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solid BaTiO3:Dy3+ microspheres and their applications in effective detection of latent fingerprints and lip prints

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LFPs were visualized using an optimized powder undoubtedly with high contrast, selectivity and low background interference on various porous and non-porous surfaces.. The photometric stu[r]

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M Dhanalakshmia,b, H Nagabhushanac,*, G.P Darshand, R.B Basavarajc,

a Department of Physics, Govt Science College, Bengaluru 560 001, India

b Research and Development Center, Bharathiar University, Coimbatore 641046, India

c Prof C.N.R Rao Centre for Advanced Materials, Tumkur University, Tumakuru 572103, India

d Department of Physics, Acharya Institute of Graduate Studies, Bangalore 560 107, India

e Department of Physics, BMS Institute of Technology and Management, VTU, Belagavi-affiliated, Bangalore 560 064, India

a r t i c l e i n f o

Article history:

Received 19 December 2016

Received in revised form

31 January 2017

Accepted 9 February 2017

Available online 16 February 2017

Keywords:

Sonochemical synthesis

Latent fingerprint

Cheiloscopy

JuddeOfelt analysis

a b s t r a c t

Nanostructured materialsfind potential benefits for surface-based science such as latent fingerprints (LFPs) and lip print detection on porous and non-porous surfaces To encounter the drawbacks viz low sensitivity, high background hindrance, complicated procedure and high toxicity associated with traditional fluo-rescent powders were resolved by using hollow/solid BaTiO3:Dy3þ(1e5 mol %) microspheres The visu-alization of LFPs stained by the optimized BaTiO3:Dy3þ(2 mol %) hollow/solid microspheres exhibits

well-defined ridge patterns with high sensitivity, low background hindrance, high efficiency and low toxicity on various surfaces The powder X-ray diffraction results revealed the body centered cubic phase of the pre-pared samples The emission spectra exhibit intensive peaks at ~480, 575, and 637 nm, which were attributed to transitions4F9/2/6HJ(J¼ 15/2, 13/2, 11/2) of Dy3þions, respectively Surface morphologies were extensively studied with different sonication times and concentrations of the used barbituric acid The Commission International De I-Eclairage (CIE) and Correlated Color Temperature (CCT) analyses revealed that the present phosphor is highly useful for the fabrication of white light emitting diodes

© 2017 The Authors Publishing services by Elsevier B.V on behalf of Vietnam National University, Hanoi This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/)

1 Introduction

In a crime spot investigation, LFPs are the most important

physical evidence for identification of criminals [1,2] When a

criminal touches any surface in a spot, skin sweat transferred to the

surface through pores leading to an invisible ridge pattern is well

known as latentfingerprints In a forensic analysis, LFPs are the most

influential method due to its unique and immutable features[3,4]

Because of invisibility of LFPs, enhancement of LFPs was required for

identification and visualization Nowadays, several methods have

been used to make LFPs visible Among them, the powder dusting

method allows for LFPs to be visualized within a short period of time

and without any complicated requirements The conventional

dusting powders were mainly classified into regular, metallic and

luminescent materials Regular and metallic powders constituent of resinous polymers and meshed metals which are hazard to in-vestigators' health[5] These conventional powders are not capable

of enhancing LFPs on some complicated surfaces Luminescent nanopowders are potential solutions to overtake such limitations, making LFPs visible Luminescent nanopowders were explored as labeling agents for visualization of LFPs and exhibit good contrast, sensitivity and adhesion efficiency These factors provide new possible applications of nano powders in surface science

In addition, lip prints are form of wrinkles and grooves including normal lines,fissures and are present in the zone of transition of human lip between the inner labial mucosa and outer skin[6] Lip prints are also a main evidence for identification of an individual in

a forensic dentistry due to its uniqueness, except in monozygotic twins The revelation of lip prints was well known as cheiloscopy

[7] The cheiloscopy plays a major role in forensic science for person identification in crime investigations, ethnic studies, mass di-sasters,fire victims, and vehicle accidents

* Corresponding author.

