Published at : 25 Jan 2024
Volume : IJtech
Vol 15, No 1 (2024)
DOI : https://doi.org/10.14716/ijtech.v15i1.6165
Ha Thanh Tung | Faculty of Basic Sciences, Vinh Long University of Technology Education, Vinh Long Province, Vietnam |
My Hanh Nguyen Thi | Faculty of Mechanical Engineering, Industrial University of Ho Chi Minh City, Ho Chi Minh City, Viet Nam |
Nguyen Doan Quoc Anh | Faculty of Electrical and Electronics Engineering, Ton Duc Thang University, Ho Chi Minh City, Vietnam |
The research herein concerns the composite of red
phosphor of LiLu(MoO4)2:Sm3+ (LMOS), yellow
phosphor YAG:Ce3+, SiO2 particles, and silicone gel. The
LMOS phosphor is created via the sol-gel procedure and supposed to yields
significant heat consistency. The concentration of this LMOS phosphor is fixed
at around 10 wt.% and the concentration
of SiO2 particles is modifed. This is to influence the scattering
performance of the composite to achieve the better color distribution. After
sample creation, we analyzed the luminescence of the LMOS in the composite and
the effects of the composite with different SiO2 dosages on the
commercial light-emitting diode (LED). When excited via 405-nm ultraviolet, the
samples generate red ray under 648 nm matching the shift between 4G5/2
and 6H9/2 for the ion of Sm3+. With high SiO2
amounts, the color difference is reduced, and the luminosity is enhanced. The
correlated color temperature is also lower, resulting in a warmer white light
for the packed LED. However, the color rendering index declines, which could be
attributed to the green and blue color deficiency while the red color is dominant.
From the tested outcomes, LiLu(MoO4)2:Sm3+@SiO2
composite is validated to be effective at improving chromatic uniformity
for white-ray diodes.
Blue InGaN chips; Color rendering index; Correlated color temperature; White-light-emitting diodes
Phosphors incorporated with
rare-earth ions demonstrate significant utility in the domains of solid-state
illumination, solar panels, and heat detectors, owing to their capability to
induce diverse transitions involving 4f-4f or 4f-5d energy levels. (Tung, An and Anh, 2023; Yu et
al., 2021; Yan et al., 2020). As of
today, the fluorescent as well as incandescent outdated lights can be altered
in favour of white-light-emitting diodes (WLEDs) because this light source
generation offers various qualities including significant performance, low
energy consumption, greater durability, etc (Henry and
Guruviah, 2020;
Kumar et al., 2020; Hansen et al., 2022). These
devices are often created by incorporating yellow YAG:Ce3+ phosphors
and blue InGaN chips. However, this method is deficient in red element within
the total spectrum, yielding small color rendering index (CRI) as well as
high-level correlated color temperature (CCT) (Bouchakour, Borni,
and Brahami, 2021;
Finch, Moreno, and Shapiro, 2021; Choi et al., 2019). Red phosphors such as Y2O2S:Eu3+
Following this, studies placed their aim at creating
various phosphors with null heat abatement, including those incorporated with
Eu2+, Eu3+, Mn2+, Tb3+, Mn4+,
as well as Sm3+. The sample Ca2InSbO6:Sm3+
yielded null heat abatement when heat level reaches 480 K, an outcome expected
for LED devices with significant performance (Guennoun et al., 2021).
As such, the task of augmenting phosphors’ heat abatement attributes remains
particularly difficult when it comes to creating WLED devices based on
conversion phosphor. Back to previous eras, various studies were carried out to
assess dial molybdates incorporated with rare-earth ions having composition
shown as MLn(MoO4)2 (with M being Li+, Na+
and Ln being La3+, Gd3+, Lu3+, Y3+)
in the form of inorganic substances, garnering significant notice as they can
be diversely utilized for solid-state
lasers, scintillators as well as WLED devices (Ranjith et al., 2020; Soltic
et al., 2019).
The phosphor bases possessing the CaMoO4
scheelite formation would be assessed through a unique disarrangement for the
surroundings for the ions of RE3+ with the Ca2+ locations
from CaMoO4 contingently inhabited by half of the alkali metal ion M+
as well as half of the rare earth ion Ln3+ (Attanayake, Okuya,
and Murakami, 2020).
