Re iew
Unde s anding he s uc u al and op ical e olu ion o Eu
3+
and Dy
3+
co-doped YVO
4
phospho s ac oss concen a ion se ies o
ligh ing applica ions
Houssem Eddine Sek a i
a,b,*
, Eya He gli
a,b
, S anisla Fe do
a,b
, Paulo J.G. Cou inho
a,b
,
Luis Rebou a
a,b
a
Physics Cen e o Minho and Po o Uni e si ies (CF-UM-UP), Uni e si y o Minho, B aga 4710-057, Po ugal
b
Labo a o y o Physics o Ma e ials and Eme gen Technologies, LaPMET, Uni e si y o Minho, B aga 4710-057, Po ugal
ARTICLE INFO
Keywo ds:
Nanophospho s
Whi e LED
Pho oluminescence
YVO
4
:x(Eu
3+
, Dy
3+
) Band gap
Ene gy ans e
ABSTRACT
YVO
4
nanopa icles co-doped wi h Eu
3+
and Dy
3+
ions we e success ully syn hesized using a con en ional co-
p ecipi a ion me hod. The esul ing phospho s exhibi ed a single-phase igonal YVO
4
s uc u e, wi h nano-
pa icles a e aging app oxima ely 60 nm in size, ob ained by measu emen s ca ied ou wi h scanning elec on
mic oscope images. UV– isible di use e lec ance spec oscopy analysis e eals ha he di ec band gaps o ou
samples all wi hin he ange o 3.6–3.75 eV. A e a ho ough analysis, he op imal doping concen a ion was
iden i ied as 2 a % Eu
3
⁺ and 2 a % Dy
3+
ions co-doping, exhibi ing he s onges up-con e sion emission in ensi y
unde 310 nm exci a ion. YVO
4
:x(Eu
3+
, Dy
3+
) phospho s exhibi dis inc bands co esponding o ansi ions o
Dy
3+
and Eu
3+
ions om hei
4
F
9/2
and
5
D
0
exci ed s a es, espec i ely. The ene gy ans e om Dy
3+
o Eu
3+
is
alida ed h ough elec ic dipole–dipole in e ac ion, wi h a c i ical dis ance o 15.63 Å. YVO
4
nanopa icles co-
doped wi h Eu
3+
and Dy
3+
ions exhibi wide- ange con ol o e hei pho oluminescence colo by egula ing he
concen a ion o bo h dopan s. These indings sugges g ea po en ial o applica ions in cu en indus ial
se ings.
1. In oduc ion
Reducing global ene gy consump ion is a p essing challenge o e-
sea che s wo ldwide [1]. De eloping and imp o ing whi e
ligh -emi ing diodes (WLEDs) has gained signi ican a en ion as a po-
en ial eplacemen o con en ional luo escen and incandescen
lamps [2]. This is due o WLEDs’ nume ous ad an ages, including low
ene gy consump ion, long li espan, high luminous e iciency, and
en i onmen al iendliness [3]. WLEDs a e a c ucial componen o
mode n ligh ing echnology, wi h a wide ange o applica ions in gene al
ligh ing, backligh ing, and au omo i e ligh ing. A common app oach o
achie ing whi e ligh u ilizes a blue LED chip coa ed wi h a yellow
phospho , known as he "blue-pumping" me hod [4]. Howe e , his
me hod su e s om limi a ions like low colo ende ing index (CRI) and
high co ela ed colo empe a u e (CCT) [5]. An al e na i e me hod
employs a ed, g een, and blue (RGB) LED chip combina ion, enabling a
wide colo gamu and highe CRI [5]. Howe e , his app oach neces-
si a es p ecise con ol o e he in ensi y and wa eleng h o each LED
chip, inc easing complexi y and cos . A p omising app oach u ilizes a
single, dual-emi ing phospho , like YVO
4
:Bi
3+
, Eu
3+
[6,7], which sim-
pli ies manu ac u ing and educes cos s while main aining high CRI and
low CCT. This phospho exhibi s high he mal s abili y and excellen
luminescence p ope ies, making i ideal o WLED applica ions.
Fu he mo e, Li
+
co-doping in he YPO
4
:Dy
3+
sys em p esen s exci ing
possibili ies o display de ices [8]. The co-doping enhances Dy
3+
emission in ensi y and imp o es he mal s abili y, making he phospho
sui able o high-powe WLEDs [9].
Di e en i alen a e-ea h (RE) ions, such as Eu
3+
, Dy
3+
, Tm
3+
,
and Sm
3+
, a e commonly used as ac i a o s in he anada e hos la ice
[10,11]. These RE ions can also be co-doped o enhance emission e i-
ciency h ough ene gy ans e mechanisms. Howe e , he co-doping o
di alen ions can also signi ican ly impac he emission spec a o he
ma e ial. Fu he mo e, y ium anada e (YVO
4
) doped wi h a ious RE
ions exhibi s ema kable e sa ili y, co e ing nea ly he en i e isible
spec um wi h i s di e se emission colo s. YVO
4
is a c i ical hos ma e-
ial due o i s excep ional combina ion o p ope ies. These include a
* Co esponding au ho a : Physics Cen e o Minho and Po o Uni e si ies (CF-UM-UP), Uni e si y o Minho, B aga 4710-057, Po ugal.
E-mail add ess: [email p o ec ed] (H.E. Sek a i).
