Probing plasmonic system by the simultaneous measurement of Raman and fluorescence signals of dye molecules
The simultaneous measurement of Raman and fluorescence signals was proposed to find out the molecule-metal distance. The ratio between Raman and fluorescence intensities was used to estimate molecule-metal distance in nanometer scale. A low-value intensity of the fluorescence of the dye molecules wa...
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nasplib_isofts_kiev_ua-123456789-1177182025-06-03T16:28:46Z Probing plasmonic system by the simultaneous measurement of Raman and fluorescence signals of dye molecules Dvoynenko, M.M. Kazantseva, Z.I. Strelchuk, V.V. Kolomys, O.F. Bortshagovsky, E.G. Venger, E.F. Tronc, P. The simultaneous measurement of Raman and fluorescence signals was proposed to find out the molecule-metal distance. The ratio between Raman and fluorescence intensities was used to estimate molecule-metal distance in nanometer scale. A low-value intensity of the fluorescence of the dye molecules was found using the photobleaching effect. Made was a comparison of experimental results with a theoretical model, which showed well agreement. The authors are thankful to S.A. Zenyo for preparation of Au substrate film. This work was supported by Ukrainian-French projects “Dnipro” of State fund for fundamental researches of Ukraine 2011 Article Probing plasmonic system by the simultaneous measurement of Raman and fluorescence signals of dye molecules / M.M. Dvoynenko, Z.I. Kazantseva, V.V. Strelchuk, O.F. Kolomys, E.G. Bortshagovsky, E.F. Venger // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2011. — Т. 14, № 2. — С. 195-199. — Бібліогр.: 22 назв. — англ. 1560-8034 PACS 33.50.-j, 34.35.+a, 73.20.Mf, 78.30.-j https://nasplib.isofts.kiev.ua/handle/123456789/117718 en Semiconductor Physics Quantum Electronics & Optoelectronics application/pdf Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
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The simultaneous measurement of Raman and fluorescence signals was proposed to find out the molecule-metal distance. The ratio between Raman and fluorescence intensities was used to estimate molecule-metal distance in nanometer scale. A low-value intensity of the fluorescence of the dye molecules was found using the photobleaching effect. Made was a comparison of experimental results with a theoretical model, which showed well agreement. |
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Dvoynenko, M.M. Kazantseva, Z.I. Strelchuk, V.V. Kolomys, O.F. Bortshagovsky, E.G. Venger, E.F. Tronc, P. |
| spellingShingle |
Dvoynenko, M.M. Kazantseva, Z.I. Strelchuk, V.V. Kolomys, O.F. Bortshagovsky, E.G. Venger, E.F. Tronc, P. Probing plasmonic system by the simultaneous measurement of Raman and fluorescence signals of dye molecules Semiconductor Physics Quantum Electronics & Optoelectronics |
| author_facet |
Dvoynenko, M.M. Kazantseva, Z.I. Strelchuk, V.V. Kolomys, O.F. Bortshagovsky, E.G. Venger, E.F. Tronc, P. |
| author_sort |
Dvoynenko, M.M. |
| title |
Probing plasmonic system by the simultaneous measurement of Raman and fluorescence signals of dye molecules |
| title_short |
Probing plasmonic system by the simultaneous measurement of Raman and fluorescence signals of dye molecules |
| title_full |
Probing plasmonic system by the simultaneous measurement of Raman and fluorescence signals of dye molecules |
| title_fullStr |
Probing plasmonic system by the simultaneous measurement of Raman and fluorescence signals of dye molecules |
| title_full_unstemmed |
Probing plasmonic system by the simultaneous measurement of Raman and fluorescence signals of dye molecules |
| title_sort |
probing plasmonic system by the simultaneous measurement of raman and fluorescence signals of dye molecules |
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Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
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2011 |
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https://nasplib.isofts.kiev.ua/handle/123456789/117718 |
| citation_txt |
Probing plasmonic system by the simultaneous measurement of Raman and fluorescence signals of dye molecules / M.M. Dvoynenko, Z.I. Kazantseva, V.V. Strelchuk, O.F. Kolomys, E.G. Bortshagovsky, E.F. Venger // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2011. — Т. 14, № 2. — С. 195-199. — Бібліогр.: 22 назв. — англ. |
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Semiconductor Physics Quantum Electronics & Optoelectronics |
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2025-11-24T15:46:47Z |
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| fulltext |
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2011. V. 14, N 2. P. 195-199.