Dual molybdate blends typically possess wide, potent charge shift line within
the near-ultraviolet zone as well as desirable heat consistency, proving to be
a fitting base substance that can be diversely utilized for WLED devices
incorporated with rare-earth phosphors (Praveen et al., 2021; Königs,
Mayr, and Buchner, 2019). The ions
of Sm3+ would be a typical trigger for orange-red discharge as it
has shifts between 4G5/2 and 6HJ
with J as 5/2, 7/2, 9/2, 11/2, being the best source when it comes illumination
and exhibition (Astuti et al., 2020). In
addition, certain phosphors incorporated with Sm3+ were created and
utilized for WLED at some points in the past. The LiLu(MoO4)2:Sm3+
(LMOS) phosphor created with sol-gel method could provide red-light component
for the WLED’s spectrum, which is supposed to effectively improve the chromatic
rendition of the package (Irawan et al., 2020). However,
this phosphor performance is barely investigated for conventional white LED
with blue InGaN chips. Therefore, in this work, the LMOS phosphor is utilized
for the goal of improving color uniformity and light distribution of the
conventional LED device. This work creates a phosphor composite comprising the
LMOS red phosphor, YAG:Ce3+ yellow phosphor, SiO2
scattering improvement particles, and silicone gel, called LMOS@SiO2
hereafter. This composite is applied for the white LED with blue InGaN chips.
In this composite, we adjust the doping dosage of SiO2 while keeping
the dosage of LMOS phosphor constant. This is to regulate the lighting
performance of the WLED with LMOS@SiO2 via the light-scattering
modification. Judging the outcomes, LMOS@SiO2 composite proves to be
useful for reducing color deviation level while improving luminosity for the
WLED device.
2.1. Creating LMOS phosphors
The LMOS samples were created using the sol-gel procedure. The ingredients used for the procedure were obtained in a pure, uncontaminated form. Table 1 lists said ingredients along with the procedure’s steps, which also apply to LiLu(1- x)(MoO4)2:x% Sm3+ with x values of 0.5, 1, 3, 5, 7, 10 (Winberg-Wang, 2019).
Table 1 Ingredients and steps to create LMOS
Ingredients |
Steps |
Lu2O3 |
- First, we dissolve Lu2O3 as well as Sm2O3
using dilute nitric acid to get the rare-earth nitrates. - Next, Li2CO3
is incorporated to the said nitrates to form a new compound, called compound
1 herein. - Then, we dissolve (NH4)6Mo7O24.4H2O
along with C6H8O7,H2O (in the form of
chelating substance) with proportion between citric acid and metal ion as 2:1
using deionized H2O to get a solution called compound 2. - The compound 2 is
subsequently added to compound 1 and the new mixture is created. The pH of
this new mixture is fixated to 6 using NH3,H2O. -
Continuously, a heating and then stirring process under 353 K is carried out
for the mixture to create a dry gel in yellow. - To get the final product from
the attained gel, we pulverize the gel within agate mortal, then calcine it
within a muffle furnace under 973 K within five hours. The obtained phosphor
substances yield white hue. |
Sm2O3 | |
Li2CO3 | |
(NH4)6Mo7O24.4H2O | |
C6H8O7,H2O | |
HNO3 | |
NH3,H2O |
2.2. Assessing attributes
Following the creation of the
samples, assessments were carried out to determine their attributes.
Appropriate tools were utilized for this task. Table 2 below details attributes
along the tools used (Altenberg-Vaz and Inanici., 2021).
Table 2
Attributes and associated tools used for the samples
Attributes |
Assessing tools |
Stage data |
X-ray powder diffraction (XRD) via Panalytical X’Pert diffractometer with radioactivity within the scanning scope of = 10–80? at scanning rate reaching 10each minute |
Rietveld
formation rectification |
Smart
Lab Studio II program |
Form |
Field
discharge scanning electron microscope (SEM JSM-6700F) accompanied by
power-dispersal spectrometer spectra |
Ultraviolet–observable
dispersal reflectance spectrum along with Fourier Infrared spectrum |
UV-2500
UV–Vis spectrophotometer along with ALPHA infrared spectrometer |
Photoluminescent
spectra as well as luminescent degradation arches based on heat level |
Fluorolog-3
fluorescent spectrometer (Fluorolog-3, Jobin Yvon, USA) |
3.1. Luminescence calculation for LMOS
The power gap will be determined via ultraviolet-observable absorbing spectra by applying the expression below (equation 1) (Nahon, Beckers, and Blanpain, 2019):
? signifies the absorptivity
coefficient. h signifies Planck constant. v signifies optical
periodicity. K signifies constant. n signifies constant corresponding to
various forms of electron shifts with values of 1/2, 2, 3/2, 3 respectively
applying to directly allowed, indirectly allowed, directly forbidden,
indirectly forbidden shifts.