E-mail address: bhushanvlc@gmail.com (H Nagabhushana).

Peer review under responsibility of Vietnam National University, Hanoi.

http://dx.doi.org/10.1016/j.jsamd.2017.02.004

2468-2179/© 2017 The Authors Publishing services by Elsevier B.V on behalf of Vietnam National University, Hanoi This is an open access article under the CC BY license

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The ultrasonic sonochemical method has received a great

attention for the fabrication of phosphors with unusual and

tailored properties Further, an ultrasound assisted synthesis route

has great commercial potential advantages with high production

rates, syntheticflexibility on choosing host materials as high

pu-rity nano powders, rapid reaction rate, narrow size distribution,

stable colloidal dispersion, uniform mixing, less synthesis time,

and less energy usage[8] In this method, the chemical reactions

arise from acoustic cavitations, i.e., formation, growth and

implosive collapse of bubbles in the liquid The growth of the

bubble happens through the diffusion of solute vapor into the

volume of the bubble, while the collapse of the bubble arises when

the bubble size reaches its maximum value When the solution was

exposed to ultrasound irradiation, the bubbles were implosively

collapsed by acousticfields in the solution[9] According to the hot

spot theory, very high temperatures (>5000 K) were achieved

upon the collapse of a bubble Since this collapse occurs in less

than a nanosecond, very high cooling rates (>1010 K/s) was also

obtained These extreme environments can drive several chemical

reactions and physical modifications occur as a result, allowing

shape and size of the phosphors to be effectively tuned[10] There

is a pressing need for synthesis of nano/micro structured materials

at reasonably low temperature for industrial applications

To the best of our knowledge, there have been no reports on an

ultrasound assisted sonochemical method for fabrication of

BaTiO3:Dy3þ (1e5 mol %) powders using Barbituric acid as a

sur-factant The prepared optimized samples were employed to

visu-alize LFTs and lip prints on various porous and non-porous surfaces

In addition, the structural and photoluminescent properties were

analyzed, and photometric properties were systematically studied

2 Experimental

Titanyl nitrate was prepared by taking N-butyl titanate in a petri

dish and a minimum quantity of doubled distilled water was added

to yield titanyl hydroxide Further, nitric acid was added to this

redox mixture which gave titanyl nitrate The corresponding chemical reactions can be given by[11]

TiðOC4H9Þ4þ 3H2O/TiOðOHÞ2þ 4C4H9OH (1)

Stoichiometric amount of barium nitrate and titanyl nitrate were dissolved in 100 ml deionized water and thoroughly mixed

in a magnetic stirrer to get uniform solution The stoichiometric amount of dysprosium nitrate (1e5 mol %) was added to the above resultant solution Further, different concentrations of barbituric acid (0.05e0.25% W/V) were added to the resultant mixture slowly Ultrasound irradiation was accomplished with a high-intensity ultrasonic probe (~2.5 cm diameter; Ti horn,

20 kHz, 150 W/cm2) immersed directly in the reaction solution Then, the solution mixture was stirred with high-intensity ul-trasound irradiation under ambient air (the ultrasonic frequency ~ 20 kHz, the power ~ 150 W) at afixed temperature of

75 C and by varying ultrasonic time (1e6 h) The solution was kept undisturbed until a white precipitate was formed The pre-cipitate wasfiltered and washed several times by using distilled water and ethanol to remove any unreacted material The ob-tained product was dried at 60 C for 3 h in a vacuum oven Finally, the dried precipitate was grinded thoroughly into the powder form and used for further studies

2.1 Characterization The obtained product was well characterized by using Shimadzu

7000 powder X-ray diffractometer using Cuka radiation Morphology of the product was studied by means of TM 3000, Hitachi table top Scanning electron microscopy and Hitachi H-8100 Transmission electron microscope The Perkin Elmer (Lambda-35) spectrometer was used to study the reflectance of the samples For