PACS 33.50.-j, 34.35.+a, 73.20.Mf, 78.30.-j
Probing plasmonic system by the simultaneous measurement
of Raman and fluorescence signals of dye molecules
M.M. Dvoynenko1, Z.I. Kazantseva1, V.V. Strelchuk1, O.F. Kolomys1, E.G. Bortshagovsky1,
E.F. Venger1, P. Tronc2
1V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine,
41, prosp. Nauky, 03028 Kyiv, Ukraine
2Centre National de la Recherche Scientifique, Ecole Superieure de Physique et de Chimie Industrielles de la Ville de
Paris, 10 rue Vauquelin, 75005 Paris, France
Abstract. The simultaneous measurement of Raman and fluorescence signals was
proposed to find out the molecule-metal distance. The ratio between Raman and
fluorescence intensities was used to estimate molecule-metal distance in nanometer scale.
A low-value intensity of the fluorescence of the dye molecules was found using the
photobleaching effect. Made was a comparison of experimental results with a theoretical
model, which showed well agreement.
Keywords: SERS, photobleaching effect, fluorescence, dye molecule, Au surface.
Manuscript received 14.10.10; accepted for publication 16.03.11; published online 30.06.11.
1. Introduction
There is a great interest to surface plasmon and related
phenomena [1]. Surface and tip enhanced Raman
spectroscopies (SERS and TERS) [2], surface plasmon
enhanced light emission [3-5] are in a researchers’ focus
of interest. The intensity of surface-enhanced
fluorescence and SERS depends on the local field and
energy transfer from an excited molecule to a metal
particle, which depends on the distance between the
molecule and metal particle. Thus, to control the
molecule-metal distance is of great importance to
describe the plasmon system. Dependence of the
fluorescence lifetime of dyes on the molecule-metal
distance was studied at wavelength [6]- and nm [7]-scale
distances. The molecule – single nanoparticle distance
dependence of both fluorescence [8, 9] and TERS [10]
intensities was experimentally demonstrated. However,
separate fluorescence and Raman studies in experiments
with many molecules have a problem associated with
various molecule numbers. Additionally, the number of
molecules situated in light spot during the measurement
can be decreased due to photobleaching. Since the
photobleaching time depends on the molecule-
nanoparticle distance, the distance behaviors of the
Raman and fluorescence intensities will be changed for
different accumulation times. Simultaneous Raman and
fluorescence measurements [11] could resolve this
general problem. Indeed, on the one hand, both Raman
and fluorescence intensities are determined by the same
studying molecule’ numbers, on the other hand, there is
a difference between them. Both Raman and
fluorescence intensities depend on the electromagnetic
enhancement factor [11-13], while the fluorescence
intensity depends also on the decay rate [11-13] for
molecules, which just reflects the energy transfer from
the excited molecule to metal. As a consequence, the
ratio between simultaneously measured Raman and
fluorescence intensities, cancelling the associated
molecule quantity and electromagnetic enhancement
factor, is only a function of the decay rate of these
molecules that in its turn is strongly sensitive to the
molecule-metal distance. The simultaneous Raman and
fluorescence measurement was proposed [11] as a way
to find the chemical enhancement factor. In the absence
of the chemical enhancement it can be used [14] to find
the molecular lifetime in steady-state spectroscopy
without resorting to time-resolved spectroscopy. Note
that the simultaneous observation of Raman and
fluorescence signals was reported [15] but there was no
analysis or proposals to investigate the distance
dependence. Recently [16], the simultaneous
measurement of the Raman and fluorescence intensities
and an analysis of the molecule-metal distance
dependence were done for dye molecules of rhodamine
6G. In this paper, we experimentally study the distance
behavior of the ratio between Raman and fluorescence
intensities for dye molecules of 2-(4-(p-dimethyl-
aminophenyl)-1,3-butadienyl)-3-ethylbenzothoazolium
perchlorat (LDS 721 or styryl 8).
© 2011, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
195
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2011. V. 14, N 2. P. 195-199.
2. Experiment
In this paper, we experimentally demonstrate and
analyze the distance dependence of the ratio between
Raman and fluorescence intensities of dye molecules of
LDS 751 spaced by a thin polymer film at nm-scale
distance at a gold substrate. A smooth flat metal surface
is chosen because all measured molecules are
approximately at the same distance to the metal surface
in contrast to island metal films [15]. A smooth gold
film with the thickness about 100 nm was prepared by
thermal evaporation on a glass substrate. Monolayers
prepared using polymer (polyimide) solution in
chloroform were investigated by R&K (Wiesbaden,
Germany) equipment for Langmuir-Blodgett film (LBF)
preparation. LBFs [17] were formed in the standard way
of vertical transfer under control of the transfer
coefficient and π-A – diagrams. The LBFs were
deposited at the surface tension of 20 mN/m by
upstrokes to form Z-type structure on the substrates. The
dipping rate was 2 mm/min. The LBF thickness was
measured ellipsometrically using a laser beam
(λ = 0.623 µm; incidence angle 60°). The reversed
ellipsometric problem was solved numerically for the
“substrate-optically transparent film” model.
