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Comments on “Photophysics of rhodamine B in the nanosized water droplets: A concentration dependence study”
Comments on ”Photophysics of Rhodamine B in the nanosized water droplets: A concentration dependence study” Soheil Sharifi, Khalil Alizadeh, Seyyed Mahdi Shavakandi PII: DOI: Reference:
S0167-7322(16)32746-5 doi:10.1016/j.molliq.2016.11.057 MOLLIQ 6604
To appear in:
Journal of Molecular Liquids
Received date: Revised date: Accepted date:
14 September 2016 13 November 2016 14 November 2016
Please cite this article as: Soheil Sharifi, Khalil Alizadeh, Seyyed Mahdi Shavakandi, Comments on ”Photophysics of Rhodamine B in the nanosized water droplets: A concentration dependence study”, Journal of Molecular Liquids (2016), doi:10.1016/j.molliq.2016.11.057
This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.
ACCEPTED MANUSCRIPT Comments on "Photophysics of Rhodamine B in the nanosized water droplets: A concentration dependence study"
PT
Soheil Sharifi*, Khalil Alizadeh, Seyyed Mahdi Shavakandi
RI
Department of Physics, Faculty of Sciences, Ferdowsi University of Mashhad, Mashhad 91775-1436, Iran
SC
Abstract:
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MA
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This comment concerns some erroneous claims, which arise from the results and discussion in the recent article by A.Rahdar (Journal of Molecular Liquids 220 (2016) 395–403). The mixture of Rhodamine B with AOT/Water/n-Hexane was studied at two water to surfactant molar ratio (Y=10 and 8). Morevoer, The effect of droplet concentration was studied on fluorescence spectra of Rhodamine B-doped droplets. The size of droplet was changed by increase of water to surfactant molar ratio(Y). The results shows, by increase of droplet concentration, the fluorescence (νf) maxima wavenumbers was changed and the absorbance (νa) maxima wavenumbers was constant. We found, the value of νa−νf and νa+νf of Rhodamine B inside of droplets is quite different from the results that found before by A.Rahdar. By theory and experiments, the corrected value of the ratio of dipole moment of Rhodamine B in droplets was reported. We have proven, the ratio of dipole moment was changed between 1.82988 to 2.05972 by increase of droplet concentration at constant molar ratio Y=10. Moreover, the effect of droplet size is reported on the ratio of excited to ground states of dipole moment at Rhodamine B. Keywords:fluorescence, nano-droplets, dipole moment. *Corresponding Author: [email protected] , [email protected]
Introduction:
In this work, the photophysics of Rhodamine B (RhB) in droplet of AOT/Water/n-Hxane microemulsion at Molar Ratio 10 and 8 was studied [1]. It is well known that the nano-droplet can prepare with mixture of water, oil (n-Hxane) and surfactant (AOT). The Rhodamine B can solve inside of water droplets in the mixture of dye with microemulsion. So, The RhB/microemulsion is RhB/water droplet inside of continuous phase of oil(n-Hxane). In this work, the mixture of dye with microemulsion is studied at different concentration of droplets in the oil at two molar ratio (Y=10 and 8). By the theory, We studied, the effect of concentration and size of droplet on, the dipole moment of ground and excited state of Rhodamine B.
ACCEPTED MANUSCRIPT Experiment:
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SC
RI
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Rhodamine b (RhB), AOT (Bis(2-ethylhexyl) sulfosuccinate sodium salt) and Hexane, were obtained from Sigma-Aldrich. All materials were used as received and MilliQ water was used in preparing all samples. Microemulsions were prepared by weight, in terms of the surfactant to water molar ratio of Y=[H2O]/[AOT], (Y=10 and 8) and the different mass fraction of droplets (mf,drop=(mH2O+mAOT)/(mTotal)), that mTotal=mH2O+mAOT+mHex, which varies by the respective mass of n-Hexane (mHex), water=(mH2O) and AOT(mAOT). All experiments were done at constant room temperature. In cases of Rhodamine B-containing microemulsions, aqueous dye solutions were mixed with oil and surfactant. The concentration of dye in droplet define by mass ratio Z=mdye/mH2O that mdye was the mass of dye. The method for the sample preparation were presented in the references [1,2]. Absorption spectra of samples were recorded with a UV-1650 PC spectrometer (Shimadzu). Fluorescence spectra (excitation at 554nm) were recorded with Jasco FP-6200 spectrofluorimeter. Results and discussions:
800 600 400
(a)
300
(b)
0.01 0.03 0.05 0.07 0.1 0.15
Fluorescence Intensity (a.u.)