Fig 1 Fingerprints on the surface of glass stained by (a) TiO 2 powder (b) BaTiO 3 :Dy3þ2 mol % powder, (c) Fe 2 O 3 powder, and (d) BaTiO 3 :Dy3þpowder synthesized by mechanical

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PL measurements Jobin Yvon Spectroflourimeter Fluorolog-3

operational with 450 W Xenon lamp was used

2.2 Mechanism of visualization of LFPs and lips print using

BaTiO3:Dy3þhollow/solid microspheres

FPs collected from healthy volunteers with the age group of ~21

years were deposited on porous and non-porous surfaces namely

microscopic slides, aluminum foils, scratched CDs, leafs, coins,

magazines, pen, colored plastic bag etc Before deposition,fingers of

volunteers were thoroughly washed with water and dried in air

without touching any surfaces The optimized BaTiO3:Dy3þ(2 mol

%) powder was carefully sprinkled and gentle dusted uniformly on

LFPs using a special“Marabou” feather brush Further, an UV lamp

(4 W, 254 nm) was illuminated on the stained LFPs and then

pho-tographed using 50 mm f/2.8G ED lens Nikon D3100/AF-S digital

camera For visualization of latent lip prints, lips were cleaned

thoroughly using smooth tissue paper and then with sterile cotton The lips were lightly pressed against a glass slab for ~3e5 s The latent lips prints acquired on glass slab were visualized by spraying the optimized powder with a smooth brushing method and pho-tographed using a digital camera

3 Results and discussion

To determine effectiveness and selectivity of the prepared BaTiO3:Dy3þ(2 mol %) powder as afluorescence labeling agent for the visualization of LFPs on glass slide, conventionally used iron oxide (Fe2O3) and titanium dioxide (TiO2) powders were used as a control It was found that, LFPs developed by Fe2O3, TiO2 and BaTiO3:Dy3þpowders fabricated by mechanical stirring could not resolve fullfingerprint patterns (Fig 1(a, c& d)) However, LFP stained by BaTiO3:Dy3þ(2 mol %) hollow/solid microspheres under

254 nm UV light revealed well defined friction ridges (Fig 1b) It is

Fig 2 LFPs on (a) a green leaf, (b) a plastic sheet, (c) a plastic pen edge, (d) a steel pen edge, (e) a TV remote, (f) a mobile screen, (g) a coin, and (h) stainless steel visualized by BaTiO 3 :Dy3þ2 mol % powder under UV 254 nm.

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evident that the optimized BaTiO3:Dy3þpowder can be used as an

effective labeling agent for visualization of LFPs due to their

supe-rior white light emission Well defined fingerprint images with high

sensitivity were also visualized by BaTiO3:Dy3þ(2 mol %) hollow/

solid microspheres on non-porous materials including green leaf,

plastic sheet, plastic pen edge, steel pen edge, TV remote, mobile

screen, coin, and stainless steel (Fig 2)

In addition, aged (different time periods) LFPs were examined to

exhibit the suitability and robustness of the prepared powder in

advanced forensic detection.Fig 3(aec) shows the aged LFPs with

different time periods (1 day, 2 week, and 1 month) stained by the

optimized BaTiO3:Dy3þ powder Normally, sensitivity of labeling

powder progressively decreases as aging of the LFPs enhances, due

to evaporation of chemical constituents of the LFPs In the present work, even one month aged FP shows defined ridges, indicate the practicability of the prepared powder The LFPs on different textured marbles visualized by optimized BaTiO3:Dy3þ(2 mol %) powder under 254 nm illumination demonstrate the well-defined ridge patterns withfine contrast and without or less background hindrance (Fig 3 (def)) The differently magnified SEM images of LFP enhanced by prepared BaTiO3:Dy3þ(2 mol %) powder were shown inFig 4 The prepared powder particles provide uniform distribution and stronger adhesive ability via each static and sur-face absorption interactions and it increases the chemical stability,

