫЕ СВОЙСТВА СФОР-
МИРОВАННЫХ В СТАЦИОНАРНЫХ
МАГНИТНЫХ ПОЛЯХ МЕЗОСТРУКТУР-
НЫХ ПЛЕНОК SiO2/P123/Rh6G/Fe3O4
В.Н.Гребенников*, Е.В.Леоненко,
П.А.Манорик, Н.И.Романовская,
Н.Г.Кобылинская**, А.В.Шульженко
*Институт физической химии им. Л.В.
Писаржевского НАН Украины
**Киевский национальный университет им.
Тараса Шевченко (КНУ) Украина, 01601, го-
род Киев, ул. Владимирская, 64/13 просп.
Науки, 31, Киев 03028, Украина.
* Е-mail: _vng@ukr.net
Исследовано влияние суперпарамагнит-
mailto:_vng@ukr.net
mailto:_vng@ukr.net
V.N. Grebennikov, E.A. Leonenko, P.A. Manorik, Romanovska, N.G. Kobylinska, A.V. Shulzhenko
ISSN 0041-6045. УКР . ХІМ . ЖУРН ., 2020, т . 86, No 2 95
ных наночастиц (НЧ) Fe3O4 на спектрально-
люминесцентные свойства однородных опти-
чески прозрачных мезоструктурных кремне-
земных пленок SiO2/P123/Rh6G/Fe3O4, содер-
жащих мицеллы {P123 (Rh6G)}, состоящие из
Pluronic 123 (P123) с инкапсулированными
молекулами красителя родамина 6Ж (Rh6G),
и сформированных в стационарных магнит-
ных полях (МП) с индукцией менее 500 мТл.
Показано, что в отличие от SiO2/P123/Rh6G,
спектрально-люминесцентные свойства пле-
нок SiO2/P123/Rh6G/Fe3O4 зависят от исполь-
зованного при их формировании МП, а на-
блюдаемое для них постепенное уменьшение
интенсивности полос в спектрах Rh6G и ту-
шение люминесценции с увеличением индук-
ции МП связано со снижением доли мономера
и увеличением доли не люминесцирующих Н-
агрегатов Rh6G в мицеллах вследствие усили-
вающегося в МП взаимодействия (образова-
ния Fe3+-O связей) ориентированных в МП
суперпарамагнитных НЧ с мицеллами
{P123 (Rh6G)}, что приводит к постепенной
деформации мицелл и накоплению Н-
агрегатов. Зависимости изменений интенсив-
ности полос поглощения и флуоресценции
мономерной формы Rh6G в спектрах пленок
от изменений величины магнитной индукции
МП описываются экспоненциальной функци-
ей, а отношения интенсивности флуоресцен-
ции пленки SiO2/P123/Rh6G к интенсивно-
стям флуоресценции пленок
SiO2/P123/Rh6G/Fe3O4 линейно зависят от ис-
пользованных величин магнитной индукции
МП, которые они способны «запоминать»,
что проявляется в величинах интенсивностей
флуоресценции.
К л ю ч е в ы е с л о в а: гибридные мезо-
структурные кремнеземные пленки, спек-
трально-люминесцентные свойства, родамин
6Ж, Pluronic 123, наночастицы, магнетит,
магнитное поле.
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THE INFLUENCE OF SUPERPARAMAGNETIC Fe3O4 NANOPARTICLES ON SPECTRAL AND LUMINESCENT PROPERTIES OF MESOSTRUCTURED SiO2/P123/Rh6G/Fe3O4 FILMS FORMED IN STATIONARY MAGNETIC FIELDS
T a b l e 1
The main characteristics of permanent magnets brand N38 (Ni).
The numerical values for the difference in the intensities of the absorption bands in the electronic spectra of the film samples at these wavelengths are given in Table 2, from which it follows that the magnitudes of the difference increase in the ser...
exception is a sample No. 0 of the hybrid mesostructured (0) SiO2/P123/Rh6G/Fe3O4 film, for which at B = 0, two broad bands of low intensity with maximum peaks close to 505 and 542 nm appear in the differential spectrum.
Fig. 4. Dependence characterizing the fluorescence quenching of magnetite-containing hybrid mesostructured SiO2/P123/Rh6G/Fe3O4 films on the magnitude of the magnetic induction (No. 0, No. 1, No. 2, No. 3 and Fig. 4d) used at the formation of the films.
