Elsevier

Optik

Volume 251, February 2022, 168244
Optik

Efficient white light emission from a single silicate host with promising color quality for white light emitting diodes

https://doi.org/10.1016/j.ijleo.2021.168244Get rights and content

Abstract

Strontium silicate phosphors were synthesized via a solid-state route with different silicon sources as SiO2 and Si3N4. The phosphors synthesized with Si3N4 exhibited improved luminescence properties for white emission because of the coexistence of Sr3MgSi2O8 and Sr2SiO4 phases. Under UV excitation, white light was observed due to the combination of blue emission from Sr3MgSi2O8: Eu2+ and yellow emission from Sr2SiO4: Eu2+. The broad Eu2+ emission was explained on the basis of the dependency of crystal field strength on the site selection. The variation of Eu2+ ion concentration controlled the quality of the emitted light and at 5 mol% Eu2+, near white emission (0.30, 0.31) was obtained with external and internal quantum efficiencies of 50% and 68%, respectively. The WLEDs were fabricated by coating the present phosphors on an InGaN UV- LED chips and the EL spectrum displayed near white chromaticity (0.31, 0.33) with color rendering index of 80 and CCT of 6850 K. The results demonstrated the promising single host phosphors for near-UV white-light-emitting diodes.

Introduction

White-light emitting diodes (WLEDs) have received much attention in recent years since WLEDs with a long lifetime, energy-saving and environmentally benign properties can replace traditional incandescent and fluorescent lamps [1], [2], [3]. WLEDs are mostly fabricated from the combination of yellow-emitting YAG: Ce3+ phosphors and blue LED chips [4]. The commercial WLEDs with poor CRI (Ra=75) and high CCT (>8000 K) restrict the application in residential lighting [4]. Therefore, a new strategy has been developed by combining an InGaN LED, yellow-emitting phosphors with broad spectra, and red/ orange emitting phosphors to achieve warm white light with compatible CRI and CCT values [5].

The commercial approaches are complicated as different phosphors make the color balance difficult to control [6]. Hence, the research on the white light emission from a single phosphor has drawn more attention. The white-light emitting phosphors can be developed based on energy transfer between co-dopant pairs [7], [8], [9], [10] and Mn2+ ions are commonly used as co-activators. However, feeble Mn2+ d-d transitions may lead to the quenching paths and restrain the quantum yield (QY) and thermal stability [11]. Therefore, white-light emitting phosphors doped with a single activator ion are exceedingly favored for WLED applications to suppress the energy loss during energy transfer. Dai et al. [12] discussed a facile solid solution technique to develop a single activator doped phosphors with variable compositions to explore white-light. Various novel phosphors with promising luminescence, color tunability, and luminescence efficacy are developed with this strategy [13], [14], [15]. However, the design of the solid solution for the synthesis of the phosphors is complex. Hence, a new strategy is developed with alkali silicate materials for the synthesis of white light emitting phosphors in the present research work.

The alkali silicate materials draw significant attention owing to the promising thermal and chemical stability [16]. Several research works have been reported on alkali silicates doped with Eu2+ ions with tunable color emission including Li2SrSiO4 (580 nm), Ba9Sc2Si6O24 (500–520 nm), Ca3Si2O7 (600 nm) and Ba2MgSi2O7 (505 nm) [16], [17], [18], [19]. A thorough investigation of Eu2+ doped M3MgSi2O8 (M= Ca, Sr, Ba) system was discussed by Blasse et al. and the reported results indicated the suitability of the phosphors as a UV- pumped blue LEDs [20]. However, the investigation on the silicates phosphors doped with a single activator to emit white light is rare.

In the present research work, Eu2+ ion activated strontium silicate phosphors were synthesized to achieve white light with various silicon sources for the first time. The broad white light emission from a single host was revealed to the co-existence of variable phases and corresponding crystal field strength. The WLEDs were fabricated by encapsulating the phosphors with InGaN UV- LED chips. The obtained results demonstrated a promising approach for developing novel white-light emitting phosphors with high CRI and suitable CCT values.

Section snippets

Experimental

In the present work, Eu2+ doped strontium magnesium silicate (SMS) phosphors with nominal composition of xSrO·yMgO·zSiO2 (x = 2, 3; y = 0, 1; and z = 1, 2) were synthesized via the solid-state reaction route using different silicon sources. A certain amount of Eu2O3 was added into the phosphors to get a series of SMS materials with different silicon sources as shown in Table 1. Different raw materials of SrCO3, MgO, and Eu2O3 were used in the stoichiometric ratio. SiO2 and Si3N4 were used as

Results and discussions

The XRD pattern of SMS- 0 phosphors is shown in Fig. 1(a). All XRD diffraction peaks of the synthesized phosphors matched well with the standard pattern of Sr2MgSi2O7 (ICDD No. 75–1736). The absence of impurity phases indicated the solubility of Eu2+ ions in the host lattice sites. The doping of Eu2+ showed no significant effects on the structure of the host material since the radius of Eu2+ (0.118 nm) is similar to Sr2+ (0.117 nm). The structure of Sr2MgSi2O7 belongs to the tetragonal crystal

Conclusions

Eu2+ ions doped strontium silicate phosphors were successfully synthesized via a solid-state route with two kinds of silicon sources including SiO2 and Si3N4. The phosphors synthesized with Si3N4 exhibited improved luminescence properties for white emission. The XRD patterns of the samples synthesized with SiO2 showed the presence of Sr2MgSi2O7 phase; whereas the samples synthesized with Si3N4 had both phases of Sr3MgSi2O8 and Sr2SiO4. The broad excitation spectra (300–400 nm) of both phosphors

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgment

This work was financially supported by the “Advanced Research Center For Green Materials Science and Technology” from The Featured Area Research Center Program within the framework of the Higher Education Sprout Project by the Ministry of Education (110L9006) and the Ministry of Science and Technology in Taiwan (MOST 110-21634-F-002-043 and MOST 107–2218-E-002-022).

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