Con en s lis s a ailable a ScienceDi ec
Jou nal o Alloys and Compounds
jou nal homepage: www.else ie .com/loca e/jalcom
h ps://doi.o g/10.1016/j.jallcom.2024.177389
Recei ed 4 Sep embe 2024; Recei ed in e ised o m 28 Oc obe 2024; Accep ed 3 No embe 2024
Jou nal o Alloys and Compounds 1010 (2025) 177389
A ailable online 6 No embe 2024
0925-8388/© 2024 The Au ho (s). Published by Else ie B.V. This is an open access a icle unde he CC BY license (
h p://c ea i ecommons.o g/licenses/by/4.0/ ).
high mel ing poin o app oxima ely 1810 ◦C, iso opic ligh emission
wi h a e ac i e index o a ound 2.02, low phonon ene gy (<900 cm
−1
),
and a di ec bandgap o app oxima ely 3.6 eV [12].
Dy
3+
ions, wi h hei cha ac e is ic 4 [13] elec onic con igu a ion,
exhibi emission spec a p ima ily o igina ing om he
4
F
9/2
ene gy
le el. This esul s in wo dis inc na ow emission lines: a blue ligh
emission (470–500 nm) co esponding o he
4
F
9/2
→
6
H
15/2
ansi ion,
and a yellow ligh emission (570–600 nm) co esponding o he
4
F
9/2
→
6
H
13/2
ansi ion [13,14]. No ably, he in ensi y a io o hese yellow
and blue emissions is highly sensi i e o he su ounding c ys al en i-
onmen o he Dy
3+
ions. By ca e ully selec ing a sui able hos ma e ial
and doping i solely wi h Dy
3+
, whi e-emi ing phospho s can be ach-
ie ed h ough manipula ion o his in ensi y a io [15]. In con as , Eu
3+
ions a e widely used as e icien ac i a o s o ed-emi ing phospho s.
Thei emission lines a ise om elec onic ansi ions o igina ing om
he exci ed
5
D
0
le el o he a ious
7
F
J
(J =0, 1, 2, 3, 4, 5, 6) le els
wi hin he 4 [16,17] elec onic con igu a ion [14,18]. Impo an ly, he
emission spec a o Eu
3+
a e s ongly in luenced by he symme y o he
si es hey occupy wi hin he hos ma e ial. This sensi i i y a ises om
he combined e ec s o elec onic-dipole and magne ic-dipole in-
e ac ions o he in e nal 4 elec ons. The e o e, he selec ion o an
app op ia e hos ma e ial plays a c i ical ole in de e mining he lumi-
nescen p ope ies o ino ganic phospho s by p o iding a sui able c ys al
ield en i onmen o he ac i a o ions.
To u he enhance he luminescen cha ac e is ics o YVO
4
, doping
wi h speci ic RE ions, such as Eu
3+
and Dy
3+
, p esen s a iable s a egy.
These ions in oduce no el ene gy le els wi hin YVO
4
’s band gap,
esul ing in heigh ened luminescence e iciency and cus omizable
emission colo s.
Building on his concep , esea che s ha e in es iga ed co-doping
o ho anada es wi h Eu
3+
and Dy
3+
ions. They ypically op imize he
pho oluminescence in ensi y by i s doping he YVO
4
ma ix wi h a
single dopan (ei he Eu
3+
o Dy
3+
) a a ying concen a ions. Subse-
quen ly, hey in oduce a se ies o di e en concen a ions o Eu o Dy
in o he p e-doped YVO
4
:Eu
3+
o YVO
4
:Dy
3+
ma ix. Ou wo k p esen s
a no el app oach by di ec ly co-doping he YVO
4
ma ix wi h equal
concen a ions o bo h Eu
3+
and Dy
3+
ions. The nanophospho s o YVO
4
:
x(Eu
3+
, Dy
3+
) (whe e x=1 a %, 2 a %, 3 a %, and 5 a %, he same x
a omic concen a ion o bo h) we e syn hesized using a co-
p ecipi a ion echnique. Subsequen ly, a comp ehensi e analysis o
hei s uc u al, composi ional, and op ical cha ac e is ics was me icu-
lously conduc ed.
2. Expe imen al
2.1. Ma e ials
The aw ma e ials employed in he cu en s udy we e sou ced om
Sigma-Ald ich (S . Louis, MO, USA), including sodium o ho anada e
(Na
3
VO
4
) wi h a pu i y o 99.98 % ( ace me als basis), y ium ni a e
hexahyd a e (Y(NO
3
)
3
•6 H
2
O) wi h a pu i y o 99.9 %, eu opium (III)
ni a e pen ahyd a e (Eu (NO
3
)
3
•5 H
2
O) wi h a pu i y o 99.9 %, and
dysp osium (III) ni a e hyd a e (Dy (NO
3
)
3
•xH
2
O) wi h a pu i y o
99.9 % in he desi ed p opo ions.
2.2. Syn hesis o YVO
4
:x(Eu
3+
, Dy
3+
) (x =1–5 a %) nanopa icles
The nanophospho s we e p epa ed h ough co-p ecipi a ion ech-
nique [19]. One mmol o Na
3
VO
4
was i s dissol ed in 3.5 mL o
dis illed wa e , and hen, Y(NO
3
)
3
•6 H
2
O (1 mmol) was dissol ed in
0.5 mL o dis illed wa e . Fo each sample, he desi ed amoun s o Eu
(NO
3
)
3
•5 H
2
O and Dy(NO
3
)
3
•xH
2
O we e subsequen ly dissol ed in
sepa a e aliquo s o 0.5 mL o dis illed wa e . Di e en samples we e
p epa ed wi h Eu and Dy dopan concen a ions o 1, 2, 3, and 5 a .
pe cen (a %). The solu ion was s i ed using a magne ic s i e o
10 minu es a oom empe a u e. The esul ing p ecipi a e was hen
cen i uged, washed wi h dis illed wa e , and d ied a 50 ◦C. Subse-
quen ly, he inal p oduc was subjec ed o hea ing in an elec ic mu le
u nace a 800◦C o a du a ion o 2 h. The yield o he p oduc con-
aining bo h Eu and Dy is 65 %.