Fluorescence Intensity (a.u.)
1000
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The fluorescence spectra of RhB mixed with AOT/Hexane/Water at two constant molar ratio is presented in the fig.1. Fig.1(a) is show, the fluorescence spectra of RhB/microemulsion with Y=8 and Z=0.000479 and fig.1(b) is the fluorescence spectra of the RhB/microemulsion for Y=10 and Z=0.0000625. The red shift is observed in fluorescence spectra (λem) by increase of droplet concentration from 0.01 to 0.15. The largest observed redshift (11nm) was appeared at higher concentration of dye(Z=0.000479) and the smaller redshift (4nm) was appeared at lowest concentration of dye(Z=0.0000625). The absorbance wavelength of RhB/microemulsion and RhB/water is constant at 554±1nm.
X=8
200 0
550
600
wavelength (nm)
650
0.1 0.07 0.06 0.05 0.04 0.03 0.02 0.01
250 200 150 100
X=10
50 0
550
600
650
wavelength (nm)
Fig.1. Fluorescence emission spectra (excitation at 554nm) of Rhodamine B inside of AOT microemulsion at Y=8 and Z=0.000479(a), RhB/microemulsion with Y=10 and Z=0.0000625 (b) at the different droplet mass fractionat. All the experiment was done at room temperature.
ACCEPTED MANUSCRIPT The relation between absorption and fluorescence spectra was obtained by using the quantummechanical second orderperturbation theory [3,4] that:
a f m1 f ( , n)
2(e g )2 m1 hca3
(2)
(3)
SC
2(e2 g2 ) m2 hca3
PT
a f m2[ f ( , n) 2g(n)]
RI
(1)
NU
(4)
MA
Where νa and νf are maximum frequency of absorption and emission and μg and μe are the dipole moments in the ground and excited states, respectively, h Planck's constant, c the velocity of light in the vacuum, a Onsager's interaction radius of solute, f(ε,n) and g(n) are the solvent polarity functions given by following equations:
D
2n2 1 1 n2 1 f ( , n) 2 ( ) n 1 1 n2 2
AC CE P
(6)
TE
(5)
3 n4 1 g(n) ( 2 ) 2 (n 1)2
Where n and ε are refractive index and dielectric constant of dye solvent.The A.Rahdar[1], had mentioned that" In this case, permittivity (ε) and refractive index (n) variations of system were negligible. Because the solvent type of bulk (hexane oil) in this system was constant." Firstly, the n-Hexane isn't solvent of Rhodamine B. The Rhodamine B can solve only inside of water droplet. So, the A.Rahdar should use the permittivity and dielectric constant of water as solvent of Rhodamine B. Secondly, from the perturbation theory, it isn't possible to neglect the effect of permittivity and dielectric constant. For this reason, the A.Rahdar used incorrect procedure to find the ratio of dipole moment. The results of the spectral shifts νa-νf and νa+νf ( ) are presented in the table 1. Our results shows, the νa-νf changes from 537.40667 to 659.23717( ) with increase of droplet concentration at constant dye/water ratio (Z=0.0000625).The A.Rahdar was found, the νa-νf was changed between 1×10-5 to 2×10-5( ) for the same samples,[1] that this range of variation is not observed in the absorption and fluorescence spectra. Moreover, the A.Rahdar was found that the νa-νf was changed between 0.5×10-5 to 2×10-5( ) by increase of droplet mass fraction from 0.01 to 0.1 at samples with higher dye/water concentration (Z=0.001) that this variation isn't possible. Moreover, the A.Rahdar used incorrect parameters (νa-νf and νa+νf) for calculate the ratio of dipole moment. In the perturbation theory, we used refractive index and dielectric constant of water as solvent of dye at the equations 5 and 6. So, the f(ε,n) and g(n) become constant for our results than from equations 1-4, we obtained ratio of dipole moments (dipole moment in excited state to the dipole
ACCEPTED MANUSCRIPT
ν
,ν
RI
ν
Table 1.ν
PT