Ellipsometric measurements with a ten-layer film give
both refractive index 1.64 and thickness 0.85±0.15 nm
per layer. The refractive index 1.64 is comparable to that
obtained previously [18]. LDS 751 molecules were
deposited by the dipping with the speed 1 mm/s in water
solution of the dye with the concentration of .
The confocal micro-Raman and fluorescence spectra
were measured by the T64000 Jobin Yvons spectrometer
with a thermoelectrically cooled charge coupled device
detector. The 514.5-nm line of an Ar
M10 5−
+/Kr+-ion laser was
used as the excitation source. After being reflected from
a sharp-edge Raman filter, the laser beam was then
focused by an Olympus BX41 microscope equipped
with an objective ×100 (numerical aperture (NA) = 0.90)
on the sample surface. The net laser intensity on the
sample surface was ~5×107 W/m2. The light scattered
backward was collected through the same objective and
detected with the integration time 20 s. All spectra were
measured at the room temperature (T = 300 K).
3. Results and discussion
Due to the photobleaching effect, the studied frequency
region ( ) was chosen in such a way that
a spectrum was measured without rotating the
monochromator grating. On the other hand, this
frequency range had a maximal value in order to
compare various active Raman modes of LDS 751
molecules. The Raman and fluorescence spectra of LDS
751 deposited on a gold substrate with the accumulation
time 300 s are shown in Fig. 1.The most pronounced
Raman peaks are at 1130, 1280 and . The
peak at with the maximal magnitude is in
focus of our study. The fluorescence spectrum of LDS
751 is broad with the peak at approximately 751 nm.
The Raman and fluorescence spectra at the spacer
thicknesses 0.85, 2.55 and 4.25 nm are shown in Fig. 2,
which correspond to the number N = 1, 3, 5 of the
polyimide monolayers. At the first sight, it can seem that
the Raman intensity decreases with the thickness of the
spacer. The local field near a flat surface consists of
incident and reflected fields. At very small thicknesses
(few nanometers) of the spacer, the reflected field can be
changed insignificantly. It is likely that the surface to be
not enough smooth and the electromagnetic
enhancement factor decreases with the distance to some
inhomogeneity (the enhancement factor practically does
not depend at such nm-scale distances to the surface for
ideal plane surface). However, the main reason in the
decrease of the Raman intensity with the distance
consists in the photobleaching effect during the
measurement. As the photobleaching time being a result
of a competition between the energy transfer from
excited molecule to the metal and relaxation to a triplet
state [19] strongly decreases with the spacer thickness,
the average number of measured molecules decreases
with the distance to metal surface, too.
1cm2500500 −−
1cm1564 −
1cm1564 −
Fig. 1. The Raman and fluorescence spectra of LDS 751
deposited on a gold substrate.
Fig. 2. The confocal micro-Raman and fluorescence intensities
of the LDS 751 on the Raman shift Ω. The characters (a, b, c)
indicate curves with the numbers N = 1, 3 and 5 of the
polyimide monolayers, respectively.
© 2011, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
196
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2011. V. 14, N 2. P. 195-199.
Contrary to the Raman signal, the fluorescence
intensity cannot be found directly from the data in Fig. 2
due to a small value of the signal and the absence of the
information about zero level at the wing of the Rayleigh
line. In order to resolve this problem, we used the
photobleaching effect. Spectra of LDS 751 at N = 1
obtained for various illumination times before
measurements are presented in Fig. 3. The subtraction
between the different spectra gives the value of the
Raman and fluorescence intensities of molecules that
were photo-oxidized. For example, the subtractions Ia–Ib
between the curves a and b and Ib–Ic between the curves
b and c in Fig. 3 give the correct (without background)
Raman and fluorescence intensities of the molecules that
were photo-oxidized during the illumination times 20
and 80 s, respectively. By this way, the background level
was cancelled and the ratio between Raman and
fluorescence intensities IR / Ifl was found for the Raman
shifts for all spacer thicknesses. 1cm1564 −=Ω
© 2011, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
Fig. 3. The confocal micro-Raman and fluorescence
spectra at N = 1 measured after preliminary light
illumination at the operation wavelength and intensity for
duration 0 (a), 20 (b), and 80 s (c).
Fig. 4. Experimental (vertical lines) and theoretical (solid
curve) dependences of IR / Ifl on the monolayer number N.