For
the task of generating non-radioactive power shift among the surrounding Sm3+
triggers, two distinct forms of non-radioactive power shift exist:
reciprocating interactivity as well as multi-state interactivity. Assessing the
critical range would be necessary to identify the best one. Power shift via
multi-polar interactivity manifests if the critical range exceeds 5 Å. On the
other hand, reciprocating interactivities manifest if critical range goes below
5 Å. For the task of clarifying the concentration abatement, the critical range
will be determined by the expression below (equation 2) (Ali et al., 2019):
V
signifies cell’s volume as 289.854 Å. ?c signifies the critical concentration. N signifies the
cation amount within the latticework, equal to 2. The yielded critical range
reaches 20.974 Å, noticeably exceeding 5 Å. As such, the non-radioactive power
shift would be deemed multi-polar interactivity. Based on Dexter’s work, it is
possible to utilize an expression for the task of approximating the potential
forms of said interactivity (equation 3) (Pierson et al., 2021):
The CIE coordinates for LMOS when excited at 405 nm appeared to be
(0.5806, 0.4145), resulting in the display of red discharge within the hue
scale. For the task of illustrating the capabilities for LMOS, we assessed the
sample’s correlated color temperature (CCT) as well as hue clarity. The McCamy
expression below will determine the CCT (equation 4)
(Chen
and Wu, 2019):
xe
(0.03320) and ye (0.1858) denote hue focal points with x, y being
the CIE coordinates. The yielded correlated color temperature output reached
1692.08. The hue clarity would be essential for the task of assessing the
luminescent output for LMOS and will be determined via the expression below (equation
5) (Xue and Xie, 2020):
The
yielded hue clarity reached 98.94% with hue coordinates (x, y) for LMOS as
(0.5806, 0.4145), the white illuminating site (xi, yi) as
(0.3333, 0.3333), as well as prevalent wavelength site (xd,
yd) as (0.5834, 0.4158).
It is possible to fit the luminescent
degradation arch by utilizing dual-exponential expression (equation 6) (Mukunda, Joshi,
and Mahato, 2022):
3.2. LMOS@SiO2
effects on WLED outputs as a function of varying SiO2 amounts
In the prepared composite,
the concentration of YAG:Ce3+ phosphor must be changed corresponding
to different doping amount of the SiO2 particles. This situation is
demonstrated in Figure 1. In the graph, the amount of SiO2 varies
from 0 wt.% to 50 wt.%, followed by the decline in YAG:Ce3+
concentration. Particularly, these changes appear to be an inverse mechanism,
with the YAG:Ce amount almost linearly decreasing from its peak at 0 wt.% SiO2
to the bottom at 50 wt.% SiO2. As the amount of SiO2
surges, the scattering coefficient is heightened, leading to better dispersion
for the illumination. Besides, the generated light by blue chip can be
effectively propagated then transmitted through the phosphor composite. As a
result, the amount of re-absorbed light by phosphors is reduced, the
luminescence will be heightened when the blue-ray dispersion in the direct path
surges while the blue-ray rear-dispersion is diminished (Rubeis et al.,
2021). So, the decreasing
concentration of YAG:Ce3+ phosphor contributes to improving the
scattering performance in the presence of increasing SiO2 dosage.
With the enhancing
scattering performance, higher SiO2 dosages also affect correlated
color temperature (CCT) levels, as shown in Figure 2. In the figure, the CCT
levels recorded in the viewing angles of ±90o with SiO2
amounts range of 0-50 wt.%. In general, in ±20o, the CCT level
declines and becomes relatively flattened as we increase the SiO2
concentration. This indicates that the white light is warmer when exposing to
human eyes directly. On the other hand, in ±90o, the CCT levels
exhibit a significant fluctuation, but still lower than the value obtained with
0 wt.% SiO2 in the package. The deviation of CCT range is
particularly calculated and displayed in Figure 3. Apparently, with different
SiO2 dosages, the CCT show notable fluctuations. However, as the
SiO2 amount increases continuously to 50 wt.%, significant
CCT-deviation reduction is achieved. The CCT is at its lowest with the SiO2
amount of 50 wt.%. The other notable CCT-deviation reduction levels are also
obtained with SiO2 concentration of 30-35 wt.%. Though with the
amount of 40-45 wt.% SiO2, the CCT-level aberration sharply goes up,
it is lower than the CCT level of the composite sample without SiO2.