moment in the ground state) and finally the results are presented in the table 1. To improve the results, the effect of droplet concentration on Rhodamine B in different molar ratio (X=8) is studied. The results show, the ratio of ground to exited state (μe/μg) changes from 1.86376 to 2.55907 by increase of droplet concentration from 0.01 to 0.1. The value of μe/μg of RhB in microemulsion with smaller size (X=8) is higher than microemulsion with bigger size (X=10) because the dye/water ratio (Z) is higher. , ratio of dipole moments(
/
), the peak wavelength of
8
0.000479
Conclusion:
NU
537.40667 537.40667 568.02403 601.57973 604.62386 607.66693 628.93873 659.23717 539.32299 782.14458 871.47868
MA
0.0000625
0.01 0.02 0.03 0.04 0.05 0.06 0.07 0.1 0.01 0.07 0.1
AC CE P
10
mf
λabc (nm) 571 554 571 554 572 554 573.1 554 573.2 554 573.3 554 574 554 575 554 570 553 578 553 581 553
D
X
λem (nm)
TE
Z
SC
the absorption, λabs, and emission, λem, of Rhodamine B mixed with AOT/n-Hexane/Water for different droplet concentrations and two molar ratios (X=10 and 8) and different Z(dye/water).
35563.67637 35563.67637 35533.059 35499.5033 35496.45917 35493.4161 35472.1443 35441.84586 35627.04229 35384.2207 35294.8866
1.82988 1.82988 1.88624 1.94907 1.95482 1.96059 2.00114 2.05972 1.86376 2.35871 2.55907
The important existing mistakes in the previous published paper in this Journal have been discussed here and the correct forms of the relevant results presented. As it was mentioned, the authors have missed to consider the correct value of νa-νf and νa+νf of Rhodamine B which caused obtaining wrong results of the ratio of dipole moment. Also, the authors have missed to consider the effects of refractive index and dielectric constant of water as solvent of dye in the perturbation theory which again caused obtaining wrong results. In this work, we find the correct value of the ratio of the dipole moment of Rodamine B inside of water droplet. Moreover, the ratio of dipole moment increases with increase of droplet concentration. More change in the ratio of dipole moment is observed in samples with higher dye concentration.
Acknowledgement: This work is supported by Ferdowsi University of Mashhad Project No.2/38792.
ACCEPTED MANUSCRIPT References:
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1) Abbas Rahdar, Mohammad Almasi-Kashi ,Photophysics of Rhodamine B in the nanosized water droplets: Aconcentration dependence study,Journal of Molecular Liquids 220 (2016) 395–403. 2) Fletcher P D I, Howe A M, Robinson B H, The kinetics of solubilisate exchange between water droplets of a water-in-oil microemulsion. J. Chem. Soc. Faraday Trans.1987, 1, 985. 3) Danaf N A, Melhem R A, Assaf Kh I, Nau W M, Patra D, Photophysical properties of neutral and dissociated forms of rosmarinic acid, Journal of Luminescence 2016, 175, 50–56. 4) Ghosh S, Mitra A K, Basu S, Chakrabortyb S, Saha Ch, 5,6,7,9-Tetrahydro-[1,3]dioxolo[4,5h]carbazol-8-one: A solvatochromic PET-acceptor fluorescent probe, Journal of Luminescence 2014, 153, 296–303.
ACCEPTED MANUSCRIPT
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Graphical Abstract
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The fluorescence quenching of Rhodamine B by droplet concentration. The Redshift of Rhodamine-doped droplet. The dipole moment of Rhodamine B inside of droplet
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Highlights
S0167-7322(16)32746-5 doi:10.1016/j.molliq.2016.11.057 MOLLIQ 6604
To appear in:
Journal of Molecular Liquids
Received date: Revised date: Accepted date:
14 September 2016 13 November 2016 14 November 2016
Please cite this article as: Soheil Sharifi, Khalil Alizadeh, Seyyed Mahdi Shavakandi, Comments on ”Photophysics of Rhodamine B in the nanosized water droplets: A concentration dependence study”, Journal of Molecular Liquids (2016), doi:10.1016/j.molliq.2016.11.057
This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.