Fig 3 LFPs aged on the non-porous glass surface for various time periods ((a) 1 day, (b) 2 weeks, and (c) 1 month) and (def) on different textured marbles visualized by

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permitting the long protection of light and affording affinity with

LFPs

The above obtained results demonstrated that, the optimized

BaTiO3:Dy3þ(2 mol %) powder was explored as an efficient

fluo-rescent labeling agent for visualization of LFPs on various porous

and non-porous surfaces The prepared optimized powder can

visualize LFPs as a whole, with high sensitivity, efficiency and low

background interference

Lip prints similar tofingerprints have many elevations and

de-pressions providing evidence in individual identification and

criminal investigation in a forensic dentistry The study of such lip

prints called as Cheiloscopy Usually, lip prints can be found where

the surface in contact with the lips[12] Most commonly in glasses,

cigarettes, straws, food items etc However, some extra effort has

been required to make lip prints visible Therefore, we explored

BaTiO3:Dy3þ(2 mol %) powder for visualization of lip prints on glass

under UV 254 nm Fig 5 shows the lip print stained by the

optimized BaTiO3:Dy3þ(2 mol %) powder From thefigure, it was clearly evident that the whole lip prints with Tsuchihashi's Type V, Type I, Type I0and Type III grooves (Fig 5(bee)) were visualized with high sensitivity and contrast due uniform smaller size and adhesive nature of the powder

In the ultrasound assisted sonication method, many experi-mental parameters namely sonication time, concentration of sur-factant, pH value and sonication power etc., may affect greatly the size and morphology of the products In the present study, the morphology of the prepared samples was extensively studied with different sonication times and concentrations of the surfactant.Fig 6

(aee) shows SEM images of BaTiO3:Dy3þ(2 mol %) with different sonication times (1e5 h) with a 0.25% W/V concentrated barbituric acid When the sonication time was ~1 h, several splintered parts having small lotusflower e like morphology was observed (Fig 6

(a)) The petals offlowers started blossoming, when the sonication time was increased to 3 h Further, increase of the sonication time

Fig 4 Differently magnified SEM images of fingerprints stained by BaTiO 3 :Dy3þ(2 mol %) powder ((b) is a magnified portion of (a)).

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(4 and 5 h), large number offlowers closed to form a uniform hallow

spherical shaped morphology was obtained (Fig 6(d& e)) The

obtained spherical morphology preserved even after 5 h sonication

irradiation Series of trials were conducted to ascertain the impact of

surfactant concentration on theflower morphology and are shown

inFig 6(fej) When the concentration of barbituric acid was 0.05%

W/V, a yolk-shell shaped structure consisting of many particles was

observed (Fig 6(f)) A hallow yolk-shell shaped micro structure

appeared, when the concentration of barbituric acid was increased

to 0.10% W/V (Fig 6(g)) However, with increase of concentration to 0.15% W/V, more hallow was observed and retained even further extended concentration (0.20% W/V) When the barbituric acid concentration was increased to 0.25% W/V, significantly condensed hallow space was observed (Fig 6(j))

Fig 7depicts TEM, HRTEM, SAED patterns, and EDAX images of the BaTiO:Dy3þ(2 mol %) powder The TEM image displays layer

Fig 6 SEM images of BaTiO 3 :Dy3þ(2 mol %) powder with (aee) different sonication times (1e5 h), a barbituric acid concentration of 0.25% W/V, and (fej) different concentrations

of the barbituric acid (0.5%e0.25% W/V) for a 5 h sonication.