2.3. Cha ac e iza ion
X- ay di ac ion (XRD) pa e ns we e collec ed using a B uke D8
Disco e di ac ome e wi h CuK
α
adia ion (λ =1.5406 Å). The in-
s umen ope a ed in he θ/2θ scan mode o e a ange o 10◦-70◦wi h a
s ep size o 0.04◦and an in eg a ion ime o 1 second. Ene gy-dispe si e
X- ay spec oscopy (EDS) using an EDAX Pegasus X4M analyze , wi h an
accele a ion ol age o 15 keV, de e mined he chemical composi ion o
he pa icles. Pa icle size and mo phology we e in es iga ed using an
FEI NOVA NanoSEM 200 scanning elec on mic oscope (SEM). ImageJ
so wa e was employed o analyze he pa icle size dis ibu ions. We
manually selec ed 100 pa icles om each SEM image, excluding holes,
o size measu emen . ImageJ can cha ac e ize bo h sphe ical and non-
sphe ical pa icles using a ious pa ame e s, including longes and
sho es diame e s, pe ime e , p ojec ed a ea, o equi alen sphe ical
diame e .
The e lec ance o he compound was measu ed using a Shimadzu
UV-3600i Plus UV-Vis-NIR spec opho ome e o e a wa eleng h ange
o 250–850 nm wi h a s ep o 1 nm. The o al e lec ance was ob ained
wi h an incidence angle o 8◦using a 150 mm diame e in eg a ing
sphe e (model ISR-1503, Shimadzu).
A homemade po able se up equipped wi h a 310 nm ligh -emi ing-
diode (LED) exci a ion sou ce and a CCS200 spec ome e om Tho labs
was used o measu e he pho oluminescence o Eu
3+
and Dy
3+
co-doped
YVO
4
nanopa icles. All cha ac e iza ions we e pe o med a oom
empe a u e.
3. Resul s and discussion
3.1. XRD pa e ns, Phase s uc u e and Rie eld e inemen
Fig. 1.a displays X- ay di ac ion (XRD) pa e ns o YVO
4
phospho-
ous wi h a ying a omic pe cen ages o Eu
3+
and Dy
3+
ions, syn he-
sized using he co-p ecipi a ion me hod and subsequen ly he mally
annealed a 800 ◦C. All di ac ion peaks obse ed in he pa e ns can be
assigned o he e e ence YVO
4
phase ( e agonal, space g oup I41/amd,
JCPDS 00–016–0250). B oad and in ense peaks in he X- ay di ac ion
pa e n indica e ha he nanophospho s syn hesized a e well-
c ys allized and ha e dimensions on he nanoscale [20]. No e idence
o addi ional c ys alline phases was ound.
The Rie eld e inemen analysis o YVO
4
:3 % (Eu
3+
, Dy
3+
), chosen
as he subjec o analysis, was pe o med using he FULLPROF sui e
p og am. The Pseudo-Voig unc ion was u ilized o i mul iple pa-
ame e s o he da a poin s [21]. Fig. 1.b illus a es he Rie eld
e inemen o he XRD pa e n o selec ed nanophospho samples wi h
x=3 mol%. The e agonal s uc u e o YVO
4
was ini ially used as a
e e ence o e ine he da a owa ds he ac ual c ys al s uc u e. In he
e inemen plo , he solid line ep esen s he calcula ed XRD pa e n,
while do s depic he obse ed XRD pa e ns. Ve ical g een ba s indi-
ca e he B agg posi ions o he e agonal phase, and he lowe p o ile
shows he disc epancy be ween obse ed and calcula ed XRD pa e ns.
The quali y o he e ined da a was assessed by lowe alues o goodness
o i (GOF) =
χ
2
; o op imal e inemen esul s, GOF should app oach
uni y. Table 1 summa izes he calcula ed la ice pa ame e s (a, b, c), as
well as he uni cell olume (V). In he same able, we ha e also compiled
he eliabili y ac o (R
F
), he B agg R- ac o , and he GOF. Based on he
calcula ed alues, i is e iden ha he e ined pa ame e s show mino
de ia ions om he s anda d da a o YVO
4
. This obse a ion indica es
he e ec i e and consis en in eg a ion o Eu opium and Dysp osium
ions in o he YVO
4
hos ma ix. This in eg a ion is made possible by he
simila ionic adius and chemical eac i i y sha ed among Eu
3+
, Dy
3+
,
H.E. Sek a i e al.
Jou nal o Alloys and Compounds 1010 (2025) 177389
2
and Y
3+
ions [22,23]. Mo eo e , his subs i u ion can po en ially impac
he pho oluminescen p ope ies o he ma e ial, pa icula ly he emis-
sion spec um.
The c ys alli e size o he nanophospho was de e mined by u ilizing
he mos p ominen di ac ion peak (200) and applying Debye-Sche -
e ’s o mula as p esen ed in Equa ion [24,25]:
DSC =Kλ
βcosθ(1)
D
SC
ep esen s he c ys alli e size, whe e K is a cons an (K ≈0.89), λ
deno es he wa eleng h o he x- ays used (0.15406 nm), θ co esponds
o he angle o di ac ion, and β ep esen s he ull wid h a hal
maximum (FWHM in adian). The calcula ed alues o c ys alli e size
e ealed a ange o 20–36 nm, as lis ed in he Table 1. The FWHM o
XRD di ac ion peaks e lec s bo h la ice s ain and c ys alli e size [26].