ACCEPTED MANUSCRIPT Comments on "Photophysics of Rhodamine B in the nanosized water droplets: A concentration dependence study"
PT
Soheil Sharifi*, Khalil Alizadeh, Seyyed Mahdi Shavakandi
RI
Department of Physics, Faculty of Sciences, Ferdowsi University of Mashhad, Mashhad 91775-1436, Iran
SC
Abstract:
AC CE P
TE
D
MA
NU
This comment concerns some erroneous claims, which arise from the results and discussion in the recent article by A.Rahdar (Journal of Molecular Liquids 220 (2016) 395–403). The mixture of Rhodamine B with AOT/Water/n-Hexane was studied at two water to surfactant molar ratio (Y=10 and 8). Morevoer, The effect of droplet concentration was studied on fluorescence spectra of Rhodamine B-doped droplets. The size of droplet was changed by increase of water to surfactant molar ratio(Y). The results shows, by increase of droplet concentration, the fluorescence (νf) maxima wavenumbers was changed and the absorbance (νa) maxima wavenumbers was constant. We found, the value of νa−νf and νa+νf of Rhodamine B inside of droplets is quite different from the results that found before by A.Rahdar. By theory and experiments, the corrected value of the ratio of dipole moment of Rhodamine B in droplets was reported. We have proven, the ratio of dipole moment was changed between 1.82988 to 2.05972 by increase of droplet concentration at constant molar ratio Y=10. Moreover, the effect of droplet size is reported on the ratio of excited to ground states of dipole moment at Rhodamine B. Keywords:fluorescence, nano-droplets, dipole moment. *Corresponding Author: [email protected] , [email protected]
Introduction:
In this work, the photophysics of Rhodamine B (RhB) in droplet of AOT/Water/n-Hxane microemulsion at Molar Ratio 10 and 8 was studied [1]. It is well known that the nano-droplet can prepare with mixture of water, oil (n-Hxane) and surfactant (AOT). The Rhodamine B can solve inside of water droplets in the mixture of dye with microemulsion. So, The RhB/microemulsion is RhB/water droplet inside of continuous phase of oil(n-Hxane). In this work, the mixture of dye with microemulsion is studied at different concentration of droplets in the oil at two molar ratio (Y=10 and 8). By the theory, We studied, the effect of concentration and size of droplet on, the dipole moment of ground and excited state of Rhodamine B.
ACCEPTED MANUSCRIPT Experiment:
NU
SC
RI
PT
Rhodamine b (RhB), AOT (Bis(2-ethylhexyl) sulfosuccinate sodium salt) and Hexane, were obtained from Sigma-Aldrich. All materials were used as received and MilliQ water was used in preparing all samples. Microemulsions were prepared by weight, in terms of the surfactant to water molar ratio of Y=[H2O]/[AOT], (Y=10 and 8) and the different mass fraction of droplets (mf,drop=(mH2O+mAOT)/(mTotal)), that mTotal=mH2O+mAOT+mHex, which varies by the respective mass of n-Hexane (mHex), water=(mH2O) and AOT(mAOT). All experiments were done at constant room temperature. In cases of Rhodamine B-containing microemulsions, aqueous dye solutions were mixed with oil and surfactant. The concentration of dye in droplet define by mass ratio Z=mdye/mH2O that mdye was the mass of dye. The method for the sample preparation were presented in the references [1,2]. Absorption spectra of samples were recorded with a UV-1650 PC spectrometer (Shimadzu). Fluorescence spectra (excitation at 554nm) were recorded with Jasco FP-6200 spectrofluorimeter. Results and discussions:
800 600 400
(a)
300
(b)
0.01 0.03 0.05 0.07 0.1 0.15
Fluorescence Intensity (a.u.)