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morphology and size ranged from 30 to 50 nm (Fig 7(a)) The lattice

spacing (d) was estimated from an HRTEM image (Fig 7(b)) and

found to be ~0.26 nm and the value was well matched with PXRD

values.Fig 7(c) shows the SAED pattern of the prepared sample and

it confirms the polycrystalline nature of the prepared powder

Further, elemental compositions such as atomic and molecular

weight were obtained from EDAX, which is shown inFig 7(d)

Fig 8(a) shows the PXRD profiles of BaTiO3:Dy3þ(1e5 mol %)

powder fabricated with a 6 h sonication time and barbituric acid

(0.25% W/V) The sharp and intense diffraction peaks were in good

agreement with the cubic phase with JCPDS no 31-0174 [13]

Further, it was observed that small impurity peak of dopant Dy2O3

ions was identified, indicating the successful substitution of Dy3þ

ions in the Ba2þsites The intensity of impurity peak increases with

increasing the concentration of dopant ions

The average crystallite size (D) was estimated using the

Scher-rer's formula[14]and listed inTable 1 It was evident from the table

that, the variation in crystalline size is dependent on dopant Dy3þ

concentration This was due to the increase in strain, leading to the

replacement of Ba2þions by smaller radius Dy3þions Generally,

broadening of the PXRD peaks was associated with crystallite sizes

or the strains present within the sample or both Therefore, the

WilliamsoneHall fitting method (Fig 8 (b)) [15]was utilized to

estimate the strain induced in the prepared samples and the

ob-tained results were given inTable 1

Fig 8(c) displays the diffuse reflectance spectra of the pure and

Dy3þdoped BaTiO3powders The spectra exhibited peaks at ~1071,

887, 796, 381, 364, 348 and 320 nm, which were due to the 4fe4f transition of the Dy3þions[16] The KubelkaeMunk (KeM) theory was utilized to estimate optical energy band gap of BaTiO3:Dy3þ (1e5 mol %) powders from the DRS spectra[17] The optical energy band gaps (Eg) values of the prepared powders were shown in

Fig 10(d) and inTable 1 The changes in Egwere mainly ascribed to degree of order and disorder in the matrix as well as variations in distribution of energy levels within the band gap[18]

The PL excitation spectrum of BaTiO3:Dy3þ (2 mol %) under

480 nm as emission was shown inFig 9(a) The spectrum exhibited peaks at ~350, 365, 387 and 435 nm, which were attributed to6H15/

2 / 6P7/2, 6H15/2 / 6P5/2, 6H15/2 / 4I13/2 and 6H15/2 / 4G11/2 respectively.Fig 9(b) shows the PL emission spectra of BaTiO3:Dy3þ (1e5 mol %) excited at 387 nm at RT The spectra exhibited distinct emission peaks at ~480, 574 and 637 nm, which were attributed to

4F9/2/6H15/2,4F9/2/6H13/2and4F9/2/6H11/2respectively[19] From thefigure, it was clear that peak at ~574 nm was more prom-inent as compared to other two peaks, which was due to a forced electric dipole transition The peak at ~480 nm was due to magnetic dipole transitions and is much less sensitive to the coordination environment The yellow emission peak at 574 nm (4F9/2/6H13/2) was stronger than the blue emission 480 (4F9/2/6H15/2), indicating that Dy3þwas located in a more non centro-symmetric position in

Fig 7 (a) TEM, (b) HRTEM images, (c) SAED pattern, and (d) EDAX spectra of BaTiO 3 :Dy3þ(2 mol %) powders prepared with a 5 h sonication time and 0.25% W/V barbituric acid.