The Williamson-Hall equa ion quan i ies his ela ionship, as shown
below [25,27]:
βcosθ=4
ε
sinθ+Kλ
DW−H
(2)
By u ilizing a linea eg ession model o analyze he cu e, ocusing
on he ela ionship be ween 4sin (θ) (x-axis) and βcos (θ) (y-axis) as
shown in Fig. 2, we success ully calcula ed he s ain
ε
by iden i ying he
slope o his g aph. Simul aneously, he c ys alli e size D
W-H
was
de e mined by loca ing he poin whe e he cu e in e sec s he e ical
axis a sin (θ) =0. The ob ained alues a e de ailed in Table 2. The
c ys alli e size es ima es ob ained om he Sche e ’s and Williamson-
Hall (W-H) plo s exhibi minimal a ia ion. This is because he s ain
componen in Sche e ’s equa ion is ypically assumed o be negligible.
Howe e , he W-H plo e eals ha he 2 % and 5 % co-doped samples
o Eu
3+
and Dy
3+
ions exhibi ela i ely lowe s ain alues and highe
c ys alli e sizes, which is ce ainly co ela ed. In his con ex , i is sug-
ges ed ha ele a ed s ain le els could po en ially esul in a educ ion
o luo escence in ensi y [28]. The Table 2 also includes disloca ion
densi y (δ), calcula ed as δ =1/D
2
(D =c ys alli e size om
Fig. 1. (a) X- ay di ac ion pa e n o YVO
4
:x(Eu
3+
, Dy
3+
) wi h x=1, 2, 3 and
5 mol% (b) Rie eld e inemen was pe o med on he XRD pa e n o he
selec ed compound a a concen a ion o 3 mol%.
Table 1
Re inemen esul s and c ys al s uc u e da a o he YVO
4
:x(Eu
3+
, Dy
3+
) se ies
(x =1 %, 2 %, 3 %, and 5 %) we e compa ed o he e e ence s anda d o YVO
4
(space g oup I41/amd, JCPDS 1–0250).
Pa ame e s YVO
4
PDF#16–0250
YVO
4
:x(Eu
3þ
, Dy
3þ
)
0 % 1 % 2 % 3 % 5 %
a ¼b (Å) 7.1230 7.116
(3)
7.1164
(12)
7.114
(3)
7.1230
(17)
c (Å) 6.2910 6.290
(3)
6.2888
(10)
6.289
(2)
6.2919
(14)
c/b 0.8832 0.8839 0.8837 0.8840 0.8833
V (Å
3
)319.19 318.51 318.48 318.31 319.24
Space
g oup
I41/amd (141)
Y/Eu/Dy
X
Y
Z
- 0.0000
0.7500
0.1250
0.0000
0.7500
0.1250
0.0000
0.7500
0.1250
0.0000
0.7500
0.1250
V
X
Y
Z
- 0.0000
0.2500
0.3750
0.0000
0.2500
0.3750
0.0000
0.2500
0.3750
0.0000
0.2500
0.3750
O
X
Y
Z
- 0.0000
0.4360
0.2038
0.0000
0.4376
0.2045
0.0000
0.4350
0.1990
0.0000
0.4370
0.2030
R
B agg
- 7.88 7.02 8.39 9.03
R
F
- 5.83 7.35 7.28 8.18
GoF - 1.28 1.62 1.31 1.41
Fig. 2. W-H plo o YVO
4
:x(Eu
3+
, Dy
3+
) nanophospho s om x=1, 2, 3 and
5 mol%.
H.E. Sek a i e al.
Jou nal o Alloys and Compounds 1010 (2025) 177389
3
Debye-Sche e ) [29]. The da a e eals an in e se ela ionship be ween
c ys alli e size, disloca ion densi y, and s ain alue. This is due o he
su ace a ea e ec : smalle c ys alli es ha e a highe su ace a ea o
olume a io, leading o inc eased s ain and disloca ion densi y in
nanoma e ials [30].
3.2. Mo phological analysis
The su ace mo phology o a luminescen ma e ial is a c i ical ac o
ha signi ican ly in luences i s op ical p ope ies [31]. Su ace ea u es,
i egula i ies, and nanos uc u es can al e ligh abso p ion, emission
e iciency, and o e all op ical pe o mance. Con olling and unde -
s anding he su ace mo phology is essen ial o op imizing he op ical
cha ac e is ics and pe o mance o luminescen ma e ials ac oss a ious
applica ions. Fig. 3.a displays he SEM mic og aphs o as-syn he ized
YVO
4
:x (Eu
3+
, Dy
3+
) ( o x=1 %, 2 %, 3 %, and 5 %) nanopa icles.
The SEM esul s e eal a po ous and agglome a ed mo phology, con-
sis ing o polyc ys alline nanopa icles. The po ous s uc u e p o ides a
high su ace a ea- o- olume a io, which can be bene icial o a ious
applica ions, such as ca alysis, adso p ion, o ene gy s o age. The
agglome a ion o he nanopa icles is a common phenomenon due o he
high su ace ene gy o he nanoscale ma e ials, leading o he o ma ion
o la ge , polyc ys alline s uc u es. By compa ing he SEM images, i
was ound ha he ma e ial co-doped wi h 2 % Eu
3+
and Dy
3+
exhibi s
uni o m and well-dispe sed quasi-sphe ical nanopa icles. Con e sely,
he sample co-doped wi h 5 % dopan s displays signi ican ly la ge g ain
sizes, sugges ing hei o ma ion du ing p ecipi a ion h ough he usion
o smalle p ecu so pa icles. This obse a ion aligns wi h p e ious
s udies, indica ing ha dopan concen a ion in luences he deg ee o
pa icle agg ega ion and size [19]. The a e age pa icle sizes obse ed in
he SEM images (Fig. 3.b) ange om 35 o 65 nm. This is la ge han he
co esponding c ys alli e sizes ob ained om he XRD esul s, which
con i ms he agglome a ion o he nanophospho pa icles. The EDS
analysis was employed o assess he chemical pu i y and elemen al
composi ion o he YVO
4
:x(Eu
3+
, Dy
3+
) ma e ials (Fig. 4). The EDX
spec a con i med he p esence o Y, V, Eu, Dy, and O h ough he
obse a ion o hei cha ac e is ic peaks. The absence o any addi ional
peaks sugges s ha he p epa ed samples a e ee om signi ican
elemen al impu i ies.