Fluorescence Intensity (a.u.)
1000
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TE
D
MA
The fluorescence spectra of RhB mixed with AOT/Hexane/Water at two constant molar ratio is presented in the fig.1. Fig.1(a) is show, the fluorescence spectra of RhB/microemulsion with Y=8 and Z=0.000479 and fig.1(b) is the fluorescence spectra of the RhB/microemulsion for Y=10 and Z=0.0000625. The red shift is observed in fluorescence spectra (λem) by increase of droplet concentration from 0.01 to 0.15. The largest observed redshift (11nm) was appeared at higher concentration of dye(Z=0.000479) and the smaller redshift (4nm) was appeared at lowest concentration of dye(Z=0.0000625). The absorbance wavelength of RhB/microemulsion and RhB/water is constant at 554±1nm.
X=8
200 0
550
600
wavelength (nm)
650
0.1 0.07 0.06 0.05 0.04 0.03 0.02 0.01
250 200 150 100
X=10
50 0
550
600
650
wavelength (nm)
Fig.1. Fluorescence emission spectra (excitation at 554nm) of Rhodamine B inside of AOT microemulsion at Y=8 and Z=0.000479(a), RhB/microemulsion with Y=10 and Z=0.0000625 (b) at the different droplet mass fractionat. All the experiment was done at room temperature.
ACCEPTED MANUSCRIPT The relation between absorption and fluorescence spectra was obtained by using the quantummechanical second orderperturbation theory [3,4] that:
a f m1 f ( , n)
2(e g )2 m1 hca3
(2)
(3)
SC
2(e2 g2 ) m2 hca3
PT
a f m2[ f ( , n) 2g(n)]
RI
(1)
NU
(4)
MA
Where νa and νf are maximum frequency of absorption and emission and μg and μe are the dipole moments in the ground and excited states, respectively, h Planck's constant, c the velocity of light in the vacuum, a Onsager's interaction radius of solute, f(ε,n) and g(n) are the solvent polarity functions given by following equations:
D
2n2 1 1 n2 1 f ( , n) 2 ( ) n 1 1 n2 2
AC CE P
(6)
TE
(5)
3 n4 1 g(n) ( 2 ) 2 (n 1)2
Where n and ε are refractive index and dielectric constant of dye solvent.The A.Rahdar[1], had mentioned that" In this case, permittivity (ε) and refractive index (n) variations of system were negligible. Because the solvent type of bulk (hexane oil) in this system was constant." Firstly, the n-Hexane isn't solvent of Rhodamine B. The Rhodamine B can solve only inside of water droplet. So, the A.Rahdar should use the permittivity and dielectric constant of water as solvent of Rhodamine B. Secondly, from the perturbation theory, it isn't possible to neglect the effect of permittivity and dielectric constant. For this reason, the A.Rahdar used incorrect procedure to find the ratio of dipole moment. The results of the spectral shifts νa-νf and νa+νf ( ) are presented in the table 1. Our results shows, the νa-νf changes from 537.40667 to 659.23717( ) with increase of droplet concentration at constant dye/water ratio (Z=0.0000625).The A.Rahdar was found, the νa-νf was changed between 1×10-5 to 2×10-5( ) for the same samples,[1] that this range of variation is not observed in the absorption and fluorescence spectra. Moreover, the A.Rahdar was found that the νa-νf was changed between 0.5×10-5 to 2×10-5( ) by increase of droplet mass fraction from 0.01 to 0.1 at samples with higher dye/water concentration (Z=0.001) that this variation isn't possible. Moreover, the A.Rahdar used incorrect parameters (νa-νf and νa+νf) for calculate the ratio of dipole moment. In the perturbation theory, we used refractive index and dielectric constant of water as solvent of dye at the equations 5 and 6. So, the f(ε,n) and g(n) become constant for our results than from equations 1-4, we obtained ratio of dipole moments (dipole moment in excited state to the dipole
ACCEPTED MANUSCRIPT
ν
,ν
RI
ν
Table 1.ν
PT
moment in the ground state) and finally the results are presented in the table 1. To improve the results, the effect of droplet concentration on Rhodamine B in different molar ratio (X=8) is studied. The results show, the ratio of ground to exited state (μe/μg) changes from 1.86376 to 2.55907 by increase of droplet concentration from 0.01 to 0.1. The value of μe/μg of RhB in microemulsion with smaller size (X=8) is higher than microemulsion with bigger size (X=10) because the dye/water ratio (Z) is higher. , ratio of dipole moments(
/
), the peak wavelength of
8
0.000479
Conclusion:
NU
537.40667 537.40667 568.02403 601.57973 604.62386 607.66693 628.93873 659.23717 539.32299 782.14458 871.47868
MA
0.0000625
0.01 0.02 0.03 0.04 0.05 0.06 0.07 0.1 0.01 0.07 0.1
AC CE P
10
mf
λabc (nm) 571 554 571 554 572 554 573.1 554 573.2 554 573.3 554 574 554 575 554 570 553 578 553 581 553
D
X
λem (nm)
TE
Z
SC
the absorption, λabs, and emission, λem, of Rhodamine B mixed with AOT/n-Hexane/Water for different droplet concentrations and two molar ratios (X=10 and 8) and different Z(dye/water).