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the BaTiO3host[20].Fig 9(c) shows the partial energy-level diagram

indicating the different excitation and emission mechanism of

BaTiO3:Dy3þpowder Asymmetry ratio (A21) was used to determine

the degree of distortion from the inversion symmetry of the local

environment of the Dy3þions in a host matrix[21]

A21¼

H

I2

4F9=2/6H13=2

dl H

I1

4F9=2/6H15=2

where I1and I2the intensities of a magnetic dipole transition at

480 nm and the electric dipole transition at 574 nm, respectively

The variation of A21 with varying Dy3þ concentration in

BaTiO3:Dy3þ(1e5 mol %) powder was shown inFig 10(a) and its

estimated values were listed inTable 3

The effect of doping concentration (Dy3þ) on PL emission

in-tensity in the BaTiO3host was shown inFig 10(a) It was clear from

the figure that, the PL intensity increased with an increase of

concentration of Dy3þup to 2 mol % and afterwards it diminished

The decrease in the PL intensity was due to the well-known

phe-nomenon called as a self-concentration quenching, resulting from

the resonance energy transfer between neighboring Dy3þions[22]

From energy match rule, cross-relaxation lines among Dy3þions

are responsible for population decrease of4F level as follows:

4F9=2þ6H15=2/6H9=2

6F11=2þ6F5=2 (4)

4F9=2þ6H15=2/6H7=2

4F9=2þ6H15=2/6F1=2

6H9=2

In the above process, the excitation energy was transferred from

a Dy3þion in a higher excited state to a neighboring Dy3þion and promotes the latter from the ground state to the metastable level The Dy3þions at4F9/2level undergo de-excitation through a cross relaxation process while Dy3þions in the ground state will allow the energies from Dy3þat6H15/2level simultaneously Finally, all the Dy3þ ions will go in their ground states and thus the lumi-nescence related to4F9/2level was quenched[23]

The non radiative energy transfer among Dy3þions leads to a concentration quenching effect By knowing the critical distance (Rc) between the neighboring Dy3þions, the type of the interaction mechanism can be explored[24] The calculated value of Rc was found to be ~4.47 Å and was almost equal to 5 Å, which leads to the multipoleemultipole interaction in the BaTiO3host and is the main cause for concentration quenching of Dy3þin the powder There were several types of electric multi-polar interactions, which may

be possible, namely, dipoleedipole (ded), dipoleequadrupole (deq), quadrupoleequadrupole (qeq), etc[25] Therefore, it was a

Fig 8 (a) PXRD patterns (b) WeH plots, (c) DR spectra and (d) optical band gap plot of pure and BaTiO 3 :Dy3þ(1e5 mol %) powders prepared with a 5 h sonication time and 0.25% W/V barbituric acid.

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necessity to know which type of interaction responsible in the

energy transfer between Dy3þions According to the Dexter and

Schulman theory[26], the ratio emission intensity (I) to

concen-tration of activator ion follows the equation;

I

where X; the activator concentration, Q; a constant of multi-polar

interaction and equals 6, 8, or 10 and less than 6 for dipoleedipole;

dipoleequadrupole or quadrupoleequadrupole interactions and

charge transfer mechanism respectively, and K andb; constants for

the given host lattice under the same excitation condition

LogI

whereðA ¼ log k  logbÞ.Fig 10(b) shows thefitted linear curve of log (I/X) vs log (X) in BaTiO3:Dy3þ(1e11 mol %) powder and the value of the slope to be ~1.205 The calculated value Q was found

to be 6.346 and was almost equal 6 This result indicates that, the charge transfer mechanism was due to the ded interaction for the concentration quenching in the present powder

The Commission International De I-Eclairage (CIE) chromaticity co-ordinates of the BaTiO3:Dy3þ (1e5 mol %) powders were calculated and listed inTable 2 It was noticed that, the CIE co-ordinates for the present powders were located well within the white region (Fig 10(c)) The Correlated Color Temperature (CCT) was estimated by Planckian locus and their values are listed in

Table 2 The quality of the white light in terms of CCT (Fig 10(d)) was also studied using the McCamy empirical theoretical relation

[27] And the color purity of the powder was estimated according

to the work[28]and their values are shown inTable 2 These re-sults clearly show that the present powder may be quite useful for solid state lighting applications

The JuddeOfelt (JeO) theory has been widely utilized to study the radiative transitions of rare-earth ions in several host materials