3.3. UV-Visible e lec ance spec oscopy
UV–Visible o al e lec ance spec a o YVO
4
:x (Eu
3+
, Dy
3+
) doped
wi h di e en concen a ions o Eu
3+
and Dy
3+
(1, 2, 3, 5 mol%) has
been depic ed in Fig. 5. These measu emen s we e ca ied ou a
ambien empe a u e o e a wa eleng h ange spanning om 250 nm o
850 nm. The uni o m doping a ia ion in e lec ance occu s be ween
1 % and 5 % o he Eu
3+
and Dy
3+
dopan s. The inse o Fig. 5 high-
ligh s he p esence o a sha p abso p ion band a app oxima ely 305 nm,
a ibu ed o he pho oexci a ion o elec ons om he alence band o
O
2-
(2p elec ons) o he conduc ion band o Y
3+
(4d le el) wi hin he
hos la ice [32]. This phenomenon can be u he elucida ed as ollows:
he g anula shape mo phology has e ealed he p esence o oids in
Eu
3+
and Dy
3+
doped YVO
4
samples. Addi ionally, su ace de ec s such
as F enkel de ec s exis ing in he la ice s uc u e con ibu e o abso p-
ion a a ious wa eleng hs [33]. The e a e also small peaks a 756 nm
and 810 nm due o he - ansi ion o Dy
3+
and Eu
3+
ions [34].
I is no ewo hy ha while indi ec ansi ions may occu concu -
en ly wi h di ec ansi ions, hey o en go unde ec ed in he abso p ion
spec um due o hei high ene gy and low p obabili y. The mos sig-
ni ican ansi ion go e ns he semiconduc o ’s beha io ; ne e heless,
es ablishing he co esponding ansi ion expe imen ally poses consid-
e able challenges. The band gap ene gy o he co-doped YVO
4
:Eu
3+
,
Dy
3+
nanophospho s was de e mined by analyzing he e lec ance
spec a using he Kubelka-Munk (K-M o F(R)) me hod. The K-M unc-
ion is exp essed as ollows [35]:
F(R) = (1−R)2
2R(3)
In his con ex , R ep esen s he e lec ance o an in ini ely hick
sample, while he unc ion F(R) is di ec ly p opo ional o he ex inc ion
coe icien (
α
). The ela ion gi en by [36] allows us o isualize he
spec a based on he calcula ed e lec ance alues:
[F(R).h ]n=A(h −Eg)(4)
In abo e equa ion, h
υ
deno es he ene gy o he inciden pho on, E
g
s ands o he ene gy o he op ical bandgap, and A deno es a cons an
e e ed o as he band ailo ing pa ame e . The alue o ’n’ a ies
depending on he ype o ansi ion: 2 o di ec allowed ansi ions, 3
o di ec o bidden ansi ions, 1/2 o indi ec allowed ansi ions, and
3/2 o indi ec o bidden ansi ions.
The di ec band gap ene gy (E
gd
) o co-doped YVO
4
: Eu
3+
, Dy
3+
(1, 2,
3, and 5 %) was calcula ed by plo ing he squa e o he K–M unc ion [F
(R).h
ν
]
2
e sus he ene gy in elec on ol s and shown in Fig. 6.a. The
linea pa o he cu e was ex ended o F(R)
2
=0 in o de o de e mine
he di ec band gap ene gy. As shown, he band gap ene gy exhibi s a
sligh inc ease wi h he concu en co-doping o Eu and Dy, esul ing in
E
gd
alues o 3.6 eV, 3.65 eV, 3.69 eV, and 3.72 eV o doping le els o
1 %, 2 %, 3 %, and 5 %, espec i ely. The de e mined op ical bandgap
alue indica es ha he analyzed compound quali ies as a semi-
conduc o ma e ial, gi en ha E
g
is lowe s ic ly han 4 eV [37].
The obse ed ise in he op ical band gap esul ing om doping could
be associa ed wi h changes in he local a omic s uc u e o la ice
con igu a ion [38]. Ano he in e p e a ion is associa ed wi h he
Bu s ein-Moss e ec (BM) [39], which cla i ies he ela ionship be ween
he band gap (E
g
) and doping concen a ion. In hea ily doped semi-
conduc o s, he Fe mi le el can shi in o he conduc ion band (CB) due
o he abundance o ee cha ge ca ie s. This ansi ion esul s in a
no able change in he semiconduc o ’s op ical p ope ies, leading o an
appa en widening o he band gap [40].
To alida e he bandgap alue and i s na u e, Fig. 6.b shows he i s
de i a i e o e lec ance (dR/dλ) o ou compounds. This de i a i e
e eals peaks a app oxima ely 3.67 eV, 3.65 eV, 3.72 eV, and 3.76 eV,
co esponding o each doping le el, espec i ely. These peaks con i m a
di ec bandgap, consis en wi h Ma o i e al. [41].
3.4. Pho oluminescence
Ra e ea h phospho s can be b oadly ca ego ized in o wo ypes
based on hei emission cha ac e is ics: b oad-band emission phospho s
and na ow-band emission phospho s. B oad-band emission phospho s,
such as hose doped wi h Eu
2+
o Ce
3+
, demons a e emission due o 5d-
4 elec onic ansi ions [42]. In con as , na ow-band emission phos-
pho s, such as hose doped wi h Eu
3+
, Gd
3+
, Sm
3+
, Dy
3+
, Nd
3+
, Tm
3+
o
E
3+
exhibi emission a ising om 4 -4 elec onic ansi ions [43].