This indicates that the light dispersion is influenced and enhanced with the
presence of SiO2, revealing the enhancement in converted red-light
proportion by LMOS phosphor.
Conversely, for the lumen of the WLED
shown in Figure 5, the considerable and continuous rise is noticed regarding
the higher SiO2 doping amounts. This event could be a result from
the better blue-light discharge induced by greater forward light dispersion and
lower light re-absorbance. It is noteworthy that increasing the particle
concentration of SiO2 can enhance the transformation of illumination
from blue to yellow or red-orange. This effect is primarily attributed to the
broader scattering range, allowing more blue light to be mixed, to interact
with the phosphor particles in the composite, and be converted. However, if the
scattering is too much, the transformed light may undergo rear-reflection,
thereby possibly reducing the intensity of luminescence and resulting in a
higher correlated color temperature (CCT) level (Costa et al., 2019). Thus, we predict that if the SiO2 is more
than 50 wt.%, the luminous flux of the WLED with LMOS@SiO2 sheet
will decline. Yet, this will be analyzed in future works.
Figure 1 YAG:Ce
concentration under influence of increasing SiO2 amount
Figure 2 Angular CCT range monitored with different SiO2 amounts
Figure 3
CCT-range deviation responding to different SiO2 amounts
Figure 4 LED
lumen responding to different SiO2 amounts
The output of hue generation of the WLED device is also affected by the dosage of SiO2. As the particle size increases from 0 wt.% to 50 wt.%, color rendering index (CRI) and color quality scale (CQS) shows a noticeable deterioration in a relatively linear manner, see Figures 5 and 6, respectively. This observed decline is possibly the result of the lack of green and blue spectra in the white light emission. Under great dosages of SiO2, the heightened dispersion generates more orange-yellow elements, resulting in the mentioned emission-color deficiency since the ray’s discharge hue generally favors the orange-yellow zone. As such, unnecessary dispersion can cause inferior CRI as well as CQS (Guerra et al., 2020).
Figure 5 CRI
under influence of SiO2 particle size
Figure 6 CQS
under influence of SiO2 particle size
In the previous eras where
the scientific fields were unfamiliar with hue assessment, color
rendering index (CRI) was created and
was deemed the only way to evaluate the quality of hue generation in a ray when
compared to natural lights. Eventually, the flaws of CRI became a concern (Danny et al.,
2020). Notably, its mechanism to
measure hue desirability in lighting devices was not reliable for utilizing outdated hue samples and inaccurate hue
scale. In the case of incandescent
lights with perfect CRI output of 100, it was reported that the human sight did
not witness the correct hue recreation based on the standard of sun ray (Thi et al.,
2023). For fluorescent light which
yielded a low CRI output, its ability to
illuminate the environment was found to be superior. When it comes to LED
devices, they generate desirable light while not generating significant
temperature, a factor that is heavily assessed by CRI considering that
luminescent light was unheard of back in the old times. As a result,
high-quality WLED devices end up yielding an inferior CRI when compared to the
more outdated lights mentioned above. Color quality scale (CQS), on the other hand, overcome the drawbacks of its
predecessor by assessing more facets, such as human preference as well as
additional hue samples, thus yielding more accurate results that fit our
perception and proven to be a better hue-output indicator for WLED devices (Thai et al., 2023).
The study herein concerns phosphor LiLu(MoO4)2:Sm3+@SiO2
composite for the conventional WLED model with blue chips. The LMOS
phosphor possesses the tetragonal setting and generates red ray under 648 nm
when excited via near-ultraviolet ray under 405 nm. The primary concentration
abatement nature in Sm3+ appeared to be the result of dipole-dipole
interactivities. By fixing the concentration of LMOS phosphor and varying the
SiO2 doping amount, the illumination properties including color
distribution and luminosity of the WLED can be regulated. Specifically,
increasing the SiO2 content leads to a decrease in color discrepancy
and an improvement in brightness. Additionally, it results in a lower
correlated color temperature, creating a warmer white light for the compact
LED. However, this increase in SiO2 content also causes a decline in
the color rendering index, which can be attributed to a deficiency in green and
blue colors while the red color remains dominant. The outcomes prove that LiLu(MoO4)2:Sm3+@SiO2
can be used to generate red rays and induce color uniformity for conventional
WLED devices.
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