Typically, IR / Ifl little increases with the illumination
time. It can be simply explained. Indeed, in the absence of
the chemical enhancement IR / Ifl ~ γ [11], where γ is the
decay rate of the molecule that is the value to be inversed
to the lifetime of the excited molecule. The higher lifetime
of an excited molecule leads to a higher probability to be
situated in a metastable triplet energy state and
consequently to transfer of the energy to oxygen. Thus,
the photo-oxidation of the molecules having the higher
lifetime has the higher probability. Since in the
electrostatic approximation and in the absence of the
physical spacer layer γ ~ z–3 (z is the molecule-surface
distance) for the case of the volume damping [20], one
can say that the photobleaching is able to selectively
“delete” the most remote dye molecules. One more trend-
like property is an increase of the fluctuation of IR / Ifl with
the spacer thickness decrease. The highest fluctuations are
at N = 1. This property is clearly seen taking into account
the distance dependence of the decay rate. Indeed,
z
zΔ
=
γ
γΔ 3 for the case of the volume damping. Thus,
the fluctuation of the molecule-surface distance essentially
increases at small mean distances. If there is the spacer
layer and the distance between the molecule and surface
of the spacer is not equal to zero, then we obtain even in
the electrostatic approximation
γ ~
( ) ( ) ( ) ⎟
⎟
⎠
⎞
⎜
⎜
⎝
⎛
+
+
+
+
+
+
...
32 3
3
3
2
3
1
hz
A
hz
A
hz
A , where
are some coefficients. The latter expression
represents multiple reflections in the spacer film. Note
that the multiple reflections still keeps the general feature
about an increase of the fluctuations at smaller spacer
thicknesses.
,...,, 321 AAA
The main result of the molecule-surface distance
behavior is depicted in Fig. 4. The diapasons of the
values IR / Ifl for the Raman shift are
presented as vertical lines at the five number values of
the spacer layers. It is seen that the fluctuation decreases
with the spacer thickness. Theoretical calculation is
presented by the solid line supposing that I
1cm1564 −=Ω
R / Ifl = 1.23 at
N = 1. This calculation is made at the following
parameters: the distance of the point-like source to
surface should be 1 nm and the thickness of one
monolayer should be 0.85 nm. The dielectric function ε
of the polyimide spacer is taken as ε = 2.8. Theoretical
calculation of the non-radiative relaxation rate based on
the classical theory delineated in Ref. [20] was
performed. Briefly, the relaxation rate of a dipole, p,
placed near a metallic surface is given by γ ∝ Im (p∗·ER),
where ER is the reaction field containing direct incident
(radiated) field and reflected field from the surface.
From the latter equation, one can get
γ ∝ (( rrGp ii ))rr,,Im2 ω , where (( rrGii ))rr,,ω is the
corresponding component of the electrodynamics Green
tensor. In the case of a substrate with the spacer layer,
the Green function can be found elsewhere [21].
Supposing the case of the physical adsorbed molecule
197
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2011. V. 14, N 2. P. 195-199.
© 2011, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
))
(the dipole moment does not change), one can get
IR / Ifl ~ (( rrGii
rr
,,Im ω . This expression is presented in
Fig. 4 by the solid line. Of course, the coefficient in the
equation IR / Ifl ~ (( rrGii ))rr,,Im ω depends on many
parameters, in particular, on the excitation and radiation
wavelengths, kind of molecules, temperature, etc.
However, it does not depend on the nanoplasmon
system. Thus, finding once the coefficient at the fixed
above mentioned parameters, one can make a diagnostic
of the nanoplasmonic system only on the basis of the
ratio between Raman and fluorescence intensities.
One can see that the theoretical dependence
describes the experimental behavior quite well.
However, there is a tendency for this behavior to be
disagreed with theoretical dependence at small spacer
thicknesses. A similar tendency [16] took place in the
case of rhodamine 6G molecules. This tendency can be
caused by both certain inhomogeneity in the spacer layer
and the deposited dye film as well as by the presence of
background. One can see that the value of the ratio IR / Ifl
is less than the theoretical prediction. It looks like there
is an additional fluorescence not taken into account. This
fluorescence can be caused by an additional background.
Nevertheless, though the subtraction should cancel the
background associated with the fluorescence of Au and
the wing of the Rayleigh scattering, an additional
background can exist. Indeed, it has been reported
recently [22] that non-fluorescent molecules (in our case
dye molecules) can give some background. This
background cannot be cancelled by the proposed
subtraction procedure.
4. Conclusion
In conclusion, we have performed an experiment on
simultaneous measurement of Raman and fluorescence
intensities of molecules LDS 751 located at various
distances from a flat Au surface. It was shown that the
ratio between the Raman and fluorescence intensities is
well described by the classical model of the energy
transfer from the molecule to metal. We believe that this
ratio can be used to find the distance between molecule
and metal surface.
The authors are thankful to S.A. Zenyo for
preparation of Au substrate film.
This work was supported by Ukrainian-French
projects “Dnipro” of State fund for fundamental
researches of Ukraine
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