Conside ing he 310 nm exci a ion wa eleng h used in p e ious
wo k wi h YVO
4
:Eu
3+
2 a % [19] and indings epo ed in he li e a u e
o YVO
4
:Dy
3+
2 a % [44] phospho s, we adop ed he same exci a ion
Table 2
The a e age c ys alli e size and la ice s ain in he syn hesized samples we e
es ima ed using Debye-Sche e ’s o mula and he Williamson-Hall equa ion.
Phospho YVO
4
:x
(Eu
3+
, Dy
3+
) (a .
mole%)
C ys alli e
size D (nm)
S ain
ε
(×10
−3
)
Disloca ion densi y (nm
−2
)
om Sche e o mula δ
(×10
−4
)
D
SC
D
W-
H
1 20 25 1.12±0.02 25
2 35 43 0.59±0.01 8
3 25 30 1.35±0.02 16
5 34 44 0.65±0.03 8
H.E. Sek a i e al.
Jou nal o Alloys and Compounds 1010 (2025) 177389
4
wa eleng h o ou cu en in es iga ion. Fig. 7 displays he emission
spec a o he YVO
4
:Ln
3+
(Ln=Eu and/o Dy) nanoc ys als, each doped
wi h 2 a % Ln, unde UV exci a ion. Fo Dy
3+
ions, he emission peaks
a e cen e ed a 486 nm (
4
F
9/2
→
6
H
15/2
) and 577 nm (
4
F
9/2
→
6
H
13/2
),
which can p oduce a yellow-g een ligh om he YVO
4
:Dy
3+
phospho s
[45,46]. The in ensi y o he yellow emission is s onge han he g een
emission due o he D
2d
poin symme y o Dy
3+
ions wi hou an
in e sion cen e in he YVO
4
hos . The
4
F
9/2
→
6
H
13/2
ansi ion is a hy-
pe sensi i e o ced elec ic dipole ansi ion [47]. I s in ensi y can a y
signi ican ly by o de s o magni ude depending on he local si e sym-
me y o he emi ing ion. In con as , he in ensi y o he
4
F
9/2
→
6
H
15/2
ansi ion is ela i ely insensi i e o he su ounding en i onmen [48].
The emission spec um o YVO
4
:Eu
3+
a ises om he
5
D
1
→
7
F
1
,
5
D
1
→
7
F
2
and
5
D
0
→
7
F
J
(J =1, 2, 3, 4) ansi ions o Eu
3+
a 597 nm,
619 nm, 622 nm, 652 nm and 702 nm, which is cha ac e is ic o ed
phospho s [19,49]. The p esence o a ed peak a 619 nm and 622 nm
signi ies he
5
D
0
→
7
F
2
ansi ion o eu opium ions wi hin he YVO
4
la -
ice. This ansi ion is hype sensi i e, u he con i ming he eu opium
ions occupy si es lacking in e sion symme y [50].
PL spec a (Fig. 7) e eal ha YVO
4
:2 %Dy
3+
and YVO
4
:2 %Eu
3+
phospho s emi yellow and ed ligh , espec i ely. No ably, bo h possess
in insic exci a ion peaks in he UV– isible egion. The e o e,
Fig. 3. (a) SEM images (b) pa icle dis ibu ions his og am o YVO
4
:x(Eu
3+
, Dy
3+
) (wi h x=1 %, 2 %, 3 % and 5 %).
H.E. Sek a i e al.
Jou nal o Alloys and Compounds 1010 (2025) 177389
5
inco po a ing Dy
3+
and Eu
3+
ions simul aneously in o he YVO
4
hos
la ice is expec ed o achie e unable colo in a single-phase phospho by
adjus ing he ac i a o concen a ion. Rema kably, he in ensi y o
YVO
4
:(Eu
3+
, Dy
3+
) 2 a % is highe han ha o bo h Eu-YVO
4
and Dy-
YVO
4
. This obse a ion sugges s ha he p esence o an ene gy ans e
mechanism be ween Eu
3+
and Dy
3+
wi hin he YVO
4
hos ma e ial, as
al eady epo ed [51,52].
To in es iga e he e ec o co-doping concen a ion on pho o-
luminescence and de e mine he maximum allowable co-doping con-
cen a ion, a se ies o samples we e p epa ed wi h a ying co-doping
amoun s o Eu
3+
and Dy
3+
(1 %, 2 %, 3 %, and 5 %), as shown in Fig. 8.
The PL spec a consis o peaks a 486, 577, 597, 612, 619, 622, 655,
702, and 707 nm. The e a e no shi s in he peak posi ions o Eu
3+
and
Dy
3+
; howe e , he in ensi y o he dopan ions inc eases wi h a ying
co-dopan concen a ions. Inse o Fig. 8 e eals a signi ican enhance-
men in he emission in ensi y o YVO
4
:(Eu
3+
, Dy
3+
) 2 a % nano-
phospho compa ed o o he co-doping concen a ions. This inc ease in
luminescence in ensi y migh be a ibu ed o a dec ease in he s ain
wi hin he c ys al la ice, when compa ed wi h sample wi h 1 a %. In
con as , he in ensi y signi ican ly dec eased when he doping con-
cen a ion exceeded 3 mol%. This dec ease in in ensi y, obse ed wi h
inc easing concen a ions o Eu
3+
and Dy
3+
, can be a ibu ed o a well-
known phenomenon in phospho s called concen a ion quenching [53,
54].
