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https://doi.org/10.1007/s11356-021-14551-9
RESEARCH ARTICLE
Received: 28 July 2020 / Accepted: 19 May 2021 / Published online: 7 June 2021
# The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2021
Abstract
New experimental results of morphological and optical properties of Curcuma longa dye thin film were investigated. The thin
films were deposited by physical vapor deposition technique. Morphological properties were measured using atomic force
microscopy technique and they show a granular structure which above there are nanotubes shapes. Photoluminescence of
Curcuma longa at low temperature was investigated and discussed for the first time. The temperature effect from 77 to 300 K
of Curcuma longa thin film has been shown and luminescence was strongly observed. Photoelectrochemical parameters of the
dye-sensitized solar cell based on Curcuma longa have been computed via the finite element method. The power conversion
efficiency is about 0.86% obtained from short circuit current, open-circuit voltage, and fill factor of 0.13 mA/cm2, 0.52 mV, and
0.83, respectively. As a result, Curcuma longa dye can be applied to dye-sensitized solar cells.
Keywords Dye-sensitized solar cell (DSSC) . Natural dyes . Curcuma longa dye . Physical vapor deposition (PVD) . Atomic force
microscopy (AFM) . Transmittance . Photoluminescence . Decay time
Introduction
Hossain et al. 2018a). Nevertheless, the procedures for the measurements of Curcuma longa were generated at low tem-
synthesis of efficient synthetic dyes are extremely consuming peratures going from 77 to 300 K, and the temperature effect
and require expensive and complicated dye materials. is noticed and discussed. A numerical study of DSSC based
Consequently, natural dyes are considered as a viable alterna- on Curcuma longa dye using the finite element method was
tive to inorganic dyes, this is due to its outstanding remarkable computed.
advantages, i.e., low manufacturing cost, easy extrac-
tion, energy recovery time, flexibility, availability of
raw materials, environment friendly, and multicolor Deposition technique of Curcuma longa thin
(Hossain et al. 2017, 2018d). films
The natural dye such as Curcuma longa is one of the most
promising candidate for DSSC. Curcuma longa is a yellow- Thin films of Curcuma longa dye were deposited on silicon
orange powder extracted from turmeric, with a chemical for- and glass substrates by means of physical vapor deposition
mula of C21H20O6 and it is formed by two feruloyl (aryl technique (Zawadzka et al. 2012; Korcala et al. 2019;
buten-2-one) chromophores linked by a methylene group Aamoum et al. 2019, p.). It was better to deposit the thin film
(Chignell et al. 1994). Various attempts have been devoted on silicon for AFM to have clear measurements, and on the
experimentally and theoretically to study Curcuma longa. In glass for transmittance and photoluminescence measurements
the experimental point of view, Buddee et al. and Suresh et al. (Anoua et al. 2019, 2020; Lougdali et al. 2019).
reported that Curcuma longa has a strong absorption visible The description of PVD apparatus used in this work is
range from 420 to 580 nm using the asorbance spectrum and shown in Fig. 1. The chamber reaches the high vacuum pres-
from 380 to 520 nm using the diffuse reflectance spectrum sure at 2 × 10−5 Torr via the rotary pump following by the
(DRS), respectively (Buddee et al. 2014; Suresh et al. 2015). diffusion pump. The temperature of the evaporation (80 °C) of
These optical properties have shown that Curcuma longa the Curcuma longa dye was reached, by supplying the tem-
would certainly be interesting as a natural dye to extend visi- perature that was manually controlled by coil heating resis-
ble light response of the SC. By varing the TiO2 film thickness tance tungsten filament wire. The temperature was slightly
in the range of 5–25 μm, Hossain et al. showed that Curcuma increased around 20 °C to raise the efficiency of the process.
longa dye can be used as a sensitizer in DSSCs with photo-
current densities of 0.17 to 0.49 mA·cm2 (Hossain et al.
2018c). From the cyclic voltammetry, Sinha et al. reported Results and discussion
that the redox response of the Curcuma longa is completely
irreversible. Curcuma longa has a broad energy band gap with Morphological proprieties
high electron affinity and oxidation peak, as well as a low
driving energy. Consequently, it is more suitable and stable Atomic force microscopy characterization is a non-destructive
for DSSC application (Sinha et al. 2018). On the other hand, method of analyzing the topography of the given sample. The
from a theoretical point of view using density functional the- obtained information are the three-dimensional morphology
ory (DFT), Ilić and Paunović have investigated the electronic and the toughness of the analyzed surface (Chelouche 2018).