35563.67637 35563.67637 35533.059 35499.5033 35496.45917 35493.4161 35472.1443 35441.84586 35627.04229 35384.2207 35294.8866
1.82988 1.82988 1.88624 1.94907 1.95482 1.96059 2.00114 2.05972 1.86376 2.35871 2.55907
The important existing mistakes in the previous published paper in this Journal have been discussed here and the correct forms of the relevant results presented. As it was mentioned, the authors have missed to consider the correct value of νa-νf and νa+νf of Rhodamine B which caused obtaining wrong results of the ratio of dipole moment. Also, the authors have missed to consider the effects of refractive index and dielectric constant of water as solvent of dye in the perturbation theory which again caused obtaining wrong results. In this work, we find the correct value of the ratio of the dipole moment of Rodamine B inside of water droplet. Moreover, the ratio of dipole moment increases with increase of droplet concentration. More change in the ratio of dipole moment is observed in samples with higher dye concentration.
Acknowledgement: This work is supported by Ferdowsi University of Mashhad Project No.2/38792.
ACCEPTED MANUSCRIPT References:
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TE
D
MA
NU
SC
RI
PT
1) Abbas Rahdar, Mohammad Almasi-Kashi ,Photophysics of Rhodamine B in the nanosized water droplets: Aconcentration dependence study,Journal of Molecular Liquids 220 (2016) 395–403. 2) Fletcher P D I, Howe A M, Robinson B H, The kinetics of solubilisate exchange between water droplets of a water-in-oil microemulsion. J. Chem. Soc. Faraday Trans.1987, 1, 985. 3) Danaf N A, Melhem R A, Assaf Kh I, Nau W M, Patra D, Photophysical properties of neutral and dissociated forms of rosmarinic acid, Journal of Luminescence 2016, 175, 50–56. 4) Ghosh S, Mitra A K, Basu S, Chakrabortyb S, Saha Ch, 5,6,7,9-Tetrahydro-[1,3]dioxolo[4,5h]carbazol-8-one: A solvatochromic PET-acceptor fluorescent probe, Journal of Luminescence 2014, 153, 296–303.
ACCEPTED MANUSCRIPT
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Graphical Abstract
Lower Size
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600
wavelength (nm)
650
D
550
TE
0
MA
200
200 150
NU
X=8
250
0.1 0.07 0.06 0.05 0.04 0.03 0.02 0.01
SC
600
Fluorescence Intensity (a.u.)
800
AC CE P
Fluorescence Intensity (a.u.)
1000
RI
300
0.01 0.03 0.05 0.07 0.1 0.15
X=10 Higher Size
100
50 0
550
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wavelength (nm)
650
ACCEPTED MANUSCRIPT
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The fluorescence quenching of Rhodamine B by droplet concentration. The Redshift of Rhodamine-doped droplet. The dipole moment of Rhodamine B inside of droplet
AC CE P
• • •
PT
Highlights