ВПЛИВ СУПЕРПАРАМАГНІТНИХ НАНО-ЧАСТИНОК Fe3O4 НА СПЕКТРАЛЬНО-ЛЮМІНЕСЦЕНТНІ ВЛАСТИВОСТІ СФОР-МОВАНИХ В СТАЦІОНАРНИХ МАГНІТ-НИХ ПОЛЯХ МЕЗОСТРУКТУРНИХ ПЛІ-ВОК SiO2/P123/Rh6G/Fe3O4
ВЛИЯНИЕ СУПЕРПАРАМАГНИТНЫХ НАНОЧАСТИЦ Fe3O4 НА СПЕКТРАЛЬНО-ЛЮМИНЕСЦЕНТНЫЕ СВОЙСТВА СФОР-МИРОВАННЫХ В СТАЦИОНАРНЫХ МАГНИТНЫХ ПОЛЯХ МЕЗОСТРУКТУР-НЫХ ПЛЕНОК SiO2/P123/Rh6G/Fe3O4
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| id | oai:ojs2.1444248.nisspano.web.hosting-test.net:article-123 |
| institution | Ukrainian Chemistry Journal |
| keywords_txt_mv | keywords |
| language | English |
| last_indexed | 2026-07-23T01:01:34Z |
| publishDate | 2020 |
| publisher | V.I.Vernadsky Institute of General and Inorganic Chemistry |
| record_format | ojs |
| resource_txt_mv | ucjorgua/33/60f5e8b1eb72fbe956e7bbe20a20e033.pdf |
| spelling | oai:ojs2.1444248.nisspano.web.hosting-test.net:article-1232026-07-22T08:23:42Z THE INFLUENCE OF SUPERPARAMAGNETIC Fe3O4 NANOPARTICLES ON SPECTRAL AND LUMINESCENT PROPERTIES OF MESOSTRUCTURED SiO2/P123/Rh6G/Fe3O4 FILMS FORMED IN STATIONARY MAGNETIC FIELDS ВЛИЯНИЕ СУПЕРПАРАМАГНИТНЫХ НАНОЧАСТИЦ Fe3O4 НА СПЕКТРАЛЬНО-ЛЮМИНЕСЦЕНТНЫЕ СВОЙСТВА СФОРМИРОВАННЫХ В СТАЦИОНАРНЫХ МАГНИТНЫХ ПОЛЯХ МЕЗОСТРУКТУРНЫХ ПЛЕНОК SiO2/P123/Rh6G/Fe3O4 ВПЛИВ СУПЕРПАРАМАГНІТНИХ НАНОЧАСТИНОК Fe3O4 НА СПЕКТРАЛЬНО-ЛЮМІНЕСЦЕНТНІ ВЛАСТИВОСТІ СФОРМОВАНИХ В СТАЦІОНАРНИХ МАГНІТНИХ ПОЛЯХ МЕЗОСТРУКТУРНИХ ПЛІВОК SiO2/P123/Rh6G/Fe3O4 Grebennikov, Volodimir Leonenko , Evgen Manorik, Petro Romanovska, Natalia Kobylinska, Natalia Shulzhenko, Olexandr hybrid mesostructured silica films, spectral luminescent properties, Rhodamine 6G, Pluronic 123, nanoparticles, magnetite, a magnetic field. The effect of superparamagnetic Fe3O4 nanoparticles (NPs) on the spectral luminescence properties of homogeneous optically transparent mesostructured silica films of SiO2/P123/Rh6G/Fe3O4, containing {P123&nbsp;(Rh6G)} micelles consisting of Pluronic&nbsp;123 with encapsulated Rh6G, and formed in stationary magnetic fields (MF) with an induction of less than 500 mT, was investigated. It was shown that, unlike SiO2/P123/Rh6G, the spectral and luminescent properties of SiO2/P123/Rh6G/Fe3O4 films depend on the MF used during their formation, and a gradual decrease in the band intensities in Rh6G spectra and quenching of luminescence with increasing of MF induction was observed. It is associated with a decrease in the monomer fraction and an increase in the fraction of non-luminescent Rh6G H-aggregates in micelles due to the interaction intensifying in the MF (formation of Fe3+&nbsp;-O bonds) of superparamagnetic NPs with micelles {P123&nbsp;(Rh6G)}, oriented in the MF, which leads to a gradual deformation of micelles and accumulation in them of H-aggregate. The dependences of the changes in the absorption bands intensity and fluorescence of the monomeric form of Rh6G in the spectra of the films on the changes in the magnetic induction of the MF are described by an exponential function, and the ratio of the fluorescence intensities of the SiO2/P123/Rh6G films to the