properties of Curcuma longa and they confirm that the elec- The morphology of Curcuma longa dye thin film deposited
trons have a higher probability of reaching the CB, which on silicon substrat was performed by atomic force microscopy
points to another reason why DSSC based on Curcuma longa technique. The AFM imaging was investigated in contact
could have greater efficiency (Ilić and Paunović 2019). Other mode, with a Nanosurf Easyscan 2 AFM equipment. Fig. 2
researchers studied also the electronic properties and con- presents AFM images at room temperature of the deposited
firmed that the lowest unoccupied molecular orbital thin film of Curcuma longa dye at three different sizes. From
(LUMO) of Curcuma longa dye is above the conducting band Fig. 2a, the particles are randomly spread all over the surface
(CB) of TiO2 (Abduljalil et al. 2018), which is a necessary of the sample. A non-uniform granular structure of the layer is
property that allow the confirmation of the use of the dye as a presented in Fig. 2c. The grains are very small and
sensitizer to DSSC. nanometric, which above the growth of nanowires as shown
In this work, Curcuma longa is used as a natural sensitizer. in Fig. 2b.
As a novelty, Curcuma longa is deposited as a thin film by
physical vapor deposition (PVD) technique. The obtained Optical properties
morphological properties of the thin film were investigated
by atomic force microscopy (AFM). In order to validate the Transmittance
use of Curcuma longa as a dye for DSSC, optical properties
using transmittance and photoluminescence (PL) spectros- The optical transmittance spectrum of Curcuma longa dye
copies were performed. New photoluminescence thin film was performed at room temperature, by using
57862 Environ Sci Pollut Res (2021) 28:57860–57871
Fig. 2 AFM 3D images of the surface morphology of Curcuma longa dye thin film deposited by the PL technique: a 50 × 50 μm area, b 10 × 10 μm
area, c 2 × 2 μm area
Environ Sci Pollut Res (2021) 28:57860–57871 57863
Perkin Elmer Lambda 2 Spectrophotometer. Fig. 3a shows the where A is the absorbance that is extracted from transmit-
transmittance spectrum as a function of the wavelength tance, T (A = − log T), and x is the thickness of the thin film.
in the spectral range of 280–1100 nm of Curcuma The thickness measured by the profilometer is 447.4 nm.
longa dye, and Fig. 3b its absorbance obtained from The analysis of the absorbance coefficient as a function of
the equation A = − log T. wavelength allows to determine the optical energy band gap
In the ultraviolet range, there is an average transmittance of for the material based on Eq. (2) (Tauc et al. 1966; Pankove
about 0.4 U.E between 320 and 400 nm. However, in the and Kiewit 1972).
c c r
visible range, particularly from 400 to 500 nm, the material αh ¼ B h −Eg ð2Þ
absorbs the light. From 500 nm, the transmittance increases λ λ
slightly to stabilize reaching 0.9 U.E. The absorption in the
where α is the absorbance coefficient, h is the Planck con-
range of 400–500 nm is in good agreement with the previous
stant, c means the speed of light, λ is the wavelength, Eg
published works (Soltani Rad et al. 2015; Condat et al.
represents the energy gap value, B represents a parameter de-
2015; Hatamie et al. 2018; Ilić and Paunović 2019).
pending on the optical probability, and r defines the type of
Fig. 4a presents the absorbance coefficient of Curcuma
the optical transition.
longa dye, and this coefficient is calculated by the fol-
The best fit of Eq. (2) was obtained for r = 1/2. It means that
lowing equation (Kodigala 2010):
the nature of the transition is direct permitted optical transi-
tions. Therefore, Eq. (2) becomes:
A
α¼ ð11Þ c
0; 4343 x ðαEÞ2 ¼ B E−E g where E ¼ h ð3Þ
λ
Fig. 4 a Absorbance coefficient spectra and b energy band gap determination plots of Curcuma longa dye
57864 Environ Sci Pollut Res (2021) 28:57860–57871
Photoluminescence
Fig. 6 3D excitation-emission
luminescence spectrum at room
temperature of Curcuma longa
dye thin film
Environ Sci Pollut Res (2021) 28:57860–57871 57865
Fig. 7 Photoluminescence
emission spectra of Curcuma
longa dye at different
temperatures
ature range from 77 to 300 K. The sample was placed in a longa dye thin film is about nanoseconds. Consequently, the
vacuum chamber and cooled using nitrogen gas. Fig. 7 shows emission is fluorescence, because the average lifetime of fluo-
the plot of photoluminescence of Curcuma longa dye at dif- rescence is 1 to 104 nanoseconds which is shorter than phos-
ferent temperatures. phorescence (usually seconds to minutes) (Khopkar 1998).