The concen a ion quenching ends o dec ease he in ensi y. This is
due o he c oss- elaxa ion mechanisms o Eu
+3
and Dy
+3
, which exhibi
s ong quenching beha io [55]. Ene gy ans e om sensi ize (Dy
3+
)
o ac i a o (Eu
3+
) ions in he YVO
4
ma ix is a mul is age in e ac ion
ha ypically occu s ia wo p ima y mechanisms: exchange in e ac ion
and mul ipola in e ac ion [56,57].
The exchange in e ac ions domina e when he c i ical dis ance (R
c
)is
less han 5 Å, while o he in e ac ions a e p ominen when R
c
exceeds
5 Å. Acco ding o Blasse’s o mula [58], he c i ical dis ance is oughly
equi alen o wice he adius o a sphe e ha has he same olume:
RC≈2(3V
4
π
XcN)1/3
(5)
In Equa ion (5), V, X
C
and N deno e he uni cell olume, he c i ical
concen a ion, and he numbe o la ice si es ha can occupied by he
ac i a o ions, espec i ely. Fo YVO
4
: Eu
3+
, Dy
3+
(1, 2, 3, and 5 %)
phospho s, he alues o hese a iables a e known and equal o V =
319.19 Å
3
, N =4, and X
C
=0.04. No ably, X
C
ep esen s he o al con-
cen a ion o dopan s equi ed o achie e maximum ene gy ans e
e iciency. Based on he a o emen ioned pa ame e s, R
c
was de e mined
o be 15.63 Å, exceeding he e ec i e dis ance o 5 Å o ene gy ex-
change in e ac ions. Consequen ly, in his pho oluminescen sys em,
ene gy ans e occu s h ough he mul ipola in e ac ion mechanism,
which is also he p ima y cause o concen a ion quenching. Acco ding
o Dex e ’s ene gy esonance heo y, he in e ac ion ype, deno ed by
he symbol (θ), can be exp essed by he ollowing o mula [59]:
I
x=k(1+β(x)θ/3)−1(6)
Fig. 4. The analysis o chemical elemen s in YVO
4
nanopa icles co-doped wi h Eu
3+
and Dy
3+
we e analyzed using EDS (wi h x=2 % selec ed).
Fig. 5. Expe imen al UV– isible e lec ance spec um o YVO
4
:x(Eu
3+
, Dy
3+
)
(wi h x=1 %, 2 %, 3 % and 5 %). The inse p esen he abso p ion spec um.
H.E. Sek a i e al.
Jou nal o Alloys and Compounds 1010 (2025) 177389
6
The Eq. (6) desc ibes he ela ionship be ween in eg al in ensi y (I),
ac i a o concen a ion (x), and a cons an e m (k). The pa ame e β is
ano he cons an speci ic o he exci a ion condi ions o he hos c ys al.
Acco ding o his equa ion, he alue o θ e lec s he ype o ene gy
ans e occu ing. A alue o θ =3 indica es ene gy ans e be ween
nea es neighbo ions. Con e sely, alues o θ =6, 8, and 10 co espond
o dipole-dipole (d-d), dipole-quad upole (d-q), and quad upole-
quad upole (q-q) in e ac ions, espec i ely [60].
The mul ipola cha ac e (θ) can be de e mined by plo ing a g aph
o Log (I/x) e sus Log (x), as shown in Fig. 9. The slope o he line, θ/3,
was app oxima ed o be −2.23 o ou samples, which leads o a
calcula ed alue o θ ha is app oxima ely 6. The e o e, he concen-
a ion quenching obse ed in he Eu and Dy co-doped YVO
4
nano-
phospho can be a ibu ed o d-d in e ac ions.
3.5. CIE ch oma ici y
The Ch oma ici y Coo dina es (CIE, Commission In e na ional de
l’Eclai age [61]) o YVO
4
:x(Eu
3+
, Dy
3+
) phospho s we e de e mined
om he emission spec a a di e en x alues, which a e depic ed in
Fig. 10. The emi ed ligh exhibi s a wide colo gamu , ansi ioning
smoo hly om yellow o o ange and ul ima ely o ed. This unabili y
sugges s ha he composi ion o YVO
4
:x(Eu
3+
, Dy
3+
) can be p ecisely
con olled by adjus ing he x alue, allowing o he a ge ed manipu-
la ion o he luminescen ma e ial’s ou pu colo .
The quali y o a ligh sou ce can be o en cha ac e ized by i s
co ela ed colo empe a u e (CCT). This me ic can also be de e mined
o YVO
4
:x(Eu
3+
, Dy
3+
) phospho s using McCamy’s well-es ablished
empi ical o mula [62], as shown below:
CCT = − 449n3+3525n2−6823n+5520.33 (7)
Fig. 6. Kubelka–Munk plo s o o YVO
4
:x(Eu
3+
, Dy
3+
) (wi h x=1 %, 2 %, 3 % and 5 %): (a) dependence o F(R)
2
and (b) dependence o F(R)
1/2
wi h gap ene gy. (c)
Po ays he e olu ion o dR/dλ wi h wa eleng h.
H.E. Sek a i e al.
Jou nal o Alloys and Compounds 1010 (2025) 177389
7
He e, n= (x−xe)/(x−ye) ep esen s he in e se slope o he line,
wi h x
e
=0.332 and y
e
=0.186 deno ing he coo dina es o he
epicen e . Table 3 p esen s he calcula ed CCT alues o YVO
4
:x(Eu
3+
,
Dy
3+
) phospho s. Unde 310 nm exci a ion, YVO
4
: (Eu
3+
, Dy
3+
) nano-
phospho s co-doped wi h 2 % o al a e ea h ca ions display he
s onges emission in he wa me o ange- ed spec al egion, e iden
om hei 1735 K (CCT).