fluorescence intensities of the SiO2/P123/Rh6G/Fe3O4 films linearly depends on the induction of MF, which they are able to "remember", which is manifested in the values of fluorescence intensities. V.I.Vernadsky Institute of General and Inorganic Chemistry 2020-02-05 Article Article Physical chemistry Физическая xимия Фізична xімія application/pdf https://ucj.org.ua/index.php/journal/article/view/123 10.33609/0041-6045.86.2.2020.78-96 Ukrainian Chemistry Journal; Vol. 86 No. 2 (2020): Ukrainian Chemistry Journal; 78-96 Украинский химический журнал; ##issue.vol## 86 ##issue.no## 2 (2020): Украинский химический журнал; 78-96 Український хімічний журнал; Том 86 № 2 (2020): Український хімічний журнал; 78-96 2708-129X 2708-1281 en https://ucj.org.ua/index.php/journal/article/view/123/78 Copyright (c) 2020 Volodimir Grebennikov, Evgen Leonenko , Petro Manorik, Natalia Romanovska, Natalia Kobylinska, Olexandr Shulzhenko https://creativecommons.org/licenses/by-nc/4.0 |
| spellingShingle | Grebennikov, Volodimir Leonenko , Evgen Manorik, Petro Romanovska, Natalia Kobylinska, Natalia Shulzhenko, Olexandr ВПЛИВ СУПЕРПАРАМАГНІТНИХ НАНОЧАСТИНОК Fe3O4 НА СПЕКТРАЛЬНО-ЛЮМІНЕСЦЕНТНІ ВЛАСТИВОСТІ СФОРМОВАНИХ В СТАЦІОНАРНИХ МАГНІТНИХ ПОЛЯХ МЕЗОСТРУКТУРНИХ ПЛІВОК SiO2/P123/Rh6G/Fe3O4 |
| title | ВПЛИВ СУПЕРПАРАМАГНІТНИХ НАНОЧАСТИНОК Fe3O4 НА СПЕКТРАЛЬНО-ЛЮМІНЕСЦЕНТНІ ВЛАСТИВОСТІ СФОРМОВАНИХ В СТАЦІОНАРНИХ МАГНІТНИХ ПОЛЯХ МЕЗОСТРУКТУРНИХ ПЛІВОК SiO2/P123/Rh6G/Fe3O4 |
| title_alt | THE INFLUENCE OF SUPERPARAMAGNETIC Fe3O4 NANOPARTICLES ON SPECTRAL AND LUMINESCENT PROPERTIES OF MESOSTRUCTURED SiO2/P123/Rh6G/Fe3O4 FILMS FORMED IN STATIONARY MAGNETIC FIELDS ВЛИЯНИЕ СУПЕРПАРАМАГНИТНЫХ НАНОЧАСТИЦ Fe3O4 НА СПЕКТРАЛЬНО-ЛЮМИНЕСЦЕНТНЫЕ СВОЙСТВА СФОРМИРОВАННЫХ В СТАЦИОНАРНЫХ МАГНИТНЫХ ПОЛЯХ МЕЗОСТРУКТУРНЫХ ПЛЕНОК SiO2/P123/Rh6G/Fe3O4 |
| title_full | ВПЛИВ СУПЕРПАРАМАГНІТНИХ НАНОЧАСТИНОК Fe3O4 НА СПЕКТРАЛЬНО-ЛЮМІНЕСЦЕНТНІ ВЛАСТИВОСТІ СФОРМОВАНИХ В СТАЦІОНАРНИХ МАГНІТНИХ ПОЛЯХ МЕЗОСТРУКТУРНИХ ПЛІВОК SiO2/P123/Rh6G/Fe3O4 |
| title_fullStr | ВПЛИВ СУПЕРПАРАМАГНІТНИХ НАНОЧАСТИНОК Fe3O4 НА СПЕКТРАЛЬНО-ЛЮМІНЕСЦЕНТНІ ВЛАСТИВОСТІ СФОРМОВАНИХ В СТАЦІОНАРНИХ МАГНІТНИХ ПОЛЯХ МЕЗОСТРУКТУРНИХ ПЛІВОК SiO2/P123/Rh6G/Fe3O4 |
| title_full_unstemmed | ВПЛИВ СУПЕРПАРАМАГНІТНИХ НАНОЧАСТИНОК Fe3O4 НА СПЕКТРАЛЬНО-ЛЮМІНЕСЦЕНТНІ ВЛАСТИВОСТІ СФОРМОВАНИХ В СТАЦІОНАРНИХ МАГНІТНИХ ПОЛЯХ МЕЗОСТРУКТУРНИХ ПЛІВОК SiO2/P123/Rh6G/Fe3O4 |
| title_short | ВПЛИВ СУПЕРПАРАМАГНІТНИХ НАНОЧАСТИНОК Fe3O4 НА СПЕКТРАЛЬНО-ЛЮМІНЕСЦЕНТНІ ВЛАСТИВОСТІ СФОРМОВАНИХ В СТАЦІОНАРНИХ МАГНІТНИХ ПОЛЯХ МЕЗОСТРУКТУРНИХ ПЛІВОК SiO2/P123/Rh6G/Fe3O4 |
| title_sort | вплив суперпарамагнітних наночастинок fe3o4 на спектрально-люмінесцентні властивості сформованих в стаціонарних магнітних полях мезоструктурних плівок sio2/p123/rh6g/fe3o4 |
| topic_facet | hybrid mesostructured silica films spectral luminescent properties Rhodamine 6G Pluronic 123 nanoparticles magnetite a magnetic field. |
| url | https://ucj.org.ua/index.php/journal/article/view/123 |
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