At lower temperatures, the higher intensities of the lumi- The graph (Fig. 11) exhibits a decrease of the lifetime with
nescence were observed. The luminescence intensity de- increasing the temperature. It can be observed that the lifetime
creases as a consequence of increasing the temperature. The decreases by 37% from 77 K to room temperature (300 K).
data for photoluminescence measurement are listed in Table 1. And proved that photoluminescence decreases with increasing
It can be noticed that the emission wavelength corresponds to temperature due to the nonradiative transition which reduces
the maximum PL intensity shifts by 2 nm for every 25 K. the lifetimes of fluorescence.
Figure 8 presents four Gaussian fit of the emission spec-
trum for the temperatures 77 K, 175 K, and 300 K. The values
of the maximum emission wavelengths intensity (Xc), the Use οf numerical simulation
maximum PL intensities (height), and the full width at half
maximum (FWHM) are presented in Table 2. Optical-electrical mοdel is used in the numerical simulation
The luminescence decreases by increasing the temperature. coupled with a two-step, in order to take advantage of the
This behavior is explained in Fig. 9 which shows the probable
absorption and emission process. The emission of Curcuma
longa dye obtained is about fluorescence, it is attributed as a Table 1 Results of photoluminescence measurements at low
temperatures
singlet to singlet transition (Skoog et al. 2007). The tempera-
ture dependence can be explained by the extra energy given to Temperature (K) Maximum PL Emission wavelength
the electron, which allows a jump from a vibrational state to an intensity (CPS) corresponding to the
upper vibrational state when the temperature increases. By the maximum PL intensity (nm)
return of the exited electron to the ground state, the electron 77 6 × 105 524
loses the excess of vibrational energy in the form of 100 4.7 × 105 526
nonradiative vibrational relaxation, and consequently, the lu- 125 3.36 × 105 528
minescence decreases. 150 2.4 × 10 5
530
175 1.67 × 105 532
Decay time The decay time was investigated at the maximum
200 1.24 × 105 534
luminescence wavelength (524 nm) (Zawadzka et al. 2014), as
225 1 × 105 536
presented in Fig. 10, at different temperatures of the measure-
250 8.3 × 104 538
ments. A single exponential fit is applied to the obtained
275 6.5 × 104 538
curves. The values of the decay times are shown in Fig. 11.
300 6.6 × 104 540
According to Fig. 11, the lifetime of the emission of Curcuma
57866 Environ Sci Pollut Res (2021) 28:57860–57871
Fig. 8 Curves fitting for emission spectra of Curcuma longa dye thin film with changing temperature: T = 77 K (a), T = 175 K (b), T = 300 K (c)
photoanode 3D design which can be straight. It can be inte- of this cell is necessary. Fig. 12 presents the 3D DSSC. The
grated into the model as well as the effect of the trap of light unit cell of DSSC contains one single nanorod.
can be analyzed as a natural extension. The input parameters that affect the optical model are the
For the enhancement of the efficiency of charge carrier thickness οf the TiΟ2 layer, FTΟ nanοrοd length, and spacing,
extractiοn (Lee et al. 2010, 2014), a design of 3D DSSC based and the optical parameters of the dye used. The refractive
on FTO (fluorine-doped tin oxide) nanorod to develop the index οf the TiΟ2 layer is extracted frοm the literature
optical-electrical mοdel simulated to determine the physics (Rothenberger et al. 1999).
Table 2 Results of the Gaussian fitting for emission spectra by changing temperature. Xc in nm, height in CPS, and FWHM in nm
77 K 528.74 382,168.23 37.78 508.42 295,262.52 23.15 553.96 273,465.24 55.12 594.26 110,441.12 91.36
100 K 530.06 305,207.39 39.04 556.30 206,052.83 56.903 597.70 79,469.78 92.52 509.08 228,555.27 23.95
125 K 531.04 210,758.49 39.45 510.27 147,152.34 25.31 557.63 148,687.04 57.90 599.97 55,942.45 94.34
150 K 532.01 146,325.00 40.49 511.14 96,067.69 26.47 558.64 107,349.85 59.30 601.10 40,697.24 96.361
175 K 533.67 103,199.65 41.96 512.25 64,043.22 28.68 561.49 74,508.99 60.96 605.28 27,761.15 97.03
200 K 532.53 74,977.32 42.15 511.31 38,748.65 28.409 560.17 59,139.91 61.49 603.53 23,206.26 98.02
225 K 531.66 57,522.33 42.33 509.81 25,379.29 26.7877 559.16 48,153.65 61.79 601.97 19,753.59 98.79
250 K 533.84 49,002.31 44.97 511.26 20,196.2 28.05 562.82 37,491.44 66.05 607.18 13,856.33 103.56
275 K 533.38 37,359.22 44.65 510.89 15,490.32 27.33 561.92 30,511.28 65.70 604.76 11,828.50 103.18
300 K 536.04 33,674.25 45.799 513.72 15,050.76 28.90 564.99 24,973.99 67.50 607.67 9012.69 104.06
Environ Sci Pollut Res (2021) 28:57860–57871 57867
The I-V curve is obtained from the photocurrent and the Simulatiοn results
phοtοvοltage measurements from the solar simulator. To cal-
culate the EQE (External Quantum Efficiency) and IQE Figure 13 shows the electron concentration and the electron’s
(Internal Quantum Efficiency) curves, in each wavelength, recombination in the simulation for a unit cell in the center
the calculation of electrons rate and the photocurrent at shοrt section. The electrοn flοw is calculated as the gradient οf the
circuit cοnditiοns is necessary. The EQE is calculated by the electrοn cοncentratiοn in the TiΟ2 cοnductiοn band.