YVO
4
: (Eu
3+
,
Dy
3+
) nanophospho s doped wi h 2 % o al a e ea h
ca ions exhibi he mos in ense emission in he wa me o ange- ed e-
gion o he spec um, as e idenced by hei (CCT) o 1735 K unde
310 nm exci a ion.
4. Summa y
In his s udy, a se ies o YVO
4
:Eu
3+
, Dy
3+
samples we e success ully
syn hesized using he co-p ecipi a ion me hod and hen unde wen
he mal annealing a 800◦C. XRD analysis con i med he success ul
inco po a ion o Eu
3+
and Dy
3+
ions in o he YVO
4
la ice wi hou
al e ing i s e agonal c ys al s uc u e. SEM e ealed ha he YVO
4
:
Eu
3+
, Dy
3+
phospho s possess a well-de ined, sphe ically-de o med
mo phology wi h an a e age pa icle size o app oxima ely 60 nm. This
pa icle size ange sugges s p omising po en ial o p ac ical applica-
ions. EDX con i med he p esence o signals om y ium, anadium,
oxygen, eu opium, and dysp osium, indica ing also he success ul
doping o hese ions in o he YVO
4
la ice. UV– is di use e lec ance
spec a e eal abso p ion peaks co esponding o an op ical di ec band
gap in he ange o 3.6–3.75 eV. In he YVO
4
:x(Eu
3+
, Dy
3+
) phospho s,
he op imal concen a ion o Eu
3+
and Dy
3+
ions o achie ing he
maximum up-con e sion emission in ensi y unde 310 nm exci a ion is
2 mol%. This concen a ion a io esul s in he mos e icien ene gy
ans e and highes luminescence in ensi y. In YVO
4
:x(Eu
3+
, Dy
3+
)
phospho s, he ene gy ans e c i ical dis ance be ween Dy
3+
and Eu
3+
ions was calcula ed o be 15.63 Å. Concen a ion quenching in his
sys em is a ibu ed o dipole-dipole in e ac ions, which domina e he
ene gy ans e mechanism. Based on hese indings, he YVO
4
:(Eu
3+
,
Dy
3+
) 2 %a . nanophospho exhibi s signi ican po en ial o use in
solid-s a e ligh ing echnology, pa icula ly as a p omising WLED
candida e.
Fig. 7. Pho oluminescence emission spec a o YVO
4
ma ices doped wi h 2 %
Eu
3+
and Dy
3+
, as well as ma ices co-doped wi h he same concen a ion o
bo h a e-ea h ions.
Fig. 8. Pho oluminescence emission spec a o YVO
4
:x(Eu
3+
, Dy
3+
) wi h x=1,
2, 3 and 5 mol% and inse show he enla ged iew o highes emission in ensi y
wi h a se ies o concen a ions.
Fig. 9. Dual loga i hmic g aph illus a ing he ela ionship be ween he pho-
oluminescence (PL) emission in ensi y pe co-dopan (Log(I/x)) and he con-
cen a ion o Eu
3+
and Dy
3+
ions (Log(x)) in YVO
4
:x(Eu
3+
, Dy
3+
) (wi h
x=1 mol%, 2 mol%, 3 mol%, and 5 mol%) nanophospho s.
Fig. 10. CIE 1931 diag am o Eu
3+
and Dy
3+
co-doped YVO
4
phospho s
(YVO
4
:x(Eu
3+
, Dy
3+
) whe e x=1 %, 2 %, 3 %, and 5 %).
Table 3
Colo ch oma ici y coo dina es (x, y) and co ela ed colo empe a u e (CCT, K)
o he YVO
4
:x(Eu
3+
, Dy
3+
) phospho s.
Compound code Ch oma ici y coo dina es CCT(K)
x y
YVO
4
:(Eu
3+
, Dy
3+
) 1 %a . 0.569 0.371 1620
YVO
4
:(Eu
3+
, Dy
3+
) 2 %a . 0.608 0.365 1735
YVO
4
:(Eu
3+
, Dy
3+
) 3 %a . 0.546 0.367 1639
YVO
4
:(Eu
3+
, Dy
3+
) 5 %a . 0.594 0.362 1694
H.E. Sek a i e al.
Jou nal o Alloys and Compounds 1010 (2025) 177389
8
CRediT au ho ship con ibu ion s a emen
Houssem Eddine Sek a i: W i ing – o iginal d a , So wa e,
Me hodology, In es iga ion, Fo mal analysis, Da a cu a ion. Eya He gli:
In es iga ion. S anisla Fe do : W i ing – e iew & edi ing, Visuali-
za ion, Valida ion, Da a cu a ion. Paulo J. G. Cou inho: W i ing – e-
iew & edi ing, Da a cu a ion. Luis Rebou a: W i ing – e iew &
edi ing, Supe ision, Resou ces.
Decla a ion o Compe ing In e es
All au ho s con i m ha he e a e no known con lic s o in e es
associa ed wi h his publica ion and ha he e has been no signi ican
suppo o his wo k ha could ha e in luenced he p esen ed esul s.
Acknowledgemen s
“This wo k was suppo ed by he Eu opean S uc u al and In es -
men Funds in he FEDER Componen h ough he Ope a ional
Compe i i eness and In e na ionaliza ion P og amme (COMPETE 2020)
unde Ad anced Decision Making in p oduc i e sys ems h ough In el-
ligen Ne wo ks (ADM.IN) P ojec 055087 (POCI-01–0247-FEDER-
055087), and pa ially suppo ed by he Po uguese Founda ion o
Science and Technology (FCT) in he amewo k o he S a egic Funding
UIDB/04650/2020.”
Da a a ailabili y
Da a will be made a ailable on eques .
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