[29] Various radiative properties such as J-O intensity parameters (U2&U4), emission peak wavelengths (lpin nm), radiative tran-sition probability (AT), calculated radiative (trad) lifetime, branching ratio (bR) and asymmetric ratio (A21) were estimated by using the

PL emission spectra[30] The relation between radiative emission rates and the integrated emission intensities were estimated by using the equation reported elsewhere[31]

A02;4

A01 ¼I02;4

I01 ¼ hy01

Fig 9 (a) PL excitation spectra of BaTiO 3 :Dy3þ(2 mol %) powder atlemi ¼ 480 nm; (b) PL emission spectra of BaTiO 3 :Dy3þ(1e5 mol %) powder atlexc ¼ 387 nm; and (c) Energy levels diagram of Dy3þdoped BaTiO 3 powder.

Table 1

Estimated average crystallite size, strain and energy gap (E g ) values of BaTiO 3 :Dy3þ

(1e5 mol %) powders.

Dy3þconc.

(mol %)

Crystallite size

(nm) [DeS approach]

Crystallite size (nm) [WeH approach]

Strain (10 4 )

E g (eV)

Table 2

Photometric characteristics of doped BaTiO 3 :Dy3þ(1e11 mol %) powders.

BaTiO 3 :Dy3þconc.

(mol %)

1 0.33403 0.34009 0.20834 0.47728 5427 92.52

2 0.33459 0.34072 0.20848 0.47769 5403 90.48

3 0.33464 0.34082 0.20849 0.47773 5401 94.85

4 0.33468 0.34053 0.20863 0.47759 5399 89.78

5 0.3344 0.34016 0.20857 0.47737 5411 90.63

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where I0 eJand hn0 eJ; integrated emission intensity and energies

corresponding to transition4F9/2/6HJ(J¼ 15/2, 13/2 and 11/2)

respectively

The radiative emission rates A0 eJ(J ¼ 2, 4) related to forced

electric dipole transitions can be obtained and written as a function

of the J-O intensity parameters:

Að0JÞ¼ 64p4w3

J

3hð2J þ 1Þ

n

n2þ 22 9

X

l¼2;4

UlD

7F9=2UðlÞ6HJE2

(10)

where Að0JÞ; the coefficient of spontaneous emission, e; the

elec-tronic charge,wJ; the wave number of the corresponding

transi-tion, h; the Planck's constant, Smd; the strength of the magnetic

dipole and n; the RI of the prepared sample.D

4F9=2UðlÞ6HJE2

; squared reduced matrix element of Dy3þions and were 0.2457 and 0.4139 for J¼ 2 and 4 respectively and these values were inde-pendent of the chemical environment Thus, by using Eqs.(9) and (10), the values of U2 and U4 were calculated and listed in

Table 3 The JeO intensity parameters (U2andU4) for different host matrices have been observed[15]and are listed inTable 4 The total radiative transition probability (ATðjJÞ) can be calcu-lated and expressed as

ATðjJÞ ¼X

J 0

The radiative lifetime (tradðjJÞ) of an excited state in terms of

ATðjJÞ is given by

Fig 10 (a) Effect of concentration of Dy3þon the 574 nm emission and the variation of asymmetric ratio in BaTiO 3 powders, (b) Relation between log(x) and log (I/x), (c) CIE and (d) CCT diagram of BaTiO 3 :Dy3þ(1e5 mol %) powders.

Table 3

JuddeOfelt intensity parameters (U2 ,U4 ), Emission peak wavelengths (lp in nm), radiative transition probability (A T ), calculated radiative (trad ) lifetime, branching ratio (bR ) and asymmetric ratio (A 21 ) of BaTiO 3 :Dy3þ(1e5 mol %) powder (lex ¼ 387 nm).

BaTiO 3 :Dy3þconc.

(mol %)

JuddeOfelt intensity parameters (10 20 cm 2 )

Emission peak wavelengthlp in nm

A T (s1) trad (ms) bR A 21

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