ratio between the number of electrodes that are generated and Figure 14 presents the current-vοltage characteristics οf
the number of photons of monochromatic light. The IQE is sοlar cells fabricated with different cοnditiοns under
calculated by the ratio of the number οf the extracted electrοns illuminatiοn that is under 5.8 mW/cm2 halogen illumination.
and the number οf phοtοns absοrbed by the TiΟ2 layer. The dye cell, cοnsisting οf a TiΟ2/Curcuma longa dye system,
Fig. 11 The values of the decay time of Curcuma longa dye at the
maximum of luminescence wavelength at different temperatures of the
measurements
where ff is the fill factor, Im and Vm are respectively the
shοws the cοnversiοn efficiency abοut 0.86%. The shοrt cir- current and voltage that the cell can deliver, and Isc and Voc
cuit current is ~0.13 mA/cm2 and the οpen-circuit vοltage is correspond respectively to the short circuit current and open-
abοut 0.52 V. circuit voltage.
These results indicate a better electrical cοntact between all
elements οf the nanοstructure. Fig. 15 displays the P-V curves Pm ðmW=cm2 Þ
η¼ 100% ð5Þ
οf DSSC that is made from Curcuma longa dye. This figure Pi ðmW=cm2 Þ
allοws to extract the essential οperating parameters such as the
parameters listed in Table 3 by using Eqs. (4) and (5). where ff is the fill factor, η represents the power conversion
Im Vm efficiency, Pm is the output power, and Pi is the input power.
ff ¼ ð4Þ Therefore, due to the low cost, environmental friend-
I sc V oc
liness, and technical efficiency of the extracted pig-
ments, Curcuma longa is a good candidate for the de-
velopment of industrial scale DSSC production. This
approach is encouraged because the photovoltaic effect
of DSSC based on Curcuma longa dye has been
achieved and all that remains is to optimize the
Fig. 12 Illustratiοn οf the 3D DSSC structure Fig. 14 I-V curve οf DSSC based on Curcuma longa dye
Environ Sci Pollut Res (2021) 28:57860–57871 57869
Conclusion
Funding This research has been financed from the funds of the Polish Hara K, Horiguchi T, Kinoshita T et al (2000) Highly efficient photon-to-
National Science Centre (grant no. 2017/25/B/ST7/02124). The films electron conversion with mercurochrome-sensitized nanoporous ox-
used in this paper were obtained using Interdisciplinary Centre for ide semiconductor solar cells. Sol Energy Mater Sol Cells 64:115–
Modern Technologies facilities, NCU, Torun, Poland. 134. https://doi.org/10.1016/S0927-0248(00)00065-9
R. Anoua wishes to acknowledge the Centre National pour la Hatamie S, Ahadian MM, Iraji zad A et al (2018) Photoluminescence and
Recherche Scientifique et Technique CNRST (Morocco) for the funding electrochemical investigation of curcumin-reduced graphene oxide
of her doctoral scholarship (Pre-Doctoral Grants 2019). sheets. J Iran Chem Soc 15:351–357. https://doi.org/10.1007/
s13738-017-1236-4
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Hydrothermal preparation of highly photoactive TiO2 nanoparticles.
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Ethics approval and consent to participate Not applicable. 053
Hossain FM, Sheppard L, Nowotny J, Murch GE (2008) Optical proper-
Consent for publication Not applicable. ties of anatase and rutile titanium dioxide: Ab initio calculations for
pure and anion-doped material. J Phys Chem Solids 69:1820–1828.
Competing interests The authors declare no competing interests. https://doi.org/10.1016/j.jpcs.2008.01.017
Hossain MK, Pervez MF, Mia MNH, Mortuza AA, Rahaman MS, Karim
MR, Islam JMM, Ahmed F, Khan MA (2017) Effect of dye
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